甲基汞於廢水處理單元的流佈與制定其放流水標準的合理性

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余萬俊(WAN-JYUN YU) 查詢紙本館藏

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論文名稱

甲基汞於廢水處理單元的流佈與制定其放流水標準的合理性
(The distribution of methylmercury in the wastewater treatment process and the rationality of establishing its discharge regulation)

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摘要(中)

污水處理廠一直以來都是城市及工業區之污染物匯集點，也是污染物進入自然水體前的最後一道防線，因此謹慎的管控污染物的排放濃度是一項重要的課題，而汞(Hg)身為全球最具毒性的重金屬一員，理所當然的該被視為重點控制目標。台灣為了防止汞污染的加劇，於最新的放流水標準裡規範了總汞及甲基汞，其中總汞為5μg/L、甲基汞為0.2 ng/L，但若比對國外之法規標準以及相關研究文獻的數據可知，在台灣法規所列的標準裡，甲基汞占總汞的比例遠低於一般自然界中尋常的比例，這會導致處理廠在處理甲基汞時出現難以管控的現象，且此規範發布後，本實驗室陸續收到廠商的詢問，表示常遇到其放流水的甲基汞超過管制標準的情況，儘管其原物料中沒有使用汞或甲基汞。有鑑於此，為了暸解污水處理單元中甲基汞生成及放流水甲基汞超標之問題，本研究藉由分析處理廠A及處理廠B之各個處理單元間的總汞及甲基汞，來了解兩者於各單元間的濃度變化及處理效率，更透過分析其他環境因子以探討各處理單元之汞甲基化潛勢高低，並藉由總汞及甲基汞與環境因子的相關性尋找控制方法。調查結果顯示兩污水處理廠對總汞及甲基汞的處理效率良好：總汞為92%、76%，甲基汞為82%、95%，且兩廠皆符合放流水標準；通過Spearman’s相關係數分析得知總汞、甲基汞及總懸浮微粒間存在著極度顯著的正相關，而溶解態活性汞的濃度與甲基化潛勢呈現顯著負相關；在季節差異上，兩處理廠的總汞及甲基汞流佈走勢沒有發現差異性，表示其處理汞之季節穩定性良好；藉由與環境因子的相關性得出，降低水中總懸浮微粒濃度及增加水中溶氧量是控制汞及甲基汞最有效且經濟之作法。最後，由於汞及甲基汞之間的相關性以及毒性強度差異大，於法規中同時規範兩者的排放限值似乎不甚恰當，本研究最後較建議可從TMDL的角度進行甲基汞控制，搭配放流水之總汞標準的調整來對汞物種進行污染物控制，既可使處理廠較容易實施，又可達到控制污染物排放之目的。

摘要(英)

Wastewater treatment plants have always been pollutant collection points in cities and industrial areas, thus being the last line of defense before pollutants enter natural water bodies. Rigorous control of pollutant emissions is an important issue. Being one of the most toxic heavy metals, mercury (Hg) is considered the priority pollutant to be handled properly. To prevent the aggravation of Hg pollution, Taiwan has regulated total Hg (THg) and methylmercury (MeHg) in the discharge, of which total Hg is 5μg/L and MeHg is 0.2 ng/L. However, when comparing these standards with the regulations of other countries and with the reported values of effluents in literature, it is obvious that the ratio of MeHg to THg pertinent to the Taiwan regulations is much lower than those observed in the majority of natural and engineered systems. This may result in difficulties in treating and managing MeHg issues in treatment plants. In view of this, two wastewater treatment plants located in North Taiwan were selected to collect aqueous samples from each operating unit and analyze THg and MeHg concentrations in order to understand the concentration change and treatment efficiency among units. In the meantime, other important environmental factors were also analyzed to explore the Hg methylation potential of each unit. The goal was to investigate the potential correlation between THg and MeHg with key environmental factors. Results show that the treatment efficiency of THg and MeHg in the treatment plants is fairly good at present with 92% and 76% for total Hg, as well as 82% and 95% for MeHg, and the discharged effluent of the two plants meets the regulations. Through Spearman’s correlation coefficient analysis, it is found that there is an extremely significant positive correlation between THg, MeHg, and total suspended particulates, whereas the concentration of dissolved active mercury has a significant negative correlation with the methylation potential. In terms of seasonal differences, there is no difference in the distribution of THg and MeHg between the two treatment plants, indicating that the seasonal stability of the mercury treatment is good. According to the correlation with environmental factors, it is concluded that reducing the concentration of total suspended particulates in water and increasing the amount of dissolved oxygen in water would be the most effective and economical methods for controlling Hg and MeHg levels. Due to the large correlation between Hg and MeHg and the difference in toxic intensity, it may not be appropriate to regulate both THg and MeHg concurrently in the discharge. At the end of this study, it is more recommended to use TMDL to control MeHg, and to control the pollutants of Hg species with the strict THg standard only, which can make the treatment plant easier to implement and achieve the purpose of controlling pollutant emissions.

