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VIETNAM NATIONAL UNIVERSITY – HOCHIMINH CITY INTERNATIONAL UNIVERSITY STUDY ON DRUG DELIVERY FOR PACLITAXEL OF THE LACTOBACILLUS STRAINS A Thesis submitted to the School of Biotechnology, International University in partial fulfillment of the requirements for the degree of Master of Science in Biotechnology Student name: Doan Thi Thanh Vinh – MBT04015 Supervisor: Dr. Nguyen Hoang Khue Tu July 2013 Study on Drug Delivery for Paclitaxel of the Lactobacillus Strains By DOAN THI THANH VINH ABSTRACT The practice of developing molecularly targeted drugs to achieve a higher degree of cancer therapy and antibiotic resistance is indispensable. Lactobacillus strains participated in the anti-cancer effects and performed the high-level specificity for cancer cell lines. This paper discussed the ability of minicells which were generated from Lactobacillus acidophilus VTCC-B-871 and Lactobacillus rhamnosus JCM 15113 for drug delivery of paclitaxel. L. acidophilus VTCC-B-871 and L. rhamnosus JCM 15113 formed minicells with highly significant number (1,070,000 and 787,000 minicells, respectively) in modified MRS broth with the concentration of fructose 10 g/l and lactose 50 g/l, respectively. Nanoparticle size of obtained minicells ( 400 nm in diameter) was determined using scanning electron microscopy. The minicells packaged paclitaxel (10 µg/ml) and cephalosporin (10 µg/ml) for different times of incubation (10, 15 and 24 hours) at 37°C. Our results showed that drugs could be completely absorbed for 10 hours by detecting extracted solution from drug packaged minicells on antimicrobial activities. The significant influence of different concentrations of loading paclitaxel (5, 10, 20 µg/ml) on drug packaging was studied. The results indicated that after extraction of the paclitaxel packaged minicells and analysis with high performance liquid chromatography for determining the number of paclitaxel presented in a minicell, there was a huge amount of paclitaxel encapsulated in a minicell (31 million paclitaxel molecules per minicell with loading paclitaxel (20 µg/ml)). The present work was the first report on the generation of minicells from Lactobacillus acidophilus VTCC-B-871 and Lactobacillus rhamnosus JCM 15113 and the drug delivery for paclitaxel of these minicells. Key works: Lactobacillus acidophilus, Lactobacillus rhamnosus, minicells, paclitaxel, cephalosporin, antimicrobial chromatography. i activities, high performance liquid ACKNOWLEDGEMENTS First of all, it is undeniable that this thesis has taken me a great deal of time and effort. Moreover, I have to insist that this thesis cannot be well-completed without the encouragements, the nice ideas and helps from a lot of people. For these reason, I would like to thank to many people that contributed one way or another to the realization of this paper. Remarkably, I would like to express my most sincere gratitude and appreciation to Dr. Nguyen Hoang Khue Tu for all her enthusiastic supervision, patience and encouragement of this work. Her critical comments, constructive suggestions, professional directions also guided effectively my logical ideation and efficient communication skills throughout the whole research period. Furthermore, I would love to send my best wishes to all members of the School of Biotechnology of International University for their tremendous enthusiasms as well as for their nice behavior towards me, and also for give me the good chance to conduct and have my research study completed. Definitely, it is certain that I really send my thanks to Dr. Ha Dieu Ly and all the members at Department of Reference Substances, Institute of Drug Quality Controls and also all members at Scanning Electron Microscopy Laboratory Room, Vietnam Academy of Science and Technology for their assistance and technical support. Words cannot express my respect, profound gratitude for my parents who are always on me, encourage, and share their great love for me. I love to send my sincere thanks to my good friends who are being with me during my bad and good time. Last but not least, I greatly thank you who spend precious time to read this document. This actually has profound significance for me as the fruit of my labor is also gotten your acceptance. ii TABLE OF CONTENTS ABSTRACT ........................................................................................... i ACKNOWLEDGEMENTS ..........................................................................ii LIST OF FIGURES ................................................................................ v LIST OF TABLES .................................................................................. vi ACRONYMS AND ABBREVIATIONS ........................................................ vii CHAPTER 1 INTRODUCTION ............................................................. 1 CHAPTER 2 LITERATURE REVIEW ..................................................... 3 2.1 Cancer and tumor-targeted drug delivery systemsError! Bookmark not defined. 2.1.1 Worldwide cancer burden ............................................................. 3 2.1.2 Cancer treatment and recent advances in cancer therapy ................ 4 2.1.3 Obstacles in cancer therapy and targeted drug delivery systems ...... 5 2.1.4 Approaches to improve the therapeutic index of anti-cancer drugs .... 8 2.2 Bacterially-derived minicells .................................................... 10 2.2.1 Minicells ...................................................................................10 2.2.2 Bacterially-derived mincells as controlled drug delivery for cancer therapy .............................................................................................11 2.2.4 Current research of minicells in delivering anti-cancer drugs ...........12 2.3 An overview of Lactobacillus species ....................................... 14 2.3.1 The Genus Lactobacillus .............................................................14 2.3.2 Lactobacillus acidophilus .............................................................15 2.3.3 Lactobacillus rhamnosus .............................................................15 2.4 Paclitaxel ................................................................................. 16 2.5 Orientation of implementing to delivery paclitaxel using minicells derived from the lactobacillus strains .............................. 17 2.6 Process of project .................................................................... 18 CHAPTER 3 MATERIAL AND METHODS ............................................ 19 3.1 Materials .................................................................................. 19 3.1.1 Bacterial strains.........................................................................19 3.1.2 Tools and equipments ................................................................19 3.1.3 Media and chemicals ..................................................................19 3.2 Research methodology ............................................................. 21 3.2.2 Design condition for minicells production from Lactobacillus strains..21 3.2.2 Minicell isolation ........................................................................21 3.2.3 Microscopic studies for characterization of minicell morphology .......21 3.2.4 Packaging of drug into minicells ...................................................22 3.2.5 Drug extraction for measurement ................................................23 iii 3.2.6 Antimicrobial activity tests ..........................................................23 3.2.7 Paclitaxel assay using HPLC-UV/Vis Spectroscopy ..........................23 3.2.8 Calculation of the number of drug molecules .................................24 3.2.9 Data analysis ............................................................................25 CHAPTER 4 RESULTS AND DISCUSSION ......................................... 26 4.1 Screening the carbon sources for study on minicell generation from Lactobacillus strains .............................................................. 26 4.1.1 Minicells generation in Lactobacillus acidophilus VTCC-B-871 ..........30 4.1.2 Minicells generation from Lactobacillus rhamnosus JCM 15113 ........34 4.2 Microscopic studies: characterization of minicell morphology .. 37 4.3 Package of drug into minicells generated from Lactobacillus strains ............................................................................................ 39 4.3.1 Antimicrobial activity tests ..........................................................39 4.3.1.1 Drug packaging of minicells produced from L. acidophilus 39 4.3.1.2 Drug packaging of minicells produced from L. rhamnosus ..........41 4.3.2 Paclitaxel quantitation using HPLC-UV/Vis Spectroscopy .................43 4.3.2.1 The minicell drug packaging in response to incubation times ......44 4.3.2.2 The minicell drug packaging in response to concentrations .........45 CHAPTER 5 CONCLUSION AND RECOMMENDATION ........................ 49 REFERENCES ................................................................................... 50 iv LIST OF FIGURES Figure 2.1 Nanoparticle platforms for drug delivery. ..................................... 8 Figure 2.2 Schematic showing minicell formation and bispecific antibodytargeted, drug/siRNA-packaged minicells ..................................11 Figure 2.3 Chemical structure of paclitaxel . ...............................................16 Figure 3.1 Process of isolation of bacterially-derived minicells from the parent cells culture ...........................................................................21 Figure 4.1 The API 50CHL biochemical testing of Lactobacillus acidophilus......26 Figure 4.2 The API 50CHL biochemical testing of Lactobacillus rhamnosus. .....28 Figure 4.3 The number of minicells (×104) produced from L. acidophilus ........32 Figure 4.4 Photomicrographs of Lactobacillus acidophilus VTCC-B-871 and its minicells (100X)l. ....................................................................33 Figure 4.5 The number of minicells (×104) produced from L. rhamnosus ........35 Figure 4.6 Photomicrographs of Lactobacillus rhamnosus JCM 15113 and its minicells (100X). .....................................................................36 Figure 4.7 Photomicrograph showing the morphology of minicells from Lactobacillus acidophilus VTCC-B-871 under the light microscope after isolation procedure (100 X) ...............................................37 Figure 4.8 Representative SEM images showing the formation of minicells. ....38 Figure 4.9 Representative SEM images of minicells from L. acidophilus VTCC-B871with minicell size after isolation procedure ............................39 Figure 4.10 Drug quantitation in minicells when minicells incubated in the presence of different drug loading concentrations. .......................46 v LIST OF TABLES Table 2.1 Estimated (2008) and projected numbers (millions) of cancer cases and deaths, all cancers, both sexes, by development status or WHO region ............................................................................. 3 Table 2.2 The summary statistics of estimated incidences, mortality in men, women, and both sexes in Vietnam in 2008. ................................... 4 Table 2.3 Advantages of using nanoparticles as a drug delivery system ........... 9 Table 3.1 Lactobacilli MRS broth ...............................................................20 Table 4.1 The API 50CHL biochemical testing of Lactobacillus acidophilus .......27 Table 4.2 The API 50CHL biochemical testing of Lactobacillus rhamnosus .......29 Table 4.3 The number of minicells produced from L. acidophilus VTCC-B-871 in modified MRS medium .................................................................32 Table 4.4 The number of minicells produced from L. rhamnosus JCM 15113 in modified MRS medium .................................................................35 Table 4.5 Antimicrobial spectrum of extracted drugs from drug-packaged minicells of L. acidophilus VTCC-B-871 and L. rhamnosus JCM 15113 against Gram-positive and Gram-negative bacteria .........................41 Table 4.6 Antibacterial activity of extracted paclitaxel and cephalosporin from drug-packaged minicells of L. acidophilus against bacterial species ...41 Table 4.7 Antibacterial activity of extracted paclitaxel and cephalosporin from drug-packaged minicells of L. rhamnosus against bacterial species ....42 Table 4.8 HPLC analysis of paclitaxel in the loading solution in response to varying times of incubation ..........................................................44 Table 4.9 HPLC analysis of paclitaxel in minicells when incubated in the presence of different drug concentrations.......................................46 Table 4.10 Paclitaxel quantification in minicells when incubated in the presence of different drug concentrations ....................................................47 vi ACRONYMS AND ABBREVIATIONS ATCC American Type Culture Collection BsAbs Bispecific Antibodies BSG Buffer Saline Gelatin CSCs Cancer Stem Cells DDSs Drug Delivery Systems EGFR Epidermal Growth Factor Receptor EPS Exoploysaccharide FDA Food And Drug Administration GRAS Generally Recognized As Safe HPLC High Performance Liquid Chromatography IARC International Agency For Research On Cancer IFP Interstitial Fluid Pressure JCM Japanese Collection Microorganism LAB Lactic Acid Bacteria NCI National Cancer Institute PBS Phosphate Buffer Saline SEM Scanning Electron Microscope shRNA Short Hairpin RNA siRNA Small interfering RNA VTCC Vietnamese Type Culture Collection vii CHAPTER 1 INTRODUCTION Cancer is the general name for a group of more than 100 diseases which is being one of the major health problems on over the world. Despite the availability of several treatment modalities, mortality rates due to cancer are high. Therefore, effective cancer therapy continues to be a daunting challenge due mainly to considerable tumor cell heterogeneity, drug resistance of cancer cells, doselimiting toxicity of chemotherapeutics, and difficulties of targeted delivery to tumors (MacDiarmid et al., 2011). A key obstacle in the use of current chemotherapeutic anticancer drugs is their lack of specificity for cancer cells, resulting in severe toxicity when they are