The distribution and speciation of heavy metal in the agricultural contamination site by tessier method

THAI NGUYEN UNIVERSITY UNIVERSITY OF AGRICULTURE AND FORESTRY (Logo university) THAN THI NHU ANH The Distribution and Speciation of Heavy Metal in the Agricultural Contamination Site by Tessier Method BACHELOR THESIS Study Mode: Full-time Major: Environmental Science and Management Faculty: Departement Environment and Soil Science Batch: 2013-2017 Thai Nguyen, ……… i Thai Nguyen University of Agriculture and Forestry Degree Program Environmental Science and Management Student name Than Thi Nhu Anh Student ID DTN1353110012 Thesis Title The Distribution and Speciation of Heavy Metal in the Agricultural Contamination Site by Tessier Method Supervisor(s) Prof Dr Yao-Tung Lin - National Chung Hsing University, Taiwan Assoc Prof Dr Nguyen The Hung- Thai Nguyen University of Agriculture and Forestry, Vietnam Abstract: (…) Keywords Heavy Metal, Number of pages Date of submission 30th August, 2016 Supervisor’s signature ii ACKNOWLEAGEMENT Firstly, I would like to say thanks to the cooperation between Thai Nguyen University of Agriculture and Forestry and National Chung Hsing University for providing me an amazing opportunity to internship in Taiwan It brings me great pleasure to work and submit my thesis for graduation I would like to express my profound gratitude to Prof Dr Yao- Tung Lin, the facilitator, facilitator, suggestion and critic of the building that contributed greatly to the development of my ideas throughout the project and teach me about the synthesis of new knowledge about soil science and many other techniques and methods Used in the field of the environment Without their help and devotion, I will not be able to achieve this stage without your guidance, I may not have this thesis I sincerely thanks to Assoc Prof Dr Nguyen The Hung for her advices, assistance, sharing experiences before and after I went to Taiwan, helping me to understand and complete proposal and thesis I am also thankful to (Your name ) and my friends in lab … They have been very helpful in providing me with constructive feedback and suggestions on my project and helping me to successfully complete some of my experiments and reports iii I also thank to my family for providing me emotional, unceasing encouragement and physical and financial support At last, I would like to thank all those other persons who helped me in completing this report Because of my lack knowledge, the mistake is inevitable, I am very grateful if I receive the comments and opinions from teachers and others to contribute my report Sincerely, Thân Thị Như Anh iv TABLE OF CONTENT LIST OF FIGURES LIST OF TABLES LIST OF ABBREVIATIONS PART I INTRODUCTION 1.1 Research rationale: 1.2 Research questions 1.3 Limitations 10 PART II LITERATURE REVIEW 11 2.1 Heavy metals speciation in the soil 11 2.2 The source of heavy metals in the soil environment: 12 2.1.1 :Industrial production 12 2.1.2 Agricultural suction 13 2.1.3 Urban waste 13 2.3 The impact of heavy metal to plant and human health 15 2.3.1 Zinc toxicity 15 2.3.2 Copper toxicity 15 2.3.3 Nikel toxicity 16 2.3.4 Chromium toxicity 17 2.4 Heavy metals toxicity 18 2.5 The metal speciation offected by environmental conditions: 22 2.5.1 Sequential extraction process: 23 2.6 The term definition of speciation 24 v PART III MATERIALS AND METHODS 26 3.1 Chemical and instruments 26 3.1.1 Chemical materials 26 3.1.2 Intrusment 27 3.1.3 Reagent 28 3.2 Soil and sediment collection 28 3.2.1 Sample pretreatment 29 3.2.2 Metal speciation using Tessier et al (1979) scheme 26 3.2.3 Quality control 27 PART IV RESULTS 4.1 Quality control 27 4.2 Heavy metal speciation 28 4.3 Heavy metal distribution 28 4.4 Conclusion 29 4.5 Acknowledgments 26 PART V DISCUSSION AND CONCLUSION Error! 