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Chemical Remediation of Copper-Contaminated Soils Using Calcium Water Treatment Residue

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Chemical Remediation of Copper-Contaminated Soils Using Calcium Water Treatment Residue CHEMICAL REMEDIATION OF COPPER-CONTAMINATED SOILS USING CALCIUM WATER TREATMENT RESIDUE By JINGHUA FAN A DISSERTATION PRESENTED TO THE GRADUATE SCHOOL OF THE UNIVERSITY OF FLORIDA IN PARTIAL FULFILLMENT OF THE REQUIREMENTS FOR THE DEGREE OF DOCTOR OF PHILOSOPHY UNIVERSITY OF FLORIDA 2010 1 © 2010 Jinghua Fan 2 To my parents, Guangyi Fan and Shuyu Lin 3 ACKNOWLEDGMENTS First of all, I would like to thank my advisor, Dr. Zhenli He, for his expert guidance and support. Not only was he readily available for me providing comprehensive instructions in the lab, but he always read and responded to the drafts of my work in time and with patience. He reviewed my multiple versions of this dissertation, and helped me to improve my presentation and clarify my writing. His comments are always perceptive and helpful, without which this dissertation would not have been finished. My thanks go out to my co-advisor, Dr. Lena Q. Ma and colleges from the Biogeochemistry of Trace Metals group for the hospitality and support I had received during my first two semesters of course studies in Gainesville. I had benefited a lot from Dr. Ma’s insightful and pertinent suggestions for my research, especially in writing manuscripts. I would also like to give my sincere thanks to Drs. Peter J. Stoffella, Patrick C. Wilson and Maria L. Silveira for serving on my advisory committee. I am grateful for their advice, assistance and encouragement in every step towards my PhD degree. I deeply express my appreciation to my colleges in Soil and Water Science Laboratory: Drs. Xiaoe Yang, Yuangen Yang, Wenrong Chen, Zhanbei Liang, Yangbo Wang, Yunlong Liu, Xuxia Zhou, Shengke Tian, PhD students Qin Lu, Bruno Pereira, Thiago Nogueira, Santanu Bakshi, Alex Merlin, Eloise Mello, Mr. Brian Cain, Mr. Douglas J. Banks, Ms. Shaoqin Lu, and Mr. Diangao Zhang for providing useful academic and social assistance. We studied and relaxed together. Without their help and friendship, the successful completion of my PhD study would be impossible. I have always felt fortunate to be part of Dr. He’s group where I have learned, enjoyed and benefited from team work. 4 I also appreciate the people on the faculty and staff at Indian River Research Center of University of Florida for providing me wonderful environment for both studying and living for three years. Everyone from the center is so kind to me that I feel at home in the center. I am particularly thankful to Dr. Peter J. Stoffella, Ms. Laura McKeon, and Ms. Velma Spencer for their timely and efficient assistance and arrangement in the student dorm. I am also grateful to Ms. Jackie White for her help with my English language practice. It is lucky for me to have Dr. Juanjuan Qu as a roommate for one year, who taught me not only cooking but also the way to balance the research and family. Last but not least, I would like to thank my dearest parents for their parts in making me who I am today. They will always love me and be my source of strength. My enormous debt of gratitude can hardly be repaid to them for their unconditional support. 5 TABLE OF CONTENTS page ACKNOWLEDGMENTS.................................................................................................. 4 LIST OF TABLES............................................................................................................ 8 LIST OF FIGURES.......................................................................................................... 9 CHAPTER ABSTRACT ................................................................................................................... 10 1 LITERATURE REVIEW........................................................................................... 13 Copper Application in Agriculture............................................................................ 13 Copper Concentrations and Distributions in Lithosphere and Soils ........................ 14 Copper Speciation and Behavior in Soils................................................................ 15 Potential Impact on Soil Quality and Crop Production ............................................ 19 Cu Release from Soil and Transport from Land to Aqueous Environment.............. 21 Remediation of Cu-contaminated Soils................................................................... 23 Conclusions and Perspectives................................................................................ 27 2 ACCUMULATION AND AVAILABILITY OF COPPER IN CITRUS-GROVE SOILS AS AFFECTED BY FUNGICIDE APPLICATION......................................... 30 Introduction ............................................................................................................. 30 Materials and Methods............................................................................................ 31 Soil Collection and Characterization................................................................. 31 Soil Cu Analysis and Fractionation................................................................... 31 Data Analysis ................................................................................................... 33 Results and Discussion........................................................................................... 33 Copper Accumulation in Relation to Citrus Planting History............................. 33 Effects of pH on Downward Movement of Copper in Soils ............................... 34 Copper Availability as Affected by Cu Accumulation and Soil pH..................... 35 Soil Cu Fractionation and Availability ............................................................... 37 Conclusions ............................................................................................................ 39 3 IMMOBILIZATION OF CU IN CONTAMINATED SANDY SOILS USING CALCIUM-WATER TREATMENT RESIDUE.......................................................... 45 Introduction ............................................................................................................. 45 Materials and Methods............................................................................................ 46 Sampling and Characterization ........................................................................ 46 Incubation Study............................................................................................... 47 Column Leaching Study ................................................................................... 48 Statistical Analysis............................................................................................ 49 6 Results and Discussion........................................................................................... 49 Addition of Ca-WTR Increased Soil pH and Decreased Extractable Cu........... 49 Addition of Ca-WTR Converted Labile Cu to More Stable Cu Forms............... 51 Addition of Ca-WTR Reduced Leachable Cu in Soil Columns ......................... 52 Conclusions ............................................................................................................ 55 4 AMENDMENT OF CALCIUM WATER TREATMENT RESIDUE (CA-WTR) REDUCES CU BIOAVAILABILITY IN CU-CONTAMINATED SOILS...................... 65 Introduction ............................................................................................................. 65 Materials and Methods............................................................................................ 67 Soil Samples and Ca-WTR Collection.............................................................. 67 Greenhouse Experiments................................................................................. 67 Chemical Analyses of Soil and Plant Samples................................................. 68 Statistical Analysis............................................................................................ 69 Results and Discussion........................................................................................... 69 Effects of Ca-WTR Amendment on Soil pH and Extractable Cu ...................... 69 Effects of Ca-WTR Amendment on Plant Cu Concentration ............................ 71 Effects of Ca-WTR Amendment on Plant Growth/Dry Matter Yields and Cu Uptake........................................................................................................... 73 Effects of Ca-WTR Amendment on Uptake of Other Nutrients......................... 75 Conclusion .............................................................................................................. 76 5 AMENDMENT OF CALCIUM-WATER TREATMENT RESIDUE (CA-WTR) ON CITRUS GROWTH AND COPPER LOADING IN SURFACE RUNOFF IN SOUTH FLORIDA................................................................................................... 82 Introduction ............................................................................................................. 82 Materials and Methods............................................................................................ 83 Site Description and Amendment Characterization .......................................... 83 Sample Collection and Analysis ....................................................................... 84 Results and Discussion........................................................................................... 87 Soil Quality Characterization and Monitoring.................................................... 87 Water Quality and Cu Speciation ..................................................................... 88 Fruit Nutrient Contents and
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