administered systemically (Flemming, 2007). Consequently over the past decade a significant global effort has focused on the discovery and development of molecularly targeted drug delivery systems (DDSs) (MacDiarmid et al., 2007a). DDSs are being developed to achieve a higher degree of tumor cell specificity and reduce toxic side effects, as well as overcome several challenges to the treatment of cancer (Chidambaram et al., 2011), including drug resistance and metastatic disease (Alexis et al., 2010). However, current strategies that use nanoparticles (Brannon et al., 2004), liposomes (Zheng et al., 2001); or polymer therapeutics (Duncan, 2003) are hampered by shortcomings such as drug leakage in vivo, lack of versatility in terms of packaging a diverse range of different drugs, thereby reducing drug potency, and difficulties in production scale-up (Ferrari et al., 2005), particularly for nanoparticles. Recently, a new promising technology for targeted and intracellular delivery of chemotherapeutic drugs relies on using bacterially derived nano-sized particles (termed as minicells). Minicells are originated from the normal cell deleting the min gene (de Boer et al., 1989), but they can package a range of different chemotherapeutic drugs and specifically targeting the minicells to tumor cell surface receptors via bispecific antibodies coating the minicells (Flemming, 2007). This technique has been experimented successfully for both Grampositive (Listeria monocytogenes) and Gram-negative bacteria (Salmonella typhimurium, Escherichia coli, Shigella flexneri, and Pseudomonas aeruginosa); drug-packaged nano-sized particles effected apoptosis of tumor cells both in vitro and in vivo; and they also targeted to cancer cells in vivo with high specificity and, thus, delivered in high concentration in vivo without toxicity 1 (MacDiarmid et al., 2007a). Although minicells currently generated from both Gram-positive and Gram-negative bacteria and also tested for encapsulating chemotherapeutic drugs and functioning as nanovectors for drug delivery in cancer therapy (MacDiarmid et al., 2007b). This mutation may effect on the growth of bacteria under their control so far (de Boer et al., 1989). Moreover, up to now, there has not any research on generating bacterially-minicells from Lactobacillus strains using other method without min gene deletion. Especially, Lactobacillus strains are GRAS (Generally Recognized as Safe) microorganisms used as the probiotics that are very important in foods, pharmaceuticals, and animal husband (Macfarlane and Cummings, 2002). The benefits of probiotics were found protection against gastrointestinal pathogens, enhancement of the immune system, reduction of lactose intolerance, reduction of serum cholesterol level and blood pressure, anti-carcinogenic activity, improved utilization of nutrients and improved nutritional value of food. Members of the genus Lactobacillus have also been reported on the significant anti-oxidative, anticarcinogenic, and anti-bacterial activity, as well as the inhibitory effects on cancer cell growth besides being effect on human immune system (Choi et al., 2006; Kim et al., 2002). Among the tested Lactobacillus species, Lactobacillus acidophilus (Choi et al., 2006) and Lactobacillus rhamnosus (Cenci et al., 2002) strains participated in the anti-cancer effects, anti-carcinogenic ability and performed the high-level specificity for cancer cell lines. From those points, this paper presented the generation of bacterially derived minicells from Lactobacillus strains for drug delivery and investigated if minicells derived from these strains were able to package with chemotherapeutic drug (Paclitaxel); in order to detectable a robust and versatile system for in vitro drug delivery using minicell, a bacterially-derived lactic acid bacteria carrier. Moreover, this study also confirmed the ability of encapsulation of minicells with other drug as cephalosporin. This study was the primary research on the drug delivery system which was able to carry many drugs and necessary products for food and pharmaceutical fields. Therefore, the main aim of this study was to develop a new drug nano-sized carrier derived from probiotic Lactobacillus for delivery of chemotherapeutic drug with fewer side effects, and with further modification, to produce a systemic complex of molecular targeted drug delivery including probiotics properties. From this aim, those specific objectives including, performing drug-packaged bacterially-derived minicells and determining the number of drug molecules presented in minicell. 2 CHAPTER 2 LITERATURE REVIEW 2.1 CANCER AND TUMOR-TARGETED DRUG DELIVERY SYSTEMS 2.1.1 Worldwide cancer burden Cancer is a group of diseases characterized by the uncontrolled growth of abnormal cells that disrupt body tissue, metabolism, etc. and tend to spread locally and to distant parts of the body. Life-threatening cancer develops gradually as a result of a complex mix of factors such as complex interactions of viruses, a person‟s genetic make-up, their immune response and their exposure to other risk factors which may favor the cancer (Win, 2006). Based on the GLOBOCAN 2008 estimates (Ferlay et al., 2010a), the standard set of worldwide estimates of cancer incidence and mortality produced by the International Agency for Research on Cancer (IARC) for 2008, there were an estimated 12.4 million cases of cancer diagnosed and 7.6 million deaths from cancer and 28 million persons alive with cancer around the world in 2008 (Table 2.1); of these, 56% of the cases and 64% of the deaths occurred in the less developed regions of the world, many of which lack the medical resources and health systems to support the disease burden. By 2030, it could be expected that there could be 27 million incident cases of cancer, 17 million cancer deaths annually and 75 million persons alive with cancer within five years of diagnosis (Table 2.1). Table 2.1 Estimated (2008) and projected numbers (millions) of cancer cases and deaths, all cancers, both sexes, by development status or WHO region (Boyle and Levin, 2008) 20301 2008 20302 Region Cases Deaths Cases Deaths Cases Deaths World 12.4 7. 6 20.0 12.9 26.4 17.0 Africa (AFRO) 0.7 0.5 1.2 0.9 1.6 1.3 Europe (ERO) 3.4 1.8 4.1 2.6 5.5 3.4 East Mediterranean (EMRO) 0.5 0.3 0.9 0.6 1.2 0.9 Pan-America (PAHO) 2.6 1.3 4.8 2.3 6.4 3.1 South-East Asia (SEARO) 1.6 1.1 2.8 1.9 3.7 2.6 Western Pacific (WPRO) 3.7 2.6 6.1 4.4 8.1 5.9 ¹ no change in current rates ² with 1% annual increase in rates 3 Overall in 2008, based on the most recently available international data (GLOBOCAN 2008 estimates) produced by IARC, about 111,600 incident cases of cancer and 82,000 cancer deaths were estimated to have occurred in Vietnam (Table 2.2). The most commonly diagnosed cancers were liver (23,251 cases, 20.8% of the total new cancer cases), lung (20,659 cases, 18.5%) and stomach (15,068 cases, 9.7%) (Figure 2.1). Liver cancer is also the leading cause of cancer death for both sexes, accounting for 21,748 deaths, comprising 26.5% of the total cancer deaths (Ferlay et al., 2010a). Table 2.2 The summary statistics of estimated incidences, mortality in men, women, and both sexes in Vietnam in 2008; Source : GLOBOCAN 2008 (Ferlay et al., 2010a). Vietnam Male Female Both sexes Population (thousands) 42973 44122 87095 Number of new cancer cases (thousands) 55.0 56.5 111.6 15.9 12.8 14.1 43.7 38.3 82.0 12.7 8.8 10.5 Risk of getting cancer before age 75 (%) Number of cancer deaths (thousands) Risk of dying from cancer before age 75 (%) 5 most frequent cancers (ranking defined by total number of cases) Liver Liver Liver Lung Lung Lung Stomach Breast Stomach Incidence and mortality data for all ages Proportions per 100,000 2.1.2 Cancer treatment and recent advances in cancer therapy Although great effort has been made in cancer research, no substantial progress can be observed in the past fifty years in the USA or almost twenty years in Vietnam in fighting against cancer. The death rate in the USA was 193.9 per 100,000 in 1950 and remained as high as 194.0 per 100,000 in 2001 (Jemal et al., 2004). Based on the data from the Hanoi cancer registry, IARC estimated that in 1990 the mortality in Vietnam was about 82.2 per 100,000 (Pham and Nguyen, 2002) and actually stayed lower than that 94.1 per 100,000 in 2008 (Ferlay et al., 2010a). It is clear that the progress in cancer treatment has been slow and inefficient (Win, 2006). It is a multidisciplinary challenge needing more and closer collaboration between clinicians, medical and biomedical scientists and biomedical engineers to eventually find a satisfactory solution (Win, 2006). 4 The choice of treatment depends on the type and location of the cancer, whether the disease has spread, the patient's age and general health, and other factors. Clinical treatment for cancer therapy is a multidisciplinary therapy consisting of surgery, radiation therapy, chemotherapy, biological therapy and other methods (e.g., biological therapy, targeted therapy, or gene therapy for cancer (ACS, 2013). Chemotherapy is most effective against cancers that divide rapidly and have a good blood supply (Win, 2006). Aims of chemotherapy treatments are to cure; to maintain long term remission (free of disease); to increase the effectiveness of surgery or radiotherapy; to help control pain or other symptoms. However, research still continues in finding ways to make chemotherapy less toxic and also to minimize the side effects. Molecularly targeted therapy – a new generation of cancer treatments has emerged as one approach to overcome the lack of tumor specificity of conventional cancer therapies (Gerber, 2008). Currently, the pharmaceutical industry has been successful in discovering many new cytotoxic drugs that can potentially be used for the treatment of cancer, this life-threatening disease still causes over 7 million deaths every year worldwide and the number is growing (Ferlay et al., 2010a). Thus, the ongoing obligation to the design and discovery of new cancer therapy is urgent. 2.1.3 Obstacles in cancer therapy and tumor-targeted drug delivery systems There are several serious obstacles in cancer therapy including drug resistance, high tumor interstitial fluid pressure (IFP), and cancer stem cells (CSCs). 2.1.3.1 Obstacles in cancer therapy A vast array of resistance mechanisms, involving overexpression of drug transporters (which are the plasma membrane P-glycoprotein (P-gp) product of the multidrug resistance (MDR) gene as well as other associated proteins) (Gottesman, 2002), mutations or amplification of the target enzyme, decreased drug activation, increased drug degradation due to altered expression of drug metabolizing enzymes, diminished drug-target interaction, enhanced DNA repair, or failure to apoptosis, can defeat single agents, no matter how well designed and targeted (Chorawala et al., 2012). High tumor interstitial fluid pressure (IFP) is another barrier for efficient drug delivery (Heldin et al., 2004). Increased IFP contributes to a decreased transcapillary transport in tumors leads to a decreased uptake of drugs or 5 therapeutic antibodies. Cancer cells are therefore exposed to a lower effective concentration of therapeutic agent than normal cells, lowering the therapeutic efficiency and increasing toxicity. It is now well established that the IFP of most solid tumors is increased. This increase makes the uptake of therapeutic agents less efficient in solid tumors (Wu et al., 2006). There are a number of factors that contribute to increase IFP in the tumour, such as vessel leakiness, lymph vessel abnormalities, fibrosis and contraction of the interstitial matrix. The discovery of cancer stem cells (CSCs) in solid tumors has changed our view of carcinogenesis and chemotherapy. Cancer stem cells are defined as those cells within a tumour that can self-renew and drive tumorigenesis (Dean et al., 2005). The CSCs, which are also accurately called „tumor-initiating cells‟, represent a small population of cancer cells, sharing common properties with normal stem cells (SCs), that can initiate new tumors following injection into animal models, while the majority of other cancer cells cannot (Vinogradov and Wei, 2012). Natural properties of the small group of cancer stem cells involved in drug resistance to standard chemotherapy agents, metastasis and relapse of cancers can significantly affect tumor (Dean et al., 2005). In addition to the obstacles in cancer therapy, current chemotherapeutic drugs are constrained by severe systemic toxicity due to indiscriminate drug distribution and narrow therapeutic indices. A key obstacle in the use of chemotherapeutic anticancer drugs is their lack of specificity for cancer cells, resulting in severe toxicity when they are administered systemically (Sarosy and Reed, 1993). This is exacerbated by the fact that systemically delivered cancer chemotherapy drugs often must be delivered at very high dosages to overcome poor bioavailability of the drugs and the large volume of distribution within a patient. In general, cancer chemotherapy is usually accompanied by severe side effects and acquired drug resistance. Therefore, we anxiously await the development of molecularly targeted therapy that will allow greater tumor specificity and less toxicity. Over these years, cancer targeting treatment has been greatly improved by new tools and approaches based on the development of nanotechnology. Nanotechnology is the creation and utilization of materials, devices, and systems through the control of matter on the nanometer scale (Jain, 2005). Nanocarrier systems can be designed to interact with target cells and tissues or respond to stimuli in well-controlled ways to induce desired 6 physiological responses. They represent new directions for more effective diagnosis and therapy of cancer (Alexis et al., 2010). 