高级搜索

典型雌激素在水稻土中的吸附特征及高岭土和猪粪DOM对吸附的影响

,  ,  ,  ,  ,  , 

downloadPDF

上一篇

下一篇

袁哲军, 张洪昌, 胡双庆, 沈根祥, 钱晓雍, 王振旗, 张玉. 典型雌激素在水稻土中的吸附特征及高岭土和猪粪DOM对吸附的影响[J]. 环境化学, 2018, 37(4): 652-660. doi: 10.7524/j.issn.0254-6108.2017082102
引用本文: 袁哲军, 张洪昌, 胡双庆, 沈根祥, 钱晓雍, 王振旗, 张玉. 典型雌激素在水稻土中的吸附特征及高岭土和猪粪DOM对吸附的影响[J]. 环境化学, 2018, 37(4): 652-660. doi: 10.7524/j.issn.0254-6108.2017082102
shu
YUAN Zhejun, ZHANG Hongchang, HU Shuangqing, SHEN Genxiang, QIAN Xiaoyong, WANG Zhenqi, ZHANG Yu. Adsorption of typical estrogens to paddy soils and influence of kaolin and pig manure DOM[J]. Environmental Chemistry, 2018, 37(4): 652-660. doi: 10.7524/j.issn.0254-6108.2017082102
Citation: YUAN Zhejun, ZHANG Hongchang, HU Shuangqing, SHEN Genxiang, QIAN Xiaoyong, WANG Zhenqi, ZHANG Yu. Adsorption of typical estrogens to paddy soils and influence of kaolin and pig manure DOM[J]. Environmental Chemistry, 2018, 37(4): 652-660. doi: 10.7524/j.issn.0254-6108.2017082102
shu

典型雌激素在水稻土中的吸附特征及高岭土和猪粪DOM对吸附的影响

  • 1.

    上海市环境科学研究院, 上海, 200233;

  • 2.

    华东理工大学资源与环境工程学院, 上海, 200237

  • 基金项目:

    国家水体污染控制与治理科技重大专项（2017ZX07207002），国家自然科学基金青年科学基金（21607105）和上海市环保科研项目（2016-2，2016-3）资助.

Adsorption of typical estrogens to paddy soils and influence of kaolin and pig manure DOM

  • 1.

    Shanghai Academy of Environmental Sciences, Shanghai, 200233, China;

  • 2.

    College of Resources and Environmental Engineering, East China University of Science and Technology, Shanghai, 200237, China

  • Fund Project: Supported by the National Water Pollution Control and Treatment Science and Technology Major Project(2017ZX07207002), Young Scientists Fund of the National Natural Science Foundation of China(21607105) and Scientific Research Program of Shanghai Environmental Protection Bureau,China(2016-2, 2016-3).

  • 摘要: 畜禽粪污还田资源化利用的同时，带来了雌激素类物质污染风险，而吸附特性决定了雌激素的土壤环境风险和生物可利用性.为掌握雌激素在土壤中的吸附特性，采用批吸附室内模拟实验研究了典型雌激素雌酮（E1）、雌二醇（E2）和炔雌醇（EE2）在水稻土中的吸附动力学和热力学特征，以及掺杂高岭土和添加猪粪溶解性有机质（DOM）对土壤吸附雌激素的影响.结果表明，E1、E2和EE2的吸附动力学均符合拟二级反应动力学方程（R2>0.997），热力学特征可用Freundlich吸附等温式描述（R2>0.990）.总体水平上，高岭土掺杂比例与3种雌激素土壤吸附能力呈显著正相关（PKF）减小，而E2的KF值出现先增大后减小的现象.综合分析表明，高岭土能促进土壤对雌激素的吸附，且氢键作用和游离羟基是增强吸附的重要原因；而猪粪DOM会降低土壤对雌激素的吸附，从而增加雌激素从土壤迁移到地表水和地下水中的风险.
    Abstract: Extensive use of livestock and poultry manure in agriculture has increased in the risk of estrogens contamination. Soil environmental risk and bioavailability are largely influenced by estrogen adsorption properties. Batch equilibrium experiments were conducted to study the adsorption kinetics and thermodynamic characteristics of estrogen(E1), estradiol(E2) and 17a-ethinylestradiol (EE2) to paddy soil and the influence of kaolin and dissolved organic matter(DOM) derived from pig manure on the sorption. The results indicated that the adsorption kinetics of E1, E2 and EE2 were fit well with the pseudo second order reaction kinetics equation(R2>0.997). Additionally, the thermodynamic characteristics can be statistically described by Freundlich isotherm(R2>0.990). In general, each estrogen adsorption capacity showed a significant positive relation to the kaolin content(PKF) of E1 and EE2 decreased, while the KF value of E2 increased first and then decreased. In conclusion, kaolin could promote the adsorption of estrogens on the soil. The hydrogen bonding and free hydroxyl groups play an important role in enhancings the adsorption. The pig manure DOM could reduce the adsorption of the estrogens to the soil, and thus increase the risk of estrogens migration from the soil to the surface water and groundwater.
  • 加载中
  • [1] COMBALBERT S, BELLET V, DABERT P, et al. Fate of steroid hormones and endocrine activities in swine manure disposal and treatment facilities[J]. Water Research, 2011, 46(3):895-906.
    [2] ZhANG H, SHI J H, LIU X W, 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.
    [3] KHANAL S K, XIE B, THOMPSON M L, et al. Fate, transport, and biodegradation of natural estrogens in the environment and engineered systems[J]. Environmental Science & Technology, 2006, 40(21):6537-6546.
    [4] LORENAEN A, HENDEL J G, CONN K L, et al. Survey of hormone activities in municipal biosolids and animal manures[J]. Environmental Toxicology, 2004, 19(3):216-225.
    [5] CHUN S, LEE J, RADOSEVICH M, et al. Influence of agricultural antibiotics and 17beta-estradiol on the microbial community of soil[J]. Journal of Environmental Science & Health.part.b Pesticides Food Contaminants & Agricultural Wastes, 2006, 41(6):923-935.
    [6] 田琳, 张珣. 雌酮胁迫农田土壤微生物群落结构变化研究[J]. 生物技术通报, 2017, 33(6):230-236.

