异化Mn(Ⅳ)还原菌激活及其对有机药物去除
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摘要
以嘉陵江沉积物为菌源,利用荧光绝对定量(qPCR)技术探究了不同碳源(葡萄糖和乙酸钠)和不同形态的锰氧化物(δ-Mn O_2和锰矿粉)对异化Mn(Ⅳ)还原菌激活效果的影响.在此基础上,研究了激活效果最佳的异化Mn(Ⅳ)还原菌对卡马西平、布洛芬、萘普生、雌激素和双氯芬酸5种有机药物的去除效果.结果表明,葡萄糖作为碳源,δ-Mn O_2作为电子受体时激活效果最佳,Mn~2+10d累计生成浓度达416.03mg/L,TOC消耗率达88.24%.激活后的异化金属还原菌在有无外加碳源时对卡马西平和布洛芬均无明显去除,对萘普生在外加碳源时能实现11.88%的去除.雌二醇和双氯芬酸可以作为异化Mn(Ⅳ)还原菌唯一碳源,其去除率可达75.70%和58.25%.
In this study, sediment from JiaLing River was cultivated as inoculum of dissimilatory Mn(Ⅳ)-reducing bacteria. By using qPCR technique, this study investigated the effects of different carbon sources(glucose and Na-acetate) and different forms of manganese oxides(δ-MnO_2 and manganese ore powders) on activating dissimilatory Mn(Ⅳ)-reducing bacteria. Moreover, the most active dissimilatory Mn(Ⅳ) reducing bacteria was further tested the performance of removing 5 typical pharmaceuticals, namely carbamazepine, ibuprofen, naproxen, estradiol and diclofenac. Results demonstrated that glucose was the most suitable carbon sources while the δ-MnO_2 was the most suitable electron acceptor for the activation of dissimilatory Mn(Ⅳ)-reducing bacteria. The accumulated concentration of Mn2+ reached 416.03mg/L after 10 d cultivation, while the total consumption of TOC was 88.24%. After 5d cultivation, removal of carbamazepine and ibuprofen by the activated dissimilatory Mn(Ⅳ)-reducing bacteria was insufficient with or without additional carbon sources. Only 11.88% of naproxen was removed by the bacteria in the presence of additional carbon sources. However, the activated dissimilatory Mn(Ⅳ)-reducing bacteria could use estradiol and diclofenac as the sole carbon source, with removal efficiency of 75.70% and 58.25%, respectively.
In this study, sediment from JiaLing River was cultivated as inoculum of dissimilatory Mn(Ⅳ)-reducing bacteria. By using qPCR technique, this study investigated the effects of different carbon sources(glucose and Na-acetate) and different forms of manganese oxides(δ-MnO_2 and manganese ore powders) on activating dissimilatory Mn(Ⅳ)-reducing bacteria. Moreover, the most active dissimilatory Mn(Ⅳ) reducing bacteria was further tested the performance of removing 5 typical pharmaceuticals, namely carbamazepine, ibuprofen, naproxen, estradiol and diclofenac. Results demonstrated that glucose was the most suitable carbon sources while the δ-MnO_2 was the most suitable electron acceptor for the activation of dissimilatory Mn(Ⅳ)-reducing bacteria. The accumulated concentration of Mn2+ reached 416.03mg/L after 10 d cultivation, while the total consumption of TOC was 88.24%. After 5d cultivation, removal of carbamazepine and ibuprofen by the activated dissimilatory Mn(Ⅳ)-reducing bacteria was insufficient with or without additional carbon sources. Only 11.88% of naproxen was removed by the bacteria in the presence of additional carbon sources. However, the activated dissimilatory Mn(Ⅳ)-reducing bacteria could use estradiol and diclofenac as the sole carbon source, with removal efficiency of 75.70% and 58.25%, respectively.
引文
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[7]Xiong J Q,Kurade M B,Jeon B H.Can Microalgae Remove Pharmaceutical Contaminants from Water?[J].Trends in Biotechnology,2017,36(1):30-44.
[8]Gagne F,Blaise C,Andre C.Occurrence of pharmaceutical products in a municipal effluent and toxicity to rainbow trout(Oncorhynchus mykiss)hepatocytes[J].Ecotoxicology and Environmental Safety,2006,64(3):329-336.
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[11]生贺,于锦秋,刘登峰,等.乳化植物油强化地下水中Cr(Ⅵ)的生物地球化学还原研究[J].中国环境科学,2015,35(6):1693-1699.Sheng H,Yu J Q,Liu D F,et al.Biogeochemical Cr(VI)reduction in groundwater enhanced by emulsified vegetable oil[J].China Environmental Science.2015,35(6):1693-1699.