2.1.3.2 Tumor-targeted drug delivery nanoparticles In recent years, the rapid advent of nanotechnology has stimulated the development of many novel drug delivery strategies (Wang et al., 2007). Nanoparticles applied as nanoscale drug delivery vehicles have shown the ability to encapsulate a variety of therapeutic agents such as small molecules (hydrophilic and/or hydrophobic), peptides, protein-based drugs, and nucleic acids, and protect them against enzymatic and hydrolytic degradation (Mohanraj and Chen, 2006). By encapsulating these molecules inside a nanocarrier, the known shortcomings of many anticancer drugs can be potentially overcome, such as low aqueous solubility, stability, high nonspecific toxicity or lack of selectivity of anticancer drugs (Chidambaram et al., 2011), while at the same time increasing the circulation time and bioavailability of encapsulated drugs (Langer, 1998). Through encapsulation of drugs in a macromolecular carrier, such as a liposome, the volume of distribution is significantly reduced and the concentration of drug in a tumor is increased. This causes a decrease in the amounts and types of nonspecific toxicities, and an increase in the amounts of drug that can be effectively delivery to a tumor (Moghimi, 2006). The surface of the nanocarrier can be engineered to increase the blood circulation half-life and influence the biodistribution, while attachment of targeting ligands to the surface can result in enhanced uptake by target tissues (Gref et al., 1994; Moghimi et al., 2001). The small size allows nanocarriers to overcome biological barriers and achieve cellular uptake (Brigger et al., 2002). The net result of these properties is to lower the systemic toxicity of the therapeutic agent while increasing the concentration of the agent in the area of interest, resulting in a higher therapeutic index for the therapeutic agent (Gilstrap et al., 2011) against the most difficult cancer challenges (Chidambaram et al., 2011), including drug resistance and metastatic disease (Alexis et al., 2010). 7 Polymeric Nanoparticle Dendrimer Liposome Polymeric Micelle Inorganic Nanoparticle Polymerosome Protein Carrier Biological Nanoparticle Polymer-drug Conjugate Hybrid Nanoparticle Hydrophobic Polymer Therapeutic load Hydrophilic Polymer Targeting Ligand Lipid Figure 2.1 Nanoparticle platforms for drug delivery. Nanoparticle platforms are characterized by their physicochemical structures, including polymer-drug conjugates, lipid-based nanoparticles, polymeric nanoparticles, protein-based nanoparticles, biological nanoparticles, and hybrid nanoparticles (Alexis et al., 2010). Nanoparticles applied as drug delivery systems are submicronsized particles (10 to 1000 nm) (Shim and Turos, 2007), devices, or systems that can be made using a variety of materials including polymers (polymeric nanoparticles, micelles, or dendrimers), lipids (liposomes), magnetic, even inorganic/metallic compounds (iron, silica) and bacteria (bacterial nanoparticles or “minicells”) (MacDiarmid and Brahmbhatt, 2011; MacDiarmid et al., 2007b, 2009) (Figure 2.2). 2.1.4 Principle approaches to improve the therapeutic index of anticancer drugs Nanoparticle drug delivery systems are being studied to overcome limitation of conventional therapeutic areas particularly in cancer chemotherapy. As mentioned in subheading 2.1.3.2, nanomedicine performed a strong potential to accelerate the development of effective approaches to the treatment of drug8 resistant and recurrent cancers. However, despite the significant progress made in the development of drug delivery system (DDS) and other nanoplatformbased approaches, serious limitations have also been identified in applications of these therapies in vivo (Vinogradov and Wei, 2012). Several important limitations of nanoparticles are highlighted (mostly liposomes (Table 2.4)), such as ineffective uptake and distribution in tumor tissue, retention in bypassing organs and by macrophages of the reticuloendothelial system after systemic administration, and limited oral availability (Yun et al., 2012). Other nanovector systems such as synthetic biodegradable nanoparticles, polymer micelles, and several others, are also hampered by drug leakage in vivo, lack of versatility in terms packaging a diverse range of different drugs, thereby reducing drug potency, and difficulties in production scale-up (Ferrari, 2005). Despite the enhanced efficacy demonstrated by many targeted nanoparticles, they also face three major limitations: immunogenicity or non-specificity of the targeting ligand leading to accelerated blood clearance; further impaired tumor penetration compared to the nontargeted nanoparticles; and receptor-mediated endocytosis and subsequent lysosomal digestion resulting in a major dose loss by the lysosomal digestion (Chen et al., 2012). Table 2.3 Advantages and disadvantages of liposome (Anwekar et al., 2011) Advantages of liposome Disadvantages of liposome 1. Liposomes increased efficacy and therapeutic Low solubility index of drug (actinomycin-D) 2. Liposome increased stability via Short half-life encapsulation 3. Liposomes are non-toxic, flexible, Sometimes phospholipid biocompatible, completely biodegradable, undergoes oxidation and and non-immunogenic for systemic and non- hydrolysis-like reaction systemic administrations 4. Liposomes reduce the toxicity of the Leakage and fusion of encapsulated agent (amphotericin B, Taxol) 5. Liposomes help reduce the exposure of encapsulated drug/molecules Production cost is high sensitive tissues to toxic drugs 6. Site avoidance effect Fewer stables 7. Flexibility to couple with site-specific ligands to achieve active targeting 9 Because problems continue to hamper significantly the success of cancer therapeutics, an urgent need exists for new targeted drug delivery strategies that will either selectively deliver drugs to tumor cells and target organs, protect normal tissues from administered antineoplastic agents, or prevent existing problems in cancer therapies. The present invention relates to ongoing efforts to achieve a targeted drug delivery by means of intact bacterial minicells, which are able to delivery drugs intracellular, within desired target cells in vivo and in vitro (MacDiarmid et al., 2007a, 2007b, 2009). Minicells containing chemical or biochemical drugs constitute novel delivery vehicles, capable of being targeted to specific cells. Because of the benefits of delivering chemotherapeutics drugs for cancer treatment, the practice of synthesizing and packagage of cytotoxic drug into minicells is the key point of this study. The present study builds on these recent discoveries relating to minicells, and addresses the continuing needs for improved drug delivery strategies, especially in the context of cancer chemotherapy. 2.2 BACTERIALLY-DERIVED MINICELLS 2.2.1 Minicells Minicells were first observed and described by Howard Adler and colleagues in 1967, who also coined the term “minicell” with the first description of a mutation that led to the minicell phenotype in Escherichia coli (Adler et al., 1967), and to more accurately describe the particle, people propose the new term “nanocell‟ instead of “minicell” since the scale size of the vector is nanometer and is not in the mini- or micro-range (MacDiarmid et al., 2007a). They are anucleate, nonliving nano-sized cells (100 – 400 nm in diameter) and are produced as a result of mutations in genes that control normal bacterial cell division (de Boer et al., 1989; Lutkenhaus, 2007; Ma et al., 2004) there-by depressing polar sties of cell fission (Figure 2.3). The resultant minicells do not contain any of the original DNA and the chromosome present in its larger sister, but may contain all of the molecular components of the parent cell. The minicells are capable of protein synthesis and normal metabolic functions but are incapable of undergoing further rounds of cell division. Minicell formation has since been described in a number of other Gram-positive and Gram-negative species. First discovered over 70 years ago, minicells are becoming of interest to researchers in their potential as anti-tumor agents. 10 Figure 2.22 Schematic showing minicell formation and bispecific antibodytargeted, drug/siRNA-packaged minicells. Minicells can be loaded with siRNAs (purple), shRNA (green) or chemotherapeutics (black). Loaded minicells are then functionalized via bispecific antibody conjugates, with one arm specific for minicell-surface O-polysaccharide (red) and the other specific for the tumor cell-surface receptor (blue) (Karagiannis and Anderson, 2009). 2.2.2 Bacterially-derived mincells as controlled drug delivery for cancer therapy Minicells are small, semi-spherical, bacterial nano-size particles that contain all of the components of the parental bacteria, except chromosomes. Without chromosomes, they cannot divide and are non-infectious, making them highly suitable for development as in vivo delivery products. So far, clever attempts at delivering potent drugs straight to the cancer cells using techniques such as conjugating them to antibodies specific to those cells, have been inconclusive at best. The use of molecularly targeted minicell nanovectors affords multiple potential advantages over conventional cancer therapy (MacDiarmid et al., 2007a). Firstly, minicells possess the ability to easily package therapeutically significant concentrations of different cytotoxic or molecularly targeted drugs into the minicell, ability to encapsulate both hydrophilic and hydrophobic drugs. Secondly, minicells have the ability to readily attach different bispecific antibodies (BsAbs) on the minicell surface in order to target a receptor found on the surface of a tumor cell. Thirdly, minicells are able to deliver the drug intracellularly within a tumor cell and without leakage of drug/siRNA/shRNA from the vector during systemic circulation. In addition, minicells also provide a dramatic increase in the therapeutic index with minimal to no toxic side effects. This also enables the use of potent cytotoxics that have failed toxicity trails but have the potential to be highly potent anti-cancer drugs. Moreover, minicells are 11 easily purified to homogeneity and the long standing pharmaceutical industry experience in bacterial fermentation and production of bacterial vaccines shows that such processes are relatively cheap. The minicells nanovector has the potential to significantly reduce cost of goods particularly since a minicell-based anti-cancer therapeutic would carry tiny fractions of the drug and the targeting antibody compared to free drug or free antibody therapy. Finally, obstacles in anticancer therapy such as multi-drug resistance of tumor can also be overcome via receptor-mediated endocytosis which triggered by the adhesion of the minicells to tumor-surface receptors, or via sequential minicell-mediated delivery of siRNA followed by drugs (MacDiarmid et al., 2009). 2.2.4 Current research situation of minicells in delivering anti-cancer drugs Minicell has been observed and described in the studies on the bacteria cell division from long time ago. However, it is actually noticeable in recent years as Himanshu Brahmbhatt, Jennifer MacDiarmid and colleagues firstly showed that report promising results using bacterial minicells as the drug delivery system in 2007 (MacDiarmid et al., 2007a). The unusual drug delivery vehicle was generated by inactivating genes that control normal cell division in bacteria. This led to the formation of anucleate particles that have a uniform diameter of 400 nm, and high yields are readily produced from Gram-positive (Listeria monocytogenes (L. monocytogenes)) and Gram-negative bacteria (Salmonella enterica serovar Typhimurium (S. typhimurium), Escherichia coli (E. coli), Shigella flexneri (S. flesneri), and Pseudomonas aeruginosa (P. aeruginosa)). These minicells were loaded with a range of therapeutically significant concentrations of chemotherapeutics (such as doxorubicin, paclitaxel, irinotecan, 5-flourouracil, cisplatin, carboplatin, and vinblastine) with differing charge, hydrophobicity and solubility by simple co-incubation in few hours. Minicell has also been demonstrated that a minicell can be efficiently loaded with si/shRNA (MacDiarmid et al., 2009). The ability of minicells encapsulated a large number of drug molecules (1- 10 million per minicell), and they loaded with doublestranded siRNA to an estimated density of nearly 12,000 molecules per minicell. These minicells selectively targeted to cancer cells via BsAbs. Cancer-cell targeting was achieved by coupling minicells to bispecific antibodies, in which one arm recognizes surface lipopolysaccharide (LPS), and the other a surface receptor on the targeted cell. 12 In vivo experiments with targeted doxorubicin-loaded minicells led to the dramatic inhibition and regression of tumour growth in mice that had human breast, ovarian, leukaemia or lung cancer xenografts. Furthermore, the drug was undetectable in the plasma of minicell-treated animals, and none of the animals developed any signs of toxicity. The anticancer efficacy of the minicells was further evaluated in dogs with advanced T-cell non Hodgkin‟s lymphoma; treatment led to marked tumour regression and tumour lysis. Importantly, the treatment was tolerated without adverse side effects despite repeat dosing, and there was no increase in pro-inflammatory cytokines. Further experiments in pigs confirmed no adverse reactions in terms of haematological indices, serum chemistries, food intake or growth, and surprisingly anti-LPS titers remained at background levels. The team tested this using a form of siRNA designed to prevent the production of a protein that causes multi-drug resistance in cancer cells. Recently, an early phase clinical trial using the platform of minicell nanoparticle for drug delivery has been tested for the first time on patients with advanced cancer and found to be safe, well-tolerated and even induced stable disease in patients with advanced, incurable cancers with no treatment options remaining. This clinical trial phase I was implemented by Associate Professor Benjamin Solomon at the Peter MaCallum Cancer Centre in Melbourne, Australia with colleagues. In a Phase I trial, minicells were loaded with with a cytotoxic chemotherapy drug called paclitaxel and coated with cetuximab, antibodies that target the epidermal growth factor receptor (EGFR) which is often overexpressed in a number of cancers, as a „homing‟ device to the tumor cells. The treatment, code-named EGFRminicellsPac, was well tolerated, and of the 28 people treated, 10 had stable disease at 6 weeks, and one patient safely received 45 doses over 15 months (ECCO, 2012) . This important study shows for the first time that these bacterially-derived minicells can be given safely to patients with cancer. It thereby allows further clinical exploration of a completely new paradigm of targeted drug delivery using this platform coupled with different concentration of cell-killing drugs or other treatments such as RNA interference, and with different targeting antibodies. After all, the minicell technology is actually a platform for the targeted delivery of many different molecules, including drugs and molecules for silencing rogue genes which cause drug resistance in late stage cancer. The technology can also be viewed as a powerful antibody drug conjugate where up to a million 13 molecules of drug can be attached to targeting antibodies and delivered to the body in a safe way. In the future this will enable a truly personalized medicine approach to cancer treatment, since the minicell payload can be adjusted depending on the genetic profile of the patient. Approaches resulting in selective delivery of anti-cancer drugs to tumour cells are highly interesting as it may lead to a reduction in adverse side-effects and improved anti-tumour activity. In this respect, the use of minicells is a novel and promising technique (ECCO, 2012). 