Synergistic effect of co-metabolism and nitration for the removal of EE2 by AOB
WANG Li-li, JIANG Xiao-man, Li An-jie
Key Laboratory of Water and Sand Science, Ministry of Education, State Key Laboratory of Water Environment Simulation, School of Environment, Beijing Normal University, Beijing 100875, China
Abstract:In this study, Nitrosomonas europaea, one type of ammonia oxidizing bacteria, was used to remove 17α-ethinylestradiol (EE2). The role of ammonia nitrogen in EE2 degradation by AOB and the degradation mechanism of EE2 were investigated. The results showed that degradation of EE2 by N. europaea was a co-metabolic process, and ammonia nitrogen was necessary for co-metabolism of EE2. The NO2--N produced during the ammonia oxidation process could nitrate EE2 under acidic condition. The nitration of EE2 obeyed first-order reaction kinetics and the degradation rate constants were positively correlated with the concentration of nitrite, H+ and FNA. The biodegradation of EE2 by N. europaea was proved by suppressing nitration of EE2 through controlling pH higher than 7.5. The co-metabolism reaction fitted first-order kinetic model with the degradation rate constant of 0.0069h-1. Biodegradation and nitration of EE2 were synergistic for EE2 removal when pH was lower than 7.5 during ammonia oxidation process. And EE2 removal by synergistic function obeyed first-order reaction kinetics with the degradation rate constant of 0.0093h-1. In addition, unreported EE2 biodegradation product M613 was found in this study. Its estrogen effect and toxicity need to be further investigated.
王丽丽, 姜晓满, 李安婕. AOB去除炔雌醇的共代谢与硝基化协同作用[J]. 中国环境科学, 2020, 40(12): 5246-5252.
WANG Li-li, JIANG Xiao-man, Li An-jie. Synergistic effect of co-metabolism and nitration for the removal of EE2 by AOB. CHINA ENVIRONMENTAL SCIENCECE, 2020, 40(12): 5246-5252.
胡双庆,袁哲军,沈根祥.典型畜禽粪污中雌激素排放特征[J]. 环境科学研究, 2020,33(1):227-234. Hu S Q, Yuan Z J, Shen G X. Characteristics of estrogen emission in typical animal manure[J]. Environmental Science Research, 2020, 33(1):227-234.
[2]
De Gusseme B, Pycke B, Hennebel T, et al. Biological removal of 17α-ethinylestradiol by a nitrifier enrichment culture in a membrane bioreactor[J]. Water Research, 2009,43(9):2493-2503.
[3]
Hamid H, Eskicioglu C. Fate of estrogenic hormones in wastewater and sludge treatment:A review of properties and analytical detection techniques in sludge matrix[J]. Water Research, 2012,46(18):5813-5833.
[4]
Kruglova A, Krakstrom M, Riska M, et al. Comparative study of emerging micropollutants removal by aerobic activated sludge of large laboratory-scale membrane bioreactors and sequencing batch reactors under low-temperature conditions[J]. Bioresource Technology, 2016, 214:81-88.
[5]
Song H L, Yang X L, Xia M Q, et al. Co-metabolic degradation of steroid estrogens by heterotrophic bacteria and nitrifying bacteria in MBRs[J]. Journal of Environmental Science and Health Part A-Toxic/Hazardous Substances & Environmental Engineering, 2017, 52(8):778-784.
[6]
Suarez S, Lema J M, Omil F. Removal of Pharmaceutical and Personal Care Products (PPCPs) under nitrifying and denitrifying conditions[J]. Water Research, 2010,44(10):3214-3224.
[7]
Zhang Z, Feng Y, Su H, et al. Influence of operating parameters on the fate and removal of three estrogens in a laboratory-scale AAO system[J]. Water Science and Technology, 2015,71(11):1701-1708.
[8]
Dytczak M A, Londry K L, Oleszkiewicz J A. Biotransformation of estrogens in nitrifying activated sludge under aerobic and alternating anoxic/aerobic conditions[J]. Water Environment Research, 2008, 80(1):47-52.
[9]
Jantanaprasartporn A, Maneerat S, Rongsayamanont C. Importance of culture history on 17alpha-ethinylestradiol cometabolism by nitrifying sludge[J]. Environmental Engineering Research, 2018,23(1):28-35.
[10]
Vader J S, van Ginkel C G, Sperling F M G M, et al. Degradation of ethinyl estradiol by nitrifying activated sludge[J]. Chemosphere, 2000,41(8):1239-1243.
[11]
Zhou X, Oleszkiewicz J A. Biodegradation of oestrogens in nitrifying activated sludge[J]. Environmental Technology, 2010,31:1263-1269.
[12]
Khunjar W O, Mackintosh S A, Skotnicka-Pitak J, et al. Elucidating the relative roles of ammonia oxidizing and heterotrophic bacteria during the biotransformation of 17α-ethinylestradiol and trimethoprim[J]. Environmental Science & Technology, 2011,45(8):3605-3612.
[13]
Skotnicka-Pitak J, Khunjar W O, Love N G, et al. Characterization of Metabolites Formed During the Biotransformation of 17alpha-ethinylestradiol by Nitrosomonas europaea in Batch and Continuous Flow Bioreactors[J]. Environmental Science & Technology, 2009, 43(10):3549-3555.
