滇池泥炭土对两种抗生素和双酚A的吸附
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摘要
用不同浓度Na OH溶液处理采集自云南滇池的泥炭土,研究处理前后的泥炭土对两种抗生素磺胺甲恶唑(SMX)、卡马西平(CBZ)及双酚A(BPA)的吸附机理,并深入探讨3种污染物及泥炭土性质对吸附特性的影响.吸附等温线拟合结果表明,Freundlich模型对3种物质在泥炭土上的吸附等温线有较好的拟合优度.3种物质中,BPA的非线性指数n值最低,这可能是由于其不对称的结构特征导致.随着处理泥炭土的NaOH浓度增加,3种吸附质在泥炭土上的吸附顺序为BPA> CBZ> SMX, BPA的吸附最高可能是由于其含有两个酚羟基,与泥炭土有较强的极性作用导致,而CBZ的吸附比SMX的吸附高是由憎水性作用引起.Na OH处理后并没有增加泥炭土对这3种吸附质的吸附,说明对于离子型化合物,吸附过程和机理复杂,BPA蝴蝶状结构及苯环上含有两个羟基可能导致其在泥炭土上出现特异性吸附,这导致其吸附系数最高;NaOH处理后泥炭土的有机碳含量增加但比表面积可能降低,从而使3种污染物的吸附降低.因此,本研究3种离子型化合物在泥炭土上的吸附受到吸附质的官能团及溶解度、泥炭土的有机碳含量及官能团等多种因素的影响.
The Dianchi peat soil was collected from Dianchi Lake in Kunming, Yunnan, China. The peat soil was treated by different concentrations of NaOH solutions, and effect of alkali solution for the properties of peat soil and the sorption characteristics of contaminants was evaluated. Adsorption mechanisms of two antibiotics, sulfamethoxazole(SMX), carbamazepine(CBZ), and bisphenol A(BPA) on peat soils before/after NaOH treated were discussed. Effects of the properties for contaminants as well as the peat soils on their sorption characteristics were investigated. Adsorption isotherms for SMX, CBZ and BPA were well fitted by the Freundlich model, and the fitting results showed that the Freundlich nonlinearity factor n values of BPA were the lowest among these three contaminants, which may be due to its asymmetric structural characteristics. As the concentration of NaOH increased, adsorption of these three contaminants on peat soils was BPA > CBZ > SMX. BPA has two phenolic hydroxyl groups and thus it could interact with peat soils by polar interaction, this may result in the highest sorption of it on peat soils. Adsorption of CBZ was higher than that of SMX was due to the hydrophobic interactions between CBZ/SMX and peat soils. Adsorption of SMX, CBZ and BPA on peat soils treated by NaOH solutions was not increased, this suggested that the sorption processes and mechanisms of ionic compounds on peat soils were complex, many factors such as functional groups and solubility of contaminants, the contents of organic carbon and functional groups of peat soils affected the sorption. The butterfly structure and two hydroxyl groups of BPA may lead to its specific adsorption on peat soil, which resulted in the highest adsorption coefficient. The organic carbon content of peat soil increased but the specific surface area may decrease after NaOH treated, and thus reducing the adsorption of these three contaminants. Therefore, adsorption of these three ionic compounds on the peat soils was affected by various factors, including the functional groups and solubility of adsorbates, the organic carbon content and functional groups of peat soils in this study.