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Bookmark not defined vi LIST OF FIGURES ( I'll bonus later) LIST OF TABLES (I’ll bonus later) LIST OF ABBREVIATIONS AAS: Atomic absorption spectrophotometer PART I INTRODUCTION 1.1 Research rationale: Economic and social development have produced many benefits – raising standards of living and improving quality of life across the world – it has also resulted in the depletion of natural resources, the degradation of ecosystems and environmental issues Environmental pollution is a controversial issue not only in Vietnam but also in the world Soil is an important part of the environment, an invaluable resource naturally given to human Soils is a special production material that is unique in labor, a constituent element of the Earth's ecosystem Due to the rapidly growing population also development of the industry, urbanization, employment and transport It is the main reason makes the land resource is heavily exploited and environmental degradation is becoming more and more serious As such, depending on the way people treat the land, the soil can develop in a good way as well as can develop in a bad way Therefore, protecting the soil environment and maintaining the long-term productivity of the soil is one of the key strategies in the sustainable use of natural resources The contamination of sediments, soils, and biota by heavy metals are of major concern, especially in many industrialized countries, because of their toxicity, persistence and bio-accumulative nature Sediment samples have been found to be carriers of most metals and some elements may be recycled through biological and chemical reactions within the water column Metals and metalloids accumulated in sediments, sludge and soils may therefore pose an environmental problem concerning possible metal transfer from these samples to the aquatic medium, and thereby including them in the food chain The total metal content in polluted environmental samples is a poor indicator of bioavailability, mobility or toxicity; these properties basically depend on the different chemical forms of binding between trace metals and solid phases of the samples Different metal extraction methods for environmental samples have been extensively studied in many countries Metal ions in sediments are partitioned between the different phases, i.e., organic matter, oxyhydroxides of iron, aluminum and manganese, phyllosilicate minerals, carbonates and sulphides In addition, metal ions are retained in these solid phases by different mechanisms (ion exchange, outer- and inner-sphere surface complexation (adsorption), precipitation or co-precipitation) Although the separation of various chemical forms of heavy metals is very difficult, the use of sequential extraction method proves to be an important and effective approach Trace element speciation in soils is often accomplished by a variety of different empirical single as well as sequential extractions These extraction tests are commonly used to study the mobility of metals in soils and sediments by mimicking different environmental conditions or dramatic changes on them A variety of leaching techniques are used to emulate differing environmental conditions, with strong acids being used to determine total abundances of potentially harmful elements, and weaker solutions to determine compounds that are relatively soluble and bioavailable Numerous selective extraction schemes have been used for discriminating individual geochemical phases, ranging from simplistic methods for differentiating “labile” and “residual” fractions Single leaching and combined sequential extraction schemes have been developed to estimate the relative phase associations of sedimentary metals in various aquatic environments The most widely utilized protocol is the Tessier et al (1979) procedure However, many schemes were developed base on the concept of Tessier et al (1979) method Therefore, this research was followed Tessier method for estimate the heavy metal speciation and distribution in soil and sediment 1.2 Research’s objectives 1) To investigate the total concentration and species distribution of heavy metal (i.e Cr, Cu, Zn and Ni) in contaminated soil and sediment in irrigation channels 2) To determine the heavy metal speciation distribution in contaminated soil and sediment in irrigation channels 1.2 Research questions 1) How to know the heavy metal speciation that affected by environmental conditions 2) What is the main speciation of heavy metal in the soil and sediment 3) What is the heavy metal concentration in the soil and sediment 4) How to assess the heavy metal contaminate in soil and sediment 1.3 Limitations The author got the good experience for exchange student to department of Soil and Environmental science, National Chung Hsing