BS-12+DAS复配修饰膨润土对苯酚、菲的不同吸附模式和机理
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摘要
为探究阴离子型表面修饰剂对两性修饰膨润土吸附不同类型有机污染物的影响,采用阴离子型表面修饰剂正十烷基磺酸钠(DAS)对两性修饰剂十二烷基二甲基甜菜碱(BS-12)修饰膨润土进行复配修饰,恒温浸泡处理法研究复配修饰膨润土对疏水性不同的有机污染物苯酚和菲的吸附模式差异及原因,并对比了不同温度、pH和离子强度条件下供试土样吸附苯酚及菲的吸附量及表观热力学参数。结果表明:BS+DAS复配修饰土样对苯酚及菲的吸附量随DAS修饰比例的增大而减小,且苯酚吸附量变化更为显著,复配修饰土样对苯酚的吸附模式为"无限"型分配吸附,对菲为"有限"型分配吸附;供试土样对苯酚及菲的吸附均为物理吸附,呈现增温负效应;pH升高促进了供试土样对苯酚的吸附,抑制了菲的吸附;离子强度在0.001~0.1 mol L~(-1)范围内,可促进供试土样对苯酚及菲的吸附;热力学参数结果表明,BS+DAS两性复配修饰膨润土对苯酚及菲的吸附是自发的物理吸附过程,DAS增大了土样表面正辛醇/水分配系数的对数(logP),造成了苯酚及菲吸附模式的不同,结果证实,以化学修饰方式增强土样有机碳含量以增加对不同疏水性有机污染物的吸附,不但要考虑有机碳含量的影响,同时也要考虑土样表面有机相和污染物之间"相溶性"的差异。
【Objective】Bentonite is a cheap and efficient adsorbent that reduces the mobility of organic and inorganic pollutants in soil.Once chemically modified, the bentonite can increase its organic pollutantsadsorption capacity. As organic pollutants are different in hydrophobicity, they are adsorbed by different mechanisms, such as distribution, surface, charge attraction,even on the same surface. However, the current researchesare focusing mainly on single surface modification of bentonite adsorbing a single organic pollutant, with little attention to complex amphoteric anionic compound modified bentonite adsorbing organic pollutants different in hydrophobicity on its surface via different mechanisms and its causes.In this paper, Dodecyl dimethyl betaine(BS) modified bentonite was remodified with anionic surfactant Sodium 1-decanesulfonate(DAS). Analysis was done of effects of modification rates on adsorption capacity of the modified bentonite and its apparent thermodynamic parameters of phenol and phenanthrene, and further of differences in adsorption of organic pollutants different in hydrophobicity and its causes.【Method】Sodium bentonite was purchased from the Xinyang Tongchuang Bentonite Company and further purified. BS is an amphoteric surface modifier and DAS an anionic surface modifier. BS modified bentonite and BS+-DAS combined modified bentonite were prepared with the wet method. 50 BS means that the modification ratio of BSis 50% CEC, whereas 100 BS+100 DAS means indicates that the modification ratio of both BSand DAS was 100% CEC. Phenol and phenanthrene had 9 levels of concentration forming a gradient. A batch adsorption experiment was done, placing 0.2000 g of soil sample into each 50 mlcentrifuge tube(plastic or glass), adding 20.00 mlof phenol or phenanthrene solution(25% v/v, Dimethyl sulfoxide as solvent), separately into plastic tube or glass tube, covering each tube with a lid andsealing the lid with glue to prevent volatilation of phenol and phenanthrene,putting the tubes on an oscillator with constant temperature for 24 hours of oscillation and then on a centrifugeforcentrifugation, determining equilibrium concentration of phenol or phenanthrene in the supernatant, and in the end calculating adsorption of phenol or phenanthrene in the solution using the subtraction method.【Result】Results show that adsorption of phenol and phenanthrene on BS+DAS bentonite decreased with increasing anionic modification ratio, the effect of the BS+-DAS bentonite inhibiting phenol adsorption was more significant; the sorption of phenol on the bentonite were of the mode of "unsaturated"partitioning, while the sorption of phenanthrene of the mode of"saturated"partitioning; and both were physisorption. rising temperatureinhibited the sorption of both, but rising pH promoted the adsorption of phenol while inhibiting the adsorption of phenanthrene; Ionic strength, in the solution varying in the range ofof 0.001 mol L~(-1)~0.1 mol L~(-1) KNO_3 in concentration, enhanced phenol and phenanthrene adsorption; the analysis of thermodynamic parameter shows that the adsorptions of phenol and phenanthrene on BS+DAS bentonite were spontaneous process, while the adsorptions triggered by improvement of the logarithmic n-octanol/water partition coefficient(logP) by DAS on the surface of BS+DAS bentonite were different in mechanism.【Conclusion】To improve the soil sample's capacity of adsorbing organic pollutants different in hydrophobicity by modifying the soil sample chemically to increase its organic carbon content, it is essential not only to take into consideration the effect of organic carbon content, but also to take into account variation of the intermiscibilitybetween organic phase of the soil surface and pollutions.
