土壤酸化作用对磺胺氯哒嗪吸附行为的影响
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摘要
参照OECD guideline 106批平衡方法研究酸化作用对磺胺氯哒嗪在黑土中的吸附动力学、吸附热力学以及有机质和离子强度对其吸附的影响。结果显示:酸化作用下磺胺氯哒嗪在黑土中吸附平衡时间为12 h,准二级动力学方程拟合的酸化黑土中的吸附速率常数(k_2)为216.275 5 mg/(g·h),大于对照黑土中的15.722 2 mg/(g·h);从吸附热力学结果看,酸化作用明显提高磺胺氯哒嗪与黑土的结合能力,其吸附量与温度呈负相关;从吸附自由能(ΔG)结果看,其吸附过程是以物理吸附为主的自发反应,但酸化作用使|ΔG|增大,体系更稳定且更易进行自发反应;添加有机质可以增加黑土对磺胺氯哒嗪的吸附,但在酸化黑土中增加效果不如对照黑土;磺胺氯哒嗪在黑土中的吸附能力随背景溶液Ca~(2+)浓度增大而减小,酸化作用下使其与Ca~(2+)产生竞争关系,离子浓度越大竞争能力越强,黑土对磺胺氯哒嗪的吸附量则越少。
The adsorption kinetics, adsorption thermodynamics and the effects of organic matter and ionic strength on the adsorption of sulfachlorpyridazine(SCP) by black soil were studied according to OECD guideline 106. The results showed that the equilibrium time of SCP adsorption by black soil was 12 h under the effect of acidification, the fitting constant(k_2) of adsorption rate of quasi two order kinetic equation was 216.275 5 mg/(g·h) for acidified black soil, higher than that of the control black soil, which was 15.722 2 mg/(g·h). The results of adsorption thermodynamics showed acidification significantly improved the binding capacity of SCP and soil, the adsorption capacity was negatively correlated with temperature. The adsorption free energy(ΔG) showed that the adsorption process was spontaneous reaction mainly by physical adsorption, but acidification increased |ΔG|, which made the system more stable and easier to spontaneous reaction. Adding organic matter increased the SCP adsorption more by the control black soil than acidified black soil. Adsorption capacity of SCP by black soil was decreased with the increase of Ca~(2+) concentration in background solution, which was attributed to the competition between SCP and Ca~(2+) under acidification.
The adsorption kinetics, adsorption thermodynamics and the effects of organic matter and ionic strength on the adsorption of sulfachlorpyridazine(SCP) by black soil were studied according to OECD guideline 106. The results showed that the equilibrium time of SCP adsorption by black soil was 12 h under the effect of acidification, the fitting constant(k_2) of adsorption rate of quasi two order kinetic equation was 216.275 5 mg/(g·h) for acidified black soil, higher than that of the control black soil, which was 15.722 2 mg/(g·h). The results of adsorption thermodynamics showed acidification significantly improved the binding capacity of SCP and soil, the adsorption capacity was negatively correlated with temperature. The adsorption free energy(ΔG) showed that the adsorption process was spontaneous reaction mainly by physical adsorption, but acidification increased |ΔG|, which made the system more stable and easier to spontaneous reaction. Adding organic matter increased the SCP adsorption more by the control black soil than acidified black soil. Adsorption capacity of SCP by black soil was decreased with the increase of Ca~(2+) concentration in background solution, which was attributed to the competition between SCP and Ca~(2+) under acidification.