2.3 AN OVERVIEW OF Lactobacillus SPECIES 2.3.1 The Genus Lactobacillus 2.3.1.1 General description of the genus Taxonomically, the genus Lactobacillus belongs to the phylum Firmicutes, class Bacilli, order II Lactobacillales, and family Lactobacillaceae and its closest relatives, being grouped within the same family, are the genera Paralactobacillus and Pediococcus (Felis et al., 2009). This genus includes a high number of GRAS species (Generally Recognized as Safe). Species of genus Lactobacillus are some of the most important taxa involved in food microbiology and human nutrition: several Lactobacillus species are remarkably essential in fermented food production and are used as starter cultures or food preservatives. Moreover, certain strains of human origins are being exploited as probiotics or vaccine carriers (Goh and Klaenhammer, 2009). The lactobacilli strains can be used as potential candidates for cancer prevention (Choi et al., 2006; Liu and Pan, 2010). A few particular strains of L. acidophilus, L. casei, L. paracasei, L. johnsonii, L. reuterui, L. salivarius and L. rhamnosus have been extensively studied as candidates of probiotics and their functional properties and safety have been well-documented. 2.3.1.2 The important role of Lactobacillus species in human life Many Lactobacillus species are associated with food production, because of preservative action due to acidification, and/or enhancement of flavour, texture and nutrition (Jay, 1996; Stiles, 1996). Members of the genus Lactobacillus are commonly present as members of probiotics (termed as living microorganisms that are associated with the beneficial effects for humans and animals). Lactobacilli strains have been used to study the anti-oxidative activity, antibacterial and anti-cancer discovery besides being effect on human immune system. This genus evaluated the inhibitory effects of on various human cancer 14 cell lines and attempted to demonstrate whether such effects were cancer cell selective (Choi et al., 2006). The inhibition of cancer cell growth by Lactobacillus has also been reported in other studies (Kim et al., 2002). Antioxidant activities and antiproliferative activities against breast and colon cancer cell lines in vitro gave a strong evidence of possessing significant anti-cancer activities of several local lactobacilli strains (Liu and Pan, 2010). Short chain fatty acids produced by L. acidophilus, L. rhamnosus are reported to inhibit the generation of carcinogenic products by reducing enzyme activities (Cenci et al., 2002). These results suggest that Lactobacillus can be used as adjuncts in fermentation of food and are potential candidates for cancer prevention. 2.3.2 Lactobacillus acidophilus Among many Lactobacillus species, L. acidophilus is likely the most common probiotics for dietary use (Parvez, 2006). In addition to its gram positive rod shape with rounded ends, the typical size of L. acidophilus is 1.5 - 6.0 µm in length. L. acidophilus is an obligately homofermentative LAB that growth in anaerobic condition. Because they utilize sugars (e.g. glucose, aesculin, cellobiose, galactose, lactose, maltose, salicin, and sucrose) as their substrates for fermentation, they inhabit environments with high sugar abundance, such as the GI tract in humans and animals (Vijayakumar et al., 2008). Health benefits of L. acidophilus include providing immune support for infections or cancer, providing a healthy replacement of good bacteria in the intestinal tract following antibiotic therapy, reducing occurrence of diarrhea in humans, aiding in lowering cholesterol and improving the symptoms of lactose intolerance. Moreover, some of L. acidophilus cell components have potential use in many different areas of biotechnology such as vaccine development (Jafarei and Ebrahimi, 2011). It is demonstrated that exoploysaccharide (EPS) from bacteria specially Lactobacillus sp. may contribute to human health, either as nondigestible food fraction or because of their immunomodulating or cholesterol lowering activity anti-tumoral, anti-ulcer, (Ganesh, 2006; Vuyst and Degeest, 1999). EPS has anti-carcinogenic ability mediated by the stimulation of the mitogenic activity of B lymphocytes (Ruas-Madiedo et al., 2006; Xu et al., 2010). 2.3.3 Lactobacillus rhamnosus Lactobacillus rhamnosus GG is a clinically documented bacterial strain which is used in many countries as a probiotic culture in different dairy products or in 15 pharmaceutical diet supplements (Korpela et al. 1997). L. rhamnosus GG is a rod shaped, Gram-positive, with 2.0-4.0 µm in length, and often with square ends, and occur singly or in chains. This bacterium is considered safe (GRAS) microorganism. L. rhamnosus GG is a homofermentative LAB (Berry et al. 1997). Lactobacillus rhamnosus has shown antimicrobial activity against Escherichia coli, Enterobacter aerogenes, Salmonella typhi, Shigella sp., Proteus vulgaris, Pseudomonas aeruginosa, Serratia marcescens, Staphylococcus aureus, Bacillus subtilis, Bacillus megaterium, Bacillus cereus, Helicobacter pylori, Campylobacter jejuni, and Listeria monocytogenes (Ambalam et al., 2009). L. rhamnosus are reported to inhibit the generation of carcinogenic products by reducing enzyme activities (Cenci et al., 2002). 2.4 PACLITAXEL Among the available drugs for chemotherapy, paclitaxel (Taxol®) is one of the best anti-cancer drugs and also reported to possess radio-sensitizer properties. Paclitaxel is a white to off-white crystalline powder with empirical formula of C47H51NO14 and a molecular weight of 853.91. It is highly lipophilic, insoluble in water, and melts at around 216-217°C. It is a complex, oxygen-rich diterpenoid (Rowinsky and Donehower, 1995; Rowinsky et al., 1992) and its chemical structure has been elucidated by chemists as in Figure 2.5. It consists of some benzene rings and other hydrophobic structures, which lead to its high water insolubility of paclitaxel. Figure 2.43 Chemical structure of paclitaxel 16 The major limitation of paclitaxel is also the obstacle of chemotherapy, drug resistance in the mucosa of the small and large intestine which limits the oral uptake of paclitaxel and mediates direct excretion of the drug in the intestinal lumen (Adams et al., 1993). Paclitaxel has been recognized as the most potent anticancer agent for the past few decades. However, its use as an anti-cancer drug is compromised by its intrinsically poor water solubility. The effective chemotherapy using paclitaxel is relying on the development of new delivery systems which attracted a substantial number of studies investigated to deliver paclitaxel by new formulations. 2.5 ORIENTATION OF IMPLEMENTING TO DELIVERY PACLITAXEL USING MINICELLS DERIVED FROM THE LACTOBACILLUS STRAINS It is clear that bacterially-derived minicells proved successfully their ability to encapsulate a range of different chemotherapeutic drugs, target to the specific tumor cells, and inhibit the growth of tumour in animal and human in the first clinical trial. Thanks to their proven benefits and the minicells applications as nanovectors for drug delivery in cancer therapy, it is necessary to develop new molecularly targeted drug delivery systems from bacteria. Currently, although minicells generated from both Gram-positive and Gram-negative bacteria and also tested for encapsulating chemotherapeutic drugs and functioning as nanovectors for drug delivery in cancer therapy, the minicells were prepared from genetically defined minCED(-) chromosomal deletion bacteria and then the subsequent minicells were purified (MacDiarmid et al., 2007b). This deletion of minCED(-) out of the bacteria cell may affect on their growth under their control so far (de Boer et al., 1989). Up to now, there has not any study on generating bacterially-minicells from Lactobacillus strains, or not any research on the drug delivery of this genus, one kind of largest genus within the group of lactic acid bacteria (LAB) with their properties as probiotics. According to the principle of bacteria cell division, the normal generation of two equally sized daughter cells are maintained by the regulatory protein system (Min system) which encoded by the min locus (consists of three genes, minC, minD, minE that encode three proteins, designated MinC, MinD, and MinE, respectively in E. coli). Abnormalities this regulatory system for cytokinesis results in the aberrant division near a cell pole, leading to the formation of small spherical minicells and short filaments. Recently, there were studies on detection the overexpression and characterization of minC homolog from Lactobacillus acidophilus (Nguyen et al., 2012), minD from L. acidophilus and L. rhamnosus 17 (Nguyen et al., 2013a, 2013b). These studies showed the role and function of min genes from Lactobacillus strains in cell division and minicell formation. The results of these studies also reported an interesting overexpression of E.coli carrying min genes of Lactobacillus strains showed the phenomenon of cell differentiation under different sugar stresses. From above stated points, this paper presented the investigation about the generation minicells from the rod Lactobacillus strains under different sugar stresses. Then, minicells were used for drug delivery by packaging drugs. 2.6 PROCESS OF PROJECT Screening the carbon source for culturing minicell – generating Lactobacillus strains Minicell production from Lactobacillus strains Minicells isolation Packaging of paclitaxel into minicells Drugs extraction Antimicrobial activity tests of extracted drugs Confirmation the packaging ability with cephalosporin Drug (paclitaxel) quantification and data analysis 18 CHAPTER 3 MATERIAL AND METHODS 3.1 MATERIALS 3.1.1 Bacterial strains Lactobacillus acidophilus VTCC-B-871 obtained from stock cultures maintained by the Vietnamese Type Culture Collection (Hanoi, Vietnam) Lactobacillus rhamnosus JCM 15113 was kindly provided by the Japanese Collection Microorganism (Japan). Indicator microorganisms for antimicrobial activity tests were supported from American Type Culture Collection (Manassas, USA), including: Staphylococcus aureus (S. aureus) ATCC 25923, Escherichia coli (E. coli) ATCC 9637, Salmonella typhimurium (S. typhi) ATCC 19430, Pseudomonas aeruginosa (P. aeruginosa) ATCC 27853, and Candida albicans (C. albicans) ATCC 14053. 3.1.2 Tools and equipments  Light Microscope  Filter vacuum system  Scanning Electron Microscope (SEM) JSM-7401F (Jeol, USA)  The High Performance Liquid Chromatography (HPLC) system (Shimadzu, Japan)  Neubauer hemocytometer  Syringe filters, sterilized filter membranes (pore size of 0.2 µm and 0.45 µm) (Whatman, England) 3.1.3 Media and chemicals 3.1.3.1 Chemicals  Chemotherapeutic drug – Paclitaxel T7402 (microcrystalline powder, >99.5% purity) (Sigma Aldrich, USA)  D-Glucose (Merck, Germany)  D-Fructose (Merck, Germany)  Lactose (Merck, Germany)  Maltose (Merck, Germany)  Saccharose (Merck, Germany)  Antibiotic – Cephalosporin C3270 (Sigma Aldrich, USA) 19  Gram staining kit (Sigma Aldrich, USA) 3.1.3.2 Carbohydrate fermentation testing kit  API 50 CHL Medium (BioMérieux, USA) 3.1.3.3 Buffer preparation Phosphate buffer saline (PBS, pH 7.4) and buffer saline gelatin (BSG, pH 7.0) can be referred from Appendix A. 3.1.3.4 Drug preparation Paclitaxel stock solution was prepared by dissolving completely in ethanol absolute to give a 1 mg/ml stock solution, then diluted 1:10 (vol/vol) in PBS buffer to give 100 µg/ml stock solution. Cephalosporin was dissolved totally in distilled water to perform a 1 mg/ml stock solution, and then diluted 1:10 (vol/vol) in distilled water to give 100 µg/ml stock solution. 3.1.3.5 Culture media Basic culture for bacteria growth Both strains of Lactobacillus were grown in Lactobacilli MRS broth (De Man et al., 1960). Table 3.1 Lactobacilli MRS broth (De Man et al., 1960) Ingredients Formula per Liter Peptone 10.0 g Meat extract 10.0 g Yeast extract 5.0 g 20.0 g Tri-ammonium citrate 2.0 g Sodium acetate 5.0 g Dipotassium hydrogen phosphate (K2HPO4) 2.0 g Manganese sulfateTetrahydrate (MnSO4. 4H2O) 0.05 g Magnesium sulfate Heptahydrate (MgSO4. 7H2O) 0.2 g Tween 80 1.0 ml D-Glucose Modified culture for study The modified MRS media were prepared by modifying carbon source in MRS ingredients (detail in sub-section 3.2.2). 20 3.2 RESEARCH METHODOLOGY 3.2.1 Design condition for minicells production from Lactobacillus strains In order to study the influence of various carbon sources on the minicell formation, this study implemented experiments on different kinds of sugar with different concentration in the culture medium. Lactobacillus acidophilus VTCC-B871 and Lactobacillus rhamnosus JCM 15113 were inoculated into modified Lactobacilli MRS broth which containing each of carbon sources separately: glucose, lactose, sucrose, maltose, fructose, in different concentration (0 g/l, 5 g/l, 10 g/l, 15 g/l, 20 g/l, 30 g/l, 40 g/l, 50 g/l) and incubated at 37ºC for 48 hr in order to produce minicells. 