[12]曾洪学,杨玉泉,屈兴红,等.异化Fe(Ⅲ)还原菌及其还原机制的环境意义[J].安徽农业科学,2012,(18):9843-9846.Zeng H X,Yang Y Q,Qu X H,et al.Dissimilatory Fe(III)-reducing bacteria and the environmental significance of iIts reduction mechanism[J].Journal of Anhui Agri.,2012(18):9843-9846.
[13]Lovley D.Dissimilatory metal reduction:From early life to bioremediation[M].2002:231-237.
[14]徐天生,欧杰,马晨晨.微生物还原Cr(Ⅵ)的机理研究进展[J].环境工程,2015,33(1):32-36.Xu T S,Ou J,Ma C C.Advances in mechanism about microbial reduction of Cr(VI)[J].Environmental Engineering,2015,33(1):32-36.
[15]许玫英,林培真,孔祥义,等.中国希瓦氏菌D14~T的Fe(Ⅲ)还原特性及其影响因素[J].微生物学报,2005,45(3):463-466.Xu M Y,Lin P Z,Kong X Y,et al.China shiva bacterium D14~T Fe(Ⅲ)reduction characteristics and its influencing factors[J].Acta Microbiologica Sinica,2005,45(3):463-466.
[16]刘硕,曲东.苯系物作为唯一碳源对异化铁还原过程的影响[J].西北农林科技大学学报(自然科学版),2006,34(10):101-106.Liu S,Qu D.Effect of benzene series as the only carbon source on the reduction process of dissimilated iron[J].J.of Northwest A&FUniversity(Nat.Sci.Ed.).2006,34(10):101-106.
[17]许超,董军,马小兰,等.微生物异化还原铁氧化物体系对硝基苯的降解作用[J].中国环境科学,2011,31(9):1472-1476.Xu C,Dong J,Ma X L,et al.Degradation of nitrobenzene by bacterial dissimilatory reduction of iron oxides[J].China Environmental Science,2011,31(9):1472-1476.
[18]Murray J W.Surface chemistry of hydrous manganese dioxide[J].Journal of Colloid&Interface Science,1974,46(3):357-371.
[19]Lovley D.Dissimilatory Fe(Ⅲ)-and Mn(Ⅳ)-Reducing Prokaryotes[M].Springer New York,2006:635-658.
[20]Dolores C M O,Julia M,Juan Luis S,et al.An affordable method for the simultaneous determination of the most studied pharmaceutical compounds as wastewater and surface water pollutants[J].Journal of Separation Science,2015,32(18):3064-3073.
[21]Holmes D E,Finneran K T,O'Neil R A,et al.Enrichment of members of the family Geobacteraceae associated with stimulation of dissimilatory metal reduction in uranium-contaminated aquifer sediments[J].Appl.Environ.Microbiol.,2002,68(5):2300-2306.
[22]Hung C H,Cheng C H,Cheng L H,et al.Application of Clostridiumspecific PCR primers on the analysis of dark fermentation hydrogen-producing bacterial community[J].International Journal of Hydrogen Energy,2008,33(5):1586-1592.
[23]Wu X Y,Walker M J,Hornitzky M,et al.Development of a group-specific PCR combined with ARDRA for the identification of Bacillus species of environmental significance[J].Journal of Microbiological Methods,2006,64(1):107-119.
[24]Treude N,Rosencrantz D,Liesack W,et al.Strain FAc12,a dissimilatory iron-reducing member of the Anaeromyxobacter subgroup of Myxococcales[J].Fems Microbiology Ecology,2003,44(2):261-269.
[25]水及废水监测[M].杭州:浙江大学出版社,2015:127-128.Water and wastewater monitoring[M].Hangzhou:Zhejiang University Press,2015:127-128.
[26]常慧敏,杨青惠,齐翔.TOC-L总有机碳分析仪测定总有机碳的实验方法[J].科技创新与生产力,2017,(11):118-120.Chang H M,Yang Q H,Qi X.Experimental method of total organic carbon determination based on TOC-L analyzer[J].Sci-tech Innovation and Productivity,2017,(11):118-120.
[27]Lovley D R,Holmes D E,Nevin K P.Dissimilatory Fe(Ⅲ)and Mn(Ⅳ)reduction[J].Advances in Microbial Physiology,2004,49(2):219.
