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Adsorption of Micropollutants on Ion Exchangers and Biosolids-Derived Biochar

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Adsorption of Micropollutants on Ion Exchangers and Biosolids-Derived Biochar Marquette University e-Publications@Marquette Dissertations, Theses, and Professional Dissertations (1934 -) Projects Micropollutant-Free Nutrient Recovery: Adsorption of Micropollutants on Ion Exchangers and Biosolids-Derived Biochar Yiran Tong Marquette University Follow this and additional works at: https://epublications.marquette.edu/dissertations_mu Part of the Environmental Engineering Commons Recommended Citation Tong, Yiran, "Micropollutant-Free Nutrient Recovery: Adsorption of Micropollutants on Ion Exchangers and Biosolids-Derived Biochar" (2018). Dissertations (1934 -). 764. https://epublications.marquette.edu/dissertations_mu/764 MICROPOLLUTANT-FREE NUTRIENT RECOVERY: ADSORPTION OF MICROPOLLUTANTS ON ION EXCHANGERS AND BIOSOLIDS-DERIVED BIOCHAR By Yiran Tong A Dissertation submitted to the Faculty of the Graduate School, Marquette University, in Partial Fulfillment of the Requirements for the Degree of Doctor of Philosophy Milwaukee, Wisconsin May 2018 ABSTRACT MICROPOLLUTANT-FREE NUTRIENT RECOVERY: ADSORPTION OF MICROPOLLUTANTS ON ION EXCHANGERS AND BIOSOLIDS-DERIVED BIOCHAR Yiran Tong Marquette University, 2018 The presence of excessive nutrients in treated wastewater effluent is a growing concern in terms of water quality and ecological balance. Thus, removal of nutrients is of great interest. Moreover, the removed nutrients can be recovered in forms amenable for agricultural reuse, which yields a sustainable supply of nonrenewable phosphorus that can be used to support global food production. As nutrient recovery gains interest, it is essential that the products be free of harmful contaminants. One class of contaminants of great concern is organic micropollutants. To help address these issues, this study evaluated the fate and impact of micropollutants during nutrient recovery via an ion exchange-regeneration-precipitation process. The adsorptive behavior of the micropollutants was evaluated for the ion exchangers and for a sustainable biosolids- derived biochar that may be useful for separating micropollutants from nutrients prior to ion exchange. Bench-scale batch reactors were operated for ion exchange-regeneration and adsorption tests. The surface properties of ion exchangers and biochar were characterized to help assess the mechanisms of micropollutant adhesion on solid adsorbents. The presence of micropollutants in water reduced the kinetic rates of nutrient exchange onto ion exchangers. Micropollutants were adsorbed to the phosphate exchangers and were released with phosphate ions during ion exchange regeneration. To remove micropollutants from water prior to ion exchange, biosolids-derived biochar was used since micropollutants were adsorbed to the biochar, but ionic nutrients were not. Biochar produced at higher pyrolysis temperatures increased adsorption capacity, as did higher ambient temperatures for batch sorption experiments. Under multi-solute conditions, not all target micropollutants demonstrated suppressed adsorption. Biochar, ammonium, and phosphate exchangers were accordingly arranged in sequence in a flow- through system. The biochar column removed more than 80% of influent hydrophobic micropollutants and 50% of hydrophilic micropollutants, thereby reducing the presence of micropollutants in the nutrient removal/recovery process. Thermodynamic parameters indicated an endothermic adsorption reaction and heterogeneity in adsorption site distribution on the biochar surface. The binding energy and entropy change of adsorption were not affected by the presence or absence of other solutes in the matrix. The underlying binding mechanism for biosolids-derived biochar adsorption was potentially dominated by non-specific hydrophobic interaction and non-covalent interaction including hydrogen bonding and π-stacking. i ACKNOWLEDGMENTS Yiran Tong I would like to express greatest gratitude to my advisors, Dr. Mayer and Dr. McNamara for helping me successfully achieve my education and research goals at Marquette University. Not only did I learn specific scientific knowledge and experimental techniques through their knowledgeable guidance, but it was also rewarding to learn from their ways of critical thinking and communicating, which will benefit my future work. I received a lot of encouragement from them. I absolutely will conclude my four years at Marquette University as a fruitful and happy time, because I got lucky to have such good advisors. I thank Dr. Silva, Dr. Singer and Dr. Zitomer, for their willingness to serve as my committee members and thoughtful advice to improve the quality of my research and dissertation. Gratefulness is also expressed to research funding sources including National Science