Study on the development of photocatalytic membrane reactor for the treatment of organics in water = nghiên cứu phát triển màng lọc quang xúc tác để xử lý chất hữu cơ trong nước

HỌ VÀ TÊN: TRẦN VĂN THIỆN BỘ GIÁO DỤC VÀ ĐÀO TẠO TRƯỜNG ĐẠI HỌC BÁCH KHOA HÀ NỘI - Trần Văn Thiện CHUYÊN NGÀNH KỸ THUẬT CƠ ĐIỆN TỬ ỨNG DỤNG GIẢI PHÁP SỐ TRONG VIỆC XÁC ĐỊNH BỘ THÔNG SỐ LÀM VIỆC PHÙ HỢP CHO HỆ THỐNG VÍT TẢI CẤP LIỆU DẠNG RỜI LUẬN VĂN THẠC SĨ KHOA HỌC KỸ THUẬT CƠ ĐIỆN TỬ KHOÁ 2017A Hà Nội – Năm 2019 BỘ GIÁO DỤC VÀ ĐÀO TẠO TRƯỜNG ĐẠI HỌC BÁCH KHOA HÀ NỘI Trần Văn Thiện ỨNG DỤNG GIẢI PHÁP SỐ TRONG VIỆC XÁC ĐỊNH BỘ THÔNG SỐ LÀM VIỆC PHÙ HỢP CHO HỆ THỐNG VÍT TẢI CẤP LIỆU DẠNG RỜI Chuyên ngành : Kỹ thuật Cơ Điện Tử LUẬN VĂN THẠC SĨ KHOA HỌC KỸ THUẬT CƠ ĐIỆN TỬ NGƯỜI HƯỚNG DẪN KHOA HỌC : TS Bùi Tuấn Anh Hà Nội – Năm 2019 CỘNG HÒA XÃ HỘI CHỦ NGHĨA VIỆT NAM Độc lập – Tự – Hạnh phúc BẢN XÁC NHẬN CHỈNH SỬA LUẬN VĂN THẠC SĨ Họ tên tác giả luận văn: TRẦN VĂN THIỆN Đề tài luận văn: ứng dụng giải pháp số việc xác định thông số làm việc phù hợp cho hệ thống vít tải cấp liệu dạng rời Chuyên ngành: Kỹ thuật Cơ Điện Tử Mã số HV: CA170370 Tác giả, Người hướng dẫn khoa học Hội đồng chấm luận văn xác nhận tác giả sửa chữa, bổ sung luận văn theo biên họp Hội đồng ngày với nội dung sau: - Đã sửa lỗi tả theo góp ý hội đồng - Đã trích dẫn tài liệu cơng thức chương - Trang 10 phân tích thêm ưu, nhược điểm loại vít - Viết lời mở đầu, tình hình vít tải Việt Nam, kết luận chung - Chỉnh sửa sai lệch đơn vị Ngày Giáo viên hướng dẫn CHỦ TỊCH HỘI ĐỒNG tháng năm Tác giả luận văn DECLARATION IN LIEU OF OATH By “Duong Nguyen Thi Thuy” This is to confirm my Master Thesis was independently composed/authored by myself using solely the referred sources and support I additionally assert that this Thesis has not been part of another examination process ACKNOWLEDGEMENT I would first like to sincerely express my thankfulness to my supervisors, Prof Dang Kim Chi, Dr Dirk Hollmann of Institute for Chemistry at Rostock University and Dr Ly Bich Thuy at Institute for Environmental Science and Technology Prof Dang Kim Chi was very willing to spend her time on discussing with me and give me knowledgeable advices and support whenever I ran into troubles and steer me to the right direction of my thesis Dr Dirk Hollman thoroughly instructed me a lot of experiment skills in laboratory and always supported me during my time researching in Germany Dr Ly Bich Thuy is a person always providing me valuable comments and feedback with her high responsibility and expertise on my work from time to time to help me carry out the scientific work with high efficiency I am also grateful to faculty of School of the Environmental Science and Technology - Hanoi University of Science and Technology who enthusiastically guided, taught and helped me during the process of studying, researching and completing this thesis I also would like to thank Prof Dr Le Minh Thang and ROHAN Project - Rostock Hanoi DAAD SDG Graduate School and all colleagues at Technical Chemistry Group, University of Rostock for supporting and creating favourable conditions for me to attend the Master Research Exchange Program at the Institute for Chemistry, University Rostock, Germany Finally, my great gratitude is for my family and my friends who always believed and encouraged me so much during my years of study This achievement would not have been possible without them Author, Duong Nguyen Thi Thuy ABBREVIATION ABS Absorbance PMRs