關鍵字(中)

★ 總汞與甲基汞
★ 廢水處理流程
★ 放流水標準
★ 總最大日負荷

關鍵字(英)

★ Total Hg and methyl Hg
★ wastewater treatment processes
★ discharge regulations
★ TMDL

論文目次

目錄
摘要 I
Abstract III
致謝 V
圖目錄 IX
表目錄 XI
第一章前言 1
1.1 研究緣起 1
1.2 研究目的 4
第二章文獻回顧 5
2.1 汞與甲基汞之毒性及危害性 5
2.2 微生物汞甲基化機制 7
2.3 生物可利用的汞(Bioavailable mercury) 10
2.4 汞的管理與相關法規歷程 12
2.5 每日最大負荷總量 (Total Maximum Daily Loads, TMDL) 17
2.6 污水處理廠中的汞 21
第三章研究方法與設備 22
3.1 研究流程與架構 22
3.2 實驗材料與儀器 23
3.2.1 實驗藥品與試劑 23
3.2.2 儀器與設備 24
3.3 研究廠址介紹 26
3.4 現場採樣實驗規劃與樣品前處理 28
3.4.1 樣品採集 28
3.4.2 樣品保存前處理 29
3.5 物理化學分析 30
3.5.1 總汞分析 30
3.5.2 甲基汞分析 30
3.5.3 添加實驗分析 30
3.5.4 過濾汞分析 31
3.5.5 總汞與甲基汞回收率分析 31
3.5.6 統計分析 31
3.5.7 活性汞分析 32
3.5.8 硫酸鹽類分析 32
3.5.9 總懸浮微粒分析 32
3.6 分生試驗 33
3.6.1 DNA萃取 33
3.6.2 PCR 33
3.6.3 qPCR 34
第四章結果與討論 36
4.1 總汞及甲基汞分析結果 36
4.1.1 總汞於廢水處理單元之流佈 36
4.1.2 甲基汞於廢水處理單元之流佈 38
4.1.3 總汞之季節性差異 40
4.1.4 甲基汞之季節性差異 42
4.2 汞甲基化潛勢因子分析與探討 44
4.2.1 MeHg / THg 44
4.2.2 hgcA / 16S rRNA gene 46
4.2.3 污水處理單元中汞之生物有效性探討 48
4.2.4 溶氧量分析探討 50
4.3 總汞及甲基汞與各項環境測值之相關性分析 52
4.3.1 總汞及甲基汞之相關性分析 52
4.3.2 總懸浮固體物(Total suspended solids)與總汞及甲基汞之相關性探討 53
4.3.3 甲基化潛勢影響因子相關性分析 55
4.4 添加實驗分析(Spike tests) 59
4.5 甲基汞法規限值探討 61
第五章結論與建議 65
5.1 結論 65
1. 污水處理廠中總汞濃度流佈 65
2. 污水處理廠中甲基汞濃度流佈 65
3. 總汞、甲基汞與環境因子之相關性 65
4. 總汞與甲基汞於兩大污水廠之季節變化 65
5. 污水處理廠中汞甲基化潛勢 66
5.2 建議 67
附錄 73

參考文獻

Bae, Hee-Sung, Forrest E Dierberg, Andrew Ogram, and Prentiss H Balcom. 2019. ′Periphyton and flocculent materials are important ecological compartments supporting abundant and diverse mercury methylator assemblages in the Florida Everglades′, Applied and environmental microbiology, 85: e00156-19.

Balogh, S. J., D. R. Engstrom, J. E. Almendinger, M. L. Meyer, and D. K. Johnson. 1999. ′History of mercury loading in the Upper Mississippi River reconstructed from the sediments of Lake Pepin′, Environmental science & technology, 33: 3297-302.

Balogh, Steven J, Yabing Huang, Heather J Offerman, Michael L Meyer, and D Kent Johnson. 2002. ′Episodes of elevated methylmercury concentrations in prairie streams′, Environmental science & technology, 36: 1665-70.