The Dianchi peat soil was collected from Dianchi Lake in Kunming, Yunnan, China. The peat soil was treated by different concentrations of NaOH solutions, and effect of alkali solution for the properties of peat soil and the sorption characteristics of contaminants was evaluated. Adsorption mechanisms of two antibiotics, sulfamethoxazole(SMX), carbamazepine(CBZ), and bisphenol A(BPA) on peat soils before/after NaOH treated were discussed. Effects of the properties for contaminants as well as the peat soils on their sorption characteristics were investigated. Adsorption isotherms for SMX, CBZ and BPA were well fitted by the Freundlich model, and the fitting results showed that the Freundlich nonlinearity factor n values of BPA were the lowest among these three contaminants, which may be due to its asymmetric structural characteristics. As the concentration of NaOH increased, adsorption of these three contaminants on peat soils was BPA > CBZ > SMX. BPA has two phenolic hydroxyl groups and thus it could interact with peat soils by polar interaction, this may result in the highest sorption of it on peat soils. Adsorption of CBZ was higher than that of SMX was due to the hydrophobic interactions between CBZ/SMX and peat soils. Adsorption of SMX, CBZ and BPA on peat soils treated by NaOH solutions was not increased, this suggested that the sorption processes and mechanisms of ionic compounds on peat soils were complex, many factors such as functional groups and solubility of contaminants, the contents of organic carbon and functional groups of peat soils affected the sorption. The butterfly structure and two hydroxyl groups of BPA may lead to its specific adsorption on peat soil, which resulted in the highest adsorption coefficient. The organic carbon content of peat soil increased but the specific surface area may decrease after NaOH treated, and thus reducing the adsorption of these three contaminants. Therefore, adsorption of these three ionic compounds on the peat soils was affected by various factors, including the functional groups and solubility of adsorbates, the organic carbon content and functional groups of peat soils in this study.
引文
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[3]Chen K L,Liu L C,Chen W R.Adsorption of sulfamethoxazole and sulfapyridine antibiotics in high organic content soils[J].Environmental Pollution,2017,231:1163-1171.
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[10]Liu Y,Liu X,Zhang G,et al.Adsorptive removal of sulfamethazine and sulfamethoxazole from aqueous solution by hexadecyl trimethyl ammonium bromide modified activated carbon[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2019,564:131-141.
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[12]Tobergte D R,Curtis S.Scrutinizing pharmaceuticals and personal care products in wastewater treatment[J].Journal of Chemical Information and Modeling,2013,53:0-9.
[13]Fiedler S,Dame T,Graw M.Do cemeteries emit drugs?A case study from southern Germany[J].Environmental Science and Pollution Research,2018,25(6):5393-5400.
[14]Dwivedi K,Morone A,Chakrabarti T,et al.Evaluation and optimization of Fenton pretreatment integrated with granulated activated carbon(GAC)filtration for carbamazepine removal from complex wastewater of pharmaceutical industry[J].Journal of environmental chemical engineering,2018,6(3):3681-3689.
[15]Rodríguez R V,López A L.Endocrine Disrupting compounds in surface water and their degradation by advanced oxidation process with ozone[M].Water Resources in Mexico.Springer,Berlin,Heidelberg,2012:279-297.
[16]Pahigian J M,Zuo Y.Occurrence,endocrine-related bioeffects and fate of bisphenol A chemical degradation intermediates and impurities:A review[J].Chemosphere,2018,207:469-480.
[17]Qiu W,Chen J,Li Y,et al.Oxidative stress and immune disturbance after long-term exposure to bisphenol A in juvenile common carp(Cyprinus carpio)[J].Ecotoxicology and environmental safety,2016,130:93-102.
[18]裴志国.Cu和Pb对两种苯酚化合物与甲磺隆在土壤和泥炭中吸附行为的影响及其机理研究[D].北京:中国科学院生态环境研究中心,2006.Pei Z G.Effects of Cu and Pb on adsorption behaviors and their mechanisms of two phenol compounds and methyl sulfon in soils and peat[D].Beijing:Research Center for Eco-Environmental Sciences,Chinese Academy of Sciences,2006.
[19]Abata M,Mc Laughlin M J,Kirby J K,et al.Adsorption and desorption of copper and zinc in tropical peat soils of Sarawak,Malaysia[J].Geoderma,2012,175-176:58-63.
[20]吴敏,宁平,刘书言.土壤有机质对诺氟沙星的吸附特征[J].环境化学,2013,32(1):112-117.Wu M,Ning P,Liu S Y.Adsorption characteristics of norfloxacin in soil organic matter fractions[J].Environmental Chemistry,2013,32(1):112-117.
[21]Chen B L,Zhou D D,Zhu L Z.Transitional adsorption and partition of nonpolar and polar aromatic contaminants by biochars of pine needles with different pyrolytic temperatures[J].Environmental Science&Technology,2008,42(14):5137-5143.