引文
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[34]张俊平,张新明,王长委,等.模拟酸雨对果园土壤交换性阳离子迁移及其对土壤酸化的影响[J].水土保持学报,2007,21(1):14-17
[35]李文慧,李爱民,王学军.pH值和离子强度对胡敏酸与芘之间相互作用的影响[J].环境化学,2009,28(5):636-639
[2]王嫒华,段增强,赵宇,等.积盐条件下土壤酸化过程的特异性研究[J].土壤学报,2015,52(1):228-233
[3]李玲,王继红,兰丽丽,等.长期施肥条件下土壤养分变化及其与土壤酸度的关系[J].吉林农业大学学报,2017,39(1):55-59
[4]张秀,张黎明,龙军,等.亚热带耕地土壤酸化程度差异及影响因素[J].中国生态农业学报,2017,25(3):441-450
[5]赵其国.我国红壤的退化问题[J].土壤,1995,27(6):281-285
[6]宋文峰.我国东南丘陵区酸化现状调查及长期施肥农田系统的生态化学计量学特征[D].北京:中国科学院大学,2016
[7]张喜林,周宝库,孙磊,等.长期施用化肥和有机肥料对黑土酸度的影响[J].土壤通报,2008,39(5):1221-1223
[8]王寅,张馨月,高强,等.吉林省农田耕层土壤pH的时空变化特征[J].土壤通报,2017,48(2):387-391
[9]于天一,孙秀山,石程仁,等.土壤酸化危害及防治技术研究进展[J].生态学杂志,2014,33(11):3137-3143
[10]Christian T,Schneider R J,F?rber H A,et al.Determination of antibiotics residues in manure,soil and surface waters[J].Actahydrochim Hydrobiol,2003,31:34-44
[11]尹春艳,骆永明,滕应,等.典型设施菜地土壤抗生素污染特征与积累规律研究[J].环境科学,2012,33(8):2810-2816
[12]赵方凯,杨磊,乔敏,等.土壤中抗生素的环境行为及分布特征研究进展[J].土壤,2017,49(3):428-436
[13]赵娜.珠三角地区典型菜地土壤抗生素污染特征研究[D].广州:暨南大学,2007
[14]金彩霞,司晓薇,王子英,等.养殖场周边土壤-蔬菜系统磺胺类药物残留及风险评价[J].环境科学,2016,37(4):1562-1567
[15]提清清,高增文,季慧慧,等.抗生素在土壤中的吸附行为研究进展[J].土壤,2017,49(3):437-445
[16]陈昦,董元华,王辉,等.江苏省畜禽粪便中磺胺类药物残留特征[J].农业环境科学学报,2008,27(1):385-389
[17]Hu X,Zhou Q,Yi L.Occurrence and source analysis of typical veterinary antibiotics in manure,soil,vegetables and groundwater from organic vegetable bases,northern China[J].Environmental Pollution,2010,158(9):2992-2998
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[19]边炜涛,马秀兰,王富民,等.环丙沙星在盐碱土中吸附特性的研究[J].农业环境科学学报,2016,35(10):1953-1959
[20]梅婷.典型土壤矿物对有机胂类药物吸附行为研究[D].南京:南京师范大学,2015
[21]倪进治,骆永明,魏然.土壤有机和无机组分对多环芳烃环境行为影响的研究进展[J].土壤,2006,38(5):559-564
[22]黎卫亮.2,4-二氯苯酚在黄土性土壤中的吸附及迁移转化研究[D].西安:长安大学,2009
[23]孔晶晶,裴志国,温蓓,等.磺胺嘧啶和磺胺噻唑在土壤中的吸附行为[J].环境化学,2008,27(6):736-741
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[26]Thiele-Bruhn S.Pharmaceutical antibiotic compounds in soils-A review[J].Journal of Plant Nutrition and Soil Science,2010,166(2):145-167
[27]李雪冰,付浩,林朋飞,等.p H值对活性炭吸附水中磺胺类抗生素的影响研究[J].中国给水排水,2015(1):56-60
[28]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
[29]杨克武,安凤春,莫汉宏.单甲脒在土壤中的吸附[J].环境化学,1995,14(5):431-435
[30]张妤,王帅,王玉军.乙草胺在酸化黑土中的吸附行为[J].东北林业大学学报,2013(7):137-140
[31]赵涛.不同生物炭对水中磺胺类抗生素的吸附及机理研究[D].广州:华南农业大学,2016
[32]Li W,Johnson C E.Relationships among pH,aluminum solubility and aluminum complexation with organic matter in acid forest soils of the Northeastern United States[J].Geoderma,2016,271:234-242
[33]李晓娜,宋洋,贾明云,等.生物质炭对有机污染物的吸附及机理研究进展[J].土壤学报,2017,54(6):1313-1325
[34]张俊平,张新明,王长委,等.模拟酸雨对果园土壤交换性阳离子迁移及其对土壤酸化的影响[J].水土保持学报,2007,21(1):14-17
[35]李文慧,李爱民,王学军.pH值和离子强度对胡敏酸与芘之间相互作用的影响[J].环境化学,2009,28(5):636-639