Balogh, Steven J, and Yabing H Nollet. 2008. ′Methylmercury input to the Mississippi River from a large metropolitan wastewater treatment plant′, Science of the total environment, 406: 145-53.

Bender, Michael %J Mercury. 2008. ′Facing Up to the Hazards of Mercury Tooth Fillings′.

Benoit, JM, Cynthia C Gilmour, A Heyes, RP Mason, and CL Miller. 2003. ′Geochemical and biological controls over methylmercury production and degradation in aquatic ecosystems.′ in (ACS Publications).

Choi, Anna L, and Philippe %J Environmental Chemistry Grandjean. 2008. ′Methylmercury exposure and health effects in humans′, 5: 112-20.

Christensen, Geoff A, Ann M Wymore, Andrew J King, Mircea Podar, Richard A Hurt, Eugenio U Santillan, Ally Soren, Craig C Brandt, Steven D Brown, and Anthony V Palumbo. 2016a. ′Development and validation of broad-range qualitative and clade-specific quantitative molecular probes for assessing mercury methylation in the environment′, Appl. Environ. Microbiol., 82: 6068-78.

Christensen, Geoff A, Ann M Wymore, Andrew J King, Mircea Podar, Richard A Hurt, Eugenio U Santillan, Ally Soren, Craig C Brandt, Steven D Brown, and Anthony V %J Appl. Environ. Microbiol. Palumbo. 2016b. ′Development and validation of broad-range qualitative and clade-specific quantitative molecular probes for assessing mercury methylation in the environment′, 82: 6068-78.

Christensen, Ole. 2016. An introduction to frames and Riesz bases (Springer).

Compeau, GC, and R Bartha. 1985. ′Sulfate-reducing bacteria: principal methylators of mercury in anoxic estuarine sediment′, Appl. Environ. Microbiol., 50: 498-502.

Fitzgerald, William F, Daniel R Engstrom, Carl H Lamborg, Chun-Mao Tseng, Prentiss H Balcom, and Chad R Hammerschmidt. 2005. ′Modern and historic atmospheric mercury fluxes in northern Alaska: Global sources and Arctic depletion′, Environmental science & technology, 39: 557-68.

Froh, Jeffrey J, and Acacia C Parks. 2013. Activities for teaching positive psychology: A guide for instructors (American Psychological Association).

Gbondo-Tugbawa, Solomon S, Joseph A McAlear, Charles T Driscoll, and Charles W Sharpe. 2010a. ′Total and methyl mercury transformations and mass loadings within a wastewater treatment plant and the impact of the effluent discharge to an alkaline hypereutrophic lake′, Water research, 44: 2863-75.

Gbondo-Tugbawa, Solomon S, Joseph A McAlear, Charles T Driscoll, and Charles W %J Water research Sharpe. 2010b. ′Total and methyl mercury transformations and mass loadings within a wastewater treatment plant and the impact of the effluent discharge to an alkaline hypereutrophic lake′, 44: 2863-75.

Gill, Gary A, and William F Fitzgerald. 1985. ′Mercury sampling of open ocean waters at the picomolar level′, Deep Sea Research Part A. Oceanographic Research Papers, 32: 287-97.

Gilmour, Cynthia C, Mircea Podar, Allyson L Bullock, Andrew M Graham, Steven D Brown, Anil C Somenahally, Alex Johs, Richard A Hurt Jr, Kathryn L Bailey, and Dwayne A Elias. 2013. ′Mercury methylation by novel microorganisms from new environments′, Environmental science & technology, 47: 11810-20.

Grandjean, Philippe, Pal Weihe, Roberta F White, Frodi Debes, Shunichi Araki, Kazuhito Yokoyama, Katsuyuki Murata, Nicolina Sørensen, Rasmus Dahl, Poul J %J Neurotoxicology Jørgensen, and teratology. 1997. ′Cognitive deficit in 7-year-old children with prenatal exposure to methylmercury′, 19: 417-28.

Hamelin, Stéphanie, Marc Amyot, Tamar Barkay, Yanping Wang, and Dolors Planas. 2011. ′Methanogens: principal methylators of mercury in lake periphyton′, Environmental science & technology, 45: 7693-700.

