基于位点能量分布理论对苯酚和双酚A在沉积物中的竞争吸附研究
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摘要
河流水体和沉积物中酚类EDCs因其广泛存在和危害持久受到广泛关注,为研究自然条件下河流沉积物上多种酚类EDCs共存的吸附行为,本文以苯酚(phenol)和双酚A(bisphenol A,BPA)为目标污染物,灞河表层沉积物为吸附剂,通过静态吸附实验研究二者在单溶质和双溶质体系下的吸附等温特性,在此基础上,采用位点能量分布理论分析污染物之间的竞争吸附机理.结果表明,相同浓度(1～50 mg·L~(-1))条件下,单溶质体系的苯酚吸附位点主要集中于高能量位;双酚A吸附位点主要分布于低能量区.双溶质体系下,相同浓度的两种物质位点分布函数均随着位点能量的增大而呈指数降低,苯酚下降趋势较为平缓,吸附位点分布更均匀.两种体系相比较,双溶质体系下苯酚平均位点能量和位点能量非均质性分别降低0.867%和3.473%,吸附位点数量降低1.230%;双酚A平均位点能量和位点能量非均质分别增大了6.074%和14.992%,吸附位点数量增大6.389%.即双溶质体系下,二者之间存在一定的竞争吸附,双酚A处于竞争优势.
Phenolic EDCs have been driving extensive research interests due to their prevalence and persistence in water and sediments. In this study, the static adsorption experiments, which contained single or dual species of phenol and bisphenol A(BPA) in the system, were carried out to characterize the isotherms of adsorption of the two pollutants on the surface sediments in Ba River. The theory of site energy distribution was employed to interpret the experimental data, so as to understand the mechanisms underlying the competitive adsorption of the two contaminants. In the system that contained the same concentration(1～50 mg·L~(-1)) of single contaminant, the adsorption sites of phenol were mainly in the high energy level, whereas the adsorption sites of bisphenol A were mainly in the low energy region. Compared to phenol, BPA had priority during the process of adsorption on sediments. In the system containing the same concentration(1～50 mg·L~(-1))of dual contaminants, exponential decrease was found for the distribution functions of both substances with the increasing site energy. The decline trend of phenol was more moderate, and the distribution of adsorption sites was more homogeneous. When compared to the single-contaminant system, the average site energy and site energy heterogeneity of phenol in the dual-contaminant system decreased by 0.867% and 3.473%, respectively, and the number of adsorption sites decreased by 1.230%. When compared to the single-contaminant system, the average site energy and site energy heterogeneity of BPA increased by 6.074% and 14.992%, and the number of adsorption sites increased by 6.389%. The results suggest that there is competition between phenol and BPA during the process of adsorption on the sediments, and the bisphenol A was in an advantage position.
Phenolic EDCs have been driving extensive research interests due to their prevalence and persistence in water and sediments. In this study, the static adsorption experiments, which contained single or dual species of phenol and bisphenol A(BPA) in the system, were carried out to characterize the isotherms of adsorption of the two pollutants on the surface sediments in Ba River. The theory of site energy distribution was employed to interpret the experimental data, so as to understand the mechanisms underlying the competitive adsorption of the two contaminants. In the system that contained the same concentration(1～50 mg·L~(-1)) of single contaminant, the adsorption sites of phenol were mainly in the high energy level, whereas the adsorption sites of bisphenol A were mainly in the low energy region. Compared to phenol, BPA had priority during the process of adsorption on sediments. In the system containing the same concentration(1～50 mg·L~(-1))of dual contaminants, exponential decrease was found for the distribution functions of both substances with the increasing site energy. The decline trend of phenol was more moderate, and the distribution of adsorption sites was more homogeneous. When compared to the single-contaminant system, the average site energy and site energy heterogeneity of phenol in the dual-contaminant system decreased by 0.867% and 3.473%, respectively, and the number of adsorption sites decreased by 1.230%. When compared to the single-contaminant system, the average site energy and site energy heterogeneity of BPA increased by 6.074% and 14.992%, and the number of adsorption sites increased by 6.389%. The results suggest that there is competition between phenol and BPA during the process of adsorption on the sediments, and the bisphenol A was in an advantage position.
