有机酸强化Fe(Ⅲ)还原介导的Shewanella oneidensis MR-1降解磺胺甲噁唑
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摘要
在实验室条件下,研究了Shewanella oneidensis MR-1对磺胺甲噁唑(Sulfamethoxazole,SMX)的降解特性以及低分子有机酸强化Fe(Ⅲ)还原介导的S.oneidensis MR-1对SMX的降解.结果表明,S.oneidensis MR-1对不同浓度SMX的降解能力与体系中的有机酸和Fe(Ⅲ)密切相关.低浓度SMX对其生长影响不大,高浓度时细菌生长则受到抑制,进而抑制SMX的降解率.当低分子有机酸单独加入体系后,S.oneidensis MR-1对SMX的最大降解率为58.5%;Fe(Ⅲ)单独加入体系后,S.oneidensis MR-1对SMX的最大降解率为67.6%.此外,当柠檬酸和Fe(OH)_3同时加入体系后,S.oneidensis MR-1对SMX生物降解和铁还原作用促进效果最显著,培养5 d后SMX降解率为90.3%.最后,采用液相色谱-质谱联用仪(LC-MS)对SMX的降解中间产物进行了分析,推测SMX的可能降解途径是由S—N键断裂引起的.本研究以期为地下水污染场地修复提供理论依据.
In this paper, low molecular organic acids enhanced and Fe(Ⅲ) reduction mediated SMX degradation by Shewanella oneidensis MR-1 were studied under laboratory conditions. The results indicate that the degradation of SMX at different initial concentrations by S. oneidensis MR-1 was closely related to the organic acids and Fe(Ⅲ) contents in the system. SMX at low concentration had little effect on the strains growth. Cells growth was inhibited at high SMX concentration, thereby reducing the degradation efficiency of SMX. When low molecular organic acids were added to the system alone, the maximum degradation rate of SMX by S. oneidensis MR-1 was 58.5%; When Fe(Ⅲ) were added to the system alone, the maximum degradation rate of SMX by S. oneidensis MR-1 was 67.6%. In addition, when 1.0 mmol·L~(-1) citric acid and 5.0 mmol·L~(-1) Fe(OH)_3 suspensions were simultaneously added to the system, the SMX degradation rate were 90.3%. Finally, the degradation intermediate products of SMX by S. oneidensis MR-1 were analyzed by liquid chromatography-mass spectrometry(LC-MS), and the possible degradation pathway of SMX was caused by S—N bond cleavage. This research provides a theoretical basis and technical support for the remediation of contaminated groundwater.
In this paper, low molecular organic acids enhanced and Fe(Ⅲ) reduction mediated SMX degradation by Shewanella oneidensis MR-1 were studied under laboratory conditions. The results indicate that the degradation of SMX at different initial concentrations by S. oneidensis MR-1 was closely related to the organic acids and Fe(Ⅲ) contents in the system. SMX at low concentration had little effect on the strains growth. Cells growth was inhibited at high SMX concentration, thereby reducing the degradation efficiency of SMX. When low molecular organic acids were added to the system alone, the maximum degradation rate of SMX by S. oneidensis MR-1 was 58.5%; When Fe(Ⅲ) were added to the system alone, the maximum degradation rate of SMX by S. oneidensis MR-1 was 67.6%. In addition, when 1.0 mmol·L~(-1) citric acid and 5.0 mmol·L~(-1) Fe(OH)_3 suspensions were simultaneously added to the system, the SMX degradation rate were 90.3%. Finally, the degradation intermediate products of SMX by S. oneidensis MR-1 were analyzed by liquid chromatography-mass spectrometry(LC-MS), and the possible degradation pathway of SMX was caused by S—N bond cleavage. This research provides a theoretical basis and technical support for the remediation of contaminated groundwater.