[22]Gunasekara A S,Simpson M I,Xing B S.Identification and characterization of sorption domains in soil organic matter using structurally modified humic acids[J].Environmental Science and Technology,2003,37(5):852-858.
[23]陈淼,唐文浩,葛成军,等.氧氟沙星在热带土壤中的吸附行为研究[J].广东农业科学,2015,42(10):146-152.Chen M,Tang W H,Ge C J,et al.Adsorption behavior of ofloxacin in tropical soil[J].Guangdong Agricultural Sciences,2015,42(10):146-152.
[24]Zhang D,Pan B,Wu M,et al.Adsorption of sulfamethoxazole on functionalized carbon nanotubes as affected by cations and anions[J].Environmental Pollution,2011,159(10):2616-2621.
[25]Yang W,Lu Y,Zheng F,et al.Adsorption behavior and mechanisms of norfloxacin onto porous resins and carbon nanotube[J].Chemical Engineering Journal,2012,179(1):112-118.
[26]郭欣妍,王娜,许静,等.5种磺胺类抗生素在土壤中的吸附和淋溶特性[J].环境科学学报,2013,33(11):3083-3091.Guo X Y,Wang N,Xu J,et al.Adsorption and leaching behavior of sulfonamides in soils[J].Acta Scientiae Circumstantiae,2013,33(11):3083-3091.
[27]Wang B,Zeng D,Chen Y,et al.Adsorption behaviors of phenanthrene and bisphenol A in purple paddy soils amended with straw-derived DOM in the West Sichuan Plain of China[J].Ecotoxicology and environmental safety,2019,169:737-746.
[28]Tolls J.Sorption of veterinary pharmaceuticals in soils:a review[J].Environmental Science&Technology,2001,35(17):3397.
[29]吴敏,宁平,李今今.底泥制备的生物炭对卡马西平的吸附解吸研究[J].昆明理工大学学报(自然科学版),2012,37(3):69-73.Wu M.Ning P,Li J J.Sorption/desorption behavior of carbamazepine in biochars derived from sediment of Dianchi Lake[J].Journal of Kunming University of Science and Technology(Science and Technology),2012,37(3):69-73.
[30]Peng H B,Pan B,Wu M,et al.Adsorption of ofloxacin on carbon nanotubes:Solubility,p H and cosolvent effects[J].Journal of Hazardous Materials,2012,211-212(2):342-348.
[31]张娇,耿永娟,朱世富,等.有机质对土壤吸附性能的影响研究[J].青岛理工大学学报,2007,28(6):78-81.Zhang J,Geng Y J,Zhu S F,et al.Study on abdsorption of methylence blue from aqueous solution onto soil with different organic matter contents[J].Journal of Qingdao Technological University,2007,28(6):78-81.
[32]Tang Y L,Wang R C,Huang J F.Relations between red edge characteristics and agronomic parameters of crops[J].Pedosphere,2004,14(4):467-474.
[33]毛真,吴敏,张迪,等.磺胺甲恶唑在土壤上的吸附及其与Ca2+、Mg2+、Zn2+的共吸附[J].环境化学,2013,32(4):640-645.Mao Z,Wu M,Zhang D,et al.Adsorption behavior of sulfamethoxazole on soils and its co-adsorption with Ca2+,Mg2+or Zn2+[J].Environmental Chemistry,2013,32(4):640-645.
[34]杨慧敏,李云桂,武彩霞,等.川西北沙化土壤对双酚A的吸附特征[J].中国环境科学,2018,38(4):1424-1432.Yang H M,Li Y G,Wu C X,et al.The characteristic sorption of bisphenol A on sandy soil in northwest Sichuan[J].China Environmental Science,2018,38(4):1424-1432.
[2]Wang N,Guo X,Xu J,et al.Sorption and transport of five sulfonamide antibiotics in agricultural soil and soil-manure systems[J].Journal of Environmental Science and Health,Part B,2015,50(1):23-33.