[28]Lovley D R.Microbial reduction of Iron,Manganese,and other Metals[J].Advances in Agronomy,1995,54(8):175-231.
[29]Bodegom P M V,Scholten J C M,Stams A J M.Direct inhibition of methanogenesis by ferriciron[J].Fems Microbiology Ecology,2004,49(2):261-268.
[30]冯雅丽,张茜,李浩然,等.利用异化金属还原菌和锰尾矿处理制药废水[J].中南大学学报(自然科学版),2012,43(10):4153-4158.Feng Y L,Zhang Q,Li H R,et al.Treatment of pharmaceutical wastewater using dissimilatory metal reductive microbes and manganese tailings[J].Journal of Central South University(Science and Technology),2012,43(10):4153-4158.
[31]Lentini C J,Wankel S D,Hansel C M.Enriched iron(III)-reducing bacterial communities are shaped by carbon substrate and iron oxide mineralogy[J].Frontiers in Microbiology,2012,3(3):404.
[32]张盛莉.利用异化金属还原菌降解有机药物的试验研究[D].重庆:重庆大学,2014.Zhang S L.Degradation of organmic pharmaceuticals by dissimilatory metal reduction bacteria[D].Chongqing:Chongqing Universty,2014.
[33]Shi N C,Ma Z S,He W Z,et al.Nano-solids in manganese nodules from northern part of Pacific Ocean floor--Nano-solids in minerals and prospects of its uses in industry[J].Science China Chemistry,1995,(12):87-94.
[34]易维洁.碳源对水稻土中铁还原特征和铁还原菌多样性的影响[D].杨凌:西北农林科技大学,2011.Yi W J.Effects of carbon sources on iron reduction characteristic and diversity of iron reducer isolates in paddy soils[D].Yangling:Northwest A&F University,2011.
[35]Hori T,Noll M,Igarashi Y,et al.Identification of acetate-assimilating microorganisms under methanogenic conditions in anoxic rice field soil by comparative stable isotope probing of RNA[J].Appl.Environ.Microbiol.,2007,73(1):101-109.
[36]Hammann R,Ottow J C G.Reductive dissolution of Fe_2O_3 by Saccharolytic Clostridia and Bacillus polymyxa under anaerobic Conditions[J].Journal of Plant Nutrition&Soil Science,1974,137(2):108-115.
[37]刘湛,拓晓骅,王保莉,等.厌氧富集培养对水稻土中铁还原菌种群结构的影响[J].西北农业学报,2011,20(8):175-181.Liu Z,Tuo X H,Wang B L,et al,Effect of anaerobic enrichment on iron-reducing bacterialcommunity structure in paddy soil[J].Acta Agriculturae Boreali-occidentalis Sinica,2011,20(8):175-181.
[38]Wojcieszyńska D,Domaradzka D,Hupert-Kocurek K,et al.Bacterial degradation of naproxen-Undisclosed pollutant in the environment[J].Journal of Environmental Management,2014,145(12):157-161.
[39]杨梦丽.厌氧锰矿反应柱对水环境中典型PPCPs的去除效果和机理研究[D].重庆:重庆大学,2016.Yang M L.Research on typical PPCPs removal effect and mechanism by manganese ore columnar reactor in anaerobic condition[D].Chongqing:Chongqing Universty,2016.
[2]Zhou H,Zhang Z,Wang M,et al.Enhancement with physicochemical and biological treatments in the removal of pharmaceutically active compounds during sewage sludge anaerobic digestion processes[J].Chemical Engineering Journal.2017,316:361-369.
[3]Zhai J,Rahaman H,Ji J,et al.Plant uptake of diclofenac in a mesocosm-scale freewater surface constructed wetland by Cyperus alternifolius[J].Water Science and Technology,2016,73(12):3008-3016.
[4]Falas P,Longree P,la Cour Jansen J,et al.Micropollutant removal by attached and suspended growth in a hybrid biofilm-activated sludge process[J].Water Research,2013,47(13):4498-4506.
[5]Ngoc H T,Reinhard M,Gin K Y.Occurrence and fate of emerging contaminants in municipal wastewater treatment plants from different geographical regions-a review[J].Water Research,2018,133:182-207.
[6]Archer E,Petrie B,Kasprzyk-Hordern B,et al.The fate of pharmaceuticals and personal care products(PPCPs),endocrine disrupting contaminants(EDCs),metabolites and illicit drugs in a WWTW and environmental waters[J].Chemosphere,2017,174:437-446.