Photocatalytic membrane reactors MB Methylene blue XRD X-Ray Diffraction RC Regenerated Cellulose ICP-MS Inductively coupled plasma mass spectrometry UV Ultraviolet VIS Visible MW Molecular weight SPR Surface Plasmon Resonance PTFE Poly Tetra Fluorethylene TiO2 Titanium dioxide Au/TiO2 Gold nanoparticles deposited on titanium dioxide TABLE OF CONTENTS DECLARATION IN LIEU OF OATH .1 ACKNOWLEDGEMENT ABBREVIATION .3 TABLE OF CONTENTS TABLE OF FIGURES TABLE OF TABLES INTRODUCTION .8 Chapter Literature Review 10 Introduction about photocatalyst .10 1.1 Overview of photocatalyst 10 1.2 Introduction about titanium dioxide 11 1.3 Gold nanoparticle supported on titanium dioxide (Au/TiO2) .14 Photocatalytic membrane reactor 17 2.1 Definition .17 2.2 Research works on photocatalytic membrane reactor 18 Researches and application of Au/TiO2 in water treatment 23 Organic pollutant status .24 Chapter Experimental section .26 Experimental overview 26 1.1 Experiment process .26 1.2 Chemical and materials .28 Methods .29 2.1 Synthesis of Au/TiO2 photocatalyst 29 2.1.1 Synthesis method 29 2.1.2 Au/TiO2 characteristic analysis method 30 2.2 Coating photocatalyst into membrane surface 31 2.3 Design and construction of a PMR reactor 33 2.4 Evaluation of the system in removal of organic matter from feed water 34 2.4.1 Evaluation of batch reaction .34 2.4.2 Evaluation of suspended reaction .35 2.4.3 Evaluation of immobilized system 36 Chapter Results and Discussion 37 Characteristics of photocatalyst: 37 Coating Au/TiO2 on membrane surface 38 Evaluation of photocatalyst in batch reaction 39 Evaluation of suspended PMR 40 Evaluation of immobilized PMR .43 CONCLUSIONS .46 RECOMMENDATION 47 REFERENCES 48 ANNEX .51 TABLE OF FIGURES Figure Crystal structure of titanium dioxide phases of rutile, brookite and anatase (Janzeer, 2013) .12 Figure Mechanism of photocatalytic reaction (Xu, Rangaiah, & Zhao, 2014) 13 Figure Comparison between TiO2 and Au/TiO2 reaction .16 Figure The number of publications on the topic of PMR and PMR for water treatment (Zheng et al., 2015) 19 Figure Annual average BOD5 content in major rivers in Vietnam (2005-2009) 25 Figure Process of study experiment 28 Figure Diagram of Au/TiO2 synthesis process .30 Figure Spraying Au nanoparticles on membrane surface .32 Figure Schematic diagram of a lab-scale PMR system 33 Figure 10 Schematic diagram of (a) tangential (cross) flow filtration and (b) dead– end filtration (El–Safty & Hoa, 2012) 36 Figure 11 UV-VIS absorbance of Au/TiO2 photocatalyst .37 Figure 12 Performance of Photocatalyst in different concentration 40 Figure 13 Performance of different membrane MW at different amount of Au/TiO2 41 Figure 14 Performance during the reaction time .42 Figure 15 Performance of different filtration mode in continuous flow 43 TABLE OF TABLES Table Classification of PMRs configuration 19 Table Advantages and disadvantages of different configurations of PMR 21 Table Experiments description 26 Table ICP result of Au/TiO2 sample 38 Table Mass of Au/TiO2 coated in membrane surface 38 Table Solutions used to avoid photo catalysts peeling off the membrane 44 However, it is not allowing the principle of membrane operation as recommended by producer Besides, when testing it in PMR cell, the conversion of MB did not occur much by observation 45 CONCLUSIONS In summary, the research achieved following outputs: ▪ Synthesized Au/TiO2 with gold nanoparticles with amounting of 0.64 % (average weight) and size