3.2.2 Minicell isolation (Brahmbhatt and MacDiarmid, 2004) Minicell-producing bacteria were subjected of the minicell isolation for free of contaminating parent bacterial cells, cellular debris. Overnight culture of minicell producing bacterial cells Differential centrifugation at 2000 rpm for 20 min First filtration through 0.45 µm filter Filtration through 0.45 µm filter Minicells collected Second filtration through 0.45 µm filter Filtration through 0.2 µm filter Figure 31 Process of isolation of bacterially-derived minicells from the parent cells culture. 3.2.3 Microscopic studies for characterization of minicell morphology 3.2.3.1 Light microscopy Isolated minicells were observed for scanning the microscopic minicell morphologies and cell counting using a Neubauer hemocytometer under a light microscopy with a total magnification of 100 X. Minicells were counted in five small squares (the four 1/25 sq. mm corners plus the middle square) in the central area into focus at low power. The numbers of obtained minicells per unit volume of a suspension was calculated as following equation (3.1). 21 (eq. 3.1) 3.2.3.2 Scanning electron microscopy Morphology of the isolated minicells were observed by scanning electron microscopy (SEM, Jeol JSM-7401F) at 10-15kV. Samples were examined at Scanning Electron Microscopy Laboratory Room, Vietnam Academy of Science and Technology, 1 Mac Dinh Chi Street, 1 District, Ho Chi Minh City to investigate morphological minicells. 3.2.4 Packaging of drug into minicells 3.2.4.1 Packaging of the cancer chemotherapeutic drug (Paclitaxel) into minicells (MacDiarmid et al., 2007b) To determine if minicells can be packaged with chemotherapeutic drug (Paclitaxel) and the kinetics of minicell drug packaging in response to varying concentrations of drug in the loading solution or varying times of incubation, the following methods were adopted. Preparations of purified minicells derived from LAB strains were separately incubated in a solution of the paclitaxel drug, at different final paclitaxel concentrations in minicell extracellular environment of 5, 10 and 20 µg/ml. The mixtures were incubated at 37°C with rotation. Minicells had been centrifuged at 13000 rpm for 15 min before were washed thoroughly with ten exchanges of buffered saline gelatin (BSG) solution. Drug was then extracted from packaged minicells to prepare for drug qualification and quantitation using HPLC-UV/Vis Spectroscopy system (detailed in sub-section 3.2.8). For minicells depending upon the times of incubation in the loading solution, minicells were seperately incubated with paclitaxel (10 µg/ml) for the time was shown 10, 15 and 24 hours with rotation. The minicell suspensions incubated with paclitaxel were then centrifuged at 13000 rpm for 15 min. The supernatants were used to analyze for the paclitaxel remaining using HPLC-UV/Vis Spectroscopy system (detailed in sub-section 3.2.8). Drug was extracted from packaged minicells to prepare for testing antimicrobial acitivity (in sub-section 3.2.7.). 22 3.2.4.2 Packaging of antibiotic (cephalosporin) into minicells To assist in determining the ability of the drug-packaged minicell, this study conducted on an experiment to test the encapsulation of antibiotic drug Cephalosporin into minicells. Minicells were seperately incubated with cephalosporin (10 µg/ml) at 10, 15 and 24 hours with rotation. The minicell suspensions incubated with cephalosporin was then centrifuged at 13000 rpm for 15 min. Drug was extracted from packaged minicells to prepare for testing antimicrobial acitivity (detailed in sub-section 3.2.7.). 3.2.5 Drug extraction for measurement (MacDiarmid et al., 2007b) The minicells which incubated with drugs (paclitaxel, celphalosporin) were harvested by centrifugation at 13000 rpm for 15 min and re-suspended in sterile BSG and washed 10 times with BSG. The minicells were collected and prepared for drug extraction. The minicells were centrifuged at 13000 rpm for 15 min, and supernatant was discarded. The phosphate-buffered saline (PBS) was added to re-suspend pellet, followed by five cycles of 1 minute vortexing and 1 minute sonicating. The samples were diluted with an equal volume of ultrapure water and the five cycles were repeated. The extracts were finally centrifuged for 5 min at 13000 rpm to pellet debris, thus yielding cell-free filtrates. 3.2.6 Antimicrobial activity tests Antimicrobial effects were tested on Staphylococcus aureus (S. aureus) ATCC 25923, Escherichia coli (E. coli) ATCC 9637, Salmonella typhimurium (S. typhi) ATCC 19430, aeruginosa (P. Candida albicans (C. albicans) ATCC 14053, Pseudomonas aeruginosa) ATCC 27853 by the agar diffusion method. The tested microorganisms were propagated twice and then grown for 18 to 24 hr in 10 ml of appropriate growth media. Sterile paper discs (5 mm of diameter) were then prepared and dropped on using 20 μl of cell-free filtrate. The extracted solution from minicell suspension without drugs incubation was used as the control. The inoculated plates were incubated for 18 to 24 hr at appropriate temperatures, and the diameter of the inhibition zone was measured in millimeters with calipers. 3.2.7 Paclitaxel assay using HPLC-UV/Vis Spectroscopy Extracted paclitaxel from packaged minicells (incubated in different final concentrations of 5, 10 and 20 µg/ml of paclitaxel) and supernatants from 23 paclitaxel-incubated minicell suspensions (shown at different time of incubation 10, 15 and 24 hr) were quantified and qualified by HPLC-UV/Vis Spectroscopy analyses. Samples were practiced at Department of Reference Substances, Institute of Drug Quality Controls, 200 Co Bac, Co Giang ward, 1 District, Ho Chi Minh City, Vietnam. According to the linear standard equation, the concentrations of paclitaxel in the minicells and in supernatants were measured (see Appendix K). . In order to identify the presence of paclitaxel, the variation between paclitaxel peaks of samples and standard were calculated as following equation (eq. 3.2). (eq. 3.2) Where, V (%) is the variation Rp is the retention time of sample paclitaxel Rst is the retention time of standard. The acceptable range for the variation of retention time was less than 5%. 3.2.8 Calculation of the number of drug molecules (MacDiarmid et al., 2007b) The number of molecules of drug (paclitaxel) packaged per minicell is calculated as follows. Where, MW is a molecular weight of paclitaxel Avogadro number of molecules is 6.02 x 1023 The number of paclitaxel molecules present in the loading solution (NPL) is expressed as: ( (eq. 3.3) ) Where, NPL is the number of paclitaxel molecules present in the external medium IPW is the initial amount of paclitxel loaded The number of Paclitaxel molecules present in the total minicells (NPT) is defined as: ( (eq. 3.4) ) 24 Where, NPT is the number of Paclitaxel molecules present in the total minicells EPW is the amount of Paclitaxel encapsulated in the minicells (determined by HPLC analysis) Therefore, the number of molecules of drug per minicell (NPM) can be calculated as follows: (eq. 3.5) Where, NPM is the number of paclitaxel molecules per minicells Encapsulation efficiency (EE %) is defined as: (eq. 3.6) 3.2.9 Data analysis Results are expressed as means ± standard deviations of triple replicates for all treatments. Data was analyzed using one-way ANOVA followed by post-hoc Tukey‟s test for paired comparisons of means, with p < 0.05 being considered statistically significant (SPSS 16, SPSS Inc., Chicago, USA). Data had also been tested for homogeneity of variances using Levene statistic (with p > 0.05, the Levene's test showed homogeneity of variance). 25 CHAPTER 4 RESULTS AND DISCUSSION 4.1 Screening the carbon sources for study on minicell generation from Lactobacillus strains In order to decide which sugars would be related to the investigation of the effect of carbon sources on the minicell formation, Lactobacillus acidophilus and Lactobacillus rhamnosus were used to test the carbohydrate fermentation using API 50CHL kit (BioMerieux). During fermentation of carbohydrates, the acid generated and decreased the pH by the change in color of the indicator; the positive tests corresponded to acidification revealed by the indicator contained in the medium changing to yellow. Figure 4.1, 4.2 and Table 4.1, 4.2: sugar (glucose, fructose, maltose, lactose, saccharose) fermentations showed the yellow change. It meant that those sugars had high impact on L. acidophilus, and L. rhamnosus. In order to define the effect of sugars as carbon sources on cell differentiation of L. acidophilus and L. rhamnosus, the research on screening the carbon sources for minicell generation from Lactobacillus strains was implemented. Figure 4.1 The API 50CHL biochemical testing of Lactobacillus acidophilus VTCC-B-871; Positive tests corresponded to acidification revealed by the purple indicator contained in the medium changing to yellow. 26 Table 4.1 The API 50CHL biochemical testing Lactobacillus acidophilus VTCC-B-871 Strip No. Substrate Isolate 0 Control negative 1 Glycerol negative 2 Erythritol negative 3 D-Arabinose negative 4 L- Arabinose negative 5 Ribose negative 6 D-Xylose negative 7 L-Xylose negative 8 Adonitol negative 9 Β Methyl-D-Xyloside negative 10 Galactose positive 11 Glucose positive 12 Fructose positive 13 Mannose positive 14 Sorbose negative 15 Rhamnose negative 16 Dulcitol negative 17 Inositol negative 18 Mannitol negative 19 Sorbitol negative 20 α-Methyl-D-Mannoside negative 21 α-Methyl-D-Glucoside negative 22 N-Acetyl-Glucosamine positive 23 Amygdalin positive 24 Arbutin positive 25 Esculin negative 26 Salicin positive 27 Cellobiose positive 28 Maltose positive 29 Lactose positive 30 Melibiose negative 31 Sucrose positive 27 of 32 Trehalose positive 33 Inulin negative 34 Melezitose negative 35 Raffinose negative 36 Starch negative 37 Glycogen negative 38 Xylitol negative 39 Gentiobiose positive 40 D-Turanose negative 41 D-Lyxose negative 42 D-Tagatose negative 43 D-Fucose negative 44 L-Fucose negative 45 D-Arabitol negative 46 L- Arabitol negative 47 Gluconate negative 48 2-Keto-Gluconate negative 49 5-Keto-Gluconate negative Figure 4.2 The API 50CHL biochemical testing of Lactobacillus rhamnosus JCM 15113; Positive tests corresponded to acidification revealed by the purple indicator contained in the medium 28 changing to yellow; For the Esculin test (tube no. 25), a change in color from purple to black is observed. Table 4.2 The API 50CHL biochemical Lactobacillus rhamnosus JCM 15113 testing Strip No. Substrate Isolate 0 Control negative 1 Glycerol negative 2 Erythritol negative 3 D-Arabinose negative 4 L- Arabinose negative 5 Ribose positive 6 D-Xylose negative 7 L-Xylose negative 8 Adonitol negative 9 Β Methyl-D-Xyloside negative 10 Galactose positive 11 Glucose positive 12 Fructose positive 13 Mannose positive 14 Sorbose positive 15 Rhamnose positive 16 Dulcitol negative 17 Inositol negative 18 Mannitol positive 19 Sorbitol positive 20 α-Methyl-D-Mannoside negative 21 α-Methyl-D-Glucoside negative 22 N-Acetyl-Glucosamine positive 23 Amygdalin positive 24 Arbutin positive 25 Esculin positive 26 Salicin positive 27 Cellobiose positive 28 Maltose positive 29 Lactose positive 30 Melibiose negative 31 Sucrose positive 29 of Strip No. Substrate Isolate 32 Trehalose positive 33 Inulin negative 34 Melezitose positive 35 Raffinose negative 36 Starch negative 37 Glycogen negative 38 Xylitol negative 39 Gentiobiose positive 40 D-Turanose negative 41 D-Lyxose positive 42 D-Tagatose positive 43 D-Fucose negative 44 L-Fucose negative 45 D-Arabitol negative 46 L- Arabitol negative 47 Gluconate positive 48 2-Keto-Gluconate negative 49 5-Keto-Gluconate negative 4.1.1 Minicells generation in Lactobacillus acidophilus VTCC-B-871 Lactobacillus acidophilus VTCC-B-871was cultured in selected sugars, as glucose, lactose, sucrose, maltose, fructose, with different concentrations (0 g/l, 5 g/l, 10 g/l, 15 g/l, 20 g/l, 30 g/l, 40 g/l, 50 g/l). The minicells from each culture were filtered through 0.45 µm. The minicells were collected and calculated. The results were summarized in Table 4.3 and Figure 4.3. The results of statistical analysis also identified that carbon sources influenced significantly on the minicell formation and the minicells were generated depending on the sugar concentrations (p < 0.05). It was clear from Table 4.3 that minicell generation was not changed when L. acidophilus was grown in the modified MRS media without containing sugar. The number of minicells obtained was always about 60,000 particles. This was the lowest level of producing minicells. The data presented that at all levels of factor treatment with sugars (from 5 g/l to 50 g/l), fructose was the carbon source by means of which the maximum number of minicells was obtained. It was followed by the quantity of minicells which were generated in the maltose medium. Lactose and glucose had similar levels of 30 production of minicells, such as between 270,000 to 780,000 particles each. Through the usage of saccharose, the minimum number of minicells was obtained. Since the fructose concentration changed in the culture medium from 5 g/l to 50 g/l, the number of obtained minicells in the medium containing fructose fluctuated between 378,000 particles and 1,070,000 particles. These numbers were two and a half times as much as the number of obtained minicells in the medium containing saccharose (fluctuated between 128,000 and 417,000 particles) at the same range of sugar concentration. As presented in Table 4.3, the number of obtained minicells was increased considerably when L. acidophilus was grown in the modified MRS media containing concentrations from 5 g/l to 10 g/l for all tested sugars. At level of factor treatment of 10 g/l, the generated minicells were the highest number at each of kind of sugar. In modified MRS medium with glucose, lactose, fructose, maltose, saccharose (10 g/l) the minicells obtained were about 662,000; 783,000; 1,070,000; 885,000, and 417,000 particles, respectively. The minicells obtained were decreased at high concentrations of sugars. These numbers were reduced (2.5 times) to 273,000; 310,000; 378,000, 352,000, and 128,000 particles when the concentration of glucose, lactose, fructose, maltose, saccharose increased (10 times) to 50 g/l, respectively (Table 4.3). At the concentration of 20 g/l for each of sugars (including glucose in the standard MRS medium), the number of minicells was only a half of minicells producing in the culture media with 10 g/l of each. As a result, the generation of minicells reached their maximum (over one million particles) when using fructose as carbon source in a concentration of 10 g/l. Consequently, fructose may not be suitable for the cell growth. However, this was the conventional condition in order to produce minicells. Saccharose effects on the minicell phenotype of the bacteria were the least (about 417,000 particles at concentration of 10 g/l in culture medium). In fact, during minD expression, saccharose led the filamentation in cells (Nguyen et al., 2013a). By statistical analysis, the minicell in fructose condition showed highly significant than the other sugars. Consequently, fructose (10 g/l) was used for minicell production in drug delivery of the study. 