[7]Xiong J Q,Kurade M B,Jeon B H.Can Microalgae Remove Pharmaceutical Contaminants from Water?[J].Trends in Biotechnology,2017,36(1):30-44.
[8]Gagne F,Blaise C,Andre C.Occurrence of pharmaceutical products in a municipal effluent and toxicity to rainbow trout(Oncorhynchus mykiss)hepatocytes[J].Ecotoxicology and Environmental Safety,2006,64(3):329-336.
[9]Kim I,Yamashita N,Tanaka H.Performance of UV and UV/H_2O_2processes for the removal of pharmaceuticals detected in secondary effluent of a sewage treatment plant in Japan[J].Journal of Hazardous Materials,2009,166(2):1134-1140.
[10]Snyder S A,Adham S,Redding A M,et al.Role of membranes and activated carbon in the removal of endocrine disruptors and pharmaceuticals[J].Desalination.2007,202(1):156-181.
[11]生贺,于锦秋,刘登峰,等.乳化植物油强化地下水中Cr(Ⅵ)的生物地球化学还原研究[J].中国环境科学,2015,35(6):1693-1699.Sheng H,Yu J Q,Liu D F,et al.Biogeochemical Cr(VI)reduction in groundwater enhanced by emulsified vegetable oil[J].China Environmental Science.2015,35(6):1693-1699.
[12]曾洪学,杨玉泉,屈兴红,等.异化Fe(Ⅲ)还原菌及其还原机制的环境意义[J].安徽农业科学,2012,(18):9843-9846.Zeng H X,Yang Y Q,Qu X H,et al.Dissimilatory Fe(III)-reducing bacteria and the environmental significance of iIts reduction mechanism[J].Journal of Anhui Agri.,2012(18):9843-9846.
[13]Lovley D.Dissimilatory metal reduction:From early life to bioremediation[M].2002:231-237.
[14]徐天生,欧杰,马晨晨.微生物还原Cr(Ⅵ)的机理研究进展[J].环境工程,2015,33(1):32-36.Xu T S,Ou J,Ma C C.Advances in mechanism about microbial reduction of Cr(VI)[J].Environmental Engineering,2015,33(1):32-36.
[15]许玫英,林培真,孔祥义,等.中国希瓦氏菌D14~T的Fe(Ⅲ)还原特性及其影响因素[J].微生物学报,2005,45(3):463-466.Xu M Y,Lin P Z,Kong X Y,et al.China shiva bacterium D14~T Fe(Ⅲ)reduction characteristics and its influencing factors[J].Acta Microbiologica Sinica,2005,45(3):463-466.
[16]刘硕,曲东.苯系物作为唯一碳源对异化铁还原过程的影响[J].西北农林科技大学学报(自然科学版),2006,34(10):101-106.Liu S,Qu D.Effect of benzene series as the only carbon source on the reduction process of dissimilated iron[J].J.of Northwest A&FUniversity(Nat.Sci.Ed.).2006,34(10):101-106.
[17]许超,董军,马小兰,等.微生物异化还原铁氧化物体系对硝基苯的降解作用[J].中国环境科学,2011,31(9):1472-1476.Xu C,Dong J,Ma X L,et al.Degradation of nitrobenzene by bacterial dissimilatory reduction of iron oxides[J].China Environmental Science,2011,31(9):1472-1476.
[18]Murray J W.Surface chemistry of hydrous manganese dioxide[J].Journal of Colloid&Interface Science,1974,46(3):357-371.
[19]Lovley D.Dissimilatory Fe(Ⅲ)-and Mn(Ⅳ)-Reducing Prokaryotes[M].Springer New York,2006:635-658.
[20]Dolores C M O,Julia M,Juan Luis S,et al.An affordable method for the simultaneous determination of the most studied pharmaceutical compounds as wastewater and surface water pollutants[J].Journal of Separation Science,2015,32(18):3064-3073.
[21]Holmes D E,Finneran K T,O'Neil R A,et al.Enrichment of members of the family Geobacteraceae associated with stimulation of dissimilatory metal reduction in uranium-contaminated aquifer sediments[J].Appl.Environ.Microbiol.,2002,68(5):2300-2306.
[22]Hung C H,Cheng C H,Cheng L H,et al.Application of Clostridiumspecific PCR primers on the analysis of dark fermentation hydrogen-producing bacterial community[J].International Journal of Hydrogen Energy,2008,33(5):1586-1592.