of 81.5 nm The Au/TiO2 catalyst demonstrated high performance of MB degradation under visible light illumination of 25%, 28%, 37%, 63% with the concentration of 0.2, 0.5, 1.25, 2.5 mg/mL respectively ▪ Regenerated Cellulose membrane was successfully coated by Au/TiO2 through Air-brushing coating method The result show that the amount of catalyst deposited on the membrane with perimeter of 24 mm is about 6.2 mg in average ▪ Two configurations of PMR were evaluated: - Before operating in PMR system, batch reaction was tested to verify the ability of Au/TiO2 in MB removal under VIS irradiation - Suspended system: Different molecular weight of regenerated cellulose membrane (10 KDa, 30 KDa, 100 KDa) were tested by system in continuous flow The best of membrane MW size, amount of photocatalyst, reaction time were determined at RC 30 KDa, 0.1 mg/mL (3mg), 120 minutes respectively with the highest efficiency of degradation of methylene blue is 50% - Immobilized system: The membrane of 30 KDa with Au/TiO2 coated was tested in dead-end and cross-flow mode with the MB removal performance of 63% and 57% respectively However, photocatalyst particles were peeled off membrane surface after a time of reaction causing impacts on its performance and catalyst-mixed retentate flow 46 RECOMMENDATION Given by the opportunities and difficulties during the 6-month research, further studies are recommended to improve and develop PMR system: ▪ The impacts of operation condition of PMR system such as: flow rate, pressure and larger range of contaminant concentration should be assessed ▪ For suspended PMR system, membrane fouling may occur, further studies are needed to address this problem ▪ For immobilized PMR system, photocatalyst peel off membrane problem need to be solved ▪ To use regenerated cellulose membrane, it is necessary to have more evaluation on impact of molecular weight of membrane, operation time, flow speed ▪ Coating method shows low effective then other method should be studied ▪ Other kind of membrane than regenerated cellulose can be tested to enhance the adhesion of catalyst on membrane surface ▪ Research on other solutions to reduce membrane failure to extend the system’s life ▪ Assessment of the PMR’s performance on other organic compounds 47 REFERENCES [1] Athanasekou, C P., Moustakas, N G., Morales-Torres, S., Pastrana-Martínez, L M., Figueiredo, J L., Faria, J L., Falaras, P (2015) Ceramic photocatalytic membranes for water filtration under UV and visible light Applied Catalysis B: Environmental, 178 [2] Athanasiou, D A., Romanos, G E., & Falaras, P (2016a) Design and optimization of a photocatalytic reactor for water purification combining optical fiber and membrane technologies Chemical Engineering Journal, 305, 92–103 [3] Athanasiou, D A., Romanos, G E., & Falaras, P (2016b) Design and optimization of a photocatalytic reactor for water purification combining optical fiber and membrane technologies Chemical Engineering Journal [4] Behera, S., Ghanty, S., Ahmad, F., Santra, S., & Banerjee, S (2012) J Anal Bioanal Techniques International Journal of Electrochemical Science [5] Binh, N A (2018) Nghiên cứu chế tạo & ứng dụng vật liệu quang xúc tác TiO2 xử lý Cr(VI) điều kiện ánh sáng khả kiến Hanoi University of Science and Technology [6] Chakraborty, S., Loutatidou, S., Palmisano, G., Kujawa, J., Mavukkandy, M O., Al-Gharabli, S., Arafat, H A (2017) Photocatalytic hollow fiber membranes for the degradation of pharmaceutical