University, Taiwan Therefore, all of the research schedule, method, results and discussion were followed from the experiments that have been done in Taiwan The limitation of the studied were: 1) The period for exchange student was shot time (6 months) Because the author need to lean ever thing for research such as how to collected the soil and sediment sample, 10 PART IV: RESULTS: 4.1 Quality control The detection limit (DL) of Ni, Cr, Cu, and Zn were shown in Table The exchangeable fraction, the detection limit of Ni, Cr, Cu, and Zn were 0.1, 0.1, 0.1 and 0.01 mg L-1 respectively The carbonate fraction noted Ni, Cr, Cu, and Zn lower than obtained by exchangeable fraction The DL in carbonate fraction was 0.01, 0.01, 0.05, and 0.01 mg L-1 in Ni, Cr, Cu, and Zn respectively In the Fe and Mn oxides speciation, the DL was 0.07, 0.10, 0.01, and 0.01 mg L-1 in Ni, Cr, Cu, and Zn respectively While Ni, Cr, Cu, and Zn were note 0.01, 0.03, 0.01, and 0.01 mg L-1 in organic matter fraction For the residual the DL was 0.01, 0.03, 0.01, and 0.01 mg L-1 in Ni, Cr, Cu, and Zn respectively (Table 5) Table The detection limit (DL) (mg L-1) of each element 36 4.2 Heavy metal speciation Heavy speciation concentration patterns following Tessier et al (1979) are illustrated in Figure Soil were high contained of Ni concentration higher than the soil monitoring standard values While, some sample area (CPS01, CPSO3, and TPSO3) in the top soil (0-15 cm) were higher than soil control standard value This indicated that the soil sample areas (CPS01, CPSO3, and TPSO3) were high toxicity of those elements Moreover in Taiwan, the government suggested that if the area higher than the control standard values, this area can not be used this areas for agriculture The concentration of Cr showed 116.27, 148.35, 128.82, 88.44, 20.71, and 146.67 mg kg-1 in top soil (0-15 cm) of CPS01, CPS02, CPS03, TPS01, TPS02, and TPS03 While in sun soil (15-30 cm) showed 77.32, 95.83, 112.61, 131.01, 11.27, and 143.53 mg kg-1 Table 6: The concentration of Cd, Ni, Cu, and Zn in contaminated soil Sample Name Cd (mg/kg) Ni (mg/kg) Cu (mg/kg) Zn (mg/kg) 37 CPS01(S) 116.27 226.84 92.13 295.14 CPS01(B) 77.32 191.36 41.86 129.15 CPS02(S) 148.35 173.72 61.71 240.06 CPS02(B) 95.83 71.57 50.82 133.94 CPS03(S) 128.82 222.03 92.26 295.43 CPS03(B) 112.61 143.78 55.18 167.89 TPS01(S) 88.44 131.04 32.49 124.61 TPS01(B) 131.01 148.23 67.68 172.26 TPS02(S) 20.71 54.27 12.36 48.73 TPS02(B) 11.27 49.83 10.49 37.57 TPS03(S) 146.67 268.56 83.84 351.24 TPS03(B) 143.53 170.56 60.92 122.14 Soil Note: S = top soil (0-15 cm B = sub soil (15-30 cm) Most of the heavy metal concentration, the highest Ni value was obtained from the Fe and Mn oxides fraction Residual Ni represented 4-19% of total Ni, while < ND to 3.3% was associated with OM, Fe and Mn oxides (74 - 90%), carbonate (< detection limit to 10.2%) and lower than detection limit in exchangeable fraction (Table 7) The catbonate Ni fractions were high in top soil than subsoil The amount of Ni associated with the exchangeable fraction was below the detection limit of the instrument Table 7: The distribution of Ni in contaminated soil Exchangeable Sample Soil Carbonate Fe Mn OM Name CPS01(S) Residual (%) (%) (%) oxide (%) (%) ND 3.24 74.51 2.83 19.41 38 CPS01(B) ND 3.99 77.60 1.99 16.42 CPS02(S) ND 4.00 77.47 3.30 15.23 CPS02(B) ND 3.85 81.14 0.84 14.16 CPS03(S) ND 2.55 83.19 3.00 11.26 CPS03(B) ND 1.75 85.68 0.59 11.95 TPS01(S) ND 7.18 80.09 0.80 11.93 TPS01(B) ND 10.26 76.83 0.84 12.09 TPS02(S) ND 4.14 90.97 1.80 4.63 TPS02(B) ND 3.18 91.11 0.75 4.95 TPS03(S) ND 1.53 84.14 ND 14.33 TPS03(B) ND ND 90.11 ND 9.89 Note: S = top soil (0-15 cm B = sub soil (15-30 cm) ND = Not detectable; lower than detection limit Most of the heavy metal concentration, the highest Zn value was obtained from the Fe and Mn oxides fraction Residual Zn represented 9-35% of total Zn, while to 7% was associated with OM, Fe and Mn oxides (54 - 60%), carbonate (4 to 24%) and lower than detection limit in exchangeable fraction (Table 8) The carbonate Zn fractions were high in top soil than subsoil The amount of Zn associated with the exchangeable fraction was below the detection limit of the instrument Table 8: The distribution of Zn in contaminated soil Fe Mn Exchanageble Sample Carbonate Name OM Residual (%) (%) oxide (%) (%) (%) 39 CPS01(S) ND 16.03 59.22 6.82 17.93 CPS01(B) ND 11.01 60.65 6.97 21.37 CPS02(S) ND 17.91 60.84 5.17 15.57 CPS02(B) ND 24.01 55.25 7.73 20.40 CPS03(S) ND 4.84 54.45 5.53 35.18 CPS03(B) ND 3.61 58.49 6.10 31.80 TPS01(S) ND 15.83 57.64 5.78 20.75 TPS01(B) ND 10.66 66.56 6.12 16.66 TPS02(S) ND 13.56 64.13 7.00 15.31 TPS02(B) ND 6.22 65.43 6.05 22.30 TPS03(S) ND 24.00 60.90 5.95 9.10 TPS03(B) ND 18.73 56.00 5.65 19.62 Soil Note: S = top soil (0-15 cm B = sub soil (15-30 cm) ND = Not detectable; lower than detection limit Most of the heavy metal concentration, the highest Cu value was obtained from the organic matter fraction Residual Cu represented 18 to 50% of total Cu, while 24 to 55% was associated with Fe and Mn oxides, carbonate (2 - 10%), and exchangeable (< detection limit to 3%) (Table 9) The carbonate Cu fractions were high in top soil than subsoil 40 Table The distribution of Cu in contaminated soil Fe Mn Residual Exchangeble Sample Name Carbonate(%) oxide OM (%) (%) (%) (%) CPS01(S) 1.14 7.91 27.47 40.97% 22.52 CPS01(B) 1.72 3.48 27.07 44.56 23.17 CPS02(S) 0.48 8.68 32.32 37.06 21.47 CPS02(B) 1.55 7.13 48.94 15.67 26.71 CPS03(S) 0.88 10.18 39.57 27.74 21.64 CPS03(B) 1.28 7.88 55.61 18.86 16.36 TPS01(S) 3.03 4.18 28.19 36.81 27.82 TPS01(B) 0.38 6.51 35.05 36.04 22.01 TPS02(S) 1.38 5.15 24.48 50.97 18.02 TPS02(B) 2.14 6.55 29.77 37.73 23.83 TPS03(S) ND 2.16 39.66 6.95 51.25 TPS03(B) 2.26 3.21 52.25 7.26 36.09 Soil Note: S = top soil (0-15 cm B = sub soil (15-30 cm) ND = Not detectable; lower than detection limit Most of the heavy metal concentration, the highest Cr value was obtained from the Fe and Mn oxides fraction Residual Cr represented 21-58% of total Cr, while to 19 % was associated with OM, carbonate (< detection limit to 1.85%) and lower than detection limit in exchangeable fraction (Table 10) The carbonate Cr fractions were high in top 41 soil than subsoil The amount of Cr associated with the exchangeable fraction was below the detection limit of the instrument Table 10: The distribution of Cr in contaminated soil Fe Mn Exchangeable Sample Carbonate Name OM Residual (%) (%) oxide (%) (%) (%) CPS01(S) ND 1.55 49.76 19.79 28.89 CPS01(B) ND 1.85 55.29 17.30 25.55 CPS02(S) ND 1.17 58.42 18.61 21.79 CPS02(B) ND 1.26 54.02 12.74 31.98 CPS03(S) ND 0.71 60.60 16.29 22.40 CPS03(B) ND 1.00 65.58 13.61 19.81 TPS01(S) ND 2.43 59.15 15.30 23.13 TPS01(B) ND 2.14 46.19 19.74 31.93 TPS02(S) ND 1.85 55.29 17.30 25.55 TPS02(B) ND 1.86 59.02 23.40 23.58 TPS03(S) ND 0.75 42.33 4.52 52.65 TPS03(B) ND ND 39.80 1.53 58.67 Soil Note: S = top soil (0-15 cm B = sub soil (15-30 cm) ND = Not detectable; lower than detection limit Ni, Cr and Cu concentrations in exchangeable, organically bounded, carbonate bounded, adsorbed species on Fe and Mn oxides and residual species (except silicates) in soil fractions after five step sequential extraction were given in Table 7–10 with their standard deviations The relative amounts of each metals in each fractions, expressed as a 42 percentage of the cumulative total extracted from the soil samples were presented in Table 7-10 Ascending order of metals was summarized as follow From Table 7-10, Ni in soil fractions was high content in residual > Fe and Mn oxide > carbonate > organic matter > exchangeable fraction While, Zn speciation in soil was high in Fe and Mn oxide > residual > organic matter > carbonate > exchangeable fraction For Cu speciation was high content in organic matter > residual > Fe and Mn oxides > carbonate > exchangeable fraction In the case of Cr speciation, Cr speciation was high content in organic matter > residual > Fe and Mn oxide > exchangeable and carbonate fraction Figure 10: The total concentration in Ni, Cu, Zn, and Cr (mg kg-1) in soil samples Ni, Cr and Cu concentrations in exchangeable, organically bounded, carbonate bounded, adsorbed species on Fe and Mn oxides and residual species (except silicates) in 43 sediment fractions after five step sequential extraction were given in Figure with their standard deviations The relative amounts of each metals in each fractions, expressed as a percentage of the cumulative total extracted from the soil samples were presented in Figure Ascending order of metals was summarized as follow From Figure 8, Ni in soil fractions was high