引文
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陈涛,李彦文,莫测辉,等.2010.广州污水厂磺胺和喹诺酮抗生素污染特征研究[J].环境科学与技术,33(6):144-147,180
Colon D,Weber E J,Anderson J L.2008.Effect of natural organic matter on the reduction of nitroaromatics by Fe(II) Species [J].Environmental Science and Technology,42(17):6538-6543
Druschel G K,Emerson D,Sutka R,et al.2008.Low-oxygen and chemical kinetic constraints on the geochemical niche of neutrophilic iron(Ⅱ) oxidizing microorganisms [J].Geochimica Et Cosmochimica Acta,72(14):3358-3370
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Groh J L,Luo Q W,Ballard J D,et al.2007.Genes that enhance the ecological fitness of Shewanella oneidensis MR-1 in sediments reveal the value of antibiotic resistance [J].Applied and Environmental Microbiology,73(2):492-498
何金华,丘锦荣,贺德春,等.2012.磺胺类抗生素的环境行为及其控制技术研究进展[J].广东农业科学,12(7):225-229
Jiang B C,Li A,Cui D,et al.2014.Biodegradation and metabolic pathway of sulfamethoxazole by Pseudomonas psychrophila HA-4,a newly isolated cold-adapted sulfamethoxazole-degrading bacterium [J].Applied Microbiology and Biotechnology,98(10):4671-4681
金彩霞,司晓薇,毛蕾,等.2015.磺胺类药物在土壤中的形态转化及降解研究[J].环境科学学报,35(12):3985-3990
Kang C H,So J S.2016.Antibiotic heavy metal resistance in Shewanella putrefaciens strains isolated from shellfishes collected from the West Sea,Korea [J].Marine Pollution Bulletin,112(1/2):111-116
Latta D E,Bachman J E,Scherer M M.2012.fe electron transfer and atom exchange in goethite:Influence of al-substitution and anion sorption [J].Environmental Science and Technology,46(19):10614-10623
Lovley D R.2006.Bug juice:harvesting electricity with microorganisms [J].Nature Reviews Microbiology,4(7):497-508
罗涛,李取生,陈惠君,等.2018.6种低分子有机酸对针铁矿、蒙脱石和生物炭中结合态Cd活化效果的对比[J].环境工程学报,12(7):2047-2055
毛飞.2017.Shewanella oneidensis MR-1和Shewanella sp.strain MR-4对磺胺类抗生素的降解特性研究[D].安徽:安徽农业大学.1-49
马小兰,丁琳洁,董军,等.2012.地下环境中铁氧化物生物异化还原耦合降解硝基苯的影响因素研究[J].生态环境学报,21(6):1109-1114
Mohatt J L,Hu L H,Finneran K T,et al.2011.Microbially mediated abiotic transformation of the antimicrobial agent sulfamethoxazole under iron-reducing soil conditions [J].Environmental Science and Technology,45(11):4793-4801
Qin F,Shan X Q,Wei B.2004.Effects of low-molecular-weight organic acids and residence time on desorption of Cu,Cd,and Pb from soils [J].Chemosphere,57(4):253-263
秦国建,许振成,吴根义,等.2011.残留磺胺类抗生素的来源及环境行为研究进展[J].农业灾害研究,1(1):58-60
Reis P J M,Reis A C,Ricken B,et al.2014.Biodegradation of sulfamethoxazole and other sulfonamides by Achromobacter denitrificans PR1 [J].Journal of Hazardous Materials,280:741-749
Richter K,Schicklberger M,Gescher J.2012.Dissimilatory reduction of extracellular electron acceptors in anaerobic respiration [J].Applied and Environmental Microbiology,78(4):913-921
Ricken B,Corvini P F X,Cichocka D,et al.2013.ipso-Hydroxylation and subsequent fragmentation:a novel microbial strategy to eliminate sulfonamide antibiotics [J].Applied and Environmental Microbiology,79(18):5550-5558
Sarmah A K,Meyer M T,Boxall A B A.2006.A global perspective on the use,sales,exposure pathways,occurrence,fate and effects of veterinary antibiotics (VAs) in the environment [J].Chemosphere,65(5):725-759
