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Studies of Mixture Effects of Emerging Contaminants in the Environment

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Studies of Mixture Effects of Emerging Contaminants in the Environment DOCTORAL SCHOOL UNIVERSITY OF MILANO-BICOCCA Department of Earth and Environmental Sciences (DiSAT) PhD program in Environmental Sciences – Cycle XXIX 80 R – Sciences, 80 R - 1 STUDIES OF MIXTURE EFFECTS OF EMERGING CONTAMINANTS IN THE ENVIRONMENT Candidate: Dr. Valeria Di Nica Registration number: 78782 Tutor: Prof. Antonio Finizio Co-tutor: Dr. Sara Villa Coordinator: Prof. Maria Luce Frezzotti 2015/2016 DOCTORAL SCHOOL UNIVERSITY OF MILANO-BICOCCA Department of Earth and Environmental Sciences (DiSAT) PhD program in Environmental Sciences – Cycle XXIX 80 R – Sciences, 80 R - 1 STUDIES OF MIXTURE EFFECTS OF EMERGING CONTAMINANTS IN THE ENVIRONMENT Candidate: Dr. Valeria Di Nica Registration number: 78782 Tutor: Prof. Antonio Finizio Co-tutor: Dr. Sara Villa Coordinator: Prof. Maria Luce Frezzotti 2015/2016 LIST OF PUBLICATIONS This thesis is based on the following publications: I. Di Nica V., Menaballi L., Azimonti G., Finizio A., 2015. RANKVET: A new ranking method for comparing and prioritizing the environmental risk of veterinary pharmaceuticals. Ecological Indicators, 52, 270–276. doi.org/10.1016/j.ecolind.2014.12.021 II. Di Nica V., Villa S., Finizio A., 2017. Toxicity of individual pharmaceuticals and their mixtures to Aliivibrio fischeri: experimental results for single compounds and considerations of their mechanisms of action and potential acute effects on aquatic organisms. Environmental Toxicology and Chemistry, 36, 807–814. doi: 10.1002/etc.3568. III. Di Nica V., Villa S., Finizio A., 2017. Toxicity of individual pharmaceuticals and their mixtures to Aliivibrio fischeri. Part II: Evidence of toxicological interactions in binary combinations. Environmental Toxicology and Chemistry; 36, 815–822. doi: 10.1002/etc.3686. IV. Di Nica V., Villa S., Finizio A., 2016. Experimental and predicted toxicity of binary combinations of diclofenac sodium, carbamazepine and caffeine to Aliivibrio fischeri. Environmental Engineering Management Journal, 15, 1971-1980. http://omicron.ch.tuiasi.ro/EEMJ/ IN PRESS. V. Di Nica V., Gallet J., Villa S., Mezzanotte V., 2017. Toxicity of Quaternary Ammonium Compounds (QACs) to aquatic non-target microorganisms: tests with single compounds and mixtures. ACCEPTED in Ecotoxicology and Environmental Safety. 3 8Love never fails. But where there are prophecies, they will cease; where there are tongues, they will be stilled; where there is knowledge, it will pass away. 9For we know in part and we prophesy in part, 10but when completeness comes, what is in part disappears. 1 Corinthians 13:8-10 4 ACKNOWLEDGMENTS At the end of this journey I would first like to thank God for giving me the grace to pursue a Ph.D. and carry it through. I would like to thank Him for giving me strength and confidence to persevere until the end despite the several challenges to be faced. Many thanks to my old friends from Palermo and my family who even at distance have supported and have endured me with patience during this intense time. Thanks for friends, so many, I met during my brief but intense stay in Genova, they were important for the choices that I was going to do. I am also thankful to the new friends from Milano who I had the joy to meet and who walked with me in this short trip of life. They also had an important role in the successful of this Ph.D. I would like to sincerely thank my tutor Prof. Antonio Finizio who guided and continuously encouraged me not only professionally but also at the human level and that gave me the opportunity to fill my bag with new and interesting skills. Many thanks also to my co-tutor Dr. Sara Villa who gave me the opportunity to confront myself with new challenges and get my hands dirty in the laboratory. She, too, has had the patience to continuously encourage me. I express also my appreciation to Dr. Valeria Mezzanotte with whom I had the pleasure to share a piece of the research activity. Thanks to my colleagues, students and trainees with whom I shared long days of study and efforts supporting and encouraging each other. Lastly, I would also like to thank my obstinacy which led me here until the end. Valeria 5 TABLE OF CONTENTS LIST OF PUBLICATIONS ................................................................................................................................ 3 ACKNOWLEDGMENTS ................................................................................................................................. 5 ABSTRACT ................................................................................................................................................... 8 CHAPTER I ..................................................................................................................................................11 INTRODUCTION ......................................................................................................................................11 1 Emerging contaminants in aquatic environment ........................................................................11 1.1. Pharmaceutical and personal care products as emerging contaminants ...................................13 1.1.1. Human and veterinary pharmaceuticals ...............................................................................13 1.1.1.1. Consumption ....................................................................................................................13 1.1.1.2. Sources and pathways of release to the environment .......................................................14 1.1.2. Human-use pharmaceuticals ................................................................................................15 1.1.2.1. Emissions during manufacturing ......................................................................................15 1.1.2.2. Discharge from Sewage Treatment Plants ........................................................................16 1.1.2.3. Use of sewage sludge and wastewater .............................................................................16 1.1.2.4. Disposal of unused drugs ..................................................................................................17 1.1.3. Veterinary medicinal products..............................................................................................17 1.1.3.1. Emissions form livestock production and manure .............................................................18 1.1.3.2. Aquaculture treatments ...................................................................................................18 1.1.3.3. Domestic animals .............................................................................................................19 1.1.1.3. Occurrence, environmental fate and harmful effects ........................................................19 1.1.4. Quaternary ammonium compounds .....................................................................................21 1.1.4.1. Consumption ....................................................................................................................22 2 Prioritization of chemicals of concern .........................................................................................24 2.2. General approach for the development of prioritization index ..................................................26 3 Chemical mixtures in the environment........................................................................................28 3.2. Approaches used for the assessment of mixture effects............................................................30 3.3. Principles of mixture toxicology ................................................................................................31 3.4. Mathematical concepts used for the prediction of mixture toxicity ...........................................32 3.5. Dose/Concentration Addition (CA) ...........................................................................................32 3.6. Independent Action (IA) ...........................................................................................................33 3.7. Quantitative relationship between CA and IA curves ................................................................34 3.8. Selection of predictive models ..................................................................................................35 3.9. Deviation from CA and IA predictions .......................................................................................36 6 3.10. Combination Index (CI) method ............................................................................................37 REFERENCES .......................................................................................................................................39 CHAPTER II ..........................................................................................................................................56 Aims....................................................................................................................................................56 CHAPTER III .........................................................................................................................................61 RANKVET: A new ranking method for comparing and prioritizing the environmental risk of veterinary pharmaceuticals ..................................................................................................................................61 CHAPTER IV ........................................................................................................................................74
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