compounds in wastewater Journal of Environmental Chemical Engineering, 5(5) [7] Depcik, C., Loya, S., Srinivasan, A., Wentworth, T., & Stagg-Williams, S (2013) Catalysts-03-00517.Pdf Catalysts, 3, 517–542 [8] El–Safty, S A., & Hoa, N D (2012) Noble Metals [9] Gutkowski, R., Schafer, D., Nagaiah, T C., Heras, J E Y., Busser, W., Muhler, M., & Schuhmann, W (2014) Efficient Deposition of Semiconductor Powders for Photoelectrocatalysis by Airbrush Spraying Electroanalysis, 26, 1–9 [10] Haiss, W., Thanh, N T K., Aveyard, J., & Fernig, D G (2007) Determination of Size and Concentration of Gold Nanoparticles from UV-Vis Spectra Analytical Chemistry, 79 [11] Hollmann, D., Rockstroh, N., Grabow, K., Bentrup, U., Rabeah, J., Polyakov, M., Brückner, A (2017) From the Precursor to the Active State: Monitoring Metamorphosis of Electrocatalysts During Water Oxidation by In Situ Spectroscopy Chem Electro Chem, 4(8), 2117–2122 48 [12] Ibhadon, A., & Fitzpatrick, P (2013) Heterogeneous Photocatalysis: Recent Advances and Applications Catalysts, 3(1), 189–218 [13] Kaneda, K., Yamaguchi, K., Mori, K., Mizugaki, T., & Ebitani, K (2000) Catalyst design of hydrotalcite compounds for efficient oxidations Catal Surv Jpn [14] Molinari, R., Lavorato, C., & Argurio, P (2017) Recent progress of photocatalytic membrane reactors in water treatment and in synthesis of organic compounds A review Catalysis Today [15] Mozia, S., Szymański, K., Michalkiewicz, B., Tryba, B., Toyoda, M., & Morawski, A W (2015) Effect of process parameters on fouling and stability of MF/UF TiO2 membranes in a photocatalytic membrane reactor Separation and Purification Technology, 142 [16] Nair, A K., & Jagadeesh, J B (2017) TiO2 nanosheet-graphene oxide based photocatalytic hierarchical membrane for water purification Surface and Coatings Technology, 320 [17] Nakata, K., & Fujishima, A (2012) Reviews TiO photocatalysis : Design and applications Journal of Photochemistry and Photobiology C: Photochemistry Reviews [18] Nur Hanis Hayati Hairom, Mohammad, A W., Ng, L Y., & Kadhum, A A H (2013) Utilization of Self-synthesized Zinc Oxide Nanoparticles in MPR for Industrial Dye Wastewater Treatment using NF and UF Membrane International Conference on the Challenges in Environmental Science and Engineering [19] Priebe, J B., Radnik, J., Lennox, A J J., Pohl, M M., Karnahl, M., Hollmann, D (2015) Solar Hydrogen Production by Plasmonic Au-TiO Catalysts: Impact of Synthesis Protocol and TiO2 Phase on Charge Transfer Efficiency and H2 Evolution Rates ACS Catalysis, 5(4), 2137–2148 [20] Saravanan, R., Gracia, F., & Stephen, A (2017) Basic Principles, Mechanism, and Challenges of Photocatalysis In M.M Khan et al (Ed.), Nanocomposites for Visible Light-induced Photocatalysis, (pp 19–40) Springer International Publishing AG [21] Syafei, A D., Lin, C F., & Wu, C H (2008) Removal of natural organic matter by ultrafiltration with TiO2-coated membrane under UV irradiation Journal of Colloid and Interface Science [22] Umar, M., & Aziz, H A (2013) Photocatalytic Degradation of Organic Pollutants in Water In Organic Pollutants - Monitoring, Risk and Treatment fecting (pp 195–208) 49 [23] Wang (2000) Transmission electron microscopy of shapecontrolled nanocrystals and their assemblies J Phys Chem B., 104, 1153–1175 [24] Trang, Q T., Trúc, T T M., Doanh, S C., & Viễn, V (2016) Tổng hợp tính chất xúc tác quang vật liệu [25] Xu, C., Rangaiah, G P., & Zhao, X S (2014) Photocatalytic degradation of MB