31 Table 4.3 The number of minicells produced from Lactobacillus acidophilus VTCC-B-871 in modified MRS medium containing each kind of selected sugar separately in different concentrations. Sugar concentrations (g/l) Selected sugars 0a, b 5a, b 10a, b 15a, b 20a, b 30a, b 40a, b 50a, b Glucose 6.03±0.25 41.1±2.71 66.2±3.35 38.8±2.55 35.4±4.78 33.6±4.28 31.2±4.42 27.3±2.95 Lactose 6.04±0.23 48.2±3.22 78.3±3.17 44.8±3.55 36.7±2.98 35.8±3.24 34.5±2.76 31.0±3.00 Fructose 6.07±0.20 81.0±2.59 107±6.03 69.0±3.74 56.3±2.60 41.9±4.19 38.7±2.52 37.8±3.36 Maltose 6.04±0.20 64.6±3.00 88.5±2.90 49.4±4.40 42.1±3.23 38.7±3.15 36.1±3.47 35.2±3.45 Saccharose 6.05±0.16 36.6±3.96 41.7±2.81 23.4±2.80 17.3±2.22 14.5±3.02 13.2±2.46 12.8±2.21 b Data are means ± standard deviations of triplicates for all treatments Expressed ×104 The number of minicells (×104 particles) a Glucose Lactose Fructose Maltose Saccharose 120 100 80 60 40 20 0 0 5 10 15 20 30 Sugar concentrations (g/l) 40 50 Figure 4.3 The number of minicells (×104) produced from Lactobacillus acidophilus VTCC-B-871 in modified MRS medium with differently selected sugars, as glucose, lactose, sucrose, maltose, fructose, with different concentrations (0 g/l, 5 g/l, 10 g/l, 15 g/l, 20 g/l, 30 g/l, 40 g/l, 50 g/l). Data represented means ± SD, n=3. 32 The number of obtained minicells after filtration was 1.07×106 particles from 100 ml starting culture with the density of cells before filtration about 2.57×1011 cells. It meant that every four million of parent cells, there was one minicell. In comparison with previous studies on other bacteria, a yield of approximately 1011 minicells from a 6 L starting culture being routinely obtained (MacDiarmid et al., 2007b), these showed that the number of obtained minicells in this study was not as high as expected. However, the techniques were quite simple in comparison with other studies on the world about filter system. Moreover, the minicells were usually formed by mutation during cell division whereas this study utilized carbon sources (sugars) as factors that effect on minicell generation in order to produce minicells with the normal properties of L. acidophilus. Remarkably, this study was the first research on minicell production from Lactobacillus strains using modified culture medium. In conclusion, the obtained minicells in this study were checked for the packaging of drug paclitaxel and confirmation by packaging other drug as cephalosporin in the next sections of this study. The Figure 4.4 illustrated the minicell formation at the end of L. acidophilus. As above analysis, this phenomenon was not caused by cell division. The reason was the effect of fructose on the cell development and differentiation. Moreover, the practice of formation of single or pair in rod of L. acidophilus (Figure 4.4A), gave advantages for minicell producing at the pole end and that was convenient for purification (Figure 4.4B). A B Figure 4.4 Photomicrographs of Lactobacillus acidophilus VTCC-B-871 and its minicells (100X): A) the morphology of L. acidophilus in basic MRS medium; B) the formation of minicells (black arrow) in the modified MRS medium with fructose 10 g/l. 33 4.1.2 Minicells generation from Lactobacillus rhamnosus JCM 15113 According to the results of biochemical tests of Lactobacillus rhamnosus JCM 15113 (Table 4.2 and Figure 4.2), the different sugars (glucose, lactose, sucrose, maltose, and fructose) were also used to study for testing the effect on minicell generation from L. rhamnosus (Appendix C). All analyzed data was shown in Table 4.4 and Figure 4.5. The statistical analysis identified that carbon sources influenced significantly on the minicell formation and the minicells were generated from L. rhamnosus depending on the sugar concentrations (p < 0.05). As presented in Table 4.4, the lowest level of producing minicells was found about 34,000 particles when L. rhamnosus was grown in the modified MRS media without containing sugar. The data presented that the number of obtained minicells increased gradually since raising the concentration of sugars (glucose, lactose, and maltose) from 5 g/l to 50 g/l for all tested sugars. On the other hand, in the fructose and saccharose conditions, production of minicells increased at low concentration of these sugars (from 5 g/l to 10 g/l) and then reduced at high concentration (from 15 g/l to 50 g/l). According to Table 4.4, the number of obtained minicells reached their maximum when using lactose as carbon source (from 146,000 to 787,000 particles). In the maltose medium, the quantity of minicells was lower than a half by comparison with lactose condition (from 98,700 to 351,000 particles). Through the usage of glucose, the number of minicells was a half of those numbers in maltose condition. Fructose and saccharose had similar levels of production of minicells such as between 48,200 to 151,000 particles each. At level of factor treatment of 50 g/l, the generated minicells were the highest number at each of kind of sugars (glucose, maltose, and lactose). In modified MRS media with these sugars (50 g/l), the minicells obtained were about 164,000; 351,000 and 787,000 particles, respectively. Meanwhile, the minicells obtained from L. rhamnosus in fructose and saccharose media got the highest values at concentration of 10 g/l (129,000 particles and 151,000 particles for saccharose and fructose, respectively) (Table 4.4). In summary, lactose was carbon source with a concentration of 50 g/l by means of which the highest number of minicells is generated from L. rhamnosus (around 800,000 particles). Consequently, the minicells produced from L. rhamnosus in modified MRS with lactose 50 g/l and applied to drug delivery of the study. 34 Table 4.4 The number of minicells produced from Lactobacillus rhamnosus JCM 15113 in modified MRS medium containing each kind of selected sugar separately in different concentrations. Sugar concentrations (g/l) Selected sugars 0a, b 5 a, b 10 a, b 15 a, b 20 a, b 30 a, b 40 a, b 50 a, b Glucose 3.39±0.72 3.46±0.75 6.87±1.59 7.48±2.15 8.13±2.03 9.38±1.97 11.7±1.85 16.4±1.97 Lactose 3.46±0.39 14.6±2.15 25.8±2.72 32.3±2.69 36.7±2.11 52.9±3.31 63.5±2.86 78.7±2.55 Fructose 3.41±0.36 9.61±2.77 15.1±1.40 13.9±1.76 12.6±2.11 11.9±1.93 10.5±1.57 9.68±2.54 Maltose 3.43±0.66 9.87±1.36 18.6±2.16 19.2±2.28 20.4±2.43 23.9±2.35 30.7±2.92 35.1±2.75 Saccharose 3.35±0.55 4.82±0.30 12.9±2.86 8.86±0.75 7.85±0.76 6.24±0.34 7.39±1.07 5.91±0.38 b Data are means ± standard deviations of triplicates for all treatments Expressed ×104 The number of minicells (×104 particles) a Glucose 90 Lactose 80 Fructose 70 Maltose 60 Saccharose 50 40 30 20 10 0 0 5 10 15 20 30 Sugar concentrations (g/l) 40 50 Figure 4.5 The number of minicells (×104) produced from Lactobacillus rhamnosus JCM 15113 in modified MRS medium with differently selected sugars, as glucose, lactose, sucrose, maltose, fructose, with different concentrations (0 g/l, 5 g/l, 10 g/l, 15 g/l, 20 g/l, 30 g/l, 40 g/l, 50 g/l). 35 Data represented means ± SD, n=3. In the Figure 4.6, the minicells were formed at one end of L. rhamnosus. The reason was the effect of lactose on the cell development and cell differentiation. Moreover, the practice of formation of rod chain of L. rhamnosus (Figure 4.6A), the minicells were produced in chain (Figure 4.6B). The cell culture of L. rhamnosus after cultivating in sugar was filtered through 0.45 µm; the minicells were collected and calculated. However, the yield of obtained minicells was too low (Table 4.4). Those meant that even morphological differentiation, the cell to cell connection was so rigid or the size of minicells was bigger than 0.45µm filter. Those caused the decrease of filtration efficiency. A B Figure 4.6 Photomicrographs of Lactobacillus rhamnosus JCM 15113 and its minicells (100X): A) the morphology of L. rhamnosus basic MRS culture medium; B) the formation of minicells (black arrow) in the modified MRS medium with lactose 50 g/l. Moreover, it was clear that there was difference in the influence of sugars on minicell formation between L. acidophilus and L. rhamnosus by comparison the levels of factor (sugar concentration) treatment of both of strains. The number of obtained minicells from L. acidophilus tended to decrease significantly whereas the production of minicells from L. rhamnosus rose at the high concentration of some of sugars (such as glucose, maltose and lactose). For this situation, more study should be done so far. According to the results of the yield of minicell generated from both L. acidophilus and L. rhamnosus, the quantity of minicell production from L. acidophilus was larger than that from L. rhamnosus. L. acidophilus was grown in MRS modified containing only 10 g/l of fructose, there 36 were 1,070,000 minicells obtained from culture with the density of about 2.57×1011 cells. Whereas, L. rhamnosus utilized 50 g/l lactose for generating and isolated only around 787,000 particles from the same cell density. 4.2 Microscopic studies for characterization of minicells morphology Minicells were achieved by using a procedure to homogenize and eliminated contaminants such as parent bacterial cells, cellular debris (Figure 4.7). By filtration through the filter membranes of 0.45 m and 0.2 m, the size of resultant minicells were less than 450 nm. Figure 4.27 Photomicrograph showing the morphology of minicells from Lactobacillus acidophilus VTCC-B-871 under the light microscope after isolation procedure (100 X). According to the obtained results in sub-headings 4.1.2 and 4.1.3, minicells generated from L. acidophilus in modified MRS with fructose 10 g/l and their isolated minicells that were selected as the representative samples for scanning the microscopic minicell morphologies under the scanning electron microscopy (SEM) (Figure 4.8 and 4.9). The Figure 4.8 represented the minicells formation at the end of one polar of L. acidophilus. This study used SEM for confirmation the minicell size; the minicell shape was captured, recorded and determined the nanoparticle size. 37 A B Figure 4.2 Representative SEM images showing the formation of minicells (red arrow) of Lactobacillus acidophilus VTCC-B-871. A) and B) SEM images observed with zoom out 20,000 times. As can be seen from the Figure 4.9, the SEM images of minicells with their diameter ranged from 290 nm to 410 nm. As the results, minicells were successfully generated as nano-cells. In the practice, nanoparticles were useful for drug delivery with the sizes up to 1000 nm (Shim and Turos, 2007). Therefore, they are continued to apply in drug delivery. The final minicell preparation was suggested to demonstrate the absence of bacterial colonies by plating the entire preparation on MRS agar plates and incubating it overnight at 37ºC. The result regarding minicell preparation did not contain filamentous, gram positive bacteria (such as Lactococcus, Staphylococcus genus) from environment. 38 A B C D Figure 4.29 Representative SEM images of minicells from Lactobacillus acidophilus VTCC-B-871with minicell size after isolation procedure. A) minicells observed with the zoom out 3,000 times; B) minicells with the zoom out 10,000 times; C) minicell with the zoom out 20,000 times; and D) minicell with the zoom out 50,000 times. 4.3 Package of drug into minicells generated from Lactobacillus strains 4.3.1 Antimicrobial activity tests The experiments of testing antimicrobial activity supported for determining the ability of packaging drug paclitaxel into minicells, because paclitaxel is not only anti-tumor activity but also antimicrobial activity. To test the ability and potency of drug delivery of our minicells, the minicells encapsulated with two different drugs (paclitaxel, and cephalosporin), and incubated at different time (10, 15 and 24 hours). The extracted solutions from drug-packaged minicells were centrifuged and used to test the antibacterial activities on the pathogens. 39 4.3.1.1 Drug packaging of minicells produced from Lactobacillus acidophilus The extracted solution from drug-packaged minicells was centrifuged and used to test the activities on the above mentioned pathogens. Results obtained in the present study relieved that extracted solution possess potential antibacterial activity against both of gram negative (S. 9637, P . aureus ATCC 25923, E. coli ATCC aeruginosa ATCC 27853), positive bacteria (S. typhi ATCC 19430), and yeast (C. albicans ATCC 14053) (Table 4.5). Meanwhile, extracted solution from control minicells that were not incubated with the drug did not show any antibacterial activity (Appendix D). Images showed off the antimicrobial activities of extracted drugs from drug-packaged minicells on bacteria that could be referred in Appendix D.1. The inhibition zone diameters were from around 4.6 to 23.0 mm and from 4.0 to 19.0 mm for extracted paclitaxel and cephalosporin, respectively (Table 4.6). The results of statistical analysis also showed that there were significantly different in antibacterial ability of extracted solutions when minicells from L. acidophilus loaded with drugs at different incubation times (10, 15, 24 hours) at 37°C with rotation (p < 0.05). The data concluded that the zone inhibition showed the highest activity at 10 hours of incubation with the tested drugs (table 4.6). For this condition, the highest antibacterial activity of 23.0 ± 1.5 mm for paclitaxel and 19.3 ± 0.5 mm for cephalosporin in against P. aeruginosa and least activity recorded in C. albicans measured 16.0 ± 1.0 mm and 13.0 ± 1.0 mm for paclitaxel and cephalosporin, respectively. After 24 hours of incubation of minicells with drugs, these numbers were significantly reduced to 7.6 ± 0.5 mm for paclitaxel in P. aeruginosa, and to 6.0 ± 1.0 mm for cephalosporin in P. aeruginosa as well (Table 4.6). The antibacterial activities of extracted paclitaxel and cephalosporin against the other bacteria had also the similar characteristics in P. aeruginosa. Those meant that antibacterial activity of drug extracts decreased since increasing the time of incubation for minicells loading drugs. These results indicated that time of incubation have certain effect on the drug loading into minicells. Consequently, the generated minicells could package with many drugs. 