引文
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Diao P, Chen Q, Wang R, et al. 2017. Phenolic endocrine-disrupting compounds in the Pearl River Estuary: Occurrence, bioaccumulation and risk assessment[J]. Science of the Total Environment, 584: 1100-1107
Gao P, Feng Y, Zhang Z, et al. 2011. Comparison of competitive and synergetic adsorption of three phenolic compounds on river sediment[J]. Environmental Pollution, 159(10):2876-2881
关伟,何江. 2010. 酚类化合物在黄河水体沉积物中的竞争吸附[J]. 安徽农业大学学报, 37(2):333-337
黄丽敏,靳强,杨斌,等. 2017. 位点能量分布理论及其在土壤和沉积物对污染物吸附研究中的应用[J]. 环境化学, 36(11):2424-2433
Huang L, Jin Q, Tandon P, et al. 2018. High-resolution insight into the competitive adsorption of heavy metals on natural sediment by site energy distribution[J]. Chemosphere, 197:411-419
Im J, Prevatte C W, Campagna S R, et al. 2015. Identification of 4-Hydroxycumyl alcohol as the major MnO2-mediated bisphenol A transformation product and evaluation of its environmental fate[J]. Environmental Science & Technology, 49(10):6214-6221
Li J, Jiang L, Xiang X, et al. 2013. Competitive sorption between 17alpha-ethinyl estradiol and bisphenol A/4-n-nonylphenol by soils[J]. Journal of Environmental Sciences, 25(6):1154-1163
李克斌,刘广深,刘维屏. 2003. 酰胺类除草剂在土壤上吸附的位置能量分布分析[J]. 土壤学报, 40(4):574-580
娄保锋,朱利中,杨坤. 2004.苯及其取代物与对硝基苯胺在沉积物上的竞争吸附[J]. 中国环境科学, 24(3): 327-331
路屏. 2012.渭河西安段干支流环境内分泌干扰物调查及分析[D]. 西安:长安大学
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沈伟松. 2017. 基于纳米铁酸盐材料去除染料、重金属和有机污染物及点位能量分布的研究[D].南昌:南昌航空大学
Shi H, Sun Y, Zhao X,et al. 2013. Influence on sorption property of pb by fractal and site energy distribution about sediment of yellow river[J]. Procedia Environmental Sciences, 18:464-471
USEPA. 2010. Bisphenol A Action Plan (CASRN 80-05-7) 2010[R]. U.S. Environmental Protection Agency
王彬. 2012, 酚类环境内分泌干扰物分析方法及滇池水系污染特征研究[D]. 昆明: 昆明理工大学
王驰. 2015. 磺胺甲恶唑和卡马西平在碳纳米材料上的竟争和补充吸附行为研究[D].昆明:昆明理工大学
Wang X, Sato T, Xing B. 2005. Sorption and displacement of pyrene in soils and sediments[J]. Environmental Science & Technology, 39(22): 8712-8718
吴颖虹,汪磊,商博东,等. 2009. 吸附态壬基酚对菲吸附的影响及位点能量分布分析[J]. 环境化学, 28(3):334-338
Yan B, Niu C H. 2016. Modeling and site energy distribution analysis of levofloxacin sorption by biosorbents[J]. Chemical Engineering Journal, 307:631-642
Yan B, Niu C H, Wang J. 2017. Kinetics, electron-donor-acceptor interactions, and site energy distribution analyses of norfloxacin adsorption on pretreated barley straw[J]. Chemical Engineering Journal,330:1211-1221
闫永胜. 2017.河流中酚类内分泌干扰物的污染特征及生态风险评价[D]. 西安:长安大学
杨跃志, 张海丽, 李正炎, 等. 2013.北部湾沿岸表层沉积物中酚类内分泌干扰物与多环芳烃的污染特征及生态风险评价[J]. 中国海洋大学学报: 自然科学版, 43(6): 87-92
Yuan G, Xing B. 1999. Site-energy distribution analysis of organic chemical sorption by soil organic matter[J]. Soil Science, 164(7): 503-509
Zhong W, Wang D, Wang Z. 2018. Distribution and potential ecological risk of 50 phenolic compounds in three rivers in Tianjin, China[J]. Environmental Pollution, 235: 121-128
崔小明. 2015. 国内外苯酚供需现状及发展前景分析[J]. 石油化工技术与经济, 31(3):15-20