[23]Wu X Y,Walker M J,Hornitzky M,et al.Development of a group-specific PCR combined with ARDRA for the identification of Bacillus species of environmental significance[J].Journal of Microbiological Methods,2006,64(1):107-119.
[24]Treude N,Rosencrantz D,Liesack W,et al.Strain FAc12,a dissimilatory iron-reducing member of the Anaeromyxobacter subgroup of Myxococcales[J].Fems Microbiology Ecology,2003,44(2):261-269.
[25]水及废水监测[M].杭州:浙江大学出版社,2015:127-128.Water and wastewater monitoring[M].Hangzhou:Zhejiang University Press,2015:127-128.
[26]常慧敏,杨青惠,齐翔.TOC-L总有机碳分析仪测定总有机碳的实验方法[J].科技创新与生产力,2017,(11):118-120.Chang H M,Yang Q H,Qi X.Experimental method of total organic carbon determination based on TOC-L analyzer[J].Sci-tech Innovation and Productivity,2017,(11):118-120.
[27]Lovley D R,Holmes D E,Nevin K P.Dissimilatory Fe(Ⅲ)and Mn(Ⅳ)reduction[J].Advances in Microbial Physiology,2004,49(2):219.
[28]Lovley D R.Microbial reduction of Iron,Manganese,and other Metals[J].Advances in Agronomy,1995,54(8):175-231.
[29]Bodegom P M V,Scholten J C M,Stams A J M.Direct inhibition of methanogenesis by ferriciron[J].Fems Microbiology Ecology,2004,49(2):261-268.
[30]冯雅丽,张茜,李浩然,等.利用异化金属还原菌和锰尾矿处理制药废水[J].中南大学学报(自然科学版),2012,43(10):4153-4158.Feng Y L,Zhang Q,Li H R,et al.Treatment of pharmaceutical wastewater using dissimilatory metal reductive microbes and manganese tailings[J].Journal of Central South University(Science and Technology),2012,43(10):4153-4158.
[31]Lentini C J,Wankel S D,Hansel C M.Enriched iron(III)-reducing bacterial communities are shaped by carbon substrate and iron oxide mineralogy[J].Frontiers in Microbiology,2012,3(3):404.
[32]张盛莉.利用异化金属还原菌降解有机药物的试验研究[D].重庆:重庆大学,2014.Zhang S L.Degradation of organmic pharmaceuticals by dissimilatory metal reduction bacteria[D].Chongqing:Chongqing Universty,2014.
[33]Shi N C,Ma Z S,He W Z,et al.Nano-solids in manganese nodules from northern part of Pacific Ocean floor--Nano-solids in minerals and prospects of its uses in industry[J].Science China Chemistry,1995,(12):87-94.
[34]易维洁.碳源对水稻土中铁还原特征和铁还原菌多样性的影响[D].杨凌:西北农林科技大学,2011.Yi W J.Effects of carbon sources on iron reduction characteristic and diversity of iron reducer isolates in paddy soils[D].Yangling:Northwest A&F University,2011.
[35]Hori T,Noll M,Igarashi Y,et al.Identification of acetate-assimilating microorganisms under methanogenic conditions in anoxic rice field soil by comparative stable isotope probing of RNA[J].Appl.Environ.Microbiol.,2007,73(1):101-109.
[36]Hammann R,Ottow J C G.Reductive dissolution of Fe_2O_3 by Saccharolytic Clostridia and Bacillus polymyxa under anaerobic Conditions[J].Journal of Plant Nutrition&Soil Science,1974,137(2):108-115.
[37]刘湛,拓晓骅,王保莉,等.厌氧富集培养对水稻土中铁还原菌种群结构的影响[J].西北农业学报,2011,20(8):175-181.Liu Z,Tuo X H,Wang B L,et al,Effect of anaerobic enrichment on iron-reducing bacterialcommunity structure in paddy soil[J].Acta Agriculturae Boreali-occidentalis Sinica,2011,20(8):175-181.
[38]Wojcieszyńska D,Domaradzka D,Hupert-Kocurek K,et al.Bacterial degradation of naproxen-Undisclosed pollutant in the environment[J].Journal of Environmental Management,2014,145(12):157-161.
[39]杨梦丽.厌氧锰矿反应柱对水环境中典型PPCPs的去除效果和机理研究[D].重庆:重庆大学,2016.Yang M L.Research on typical PPCPs removal effect and mechanism by manganese ore columnar reactor in anaerobic condition[D].Chongqing:Chongqing Universty,2016.