by TiO2.pdf Industrial & Engineering Chemistry Research, 53 [26] Yu, Y., Wen, W., Qian, X Y., Liu, J Bin, & Wu, J M (2017) UV and visible light photocatalytic activity of Au/TiO2 nanoforests with Anatase/Rutile phase junctions and controlled Au locations Scientific Reports 50 ANNEX Figure A1 PMR cell 51 Figure A2 Design of PMR cell in Auto-cad drawing 52 Figure A3 Whole PMR system in laboratory Figure A4 Au/TiO2 after synthesis 53 Figure A5 ICP result of Au/TiO2 photocatalyst 54 Figure A6 Coated regenerated cellulose membrane 55 1.2 y = 0.1667x - 0.0182 R² = 0.9987 UV VIS Absorbance 0.8 0.6 0.4 0.2 0 -0.2 Concentration of MB Figure A7 Standard line of MB 6ppm solution 56 Table A1 Data of experiment in batch reaction (Section 3, Chapter 3) Catalyst Conc of catalyst None VIS UV-VIS mg/mL ABS Conc Removal rate (%) 2.5 0.35 4.42 35 0.29 3.78 44 0.0097 0.33 95 1.25 0.45 5.66 16 0.41 5.18 23 0.0172 0.42 94 0.5 0.49 6.09 10 0.46 5.74 15 0.0299 0.58 91 0.2 0.50 6.22 0.48 5.98 12 0.0144 0.39 94 2.5 0.24 3.10 54 0.19 2.48 63 0.0184 0.44 94 1.25 0.39 4.87 28 0.34 4.28 37 0.0034 0.26 96 0.34 95 0.25 96 TiO2 Au/TiO2 ABS Conc Removal rate (%) ABS Conc Removal rate (%) 0.5 0.47 5.82 14 0.39 4.88 28 0.01 0.2 0.51 6.30 0.41 5.09 25 0.0023 Table A2 Data of performance of different membrane MW at different amount of Au/TiO2 (Section 4, Chapter 3) Membrane RC 10 KDa RC 30 KDa RC 100 KDa Concentration of PC (mg/mL) 0.03 0.07 0.1 0.13 4 ABS 0.3454 0.3303 0.3042 0.2914 0.2084 0.2227 0.2019 0.1845 0.1767 0.1568 0.5387 0.5369 0.51 0.5056 0.4905 Concentration of MB (ppm) 4.362328 4.181164 3.868026 3.714457 2.718656 2.890222 2.640672 2.431914 2.338332 2.09958 6.681464 6.659868 6.337133 6.284343 6.103179 Removal rate (%) 39 41 46 48 62 59 63 66 67 71 11 12 14 57 Table A3 Data of methylene (MB) removal performance during the reaction time (Section 4, Chapter 3) 30RC VIS 3mg 500-700/min Naked 30RC VIS Time (min) ABS 30 60 90 120 150 180 0.4168 0.425 0.4361 0.4125 0.3845 0.4582 210 0.4891 240 0.495 30RC VIS 3mg 700-1000/min Conc.of Removal Conc.of Removal ABS MB rate (%) MB rate (%) 5.22 28 0.4005 5.02 31 5.32 27 0.4073 5.10 30 5.45 25 0.4102 5.14 29 5.17 29 0.3462 4.37 40 4.83 34 0.3589 4.52 38 5.72 21 0.3682 4.64 36 6.09 16 0.3988 5.00 31 6.16 15 0.4192 5.25 28 ABS 0.3605 0.3631 0.3376 0.2846 0.2988 0.3245 0.3387 0.3806 Conc.of Removal MB rate (%) 4.54 38 4.57 37 4.27 41 3.63 50 3.80 48 4.11 43 4.28 41 4.78 34 Table A4 Data of methylene (MB) removal performance in different filtration mode in continuous flow (Section 5, Chapter 3) Time (min) 30 60 90 120 30RC 7mg on membrane VIS- dead end 30RC 7mg on membrane VIS- cross flow ABS Conc.of MB Removal rate (%) ABS Conc.of MB Removal rate (%) 0.2461 0.2298 0.2373 0.2422 3.17 2.98 3.07 3.12 56 59 58 57 0.2489 0.2172 0.2108 0.2044 3.20 2.82 2.75 2.67 56 61 62 63 58 Figure A8 Author in University of Rostock 59 ... running the PMR with selected catalysts and irradiation in continuous mode to research the performance of the system in near-real operation condition In this mode, the two kinds of design of the. .. possess the property of storing electrons in a quantized fashion (Ismail & Institut, 2009) Photocatalytic membrane reactor 2.1 Definition In field of water treatment, hybrid processes combining membrane. .. Evaluation of the system in removal of organic matter from feed water In this step, the performance of catalysts for photo-reaction and PMR system is evaluated basing on the change of concentration of