40 Table 4.5 Antimicrobial spectrum of extracted drugs from drug-packaged minicells of Lactobacillus acidophilus VTCC-B-871 and Lactobacillus rhamnosus JCM 15113 against Gram-positive and Gram-negative bacteria. Inhibition1 Test organism Gram-positive Staphylococcus aureus ATCC 25923 (+) Gram-negative Escherichia coli ATCC 9637 (+) Salmonella typhi ATCC 19430 (+) Pseudomonas aeruginosa ATCC 27853 (+) Yeast Candida albicans ATCC 14053 1 (+) (+) Inhibited by extracted drugs from drug-packaged minicells, (-) not inhibited. Table 4.6 Antibacterial activity of extracted paclitaxel and cephalosporin from drug-packaged minicells of Lactobacillus acidophilus against bacterial species Zone of inhibition (mm) Indicator Bacteria 10 hours 15 hours Pac Cel Pac S. typhi 18.0 ± 1.0 14.3 ± 0.5 11.0 ± 1.0 E. coli 19.3 ± 1.5 15.3 ± 0.5 C. albicans 16.0 ± 1.0 P. aeruginosa S. aureus 24 hours Cel Pac Cel 8.6 ± 0.5 5.0 ± 1.0 5.0 ± 1.0 12.3 ± 0.5 9.3 ± 0.5 5.3 ± 1.5 5.0 ± 1.0 13.0 ± 1.0 9.3 ± 0.5 7.3 ± 0.5 4.6 ± 0.5 4.0 ± 0.0 23.0 ± 1.5 19.3 ± 0.5 15.0 ± 1.0 13.3 ± 0.5 7.6 ± 0.5 6.0 ± 1.0 22.0 ± 1.0 18.3 ± 0.5 14.3 ± 0.5 12.0 ± 1.0 7.0 ± 0.0 6.3 ± 0.5 Measurements are means ± standard deviations of 3 replicates for all treatments Pac: paclitaxel; Cel: cephalosporin 4.3.1.2 Drug packaging rhamnosus of minicells produced from Lactobacillus Even though the number of obtained minicells from L. rhamnosus after filtration was less than that from L. acidophilus, this study also tried to test the packaging drug into minicells. In the practice, L. acidophilus and L. rhamnosus also had the same in applied properties as probiotics. This was clear that using L. acidophilus or L. rhamnosus as the bacteria source for producing minicells. Moreover, L. acidophilus was applied more popular than L. rhamnosus in pharmaceutical field. From those points, this study also implemented the research on the paclitaxel packaging into minicells from L. rhamnosus. To determine the ability of paclitaxel 41 packaged minicells by using antimicrobial activity testing because paclitaxel is not only anti-tumor activity but also antimicrobial activity. The study also tested the cephalosporin packaging of this kind of minicells. The minicells were incubated with two different drugs (paclitaxel, and cephalosporin) at different time (10, 15 and 24 hours). The extracted solutions from drug-packaged minicells were centrifuged and used to test the antibacterial activities on the mentioned pathogens. Table 4.7 Antibacterial activity of extracted paclitaxel and cephalosporin from drug-packaged minicells of Lactobacillus rhamnosus against bacterial species Zone of inhibition (mm) Indicator Bacteria 10 hours Pac 15 hours Cel Pac 24 hours Cel Pac Cel S. typhi 13.6 ± 0.5 11.0 ± 1.0 8.3 ± 0.5 5.3 ± 0.5 2.3 ± 0.5 3.3 ± 0.5 E. coli 14.6 ± 0.5 12.0 ± 1.0 8.0 ± 1.0 6.3 ± 0.5 4.3 ± 0.5 3.6 ± 0.5 C. albicans 12.0 ± 1.0 8.3 ± 0.5 6.0 ± 0.0 4.3 ± 0.5 4.0 ± 1.0 2.0 ± 1.0 P. aeruginosa 19.3 ± 1.0 16.6 ± 0.5 11.0 ± 1.0 8.3 ± 0.5 6.6 ± 0.5 5.0 ± 1.0 S. aureus 18.0 ± 1.0 14.6 ± 0.5 11.0 ± 1.0 8.0 ± 0.0 4.0 ± 0.0 5.0 ± 1.0 Measurements are means ± standard deviations of triplicates for all treatments Pac: paclitaxel; Cel: cephalosporin As was illustrated by the Table 4.5, the extracted solution from drug-packaging minicells of L. rhamnosus showed antimicrobial activities against both of gram negative and gram positive bacteria. Inhibited activity of the growth of tested bacteria S. aureus ATCC 25923, E. coli ATCC 9637, S. typhi ATCC 19430, C. albicans ATCC 14053 and P. aeruginosa ATCC 27853 were presented by the action of the supernatants (Appendix E). Moreover, extracted solution from control minicells that were not incubated with the drug did not show any antibacterial activity (Appendix E). As the information provided by Table 4.7, extracted solutions of drug-loading minicells showed varied in the zone of inhibition from about 2.0 - 19.3 mm against all the tested bacteria. It was similar in L. acidophilus, there were also significantly different in antibacterial ability of extracted solution when minicells from L. rhamnosus incubated with drugs at different incubation times (10, 15, 24 hours) at 37°C with rotation (P < 0.05). When minicells from L. rhamnosus had been incubated with drugs at 10 hr, the highest antibacterial activity of their drug extracts were observed in all indicator bacteria. The inhibition zone diameters of extracted solution of paclitaxel were from around 13.6 mm to 19.3 mm and from about 8.3 mm to 16.6 mm of 42 cephalosporin (Table 4.7). After 24 hours of incubation of minicells with drugs, the antibacterial activity of extracted solutions was significantly reduced from about 19.3 mm to 6.6 mm for paclitaxel in P. aeruginosa, and from 16.6 mm to 5.0 mm for cephalosporin in P. aeruginosa as well (Table 4.7). The antibacterial activities of extracted paclitaxel and cephalosporin against other bacteria had also the same characteristics as in P. aeruginosa. It was clearly that antibacterial activities vary with the extracted solutions from drug-packaged minicells which were incubated with drugs at different time. The results of present investigation about the antibacterial activity of extracted solutions clearly cephalosporin in indicated the that extracted there were solutions presence of of paclitaxel drug-packaging and minicells. Consequently, the generated minicells from Lactobacillus strains could package with many drugs. Moreover, the incubation time of minicells with drugs also affected on the drug loading into minicells. To test how the minicells could package with the drugs, more studies should be done so far. From the results in the Table 4.6 and 4.7 it was interesting that the drug extracts from L. acidophilus drug-packaged minicells were almost higher antibacterial activities when compared with the extracted solution from minicells of L. rhamnosus. This meant that the concentration of drugs in extracted solutions from drug-packaged minicells of L. acidophilus were higher than those of L. rhamnosus. In general, the efficient packaging of many drugs into minicells generated from L. acidophilus was better than that into minicells produced from L. rhamnosus. Therefore, isolated minicells from L. acidophilus in this study were selected as the representative samples for certain confirmation of packaging of chemotherapeutic drug paclitaxel using a high sensitive and accurate technique, HPLC-UV/Vis Spectroscopy. From that, the packaged paclitaxel concentration and the number of paclitaxel molecules presented per minicell were determined. 4.3.2 Paclitaxel quantitation using HPLC-UV/Vis Spectroscopy To confirm certainly if minicells can be packaged with chemotherapeutic drug (Paclitaxel) and the kinetics of minicell drug packaging in response to varying concentrations of drug in the loading solution or varying times of incubation. HPLC analysis was applied to detect the existence of paclitaxel and determined the amount of packaged paclitaxel as well as the number of paclitaxel molecules presented per minicell. 43 4.3.2.1 The minicell drug packaging in response to varying times of incubation For minicells depending upon the times of incubation in the loading solution, minicells were separately incubated with paclitaxel (10 µg/ml) for the time was shown 10, 15 and 24 hours with rotation. The minicell suspensions incubated with paclitaxel were then centrifuged at 13000 rpm for 15 min. The supernatants were used to analyze for the paclitaxel remaining. Paclitaxel supernatants were introduced to High Performance Liquid Chromatography (HPLC) for paclitaxel detection and quantification whose results were showed in Appendix G. The data obtained from HPLC analysis was analyzed by comparison with the data of standard paclitaxel. With this method, the remaining concentration of paclitaxel in the loading solution could be measured as following the linear calibration equation of paclitaxel (Appendix K) in order to determine whether paclitaxel could be absorbed by minicells in the loading solution or not. According to the HPLC chromatogram analysis (detailed in Appendix G), the retention time and the remaining paclitaxel concentration were summarized in Table 4.8. Table 4.8 HPLC analysis of paclitaxel in the loading solution in response to varying times of incubation Incubation time (hr) Retention time (minutes) Variation (%) Remaining paclitaxel concentration (µg/ml) 0 0 0 0 10 5.846 ± 0.006 2.24 ± 0.097 8.56 ± 0.025 15 5.807 ± 0.006 1.56 ± 0.105 9.16 ± 0.015 24 5.826 ± 0.006 1.88 ± 0.096 9.71 ± 0.03 Data are means ± standard deviations of triplicates for all treatments The retention time of paclitaxel standard was 5.718 min (Appendix F). As Table 4.8 underlined that the paclitaxel still remained in the supernatants after 10 hr, 15 hr to 24 hr with the retention time about at 5.846 ± 0.006, 5.807 ± 0.006, and 5.826 ± 0.006 min, respectively. The remaining paclitaxel concentration was inferred from the linear standard graph of peak area which was drawn in the appendix K. Comparing with the initial amount of paclitaxel loaded (10 (µg/ml)), data showed that the drug concentration decreased in all loading solutions after incubating time (Table 4.8). This finding therefore proved that chemotherapeutic drug (paclitaxel) was absorbed by minicells which were presented in the 44 incubated solution. This totally matched with the result of testing antimicrobial activity which indicated there were presence of paclitaxel the extracted solutions of drug-packaging minicells (sub-heading 4.3.1.1). The results of statistical analysis also showed that drug-incubating time affected significantly on the efficient packaging paclitaxel activity in minicells (p < 0.05). There was gradual raise of leftover drug concentration in the loading solutions as increasing the incubation time of minicells with drug. The data in Table 4.8 revealed increase in concentration of paclitaxel remaining according to the incubation time, from 8.56 ± 0.025 (µg/ml) with 10 hr of incubation time go up to 9.71 ± 0.03 (µg/ml) with 24 hr. Indeed, the peak area of samples after 15 hr and 24 hr of incubation were higher than that from 10 hr (Appendix G). With these points, minicells should be soaked in paclitaxel loading solution for 10 hr in order to get the highest yield of encapsulated activity. 4.3.2.2 The minicell drug packaging in response to varying concentrations Purified minicells were separately loaded in solution of the paclitaxel drug, at different final concentrations of 5 µg/ml, 10 µg/ml, and 20 µg/ml and then incubated at 37°C with rotation for 10 hr. In order to confirm certainly the drugpackaging in minicells, the extracted solutions from drug-packaged minicells were centrifuged and used to determine the concentration of drug in minicells using HPLC. This experiment also revealed quantitation of minicells loading when incubated in the presence of different paclitaxel concentrations. As mentioned in Appendix F, retention time of standard was 5.718 min whereas others were slightly varied. To identify the presence of paclitaxel, the variation between paclitaxel peaks of samples and standard were calculated as equation 3.2 (see sub-heading 3.2.8). These variations could due to noise and disturbance. However, the measured variations of retention time should be in the acceptable range (less than 5%). Since all of experiments had retention time variation less than 5% which were recognized as peak of standard paclitaxel. In addition, extracted solution from control minicells that were not incubated with the drug did not show paclitaxel peak (Appendix F). As comparing with the retention time of standard paclitaxel (5.718 min), the retention time 5.444 ± 0.007, 5.454 ± 0.006 and 5.671 ± 0.004 min for samples of 5, 10 and 20 µg/ml initial paclitaxel concentration, respectively, pointed that the existence of paclitaxel in the minicells (Table 4.9, Appendix H). 45 Table 4.9 HPLC analysis of paclitaxel loading in minicells when incubated in the presence of different drug concentrations Initial Paclitaxel Concentration (µg/ml) Retention time (minutes) Variation (%) Concentration of extracted paclitaxel (µg/ml) 0 0 0 0 5 5.444 ± 0.007 4.80 ± 0.124 0.35 ± 0.025 10 5.454 ± 0.006 4.61 ± 0.105 1.07 ± 0.026 20 5.671 ± 0.004 0.83 ± 0.071 2.22 ± 0.015 Data are means ± standard deviations of triplicates for all treatments According to the linear calibration graph of area peak as a function of concentration for paclitaxel standard solutions assayed by HPLC (Appendix K), the amount of paclitaxel packaged into the total minicells was determined. As the information provided by Table 4.9 and Figure 4.10, it was clear that paclitaxel packaging was dependent on, and directly related to the external loading concentration of paclitaxel. Indeed, the results of statistical analysis also showed that the input drug concentration in the loading solution influenced significantly on the encapsulation efficiency paclitaxel of minicells (p < 0.05) (Table 4.10). There was the raise of packaged drug concentrations in minicells from 0.35 to 2.22 µg/ml as initial drug concentrations were increased from 5 to 20 µg/ml, respectively (Table 4.9). It meant that the amount of packaged drug increased six fold as raising the input drug quantity to four times. Drug (µg) in 2.12 ×106 minicells Figure 4.10 Drug quantitation in minicells when minicells incubated in the 2.50 2.00 paclitaxel packaging 1.50 1.00 0.50 0.00 5 10 20 Initial drug concentration (µg/ml) presence of different drug loading concentrations. Data are means ± standard deviations of triplicates for all treatments. 