    TIAN L, ZHANG, X. Study on the changes of soil microbial community structure in farmland by estrone stress[J]. Biotechnology Bulletin, 2017, 33(6):230-236(in Chinese).

    [7] ARNON S, DAHAN O, ELHANANY S, et al. Transport of testosterone and estrogen from dairy-farm waste lagoons to groundwater.[J]. Environmental Science & Technology, 2008, 42(15):5521-5526.
    [8] CHEFETZ B, XING B. Relative role of aliphatic and aromatic moieties as sorption domains for organic compounds:A review[J]. Environmental Science & Technology, 2009, 43(6):1680-1688.
    [9] 赵晓丽, 毕二平. 水溶性有机质对土壤吸附有机污染物的影响[J]. 环境化学, 2014, 33(2):256-261.

    ZHAO X L, BI E P. Effects of dissolved organic matter on the sorption of organic pollutants to soils[J]. Environmental Chemistry, 2014, 33(2):256-261 (in Chinese).

    [10] 张丰松, 李艳霞, 杨明, 等. 畜禽粪便堆肥溶解态有机质三维荧光光谱特征及Cu络合[J].农业工程学报, 2011, 27(1):314-319.

    ZHANG F S, LI Y X, YANG M, et al. Change of three-dimentional excitation emission matrix fluorescence spectroscopic characterization of manure dissolved organic matter after composting and influence on its complexation with Cu[J]. Transactions of the CSAE, 2011, 27(1):314-319(in Chinese).

    [11] LUCAS S D, JONES D L. Urine enhances the leaching and persistence of estrogens in soils.[J]. Soil Biology & Biochemistry, 2009, 41(2):236-242.
    [12] 张丰松, 李艳霞, 黄泽春, 等. 雌二醇在土壤/沉积物中的吸附特征及猪粪DOM对吸附的影响[J]. 环境科学, 2012, 33(10):3542-3546.

    ZHANG F S, LI Y X, HUANG Z C, et al. Sorption of 17β-estradiol to soils and sediment and influence of pig manure DOM[J]. Environmental Science, 2012, 33(10):3542-3546(in Chinese).

    [13] 袁东海, 张孟群, 高士祥, 等. 几种粘土矿物和粘粒土壤吸附净化磷素的性能和机理[J]. 环境化学, 2005, 24(1):7-11.

    YUAN D H, ZHANG M Q, GAO S X, et al. The abilities and mechanisms of adsorption phosphorus in some clay minerls and soils[J]. Environmental Chemistry, 2005, 24(1):7-11(in Chinese).

    [14]
    [15] 李鱼, 张琛, 刘建林, 等. 掺杂MnO2土壤对多种雌激素化合物的吸附热力学特征及机理[J]. 高等学校化学学报, 2013, 34(3):634-640.

