养殖场沼液中雌激素排放特征及去除效果研究

余薇薇, 杨硕, 杨伦, 杜邦昊, 万巧玲, 陈垚, 谢明扬

中国环境科学 ›› 2020, Vol. 40 ›› Issue (5) : 2103-2109.

PDF(397 KB)
PDF(397 KB)
中国环境科学 ›› 2020, Vol. 40 ›› Issue (5) : 2103-2109.
水污染与控制

养殖场沼液中雌激素排放特征及去除效果研究

  • 余薇薇1, 杨硕1, 杨伦1, 杜邦昊1, 万巧玲2, 陈垚1, 谢明扬1
作者信息 +

Study of emission characteristics and removal efficiency of estrogens in biogas slurry at farm

  • YU Wei-wei1, YANG Shuo1, YANG Lun1, DU Bang-hao1, WAN Qiao-ling2, CHEN Yao1, XIE Ming-yang1
Author information +
文章历史 +

摘要

为探究典型奶牛养殖场沼液中类固醇雌激素的排放特征,采用固相萃取-高效液相色谱串联质谱(SPE-HPLC-MS/MS)分析方法,对重庆市某奶牛养殖场厌氧池和好氧池出水中类固醇雌激素进行夏、秋、冬3季连续监测.结果表明:类固醇雌激素(含雌酮;17α-雌二醇;17β-雌二醇;雌三醇;硫酸雌酮)在厌氧池和好氧池出水中总浓度分别在347.28~2117.65ng/L和10.75~1070.00ng/L之间,其中厌氧池出水以雌酮(E1)、17α-雌二醇(17α-E2)和17β-雌二醇(17β-E2)为主,好氧池出水以E1和17β-E2为主.研究显示:好氧处理对E1、17β-E2、17α-E2的平均去除率达85.70%、56.82%、57.32%,厌氧处理可有效去除硫酸雌酮(E1-3S).在微生物作用下,厌氧和好氧处理均存在E1、17α-E2和17β-E2的相互转化,但雌三醇(E3)的低检出率则显示体系中雌激素转化为E3的比例较低.对雌激素活性(EEQ95th)的评估显示厌氧-好氧处理后雌激素活性平均降低70.34%,但沼液的雌激素生态环境风险仍不可忽视,需持续观察及研究.

Abstract

To explore the emission characteristics of steroid estrogens in biogas slurry, the anaerobic and aerobic tank effluent samples were continuously monitored in summer, autumn, and winter by solid phase extraction-high performance liquid chromatography-tandem mass spectrometry (SPE-HPLC-MS/MS) analysis method from a typical dairy farm in Chongqing city, China. The results showed that the total amounts of five steroid estrogens (estrone; 17α-estradiol; 17β-estradiol; estriol; estrone-3-sulfate) were ranged at 347.28~2117.65ng/L and 10.75~1070.00ng/L in anaerobic and aerobic tank effluent, respectively. The anaerobic tank effluent was dominated by E1, 17α-E2, and 17β-E2, and the aerobic tank effluent was dominated by E1 and 17β-E2.The average removal efficiency of E1, 17β-E2, and 17α-E2by aerobic treatment reached 85.70%, 56.82%, and 57.32%, respectively. Moreover, E1-3S was effectively removed under anaerobic treatment. Under the effect of microorganisms, the interconversion amongE1, 17α-E2, and 17β-E2 was found both in anaerobic and aerobic treatment. However, the low detection frequency of E3 indicated that the ratio of estrogen to E3 was lower in the system. The assessment of simulated estrogen activity (EEQ95th) was reduced by an average of 70.34% after anaerobic-aerobic treatment, but the estrogens ecological risk of biogas slurry could not be ignored and required continuous monitoring.