[3]Chen K L,Liu L C,Chen W R.Adsorption of sulfamethoxazole and sulfapyridine antibiotics in high organic content soils[J].Environmental Pollution,2017,231:1163-1171.
[4]Wang N,Guo X Y,Shan Z J,et al.Prioritization of veterinary medicines in China's environment[J].Human and Ecological Risk Assessment:An International Journal,2014,20(5):1313-1328.
[5]Thiele-Bruhn S.Pharmaceutical antibiotic compounds in soils-a review[J].Journal of plant nutrition and soil science,2003,166(2):145-167.
[6]Zhang D,Pan B,Zhang H,et al.Contribution of different sulfamethoxazole species to their overall adsorption on functionalized carbon nanotubes[J].Environmental Science&Technology,2010,44(10):3806-3811.
[7]Demoling L A,B??th E,Greve G,et al.Effects of sulfamethoxazole on soil microbial communities after adding substrate[J].Soil Biology&Biochemistry,2009,41(4):840-848.
[8]Wang J,Gao M,Ding F,et al.Organo-vermiculites modified by heating and gemini pyridinium surfactants:Preparation,characterization and sulfamethoxazole adsorption[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2018,546:143-152.
[9]Marc L F,Premasis S,Sebastian Z,et al.Metabolism of 14C-labelled and non-labelled sulfadiazine after administration to pigs[J].Analytical&Bioanalytical Chemistry,2007,388(8):1733-1745.
[10]Liu Y,Liu X,Zhang G,et al.Adsorptive removal of sulfamethazine and sulfamethoxazole from aqueous solution by hexadecyl trimethyl ammonium bromide modified activated carbon[J].Colloids and Surfaces A:Physicochemical and Engineering Aspects,2019,564:131-141.
[11]Deng W,Li N,Zheng H,et al.Occurrence and risk assessment of antibiotics in river water in Hong Kong[J].Ecotoxicology and Environmental Safety,2016,125:121-127.
[12]Tobergte D R,Curtis S.Scrutinizing pharmaceuticals and personal care products in wastewater treatment[J].Journal of Chemical Information and Modeling,2013,53:0-9.
[13]Fiedler S,Dame T,Graw M.Do cemeteries emit drugs?A case study from southern Germany[J].Environmental Science and Pollution Research,2018,25(6):5393-5400.
[14]Dwivedi K,Morone A,Chakrabarti T,et al.Evaluation and optimization of Fenton pretreatment integrated with granulated activated carbon(GAC)filtration for carbamazepine removal from complex wastewater of pharmaceutical industry[J].Journal of environmental chemical engineering,2018,6(3):3681-3689.
[15]Rodríguez R V,López A L.Endocrine Disrupting compounds in surface water and their degradation by advanced oxidation process with ozone[M].Water Resources in Mexico.Springer,Berlin,Heidelberg,2012:279-297.
[16]Pahigian J M,Zuo Y.Occurrence,endocrine-related bioeffects and fate of bisphenol A chemical degradation intermediates and impurities:A review[J].Chemosphere,2018,207:469-480.
[17]Qiu W,Chen J,Li Y,et al.Oxidative stress and immune disturbance after long-term exposure to bisphenol A in juvenile common carp(Cyprinus carpio)[J].Ecotoxicology and environmental safety,2016,130:93-102.
[18]裴志国.Cu和Pb对两种苯酚化合物与甲磺隆在土壤和泥炭中吸附行为的影响及其机理研究[D].北京:中国科学院生态环境研究中心,2006.Pei Z G.Effects of Cu and Pb on adsorption behaviors and their mechanisms of two phenol compounds and methyl sulfon in soils and peat[D].Beijing:Research Center for Eco-Environmental Sciences,Chinese Academy of Sciences,2006.
[19]Abata M,Mc Laughlin M J,Kirby J K,et al.Adsorption and desorption of copper and zinc in tropical peat soils of Sarawak,Malaysia[J].Geoderma,2012,175-176:58-63.
[20]吴敏,宁平,刘书言.土壤有机质对诺氟沙星的吸附特征[J].环境化学,2013,32(1):112-117.Wu M,Ning P,Liu S Y.Adsorption characteristics of norfloxacin in soil organic matter fractions[J].Environmental Chemistry,2013,32(1):112-117.