    LI Y, ZHANG C, LIU J L, et al. Thermodynamic characteristics and mechanisms of estrogen hormones adsorption on soil doped with MnO2[J]. Chemical Journal of Chinese Universities, 2013, 34(3):634-640(in Chinese).

    [16] 高姣. 大孔树脂对硝基苯酚的吸附行为研究及其在废水处理中的应用[D]. 南京:东南大学, 2010. GAO J. Adsorptive behavior of nitrobenzenes by macroporous resin and its application to wastewater stewater tn treatment[D]. Nanjing:Southeast University, 2010(in Chinese).
    [17] TOOR M, JIN B. Adsorption characteristics, isotherm, kinetics, and diffusion of modified natural bentonite for removing diazo dye[J]. Chemical Engineering Journal, 2012, 187(2):79-88.
    [18] VENKATA M S, SHAILAJA S, RAMA K M, et al. Adsorptive removal of phthalate ester (Di-ethyl phthalate) from aqueous phase by activated carbon:A kinetic study[J]. Journal of Hazardous Materials, 2007, 146(1-2):278-282.
    [19] VIMONSES V, LEI S, JIN B, et al. Adsorption of congo red by three Australian kaolins[J]. Applied Clay Science, 2009, 43(3):465-472.
    [20] KANDPAL G, SRIVASTAVA P C, RAM B. Kinetics of desorption of heavy metals from polluted soils:influence of soil type and metal source[J]. Water Air & Soil Pollution, 2005, 161(1-4):353-363.
    [21] YU Z, XIAO B, HUANG W, et al. Sorption of steroid estrogens to soils and sediments[J]. Environmental Toxicology & Chemistry, 2004, 23(3):531-539.
    [22] 党志, 于虹, 黄伟林,等. 土壤/沉积物吸附有机污染物机理研究的进展[J]. 化学通报, 2001, 64(2):81-85.

    DANG Z, YU H, HUANG W L, et al. Research advances on the mechanism of soil/sediment adsorption of organic pollutants[J]. Chemistry, 2001, 64(2):81-85(in Chinese).

    [23] 刘建林. 雌激素化合物在土壤中的吸附行为及生物降解研究[D]. 北京:华北电力大学, 2012. LIU J L. Study on the adsorption behaviors and biodegradation of estrogen chemicals in soil system[J]. Beijing:North China Electric Power University, 2012(in Chinese).
    [24] 张锡秋, 方邺森, 胡利勋. 高岭土[M]. 北京:轻工业出版社, 1988:3-14. ZHANG X Q, FANG Y S, HU L X. Kaolinite[M]. Beijing:Light Industry Press, 1988:3

    -14(in Chinese).

    [25] 武庭, 周敏, 万建新, 等. 膨润土和高岭土对四环素吸附的影响[J]. 农业环境科学学报, 2009, 28(5):914-918.

    WU T, ZHOU M, WAN J X, et al. Influence of montmorillonite and kaolinite on tetracycline adsorption[J]. Journal of Agro-Environment Science, 2009, 28(5):914-918(in Chinese).

    [26] ZHANG Z Z, SPARKS D L, SCRIVNER N C. Sorption and desorption of quaternary amine cations on clays[J]. Environmental Science & Technology, 1993, 27(8):3958-3959.
    [27] 王玉, 张一平, 陈思根. 中国6种地带性土壤红外光谱特征研究[J]. 西北农林科技大学学报(自然科学版), 2003, 31(1

    ):57-61. WANG Y, ZHANG Y P, CHEN S G. The characteristics of infrared spectrum of 6 typical zonal soils in China[J]. Journal of Northwest Sci-Tech University of Agriculture and Forestry, 2003, 31(1):57-61(in Chinese).

    [28] SUVRAMANIAN M K, ANBARASAN P M, MANIMEGALAI S. DFT simulations and vibrational analysis of FT-IR and FT-Raman spectra of 2,4-diamino-6-hydroxypyrimidine[J]. Spectrochimica Acta Part A Molecular & Biomolecular Spectroscopy, 2009, 73(4):642-649.
    [29] SHENG G D, CHAO X, LEI X, et al. Abiotic oxidation of 17β-estradiol by soil manganese oxides.[J]. Environmental Pollution, 2009, 157(10):2710-2715.
    [30] STUMPE B, MARSCHNER B. Dissolved organic carbon from sewage sludge and manure can affect estrogen sorption and mineralization in soils.[J]. Environmental Pollution, 2010, 158(1):148-154.
    [31] FLORES-CESPEDES F, FERNANDEZ-PEREZ M, VILLAFRANCA-SANCHEZ M, et al. Cosorption study of organic pollutants and dissolved organic matter in a soil.[J]. Environmental Pollution, 2006, 142(3):449-456.
    [32] BARRIUSO E, BAER U, CALVET R. Dissolved organic matter and adsorption-desorption of dimefuron, atrazine, and carbetamide by soils[J]. Journal of Environmental Quality, 1992, 21(3):359-367.
    [33] 张丰松, 胡海平, 黄泽春, 等. 雄烯二酮在我国典型土壤中的吸附特性[J]. 生态毒理学报, 2014, 9(1):114-120.