关键词

风险评估 / 类固醇雌激素 / 厌氧-好氧处理 / 沼液

Key words

anaerobic-aerobic treatment / biogas slurry / risk assessment / steroid estrogens

引用本文

导出引用
余薇薇, 杨硕, 杨伦, 杜邦昊, 万巧玲, 陈垚, 谢明扬. 养殖场沼液中雌激素排放特征及去除效果研究[J]. 中国环境科学. 2020, 40(5): 2103-2109
YU Wei-wei, YANG Shuo, YANG Lun, DU Bang-hao, WAN Qiao-ling, CHEN Yao, XIE Ming-yang. Study of emission characteristics and removal efficiency of estrogens in biogas slurry at farm[J]. China Environmental Science. 2020, 40(5): 2103-2109
中图分类号: X703   

参考文献

[1] Douglas P, Robertson S, Gay R, et al. A systematic review of the public health risks of bioaerosols from intensive farming[J]. Int J Hyg Environ Health, 2018,221(2):134-173.
[2] 宋晓明,杨悦锁,温玉娟,等.雌激素在地下环境中的归宿及其生态调控[J]. 中国环境科学, 2016,36(9):2828-2840. Song X M, Yang Y S, Wen Y J, et al. Fate and ecological regulation of steroidal estrogens in subsurface environment[J]. China Environmental Science, 2016,36(9):2828-2840.
[3] 马晓雁,倪梦婷,倪永炯,等.UV体系中3种微量类固醇雌激素的竞争降解及同趋转化[J]. 中国环境科学, 2014,34(4):904-911. Ma X Y, Ni M T, Ni Y J, et al. Competitive degradation and transformation trend of three steroid estrogens in UV system[J]. China Environmental Science, 2014,34(4):904-911.
[4] 余薇薇,朱家悦,陈垚,等.集约化养殖场中类固醇雌激素的环境行为与处理途径[J]. 环境工程, 2017,35(3):174-178. Yu W W, Zhu J Y, Chen Y, et al. Research advances in environmental behavior and treatments of Steroid estrogens in intensive farm[J]. Environmental Engineering, 2017,35(3):174-178.
[5] Yu W W, Du B H, Yang L, et al. Occurrence, sorption, and transformation of free and conjugated natural steroid estrogens in the environment[J]. Environmental Science and Pollution Research, 2019,26(10):9443-9468.
[6] Czarny K, Szczukocki D, Krawczyk B, et al. The impact of estrogens on aquatic organisms and methods for their determination[J]. Critical Reviews in Environmental Science and Technology, 2017,47(11):909-963.
[7] Acshimoto T, Murakami T. Removal and degradation cacracteristics of natural and synthetic estrogens by activated sludge in batch experiments[J]. Water Research, 2009,43(3):573-582.
[8] Du H, Gao W, Li J, et al. Effects of digested biogas slurry application mixed with irrigation water on nitrate leaching during wheat-maize rotation in the North China Plain[J]. Agricultural Water Management, 2019,213:882-893.
[9] Zhang H, Shi J, Liu X, et al. Occurrence and removal of free estrogens, conjugated estrogens, and bisphenol A in manure treatment facilities in East China[J]. Water Research, 2014,58(7):248-257.
[10] Fang T Y, Praveena S M, deBurbure, et al. Analytical techniques for steroid estrogens in water samples-Areview[J]. Chemosphere, 2016, 165:358-368.
[11] Zhang H, Shi J, Liu X, et al. Occurrence and removal of free estrogens, conjugated estrogens, and bisphenol A in manure treatment facilities in East China[J]. Water Research, 2014,58:248-257.
[12] 阳春,纪中旭,胡碧波,等.污水中基于酶活性分析的硫酸雌酮雌激素效应[J]. 中国环境科学, 2018,38(1):369-373. Yang C, Xu J Z, Hu B B, et al. The estrogenic activity release of estrone-3-sulfate in sewage based on enzyme activity analysis[J]. China Environmental Science, 2018,38(1):369-373.
[13] Zhang Y, Snow D D, Bartelthunt S. Stereoselective degradation of estradiol and trenbolone isomers in alluvial sediment[J]. Environmental Science & Technology, 2016,50(24):13256-13264.
[14] 宋晓明.农业土壤中类固醇雌激素的潜在风险与归趋机理研究[D]. 沈阳:沈阳大学, 2018. Song X M. Study on potential risk and fate and transport mechanism of steroid estrogens in agricultural soil[D]. Shenyang:Shenyang University, 2018.