Tamtam F,Mercier F,Le Bot B,et al.2008.Occurrence and fate of antibiotics in the Seine River in various hydrological conditions [J].Science of the Total Environment,393(1):84-95
Tong L,Huang S B,Wang Y X,et al.2014.Occurrence of antibiotics in the aquatic environment of Jianghan Plain,central China [J].Science of the Total Environment,497:180-187
Wang A J,Sun D,Ren N Q,et al.2010.A rapid selection strategy for an anodophilic consortium for microbial fuel cells [J].Bioresource Technology,101(14):5733-5735
Wang L,Liu Y L,Ma J,et al.2016.Rapid degradation of sulphamethoxazole and the further transformation of 3-amino-5-methylisoxazole in a microbial fuel cell [J].Water Research,88:322-328
汪明霞,王娟,司友斌,等.2014.Shewanella oneidensis MR-1 异化还原Fe(Ⅲ)介导的As(Ⅲ)氧化转化[J].中国环境科学,34(9):2368-2373
肖湘波,唐天乐,徐浩,等.2015.医院典型废水处理工艺单元的抗生素去除效果与评价[J].环境科学与技术,38(4):121-127
许超,董军,马小兰,等.2011.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,31(9):1472-1476
叶计朋,邹世春,张干,等.2007.典型抗生素类药物在珠江三角洲水体中的污染特征[J].生态环境,16(2):384-388
张敏,李轶,敖永华,等.2011.土壤中磺胺类兽药残留的生态效应及转归[J].中国农学通报,27(3):369-373
Zhou C,Wang H Q,Si Y B,et al.2018.Electron shuttles enhance the degradation of sulfamethoxazole coupled with Fe(III) reduction by Shewanella oneidensis MR-1 [J].Environmental Toxicology and Pharmacology,62:156-163
陈涛,李彦文,莫测辉,等.2010.广州污水厂磺胺和喹诺酮抗生素污染特征研究[J].环境科学与技术,33(6):144-147,180
Colon D,Weber E J,Anderson J L.2008.Effect of natural organic matter on the reduction of nitroaromatics by Fe(II) Species [J].Environmental Science and Technology,42(17):6538-6543
Druschel G K,Emerson D,Sutka R,et al.2008.Low-oxygen and chemical kinetic constraints on the geochemical niche of neutrophilic iron(Ⅱ) oxidizing microorganisms [J].Geochimica Et Cosmochimica Acta,72(14):3358-3370
Eibes G,Debernardi G,Feijoo G,et al.2011.Oxidation of pharmaceutically active compounds by a ligninolytic fungal peroxidase [J].Biodegradation,22(3):539-550
Gao Y Z,He J Z,Ling W T,et al.2003.Effects of organic acids on copper and cadmium desorption from contaminated soils [J].Environment International,29(5):613-618
García-Galán M,Rodríguez-Rodríguez C E,Vicent T,et al.2011.Biodegradation of sulfamethazine by Trametes versicolor:Removal from sewage sludge and identification of intermediate products by UPLC-QqTOF-MS [J].Science of the Total Environment,409(24):5505-5512
Groh J L,Luo Q W,Ballard J D,et al.2007.Genes that enhance the ecological fitness of Shewanella oneidensis MR-1 in sediments reveal the value of antibiotic resistance [J].Applied and Environmental Microbiology,73(2):492-498
何金华,丘锦荣,贺德春,等.2012.磺胺类抗生素的环境行为及其控制技术研究进展[J].广东农业科学,12(7):225-229
Jiang B C,Li A,Cui D,et al.2014.Biodegradation and metabolic pathway of sulfamethoxazole by Pseudomonas psychrophila HA-4,a newly isolated cold-adapted sulfamethoxazole-degrading bacterium [J].Applied Microbiology and Biotechnology,98(10):4671-4681
金彩霞,司晓薇,毛蕾,等.2015.磺胺类药物在土壤中的形态转化及降解研究[J].环境科学学报,35(12):3985-3990
Kang C H,So J S.2016.Antibiotic heavy metal resistance in Shewanella putrefaciens strains isolated from shellfishes collected from the West Sea,Korea [J].Marine Pollution Bulletin,112(1/2):111-116