46 The number of drug molecules per minicell was calculated according to equations in sub-heading 3.2.9. The number of drug molecules in the incubation solution, in the total of minicells, and in per minicell; the encapsulation efficiency of packaging paclitaxel into minicells were summarized in Table 4.10. For the incubation of 5×107 minicells for 10 hr with different paclitaxel concentrations of 5 µg/ml, 10 µg/ml and 20 µg/ml, the amount paclitaxel packaged was 0.35 ± 0.025 µg, 1.07 ± 0.026 µg, and 2.22 ± 0.015 µg, respectively (Table 4.9). This equated to about 5 million, 15 million, and 31 million drug molecules packaged per minicell, respectively (Table 4.10). When the initial paclitaxel concentration increased to 20 µg/ml, the encapsulated efficiency achieved almost 2 times higher than at 5 µg/ml (Table 4.10). At input paclitaxel concentration of 20 µg/ml, the highest number of paclitaxel molecules (about 31 million molecules) was packaged per minicell. Table 4.10 also indicated that at paclitaxel concentration of 20 µg/ml, there were the total number of 14.1×10 15 paclitaxel molecules presented in the loading solution, and 1.57×1015 paclitaxel molecules entrapped in 5×107 minicells. Table 4.10 Paclitaxel quantification in minicells when incubated in the presence of different drug concentrations Initial Paclitaxel Concentration (µg/ml) NPL (molecules) b NPT (molecules)a, b NPM (molecules)a, c EE (%)a 0 0 0 0 0 5 352 24.9±1.77 49.8±3.55 6.6±0.503 10 705 75.4±1.87 151±3.73 10.7±0.265 20 1410 157±1.08 313±2.15 11.1±0.076 a Data are means ± standard deviations of triplicates for all treatments; Expressed ×1013 ; c Expressed ×105; NPL: the number of paclitaxel molecules present in the loading solution; NPT: the number of paclitaxel molecules present in the total minicells; NPM: the number of paclitaxel molecules per minicells; EE%: is encapsulation efficiency. b In general, this study was discovered that an unprecedented concentration of 5 million to 31 million paclitaxel molecules can be packaged within a minicell. In contrast, other bacterially deriver minicells have been shown to package 300,000 (MacDiarmid et al., 2007b) molecules of paclitaxel. This was clear that minicells generated from this study which was able to encapsulate a huge amount of drug (more than 100 times in comparison with previous study about packaging paclitaxel in minicells). Although minicells were produced in this study at low 47 yield (about 106 in comparison with 1011 minicells generated from other bacteria in previous study (MacDiarmid et al., 2007b)), the number of paclitaxel drug molecules packaged by a minicell was very large. 48 CHAPTER 5 CONCLUSION AND RECOMMENDATION The study was the first report that L. acidophilus VTCC-B-871 and L. rhamnosus JCM 15113 in the modified MRS broth with carbon source as fructose (10 g/l) and lactose (50 g/l), respectively, gave the significant minicell quantity. The number of minicells was generated from L. acidophilus VTCC-B-871 and L. rhamnosus JCM 15113 about 1,070,000 and 787,000 minicells, respectively. The result of this study revealed that carbon sources (sugars) actually affected on the minicell production or cell division of L. acidophilus VTCC-B-871 and L. rhamnosus JCM 15113 strains. This study captured and determined the nanoparticle size of obtained minicells (with their diameter ranged from 290 nm to 410 nm) using scanning electron microscopy. Minicells were performed the ability of packaging paclitaxel. The study also tested the packaging of cephalosporin to confirm the packaging ability. Moreover, the study also suggested the easy, fast and cheap way to test the paclitaxel and cephalosporin using antimicrobial activity. However, the higher technique (using HPLC) was applied in this study to measure the paclitaxel packaging in the small amount. Also, the study was optimized the minicell generation from L. rhamnosus that was able to package paclitaxel and cephalosporin by testing on antimicrobial activity. The input drug concentration in the loading solution and the incubation time of drug with minicells influenced significantly on the encapsulation efficiency paclitaxel of minicells. Surprisingly, the minicell generated from L. acidophilus could package with the drug better than that from L. rhamnosus. In addition, the ability of minicells to encapsulate a large number of drug molecules (5 million to 31 million paclitaxel molecules packaged per minicell), as well as a convenient drug-loading process that required only one-step co-incubation of a solution of the drug with the vehicle, made minicells the potentially attractive alternative to other macromolecule based drug formulations. Frequently, the following minicell production was due to the min deletion. The practice of modifying carbon sources to produce minicell had the potential role in drug delivery. 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Aaps Pharmsci 3: E15. 57 APPENDIX A Buffers preparation Table A.1 Buffered saline gelatin (BSG) preparation Ingredients Formula per Liter NaCl 8.5 g KH2PO4 0.3 g Na2HPO4. 12H2O 0.6 g Gelatin 1% 10 ml pH 7.0, autoclaved at 121°C for 15 min Table A.2 Phosphate buffered saline (PBS) preparation Ingredients Formula per Liter NaCl 8.01 g KH2PO4 0.24 g Na2HPO4. 12H2O 3.63 g KCl 0.2 g pH 7.4, autoclaved at 121°C for 15 min 58 APPENDIX B Morphology of Lactobacilus acidophilus in modified MRS broth with different concentrations of sugar (0, 5, 10, 15, 20, 30, 40, 50 (g/l)) Figure B.1 Morphology of L.acidophilus in modified MRS broth containing different concentrations of glucose (0, 5, 10, 15, 20, 30, 40, 50 g/L (w/v)) Figure B.2 Morphology of L.acidophilus in modified MRS broth containing different concentrations of lactose (0, 5, 10, 15, 20, 30, 40, 50 g/L (w/v)) 59 Figure B.3 Morphology of L.acidophilus in modified MRS broth containing different concentrations of frucose (0, 5, 10, 15, 20, 30, 40, 50 g/L (w/v)) Figure B.4 Morphology of L.acidophilus in modified MRS broth containing different concentrations of maltose (0, 5, 10, 15, 20, 30, 40, 50 g/L (w/v)) Figure B.5 Morphology of L.acidophilus in modified MRS broth containing different concentrations of sacchrose (0, 5, 10, 15, 20, 30, 40, 50 g/L (w/v)) 60 APPENDIX C Morphology of Lactobacilus rhamnosus in modified MRS broth with different concentrations of sugar (0, 5, 10, 15, 20, 30, 40, 50 (g/l)) Figure C.1 Morphology of L. rhamnosus in modified MRS broth containing different concentrations of glucose (0, 5, 10, 15, 20, 30, 40, 50 g/L (w/v)) Figure C.2 Morphology of L. rhamnosus in modified MRS broth containing different concentrations of lactose (0, 5, 10, 15, 20, 30, 40, 50 g/L (w/v)) 61 Figure C.3 Morphology of L. rhamnosus in modified MRS broth containing different concentrations of fructose (0, 5, 10, 15, 20, 30, 40, 50 g/L (w/v)) Figure C.4 Morphology of L. rhamnosus in modified MRS broth containing different concentrations of maltose (0, 5, 10, 15, 20, 30, 40, 50 g/L (w/v)) Figure C.5 Morphology of L. rhamnosus in modified MRS broth containing different concentrations of saccharose (0, 5, 10, 15, 20, 30, 40, 50 g/L (w/v)) 62 APPENDIX D Antimicrobial activity tests on bacteria of drug extracts of minicells from Lactobacillus acidophilus at different drug incubation time (10, 15, 24hr) A B C D E Figure D.1 Extracted cephalosporin showing antibacterial activity against: A) Salmonella typhi; B) Escherichia coli; C) Candida albicans; D) Pseudomonas aeruginosa; E) Staphylococcus aureus. N is negative control (minicells without drug) ; P is positive control (cephalosporin) 63 A B D C E Figure D.2 Extracted paclitaxel showing antibacterial activity against: A) Salmonella typhi; B) Escherichia coli; C) Candida albicans; D) Pseudomonas aeruginosa; E) Staphylococcus aureus. N is negative control (minicells without drug) ; P is positive control (paclitaxel) 64 APPENDIX E Antimicrobial activity tests on bacteria of drug extracts of minicells from Lactobacillus rhamnosus at different drug incubation time (10, 15, 24hr) A B C D E Figure E.1 Extracted cephalosporin showing antibacterial activity against: A) Salmonella typhi; B) Escherichia coli; C) Candida albicans; D) Pseudomonas aeruginosa; E) Staphylococcus aureus. N is negative control (minicells without drug) ; P is positive control (cephalosporin) 65 A B C D E Figure E.2 Extracted paclitaxel showing antibacterial activity against: A) Salmonella typhi; B) Escherichia coli; C) Candida albicans; D) Pseudomonas aeruginosa; E) Staphylococcus aureus. N is negative control (minicells without drug) ; P is positive control (paclitaxel) 66 APPENDIX F HPLC analysis for paclitaxel standard, incubated with paclitaxel), and blank. 67 control (minicells without APPENDIX G G.1. HPLC analysis for minicell loading paclitaxel when incubated at 10hr 68 APPENDIX G (cont.) G.2. HPLC analysis for minicell loading paclitaxel when incubated at 15hr 69 APPENDIX G (cont.) G.3. HPLC analysis for minicell loading paclitaxel when incubated at 24hr 70 APPENDIX H H.1. HPLC assay for minicell loading when incubated in the presence of 5 (µg/ml) drug concentrations 71 H.2. HPLC assay for minicell loading when incubated in the presence of 10 (µg/ml) drug concentrations 72 H.3. HPLC assay for minicell loading when incubated in the presence of 20 (µg/ml) drug concentrations 73 APPENDIX K Standard paclitaxel linear calibration graph of peak area Table K.1 Concentration of standard paclitaxel and peak areas corresponding Concentration of standard paclitaxel (µg/ml) Peak area 0 0 5 68908 10 179816 15 294356 20 381602 30 583890 50 938518 1000000 y = 19120x - 5500 R² = 0.9983 800000 Peak area 600000 400000 Paclitaxel standard 200000 Linear (Paclitaxel standard) 0 0 -200000 10 20 30 40 50 Paclitaxel Concentration (µg/ml) Figure B.1 Standard paclitaxel linear calibration graph of peak area 74 60 [...]... insolubility of paclitaxel Figure 2.43 Chemical structure of paclitaxel 16 The major limitation of paclitaxel is also the obstacle of chemotherapy, drug resistance in the mucosa of the small and large intestine which limits the oral uptake of paclitaxel and mediates direct excretion of the drug in the intestinal lumen (Adams et al., 1993) Paclitaxel has been recognized as the most potent anticancer agent for the. .. kinetics of minicell drug packaging in response to varying concentrations of drug in the loading solution or varying times of incubation, the following methods were adopted Preparations of purified minicells derived from LAB strains were separately incubated in a solution of the paclitaxel drug, at different final paclitaxel concentrations in minicell extracellular environment of 5, 10 and 20 µg/ml The. .. standard were calculated as following equation (eq 3.2) (eq 3.2) Where, V (%) is the variation Rp is the retention time of sample paclitaxel Rst is the retention time of standard The acceptable range for the variation of retention time was less than 5% 3.2.8 Calculation of the number of drug molecules (MacDiarmid et al., 2007b) The number of molecules of drug (paclitaxel) packaged per minicell is calculated... DISCUSSION 4.1 Screening the carbon sources for study on minicell generation from Lactobacillus strains In order to decide which sugars would be related to the investigation of the effect of carbon sources on the minicell formation, Lactobacillus acidophilus and Lactobacillus rhamnosus were used to test the carbohydrate fermentation using API 50CHL kit (BioMerieux) During fermentation of carbohydrates, the. .. for study The modified MRS media were prepared by modifying carbon source in MRS ingredients (detail in sub-section 3.2.2) 20 3.2 RESEARCH METHODOLOGY 3.2.1 Design condition for minicells production from Lactobacillus strains In order to study the influence of various carbon sources on the minicell formation, this study implemented experiments on different kinds of sugar with different concentration... mortality produced by the International Agency for Research on Cancer (IARC) for 2008, there were an estimated 12.4 million cases of cancer diagnosed and 7.6 million deaths from cancer and 28 million persons alive with cancer around the world in 2008 (Table 2.1); of these, 56% of the cases and 64% of the deaths occurred in the less developed regions of the world, many of which lack the medical resources... Up to now, there has not any study on generating bacterially-minicells from Lactobacillus strains, or not any research on the drug delivery of this genus, one kind of largest genus within the group of lactic acid bacteria (LAB) with their properties as probiotics According to the principle of bacteria cell division, the normal generation of two equally sized daughter cells are maintained by the regulatory... improve the therapeutic index of anticancer drugs Nanoparticle drug delivery systems are being studied to overcome limitation of conventional therapeutic areas particularly in cancer chemotherapy As mentioned in subheading 2.1.3.2, nanomedicine performed a strong potential to accelerate the development of effective approaches to the treatment of drug8 resistant and recurrent cancers However, despite the. .. with chemotherapeutic drug (Paclitaxel) ; in order to detectable a robust and versatile system for in vitro drug delivery using minicell, a bacterially-derived lactic acid bacteria carrier Moreover, this study also confirmed the ability of encapsulation of minicells with other drug as cephalosporin This study was the primary research on the drug delivery system which was able to carry many drugs and... twice and then grown for 18 to 24 hr in 10 ml of appropriate growth media Sterile paper discs (5 mm of diameter) were then prepared and dropped on using 20 μl of cell-free filtrate The extracted solution from minicell suspension without drugs incubation was used as the control The inoculated plates were incubated for 18 to 24 hr at appropriate temperatures, and the diameter of the inhibition zone was .. .Study on Drug Delivery for Paclitaxel of the Lactobacillus Strains By DOAN THI THANH VINH ABSTRACT The practice of developing molecularly targeted drugs to achieve a higher degree of cancer therapy... Rst is the retention time of standard The acceptable range for the variation of retention time was less than 5% 3.2.8 Calculation of the number of drug molecules (MacDiarmid et al., 2007b) The number... study on minicell generation from Lactobacillus strains In order to decide which sugars would be related to the investigation of the effect of carbon sources on the minicell formation, Lactobacillus

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