[15] Noguera-Oviedo K, Aga D S. Chemical and biological assessment of endocrine disrupting chemicals in a full scale dairy manure anaerobic digester with thermal pretreatment[J]. Science of The Total Environment, 2016,550:827-834.
[16] Gadd J B, Tremblay L A, Northcott G L. Steroid estrogens, conjugated estrogens and estrogenic activity in farm dairy shed effluents[J]. Environmental Pollution, 2010,158(3):730-736.
[17] 余薇薇,杜邦昊,张敏讷,等.环境中自由及结合态雌激素的酶降解转化研究进展[J]. 生物技术通报, 2019,35(4):151-162. Yu W W, Du B H, Zhang M N, et al. A review on enzymatic degradation and transformation mechanisms of free and conjugated estrogens in the environment[J]. Biotechnology Bulletin, 2019,35(4):151-162.
[18] 朱宏鹄,常志州,叶小梅,等.太湖地区规模奶牛场粪尿年产生量估算[J]. 江苏农业学报, 2010,22(3):517-521. Zhu H H, Chang Z Z, Ye X M, et al. Estimate of annual excretion in a large-scale cattle farm in Taihu district[J]. Jiangsu Journal of Agricultural Sciences, 2010,22(3):517-521.
[19] Xu N, Xu Y F, Xu S, et al. Removal of estrogens in municipal wastewater treatment plants:a Chinese perspective[J]. Environmental Pollution, 2012,165:215-224.
[20] Robinson J A, Ma Q, Staveley J P, et al. Degradation and transformation of 17α-estradiol in water-sediment systems under controlled aerobic and anaerobic conditions[J]. Environmental Toxicology and Chemistry, 2017,36(3):621-629.
[21] Dai Y N, Dan A, Yang Y, et al. Factors affecting behavior of phenolic endocrine disruptors, estrone and estradiol, in constructed wetlands for domestic sewage treatment[J]. Environmental Science & Technology, 2016,50(21):11844-11852.
[22] Stadler L B, Love N G. Impact of microbial physiology and microbial community structure on pharmaceutical fate driven by dissolved oxygen concentration in nitrifying bioreactors[J]. Water Research, 2016,104:189-199.
[23] Furuichi T, Kannan K, Suzuki K, et al. Occurrence of estrogenic compounds in and removal by a swine farm waste treatment plant[J]. Environ Sci Technol, 2006,40(24):7896-7902.
[24] Zheng W, Yates S R, Bradford S A. Analysis of Steroid Hormones in a Typical Dairy Waste Disposal System[J]. Environmental Science & Technology, 2008,42(2):530.
[25] Mashtare M L, Green D A, Lee L S. Biotransformation of 17α-and 17β-estradiol in aerobic soils[J]. Chemosphere, 2013,90(2):647-652.
[26] Thompson K, Zhang J, Zhang C. Use of fugacity model to analyze temperature-dependent removal of micro-contaminants in sewage treatment plants[J]. Chemosphere, 2011,84(8):1066-1071.
[27] Sun Y, Huang H, Sun Y, et al. Ecological risk of estrogenic endocrine disrupting chemicals in sewage plant effluent and reclaimed water[J]. Environmental Pollution, 2013,180(3):339-344.
[28] Zhao X M, Grimes K L, Colosi L M, et al. Attenuation, transport, and management of estrogens:A review[J]. Chemosphere, 2019,230:462-478.
[29] Rodriguez N C, Bjorklund E, Halling S B, et al. Biogas final digestive byproduct applied to croplands as fertilizer contains high levels of steroid hormones[J]. Environmental Pollution, 2013,180:386-371.
[30] Suzuki Y, Kubota A, Furukawa T, et al. Residual of 17beta-estradiol in digestion liquid generated from a biogas plant using livestock waste[J]. Journal of Hazardous Materials, 2009,165(1-3):667-682.

基金

国家自然科学基金资助项目(51608079;51709024);重庆交通大学河海学院研究生教育创新基金资助项目(YC2019008;YC2019004);国家内河航道整治工程技术研究中心开放基金资助项目(SLK2018A04);重庆市基础科学与前沿技术研究项目(cstc2017jcyjAX0292)


PDF(397 KB)

Accesses

Citation

Detail

段落导航
相关文章

/