Diao P, Chen Q, Wang R, et al. 2017. Phenolic endocrine-disrupting compounds in the Pearl River Estuary: Occurrence, bioaccumulation and risk assessment[J]. Science of the Total Environment, 584: 1100-1107
Gao P, Feng Y, Zhang Z, et al. 2011. Comparison of competitive and synergetic adsorption of three phenolic compounds on river sediment[J]. Environmental Pollution, 159(10):2876-2881
关伟,何江. 2010. 酚类化合物在黄河水体沉积物中的竞争吸附[J]. 安徽农业大学学报, 37(2):333-337
黄丽敏,靳强,杨斌,等. 2017. 位点能量分布理论及其在土壤和沉积物对污染物吸附研究中的应用[J]. 环境化学, 36(11):2424-2433
Huang L, Jin Q, Tandon P, et al. 2018. High-resolution insight into the competitive adsorption of heavy metals on natural sediment by site energy distribution[J]. Chemosphere, 197:411-419
Im J, Prevatte C W, Campagna S R, et al. 2015. Identification of 4-Hydroxycumyl alcohol as the major MnO2-mediated bisphenol A transformation product and evaluation of its environmental fate[J]. Environmental Science & Technology, 49(10):6214-6221
Li J, Jiang L, Xiang X, et al. 2013. Competitive sorption between 17alpha-ethinyl estradiol and bisphenol A/4-n-nonylphenol by soils[J]. Journal of Environmental Sciences, 25(6):1154-1163
李克斌,刘广深,刘维屏. 2003. 酰胺类除草剂在土壤上吸附的位置能量分布分析[J]. 土壤学报, 40(4):574-580
娄保锋,朱利中,杨坤. 2004.苯及其取代物与对硝基苯胺在沉积物上的竞争吸附[J]. 中国环境科学, 24(3): 327-331
路屏. 2012.渭河西安段干支流环境内分泌干扰物调查及分析[D]. 西安:长安大学
Ou Y H, Chang Y J, Lin F Y,et al. 2016. Competitive sorption of bisphenol A and phenol in soils and the contribution of black carbon[J]. Ecological Engineering, 92(2):270-276
沈伟松. 2017. 基于纳米铁酸盐材料去除染料、重金属和有机污染物及点位能量分布的研究[D].南昌:南昌航空大学
Shi H, Sun Y, Zhao X,et al. 2013. Influence on sorption property of pb by fractal and site energy distribution about sediment of yellow river[J]. Procedia Environmental Sciences, 18:464-471
USEPA. 2010. Bisphenol A Action Plan (CASRN 80-05-7) 2010[R]. U.S. Environmental Protection Agency
王彬. 2012, 酚类环境内分泌干扰物分析方法及滇池水系污染特征研究[D]. 昆明: 昆明理工大学
王驰. 2015. 磺胺甲恶唑和卡马西平在碳纳米材料上的竟争和补充吸附行为研究[D].昆明:昆明理工大学
Wang X, Sato T, Xing B. 2005. Sorption and displacement of pyrene in soils and sediments[J]. Environmental Science & Technology, 39(22): 8712-8718
吴颖虹,汪磊,商博东,等. 2009. 吸附态壬基酚对菲吸附的影响及位点能量分布分析[J]. 环境化学, 28(3):334-338
Yan B, Niu C H. 2016. Modeling and site energy distribution analysis of levofloxacin sorption by biosorbents[J]. Chemical Engineering Journal, 307:631-642
Yan B, Niu C H, Wang J. 2017. Kinetics, electron-donor-acceptor interactions, and site energy distribution analyses of norfloxacin adsorption on pretreated barley straw[J]. Chemical Engineering Journal,330:1211-1221
闫永胜. 2017.河流中酚类内分泌干扰物的污染特征及生态风险评价[D]. 西安:长安大学
杨跃志, 张海丽, 李正炎, 等. 2013.北部湾沿岸表层沉积物中酚类内分泌干扰物与多环芳烃的污染特征及生态风险评价[J]. 中国海洋大学学报: 自然科学版, 43(6): 87-92
Yuan G, Xing B. 1999. Site-energy distribution analysis of organic chemical sorption by soil organic matter[J]. Soil Science, 164(7): 503-509
Zhong W, Wang D, Wang Z. 2018. Distribution and potential ecological risk of 50 phenolic compounds in three rivers in Tianjin, China[J]. Environmental Pollution, 235: 121-128
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