[14]
Shi J, Fujisawa S, Nakai S, et al. Biodegradation of natural and synthetic estrogens by nitrifying activated sludge and ammonia-oxidizing bacterium Nitrosomonas europaea [J]. Water Research, 2004, 38(9):2323-2330.
[15]
吴凡,高品,薛罡,等.硝化细菌对碘普罗胺的降解及作用机制[J]. 环境工程学报, 2014,6:2225-2230. Wu F, Gao P, Xue G, et al. Degradation of ioprolamine by nitrifying bacteria and its mechanism of action[J]. Journal of Environmental Engineering. 2014,6:2225-2230.
[16]
Yi T, Jr. Harper W F. The link between nitrification and biotransformation of 17alpha-ethinylestradiol[J]. Environmental Science & Technology, 2007,41(12):4311-4316.
[17]
Gaulke L S, Strand S E, Kalhorn T F, et al. 17[alpha]-ethinylestradiol transformation via abiotic nitration in the presence of ammonia oxidizing bacteria[J]. Environmental Science & Technology, 2008, 42(20):7622.
[18]
熊英,向斯,程凯.一株高适应性Nitrosomonas eutropha CZ-4的脱氨特性[J]. 中国环境科学, 2019,39(8):3365-3372. Xiong Y, Xiang S, Cheng K. Deamination of highly adaptable Nitrosomonas Eutropha CZ-4[J]. China Environmental Science, 2019,39(8):3365-3372.
[19]
Stein L Y, Arp D J. Loss of ammonia monooxygenase activity in Nitrosomonas europaea upon exposure to nitrite[J]. Applied and Environmental Microbiology, 1998,64(10):4098-4102.
[20]
Yang L, Chang Y, Chou M. Feasibility of bioremediation of trichloroethylene contaminated sites by nitrifying bacteria through cometabolism with ammonia[J]. Journal of Hazardous Materials, 1999,69(1):111-126.
[21]
Gaulke L S, Strand S E, Kalhorn T F, et al. Estrogen nitration kinetics and implications for wastewater treatment[J]. Water Environment Research, 2009,81(8):772-778.
[22]
刘婳.氨氮与TMP对氨单加氧酶活性位点的竞争抑制作用的研究[D]. 西安:西安建筑科技大学, 2012. Liu H. Study on the Competitive inhibitory effect of ammonia nitrogen and TMP on the active site of ammonia monooxygenase[D]. Xi'an:Xi'an University of Architecture and Technology, 2012.
[23]
Wendeborn S. The chemistry, biology, and modulation of ammonium nitrification in soil[J]. Angewandte Chemie-International Edition, 2020,59(6):2182-2202.
[24]
Keener W K, Arp D J. Transformations of aromatic-compounds by Nitrosomonas europaea [J]. Applied and Environmental Microbiology, 1994,60(6):1914-1920.
[25]
Khunjar W O, Klein C, Skotnicka-Pitak J, et al. Biotransformation of pharmaceuticals and personal care products (PPCPs) during nitrification:The role of ammonia oxidizing bacteria versus heterotrophic bacteria[J]. Proceedings of the Water Environment Federation, 2008:132-145.
[26]
Li Y, Liu D, Li L, et al. Advances in co-metabolic technology of refractory organic pollutants and micro-organisms[J]. Modern Chemical Industry, 2019,39:25-28,34.
[27]
Anthonisen A C, Loehr R C, Prakasam T, et al. Inhibition of nitrification by ammonia and nitrous-acid[J]. Journal Water Pollution Control Federation, 1976,48(5):835-852.
[28]
Sun F, Wu D, Chua F D, et al. Free nitrous acid (FNA) induced transformation of sulfamethoxazole in the enriched nitrifying culture[J]. Water Research, 2019,149:432-439.
[29]
徐硕.好氧污泥氨氧化活性对雌激素降解效率的影响研究[D]. 北京:北京大学, 2013. Xu Shuo. Study on the effect of ammonia-oxidation activity of aerobic sludge on the degradation efficiency of estrogen[D]. Beijing:Peking University, 2013.
[30]
Zhu B T, Han G, Shim J, et al. Quantitative structure-activity relationship of various endogenous estrogen metabolites for human estrogen receptor alpha and beta subtypes:Insights into the structural determinants favoring a differential subtype binding[J]. Endocrinology, 2006,147(9):4132-4150.
[31]
Wang L, Zhang F, Liu R, et al. FeCl3/NaNO2:An efficient photocatalyst for the degradation of aquatic steroid estrogens under natural light irradiation[J]. Environmental Science & Technology, 2007,41(10):3747-3751.
[32]
Chapman E, Best M D, Hanson S R, et al. Sulfotransferases:Structure, mechanism, biological activity, inhibition, and synthetic utility[J]. Angewandte Chemie-International Edition, 2004,43(27):3526-3548.
[33]
Chain P, Lamerdin J, Larimer F, et al. Complete genome sequence of the ammonia-oxidizing bacterium and obligate chemolithoautotroph Nitrosomonas europae[J]. Journal Of Bacteriology, 2003,185(21):6496.