Latta D E,Bachman J E,Scherer M M.2012.fe electron transfer and atom exchange in goethite:Influence of al-substitution and anion sorption [J].Environmental Science and Technology,46(19):10614-10623
Lovley D R.2006.Bug juice:harvesting electricity with microorganisms [J].Nature Reviews Microbiology,4(7):497-508
罗涛,李取生,陈惠君,等.2018.6种低分子有机酸对针铁矿、蒙脱石和生物炭中结合态Cd活化效果的对比[J].环境工程学报,12(7):2047-2055
毛飞.2017.Shewanella oneidensis MR-1和Shewanella sp.strain MR-4对磺胺类抗生素的降解特性研究[D].安徽:安徽农业大学.1-49
马小兰,丁琳洁,董军,等.2012.地下环境中铁氧化物生物异化还原耦合降解硝基苯的影响因素研究[J].生态环境学报,21(6):1109-1114
Mohatt J L,Hu L H,Finneran K T,et al.2011.Microbially mediated abiotic transformation of the antimicrobial agent sulfamethoxazole under iron-reducing soil conditions [J].Environmental Science and Technology,45(11):4793-4801
Qin F,Shan X Q,Wei B.2004.Effects of low-molecular-weight organic acids and residence time on desorption of Cu,Cd,and Pb from soils [J].Chemosphere,57(4):253-263
秦国建,许振成,吴根义,等.2011.残留磺胺类抗生素的来源及环境行为研究进展[J].农业灾害研究,1(1):58-60
Reis P J M,Reis A C,Ricken B,et al.2014.Biodegradation of sulfamethoxazole and other sulfonamides by Achromobacter denitrificans PR1 [J].Journal of Hazardous Materials,280:741-749
Richter K,Schicklberger M,Gescher J.2012.Dissimilatory reduction of extracellular electron acceptors in anaerobic respiration [J].Applied and Environmental Microbiology,78(4):913-921
Ricken B,Corvini P F X,Cichocka D,et al.2013.ipso-Hydroxylation and subsequent fragmentation:a novel microbial strategy to eliminate sulfonamide antibiotics [J].Applied and Environmental Microbiology,79(18):5550-5558
Sarmah A K,Meyer M T,Boxall A B A.2006.A global perspective on the use,sales,exposure pathways,occurrence,fate and effects of veterinary antibiotics (VAs) in the environment [J].Chemosphere,65(5):725-759
Tamtam F,Mercier F,Le Bot B,et al.2008.Occurrence and fate of antibiotics in the Seine River in various hydrological conditions [J].Science of the Total Environment,393(1):84-95
Tong L,Huang S B,Wang Y X,et al.2014.Occurrence of antibiotics in the aquatic environment of Jianghan Plain,central China [J].Science of the Total Environment,497:180-187
Wang A J,Sun D,Ren N Q,et al.2010.A rapid selection strategy for an anodophilic consortium for microbial fuel cells [J].Bioresource Technology,101(14):5733-5735
Wang L,Liu Y L,Ma J,et al.2016.Rapid degradation of sulphamethoxazole and the further transformation of 3-amino-5-methylisoxazole in a microbial fuel cell [J].Water Research,88:322-328
汪明霞,王娟,司友斌,等.2014.Shewanella oneidensis MR-1 异化还原Fe(Ⅲ)介导的As(Ⅲ)氧化转化[J].中国环境科学,34(9):2368-2373
肖湘波,唐天乐,徐浩,等.2015.医院典型废水处理工艺单元的抗生素去除效果与评价[J].环境科学与技术,38(4):121-127
许超,董军,马小兰,等.2011.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,31(9):1472-1476
叶计朋,邹世春,张干,等.2007.典型抗生素类药物在珠江三角洲水体中的污染特征[J].生态环境,16(2):384-388
张敏,李轶,敖永华,等.2011.土壤中磺胺类兽药残留的生态效应及转归[J].中国农学通报,27(3):369-373
Zhou C,Wang H Q,Si Y B,et al.2018.Electron shuttles enhance the degradation of sulfamethoxazole coupled with Fe(III) reduction by Shewanella oneidensis MR-1 [J].Environmental Toxicology and Pharmacology,62:156-163
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