content in residual > Fe and Mn oxide > carbonate > organic matter > exchangeable fraction While, Zn speciation in soil was high in Fe and Mn oxide > residual > organic matter > carbonate > exchangeable fraction For Cu speciation was high content in organic matter > residual > Fe and Mn oxides > carbonate > exchangeable fraction In the case of Cr speciation, Cr speciation was high content in organic matter > residual > Fe and Mn oxide > exchangeable and carbonate fraction Figure 11:The total concentration in Ni, Cu, Zn, and Cr (mg kg-1) in sediment samples 44 4.3: Heavy metal distribution Most of the heavy metal concentration, the highest Ni value was obtained from the Fe and Mn oxides fraction (Figure 9) Residual Ni represented 4-90% of total Ni, while ND - 3.3% was associated with OM (0.21 - 0.78%), Fe and Mn oxides (0.36 - 0.60%), carbonate (< detection limit to 0.20%) and exchangeable K (0.36 - 1.08%) (Figure 11) Cu was obtained from the Fe and Mn oxides fraction (Figure 9) Residual Ni represented 4-90% of total Ni, while ND - 3.3% was associated with OM (0.21 - 0.78%), Fe and Mn oxides (0.36 - 0.60%), carbonate (< detection limit to 0.20%) and exchangeable K (0.36 1.08%) (Figure 11) Zn was obtained from the Fe and Mn oxides fraction (Figure 9) Residual Ni represented 4-90% of total Ni, while ND - 3.3% was associated with OM (0.21 - 0.78%), Fe and Mn oxides (0.36 - 0.60%), carbonate (< detection limit to 0.20%) and exchangeable K (0.36 - 1.08%) (Figure 11) Cr was obtained from the Fe and Mn oxides fraction (Figure 9) Residual Ni represented 4-90% of total Ni, while ND - 3.3% was associated with OM (0.21 - 0.78%), Fe and Mn oxides (0.36 - 0.60%), carbonate (< detection limit to 0.20%) and exchangeable K (0.36 - 1.08%) (Figure 11) 45 Figure 12: The distribution of Ni, Cu, Zn and Cr in soil Ni, Cr and Cu concentrations in exchangeable, organically bounded, carbonate bounded, adsorbed species on Fe and Mn oxides and residual species (except silicates) in soil fractions after five step sequential extraction were given in Figure 11 with their standard deviations The relative amounts of each metals in each fractions, expressed as a percentage of the cumulative total extracted from the sediment samples were presented in Figure 11 Ascending order of metals was summarized as follow From Tab 3, Ni in sediment fractions was high content in Fe and Mn oxide > organic matter > exchangeable 46 > residual > carbonate fraction While, Zn speciation in soil was high in Fe and Mn oxide > organic matter > residual > carbonate > exchangeable fraction For Cu speciation was high content in organic matter > residual > Fe and Mn oxides > carbonate > exchangeable fraction In the case of Cr speciation, Cr speciation was high content in residual > Fe and Mn oxide > organic matter > exchangeable or carbonate fraction PART V: DISCUSSION AND CONCLUSION 5.1: Discussion: 5.2: Conclusion Tessier et al (1979) scheme was high advantage to divide the heavy metal speciation that affected by environmental conditions The results showed that the speciation of Ni, Cr, Zn, and Cu in soil were higher than sediment and top soil showed high concentration than sub-soil Some areas were high concentration of Ni and Cr than soil monitoring and soil control standards The percentage distribution of Ni, Zn, Cu, and Cr were difference in residual, organic mater, Fe Mn oxide, carbonate and exchangeable fraction 5.3: Acknowledgments: Environmental Nano material (ENM) lan, National Chung Hsing University, Taiwan 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(2017) Occurrence, speciation and transportation of heavy metals in coastal rivers from watershed of Laizhou Bay, China Chemosphere 173:61-68 50 ... environment and maintaining the long-term productivity of the soil is one of the key strategies in the sustainable use of natural resources The contamination of sediments, soils, and biota by heavy metals... is the main speciation of heavy metal in the soil and sediment 3) What is the heavy metal concentration in the soil and sediment 4) How to assess the heavy metal contaminate in soil and sediment... survive in areas with too much heavy metal content Heavy metals accumulated in the soil into agricultural products, food and heavy metal food chains in the soil will accumulate in plants and in the