[21]Chen B L,Zhou D D,Zhu L Z.Transitional adsorption and partition of nonpolar and polar aromatic contaminants by biochars of pine needles with different pyrolytic temperatures[J].Environmental Science&Technology,2008,42(14):5137-5143.
[22]Gunasekara A S,Simpson M I,Xing B S.Identification and characterization of sorption domains in soil organic matter using structurally modified humic acids[J].Environmental Science and Technology,2003,37(5):852-858.
[23]陈淼,唐文浩,葛成军,等.氧氟沙星在热带土壤中的吸附行为研究[J].广东农业科学,2015,42(10):146-152.Chen M,Tang W H,Ge C J,et al.Adsorption behavior of ofloxacin in tropical soil[J].Guangdong Agricultural Sciences,2015,42(10):146-152.
[24]Zhang D,Pan B,Wu M,et al.Adsorption of sulfamethoxazole on functionalized carbon nanotubes as affected by cations and anions[J].Environmental Pollution,2011,159(10):2616-2621.
[25]Yang W,Lu Y,Zheng F,et al.Adsorption behavior and mechanisms of norfloxacin onto porous resins and carbon nanotube[J].Chemical Engineering Journal,2012,179(1):112-118.
[26]郭欣妍,王娜,许静,等.5种磺胺类抗生素在土壤中的吸附和淋溶特性[J].环境科学学报,2013,33(11):3083-3091.Guo X Y,Wang N,Xu J,et al.Adsorption and leaching behavior of sulfonamides in soils[J].Acta Scientiae Circumstantiae,2013,33(11):3083-3091.
[27]Wang B,Zeng D,Chen Y,et al.Adsorption behaviors of phenanthrene and bisphenol A in purple paddy soils amended with straw-derived DOM in the West Sichuan Plain of China[J].Ecotoxicology and environmental safety,2019,169:737-746.
[28]Tolls J.Sorption of veterinary pharmaceuticals in soils:a review[J].Environmental Science&Technology,2001,35(17):3397.
[29]吴敏,宁平,李今今.底泥制备的生物炭对卡马西平的吸附解吸研究[J].昆明理工大学学报(自然科学版),2012,37(3):69-73.Wu M.Ning P,Li J J.Sorption/desorption behavior of carbamazepine in biochars derived from sediment of Dianchi Lake[J].Journal of Kunming University of Science and Technology(Science and Technology),2012,37(3):69-73.
[30]Peng H B,Pan B,Wu M,et al.Adsorption of ofloxacin on carbon nanotubes:Solubility,p H and cosolvent effects[J].Journal of Hazardous Materials,2012,211-212(2):342-348.
[31]张娇,耿永娟,朱世富,等.有机质对土壤吸附性能的影响研究[J].青岛理工大学学报,2007,28(6):78-81.Zhang J,Geng Y J,Zhu S F,et al.Study on abdsorption of methylence blue from aqueous solution onto soil with different organic matter contents[J].Journal of Qingdao Technological University,2007,28(6):78-81.
[32]Tang Y L,Wang R C,Huang J F.Relations between red edge characteristics and agronomic parameters of crops[J].Pedosphere,2004,14(4):467-474.
[33]毛真,吴敏,张迪,等.磺胺甲恶唑在土壤上的吸附及其与Ca2+、Mg2+、Zn2+的共吸附[J].环境化学,2013,32(4):640-645.Mao Z,Wu M,Zhang D,et al.Adsorption behavior of sulfamethoxazole on soils and its co-adsorption with Ca2+,Mg2+or Zn2+[J].Environmental Chemistry,2013,32(4):640-645.
[34]杨慧敏,李云桂,武彩霞,等.川西北沙化土壤对双酚A的吸附特征[J].中国环境科学,2018,38(4):1424-1432.Yang H M,Li Y G,Wu C X,et al.The characteristic sorption of bisphenol A on sandy soil in northwest Sichuan[J].China Environmental Science,2018,38(4):1424-1432.
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