Hines, Mark E, Milena Horvat, Jadran Faganeli, Jean-Claude J Bonzongo, Tamar Barkay, Elaine B Major, Karen J Scott, Elizabeth A Bailey, John J Warwick, and W Berry Lyons. 2000. ′Mercury biogeochemistry in the Idrija River, Slovenia, from above the mine into the Gulf of Trieste′, Environmental research, 83: 129-39.

King, Jeffrey K, Joel E Kostka, Marc E Frischer, and F Michael Saunders. 2000. ′Sulfate-reducing bacteria methylate mercury at variable rates in pure culture and in marine sediments′, Appl. Environ. Microbiol., 66: 2430-37.

Kjellström, Tord, Paul Kennedy, Sally Wallis, Alistair Stewart, Lars Friberg, Birger Lind, Ted Wutherspoon, and Colin Mantell. 1989. Physical and mental development of children with prenatal exposure to mercury from fish. Stage 2. Interviews and psychological tests at age 6.

Krabbenhoft, DP, BA Branfireun, A Heyes, and Prentiss H Balcom. 2005. ′Biogeochemical cycles affecting the speciation, fate and transport of mercury in the environment′, Mercury: Sources, measurements, cycles, and effects.(Short course series, Vol. 34). Edited by MB Parsons and JB Percival. Mineralogical Association of Canada, Ottawa, Ont: 139-56.

Liu, Yu-Rong, Ri-Qing Yu, Yuan-Ming Zheng, and Ji-Zheng He. 2014. ′Analysis of the microbial community structure by monitoring an Hg methylation gene (hgcA) in paddy soils along an Hg gradient′, Appl. Environ. Microbiol., 80: 2874-79.

Lohren, Hanna, Lara Blagojevic, Romy Fitkau, Franziska Ebert, Stefan Schildknecht, Marcel Leist, Tanja %J Journal of Trace Elements in Medicine Schwerdtle, and Biology. 2015. ′Toxicity of organic and inorganic mercury species in differentiated human neurons and human astrocytes′, 32: 200-08.

Mao, Yuxiang, Liu Cheng, Bingjuan Ma, and Yong Cai. 2016a. ′The fate of mercury in municipal wastewater treatment plants in China: significance and implications for environmental cycling′, Journal of hazardous materials, 306: 1-7.

Mao, Yuxiang, Liu Cheng, Bingjuan Ma, and Yong %J Journal of hazardous materials Cai. 2016b. ′The fate of mercury in municipal wastewater treatment plants in China: significance and implications for environmental cycling′, 306: 1-7.

Mason, RP, and JD Dean. 2008. ”Mercury Bioaccumulation Potential from Wastewater Treatment Plants in Receiving Waters.” In AGU Fall Meeting Abstracts.

Mason, RP, WF Fitzgerald, J Hurley, AK Hanson Jr, P Lake Donaghay, JM %J Limnology Sieburth, and Oceanography. 1993. ′Mercury biogeochemical cycling in a stratified estuary′, 38: 1227-41.

Mergler, Donna, Henry A Anderson, Laurie Hing Man Chan, Kathryn R Mahaffey, Michael Murray, Mineshi Sakamoto, and Alan H Stern. 2007a. ′Methylmercury exposure and health effects in humans: a worldwide concern′, AMBIO: A Journal of the Human Environment, 36: 3-12.

Mergler, Donna, Henry A Anderson, Laurie Hing Man Chan, Kathryn R Mahaffey, Michael Murray, Mineshi Sakamoto, and Alan H %J AMBIO: A Journal of the Human Environment Stern. 2007b. ′Methylmercury exposure and health effects in humans: a worldwide concern′, 36: 3-12.
Morgan, James J, and Werner Stumm. 1970. Aquatic chemistry (Wiley).
Mutter, Joachim, Annika Curth, Johannes Naumann, Richard Deth, and Harald Walach. 2010. ′Does inorganic mercury play a role in Alzheimer′s disease? A systematic review and an integrated molecular mechanism′, Journal of Alzheimer′s Disease, 22: 357-74.

O′Driscoll, Nelson J, Stephen Beauchamp, Steven D Siciliano, Andy N Rencz, and David RS Lean. 2003. ′Continuous analysis of dissolved gaseous mercury (DGM) and mercury flux in two freshwater lakes in Kejimkujik Park, Nova Scotia: evaluating mercury flux models with quantitative data′, Environmental science & technology, 37: 2226-35.

Parks, Jerry M, Alexander Johs, Mircea Podar, Romain Bridou, Richard A Hurt, Steven D Smith, Stephen J Tomanicek, Yun Qian, Steven D Brown, and Craig C Brandt. 2013. ′The genetic basis for bacterial mercury methylation′, Science, 339: 1332-35.