    ZHANG F S, HU H P, HUANG Z C, et al. Sorption of androstenedione on typical soils of China[J]. Asian Journal of Ecotoxicology, 2014, 9(1):114-120(in Chinese).

    [34] GAO Y, XIONG W, LING W, et al. Impact of exotic and inherent dissolved organic matter on sorption of phenanthrene by soils[J]. Journal of Hazardous Materials, 2007, 140(1):138-144.
  • 加载中
WeChat 点击查看大图
计量
  • 文章访问数:  1644
  • HTML全文浏览数:  1601
  • PDF下载数:  316
  • 施引文献:  0
出版历程
  • 收稿日期:  2017-08-21
  • 刊出日期:  2018-04-15
袁哲军, 张洪昌, 胡双庆, 沈根祥, 钱晓雍, 王振旗, 张玉. 典型雌激素在水稻土中的吸附特征及高岭土和猪粪DOM对吸附的影响[J]. 环境化学, 2018, 37(4): 652-660. doi: 10.7524/j.issn.0254-6108.2017082102
引用本文: 袁哲军, 张洪昌, 胡双庆, 沈根祥, 钱晓雍, 王振旗, 张玉. 典型雌激素在水稻土中的吸附特征及高岭土和猪粪DOM对吸附的影响[J]. 环境化学, 2018, 37(4): 652-660. doi: 10.7524/j.issn.0254-6108.2017082102
shu
YUAN Zhejun, ZHANG Hongchang, HU Shuangqing, SHEN Genxiang, QIAN Xiaoyong, WANG Zhenqi, ZHANG Yu. Adsorption of typical estrogens to paddy soils and influence of kaolin and pig manure DOM[J]. Environmental Chemistry, 2018, 37(4): 652-660. doi: 10.7524/j.issn.0254-6108.2017082102
Citation: YUAN Zhejun, ZHANG Hongchang, HU Shuangqing, SHEN Genxiang, QIAN Xiaoyong, WANG Zhenqi, ZHANG Yu. Adsorption of typical estrogens to paddy soils and influence of kaolin and pig manure DOM[J]. Environmental Chemistry, 2018, 37(4): 652-660. doi: 10.7524/j.issn.0254-6108.2017082102
shu

典型雌激素在水稻土中的吸附特征及高岭土和猪粪DOM对吸附的影响

  • 1.  上海市环境科学研究院, 上海, 200233;
  • 2.  华东理工大学资源与环境工程学院, 上海, 200237
  • 收稿日期:  2017-08-21
基金项目:

国家水体污染控制与治理科技重大专项（2017ZX07207002），国家自然科学基金青年科学基金（21607105）和上海市环保科研项目（2016-2，2016-3）资助.

摘要: 畜禽粪污还田资源化利用的同时，带来了雌激素类物质污染风险，而吸附特性决定了雌激素的土壤环境风险和生物可利用性.为掌握雌激素在土壤中的吸附特性，采用批吸附室内模拟实验研究了典型雌激素雌酮（E1）、雌二醇（E2）和炔雌醇（EE2）在水稻土中的吸附动力学和热力学特征，以及掺杂高岭土和添加猪粪溶解性有机质（DOM）对土壤吸附雌激素的影响.结果表明，E1、E2和EE2的吸附动力学均符合拟二级反应动力学方程（R2>0.997），热力学特征可用Freundlich吸附等温式描述（R2>0.990）.总体水平上，高岭土掺杂比例与3种雌激素土壤吸附能力呈显著正相关（PKF）减小，而E2的KF值出现先增大后减小的现象.综合分析表明，高岭土能促进土壤对雌激素的吸附，且氢键作用和游离羟基是增强吸附的重要原因；而猪粪DOM会降低土壤对雌激素的吸附，从而增加雌激素从土壤迁移到地表水和地下水中的风险.

English Abstract

    全文HTML

参考文献 (34)

返回顶部

目录

/

返回文章
返回

Copyright © 2019 中国科学院生态环境研究中心