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1) Innehållsförteckning AN ADD-ON FILTER TECHNIQUE TO IMPROVE MICROPOLLUTANT REMOVAL AND WATER QUALITY IN ON-SITE SEWAGE TREATMENT FACILITIES Wen Zhang September 2018 TRITA-ABE-DLT-1821 ISBN: 978-91-7729-936-3 Wen Zhang TRITA-ABE-DLT-1821 © Wen Zhang 2018 Phd thesis Division of Water and Environmental Engineering Department of Sustainable Development, Environmental Science and Engineering School of Architecture and the Built Environment KTH Royal Institute of Technology SE-100 44 STOCKHOLM, Sweden Reference to this publication should be written as: Zhang, W (2018) “An add-on filter technique to improve micropollutant removal and water quality in on-site sewage treatment facilities” TRITA-ABE-DLT-1821 ii An add-on filter technique to improve micropollutant removal and water quality in on-site sewage treatment facilities SUMMARY IN SWEDISH Småskaliga (enskilda) avloppsreningsanläggningar i Sverige och på många håll i världen släpper på grund av ofullständig rening betydande mängder kväve (N) och fosfor (P) till grundvatten och ytvatten. Mikroföroreningar (MP) har också hittats i både ytvatten och grundvatten, vilket indikerar otillräckligt avlägsnande av MP i dessa anläggningar. Det övergripande syftet med denna avhandling var att undersöka olika typer av organiska och oorganiska filtermaterial (sorbent) för att identifiera en lämplig typ eller kombination av typer med hög kapacitet att ta bort en mängd MP från avloppsvatten i småskaliga anläggningar. Samtidigt har konventionella parametrar och ämnen (t ex N, P) i avloppsvattnet studerats för att undersöka om studerade sorbent även samtidigt kan avskilja dessa. Två kolonnförsök i laboratorieskala, följt av ett fältförsök, utfördes för att studera avskiljningen av en uppsättning organiska MPs genom filtrering med organiska och oorganiska sorbent. Uppsättningen MPs som tillsattes avloppsvattnet omfattade olika produktkategorier, t.ex. ett artificiellt sötningsmedel, organofosfater, parabener, personliga hygienprodukter, perfluoralkylsubstanser (PFAS), bekämpningsmedel, läkemedel, en mjukgörare, en bisfenol, stimulanter och ytaktiva ämnen. Vardera fem organiska och oorganiska sorbenter som testades visade att kolbaserade organiska sorbenter avskiljde MPs i genomsnitt 20% bättre än naturliga fibermaterial och oorganiska sorbent. Organiska sorbent med bra prestanda vid avlägsnande av MP och en konventionell sandbädd visade emellertid begränsad förmåga att avlägsna P, medan kalciumrika sorbent ökade P- avlägsnandet mycket. Fem sorbent valdes för ett långsiktigt kolonnexperiment som undersökte 31 målmikroföroreningar. De kemiska och fysikaliska egenskaperna hos de valda organiska och oorganiska filtermaterialen varierade mycket, vilket hade signifikanta effekter på deras förmåga att avlägsna målämnena från avloppsvatten. Stor specifik yta och en varierad fördelning av makroporer och mikroporer var viktiga för avlägsnande av MP, såsom demonstrerades av granulerat aktivt kol (GAC). Relativt hydrofoba MPs (log Kow ≥3) avlägsnades väl av alla organiska sorbenter. Enbart hydrofobicitet kunde emellertid inte förklara adsorptionen av MP. Negativt laddade MPs adsorberade till lignit (som var ett av testade sorbent) befanns lätt frigöras över tid från sin negativt laddade yta. För PFAS befanns molekylvikt och tillgänglig yta vara starkt positivt korrelerad med förmågan att avskilja ämnet hos materialen lignit, Xylit och sand. För andra grupper av MP var apolär och polär ytarea och förhållandet mellan dessa positivt korrelerade med avskiljningen av MP hos lignit och Xylit. Slutsatsen är att de kemiska och fysikaliska egenskaperna hos en uppsättning filtermaterial måste beaktas noga när det väljs för ett tilläggsfilter för små avloppsteknik. iii Wen Zhang TRITA-ABE-DLT-1821 Markbäddar och infiltrationslösningar är mycket vanliga i Sverige. Resultaten från denna undersökning visar att de avskiljer MP men för att uppnå effektiv behandling måste ytterligare tekniker tillämpas. Två sorbent, GAC och Xylit (xyloid lignit) testades i 24 veckor som ett tillsatsfilter i utflödet från en markbädd. Båda filtermaterialen befanns avsevärt förbättra avlägsnandet av MP. En utbytbar tilläggsenhet föreslås därför om avskiljningen av MP från små avlopp ska kunna förbättras. I denna undersökning har GAC och Xylit visat sig vara bra material som kan ingå i ett filter. Dessa material kan dock inte minska koncentrationerna av fosfor och kväve i avloppsvatten till en nivå som uppfyller svenska lagstadgade utsläppsgränser utan andra metoder måste läggas till i reningssystemet. iv An add-on filter technique to improve micropollutant removal and water quality in on-site sewage treatment facilities ACKNOWLEDGEMENTS First and foremost, I would like to express my sincere gratitude to my main supervisor, Professor Gunno