Podar, Mircea, Cynthia C Gilmour, Craig C Brandt, Allyson Soren, Steven D Brown, Bryan R Crable, Anthony V Palumbo, Anil C Somenahally, and Dwayne A Elias. 2015. ′Global prevalence and distribution of genes and microorganisms involved in mercury methylation′, Science advances, 1: e1500675.

Reg, US Environmental Protection Agency %J Fed. 2001. ′Water quality criteria: Notice of availability of water quality criterion for the protection of human health: Methylmercury′, 66: 1344-59.

Regnell, Olof, Anders Tunlid, Goran Ewald, and Olof Sangfors. 1996. ′Methyl mercury production in freshwater microcosms affected by dissolved oxygen levels: role of cobalamin and microbial community composition′, Canadian Journal of Fisheries and Aquatic Sciences, 53: 1535-45.

Rule, KL, SDW Comber, D Ross, A Thornton, CK Makropoulos, and R %J Chemosphere Rautiu. 2006. ′Diffuse sources of heavy metals entering an urban wastewater catchment′, 63: 64-72.

Schaefer, Jeffra K, Aleksandra Szczuka, François MM %J Environmental science Morel, and technology. 2014. ′Effect of divalent metals on Hg (II) uptake and methylation by bacteria′, 48: 3007-13.

Schaefer, Jeffra K, Jane Yagi, John R Reinfelder, Tamara Cardona, Kristie M Ellickson, Shoshana Tel-Or, and Tamar Barkay. 2004. ′Role of the bacterial organomercury lyase (MerB) in controlling methylmercury accumulation in mercury-contaminated natural waters′, Environmental science & technology, 38: 4304-11.

Selifonova, O, Robert Burlage, Tamar Barkay, and Prentiss H Balcom. 1993. ′Bioluminescent sensors for detection of bioavailable Hg (II) in the environment′, Appl. Environ. Microbiol., 59: 3083-90.

Smith, Steven D, Romain Bridou, Alexander Johs, Jerry M Parks, Dwayne A Elias, Richard A Hurt, Steven D Brown, Mircea Podar, and Judy D Wall. 2015. ′Site-directed mutagenesis of HgcA and HgcB reveals amino acid residues important for mercury methylation′, Appl. Environ. Microbiol., 81: 3205-17.

Thomas, Sara A, Kara E Rodby, Eric W Roth, Jinsong Wu, and Jean-François Gaillard. 2018. ′Spectroscopic and microscopic evidence of biomediated HgS species formation from Hg (II)–cysteine complexes: implications for Hg (II) bioavailability′, Environmental science & technology, 52: 10030-39.

Ullrich, Susanne M, Trevor W Tanton, and Svetlana A Abdrashitova. 2001. ′Mercury in the aquatic environment: a review of factors affecting methylation′, Critical reviews in environmental science and technology, 31: 241-93.

Wiatrowski, Heather A, Paula Marie Ward, Tamar Barkay, and Prentiss H Balcom. 2006. ′Novel reduction of mercury (II) by mercury-sensitive dissimilatory metal reducing bacteria′, Environmental science & technology, 40: 6690-96.

Winfrey, Michael R, and John WM Rudd. 1990. ′Environmental factors affecting the formation of methylmercury in low pH lakes′, Environmental Toxicology and Chemistry: An International Journal, 9: 853-69.

Zhang, Hua, Xinbin Feng, Thorjørn Larssen, Guangle Qiu, and Rolf D Vogt. 2010a. ′In inland China, rice, rather than fish, is the major pathway for methylmercury exposure′, Environmental health perspectives, 118: 1183-88.

Zhang, Hua, Xinbin Feng, Thorjørn Larssen, Guangle Qiu, and Rolf D %J Environmental health perspectives Vogt. 2010b. ′In inland China, rice, rather than fish, is the major pathway for methylmercury exposure′, 118: 1183-88.

Zhou, Jing, Micholas Dean Smith, Sarah J Cooper, Xiaolin Cheng, Jeremy C Smith, and Jerry M Parks. 2017. ′Modeling of the passive permeation of mercury and methylmercury complexes through a bacterial cytoplasmic membrane′, Environmental science & technology, 51: 10595-604.

指導教授

林居慶(Chu-Ching lin)

審核日期

2020-1-17

推文