Foundation (NSF) Water Equipment and Policy Center (WEP), the Lafferty Family Foundation and Arthur J. Schmitt Foundation for supporting my education and research. I would also acknowledge members of Water Quality Center. I thank our lab manager, Mike Dollhopf. His efforts for making the lab space, instruments, and chemicals organized was the basic quality control for my experiments. In no particular order, I would like to thank my past and present colleagues: Dr. Daniel Carey, Dr. Matthew Seib, Dr. Anthony Kappell, Dr. Zhongzhe Liu, Dr. Yu Yang, Dr. Kyana Young, Dr. Kaushik Venkiteshwaran, , Joseph Heffron, Emily Maher, Anna Avila, Saba Seyedi, ii Erik Anderson, Dylan Friss, Lee Kimbell, Paige Peters, Vinny Martino, Donald Ryan, Will Lynn, John Ross, Tom Hoffman, Carlan Johnson and Nick Benn. They are not only great friends, but also my mentors on techniques to some extent. Words just can’t describe how much thankfulness I have for my beloved mom and dad. They have always been extremely supportive and empathetic to the decisions I made. And my dearest boyfriend, Zhuozhi, I feel blessed to have him for putting our endeavors together to achieve shared life goals. iii TABLE OF CONTENTS ACKNOWLEDGMENTS ................................................................................................... i LIST OF TABLES ............................................................................................................. ix LIST OF FIGURES ............................................................................................................ x 1 INTRODUCTION .................................................................................................. 1 1.1 The Nutrients-Energy-Water Nexus at Water Resource Reclamation Facilities .................................................................................................................. 2 1.2 Anaerobic Treatment and Nutrient Recovery ............................................. 3 1.3 Pyrolysis for Biosolids Treatment .............................................................. 4 1.4 Organic Micropollutants in Wastewater ..................................................... 4 1.5 Adsorptive Behavior of Micropollutants in WRRFs .................................. 5 1.6 Research Objectives .................................................................................... 8 1.7 References ................................................................................................... 9 2 LITERATURE REVIEW: ADSORPTION OF ORGANIC MICROPOLLUTANTS ONTO SOLID ADSORBENTS................................................ 13 2.1 Introduction ............................................................................................... 14 2.2 Adsorbent surface properties and their adsorption abilities ...................... 15 2.2.1 Biochar surface properties and the adsorption of organic contaminants ............................................................................................. 16 2.2.2 Surface properties of non-carbonaceous adsorbents ..................... 19 2.3 The kinetics of adsorption of aqueous-phase organic compounds onto porous media ......................................................................................................... 20 2.3.1 Diffusion-controlled kinetics ........................................................ 21 2.3.2 Reaction-controlled kinetics .......................................................... 24 2.4 Adsorption mechanisms of organic micropollutants binding to porous sorbents ................................................................................................................. 26 iv 2.5 Quantitative methods for characterizing adsorption of organic micropollutants on porous media from water ....................................................... 32 2.5.1 Isotherms ....................................................................................... 32 2.5.2 Thermodynamics of adsorption ..................................................... 37 2.6 Conclusions and Research Gaps ............................................................... 44 2.7 References ................................................................................................. 46 3 THE FATE AND IMPACT OF ORGANIC MICROPOLLUTANTS DURING NUTRIENT REMOVAL AND RECOVERY VIA ION EXCHANGE AND STRUVITE PRECIPITATION ............................................................................................................. 57 3.1 Introduction ............................................................................................... 58 3.2 Materials and Methods .............................................................................. 61 3.2.1 Ion exchangers .............................................................................. 61 3.2.2 Ion exchanger characterization ....................................................
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