Renman, for his guidance in the research and great support in the laboratory and in the field. I appreciate his professional ideas in discussions and the rich practical experiences he shared during field studies. My gratitude also to my co-supervisor, Dr. Erik Kärrman, for great support and encouragement during the whole study. I would like to thank the professors and all the scientists with whom I collaborated in the RedMic project group: Berndt Björlenius, Patrik Andersson, Karin Wiberg, Peter Haglund, Lutz Ahrens, Kristin Blum, Pablo Gago Ferrero, Qiuju Gao, Meritxell Gros, Henrik Jernstedt, Ande Rostvall and Shiromini Gamage. Thank you all for the deep and invaluable discussions, support during the experiments and suggestions for data analysis. I am grateful to Dr. Agnieszka Renman for her enthusiastic help in the laboratory. Special thanks to Dr. Heléne Ejhed for being my mid-term exam reviewer, and Professor Elzbieta Plaza, for quality control of my thesis. Warm thanks for all the help from Aira Sarrelainen and Britt Aguggiaro regarding administrative issues. Many thanks are due to Dr. Mary McAfee for her help with English grammar. Thanks to my friends and colleagues, Ezekiel Kholoma and Raúl Rodriguez Gómez, who helped me to build my columns and taught me to be an engineer. Thanks to Anqi Li and Aibin Zhang for their assistance in my laboratory work. My sincere thanks go to Yuanying Chen, Minyu Zuo, Guillaume Vigouroux, Romain Goldenberg and Liangchao Zou, for all your kindness, friendship and the enjoyable times we shared. Extra thanks to Xi Pang and Ziyi Wang for every happy lunch time we spent together during my last year. Great thanks to my parents, Shoufeng Zhang and Huaiying Cui, for their unconditional baking and love. I would like to thank my beloved husband, Anders Larsson, and the best mother-in-law, Ingrid Larsson, for their understanding and great support during my PhD study. Thanks to my dearest son, Jack Zhang Larsson, who disturbed me every five minutes when I tried to work at home, reminding me that I have a family to take care of. Finally, thanks to the Swedish Research Council FORMAS for funding part of my work in the project RedMic (Reduction of diffuse emissions of micropollutants from on-site sewage facilities, 216-2012-2101). v Wen Zhang TRITA-ABE-DLT-1821 vi An add-on filter technique to improve micropollutant removal and water quality in on-site sewage treatment facilities TABLE OF CONTENT Summary ............................................................................................................... iii Acknowledgements ................................................................................................. v Table of Content .................................................................................................. vii List of appended papers ........................................................................................ ix List of abbreviations.............................................................................................. xi Abstract .................................................................................................................. 1 1. Introduction .................................................................................................. 1 1.1. Aims and objectives 2 2. Background ................................................................................................... 3 2.1. On-site sewage treatment technologies 3 2.2. Micropollutant removal from domestic wastewater 5 2.3. Factors affecting micropollutant removal 6 2.3.1. Physical properties and chemical structure of the sorbent 6 2.3.2. Physicochemical properties of micropollutants 8 2.3.3. Adsorption process 8 2.3.4. Effect of biofilm 8 3. Materials and methods ................................................................................... 9 3.1. Filter media 9 3.2. Target chemicals 11 3.3. Screening experiment (Paper I) 11 3.4. Long-term column experiment (Papers II and III) 14 3.5. Field study (Paper IV) 16 3.6. Analytical methodology for micropollutant analysis (see also Papers I-III) 17 3.7. Determination of surface functional groups on the sorbents 18 3.8. Determination of point of zero charge (pHpzc) of the sorbents 18 3.9. Prediction of phosphorus removal 18 3.10. Calculations and statistical analysis 19 3.11. Quality assurance and quality control 20 4. Results and discussion ................................................................................. 21 4.1. Removal of conventional contaminants (Papers I, II and IV) 21 4.1.1. Dissolved organic carbon and chemical oxygen demand 21 4.1.2. Ammonium-nitrogen 23 4.1.3. Phosphorus 25 4.2. Removal of micropollutants 27 4.2.1. Comparison of sorbent performance in micropollutant removal (Papers I and
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