【Objective】Bentonite is a cheap and efficient adsorbent that reduces the mobility of organic and inorganic pollutants in soil.Once chemically modified, the bentonite can increase its organic pollutantsadsorption capacity. As organic pollutants are different in hydrophobicity, they are adsorbed by different mechanisms, such as distribution, surface, charge attraction,even on the same surface. However, the current researchesare focusing mainly on single surface modification of bentonite adsorbing a single organic pollutant, with little attention to complex amphoteric anionic compound modified bentonite adsorbing organic pollutants different in hydrophobicity on its surface via different mechanisms and its causes.In this paper, Dodecyl dimethyl betaine(BS) modified bentonite was remodified with anionic surfactant Sodium 1-decanesulfonate(DAS). Analysis was done of effects of modification rates on adsorption capacity of the modified bentonite and its apparent thermodynamic parameters of phenol and phenanthrene, and further of differences in adsorption of organic pollutants different in hydrophobicity and its causes.【Method】Sodium bentonite was purchased from the Xinyang Tongchuang Bentonite Company and further purified. BS is an amphoteric surface modifier and DAS an anionic surface modifier. BS modified bentonite and BS+-DAS combined modified bentonite were prepared with the wet method. 50 BS means that the modification ratio of BSis 50% CEC, whereas 100 BS+100 DAS means indicates that the modification ratio of both BSand DAS was 100% CEC. Phenol and phenanthrene had 9 levels of concentration forming a gradient. A batch adsorption experiment was done, placing 0.2000 g of soil sample into each 50 mlcentrifuge tube(plastic or glass), adding 20.00 mlof phenol or phenanthrene solution(25% v/v, Dimethyl sulfoxide as solvent), separately into plastic tube or glass tube, covering each tube with a lid andsealing the lid with glue to prevent volatilation of phenol and phenanthrene,putting the tubes on an oscillator with constant temperature for 24 hours of oscillation and then on a centrifugeforcentrifugation, determining equilibrium concentration of phenol or phenanthrene in the supernatant, and in the end calculating adsorption of phenol or phenanthrene in the solution using the subtraction method.【Result】Results show that adsorption of phenol and phenanthrene on BS+DAS bentonite decreased with increasing anionic modification ratio, the effect of the BS+-DAS bentonite inhibiting phenol adsorption was more significant; the sorption of phenol on the bentonite were of the mode of "unsaturated"partitioning, while the sorption of phenanthrene of the mode of"saturated"partitioning; and both were physisorption. rising temperatureinhibited the sorption of both, but rising pH promoted the adsorption of phenol while inhibiting the adsorption of phenanthrene; Ionic strength, in the solution varying in the range ofof 0.001 mol L~(-1)~0.1 mol L~(-1) KNO_3 in concentration, enhanced phenol and phenanthrene adsorption; the analysis of thermodynamic parameter shows that the adsorptions of phenol and phenanthrene on BS+DAS bentonite were spontaneous process, while the adsorptions triggered by improvement of the logarithmic n-octanol/water partition coefficient(logP) by DAS on the surface of BS+DAS bentonite were different in mechanism.【Conclusion】To improve the soil sample's capacity of adsorbing organic pollutants different in hydrophobicity by modifying the soil sample chemically to increase its organic carbon content, it is essential not only to take into consideration the effect of organic carbon content, but also to take into account variation of the intermiscibilitybetween organic phase of the soil surface and pollutions.
引文
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[6]Jing X R,Wang Y Y,Liu W J,et al.Enhanced adsorption performance of tetracycline in aqueous solutions by methanol-modified biochar.Chemical Engineering Journal,2014,248:168-174
[7]徐仲艳,王晓蓉.改性土壤对模拟含硝基苯废水的吸附.环境化学,2002,21(3):235-239Xu Z Y,Wang X R.Sorption of nitrobenzene in simulated nitrobenzene polluted water by modified soils(In Chinese).Environmental Chemistry,2002,21(3):235-239
[8]赵景婵,郭治安,袁红安.改性土壤对苯系物的吸附行为研究.西北大学学报(自然科学版),2001,31(4):300-302Zhao J C,Guo Z A,Yuan H A.Sorption properties and mechanisms of benzene homologue on surfactantmodified soil(In Chinese).Journal of Northwest University(Natural Science Edition),2001,31(4):300-302
[9]蒋渊,李坤权,杨美蓉,等.硝酸改性对不同介孔结构生物质炭铅吸附的影响.环境工程学报,2016,10(9):4887-4894Jiang Y,Li K Q,Yang M R,et al.Effects of Pb2+adsorption on biomass-based carbons with different mesoporous structures modified with nitric acid(In Chinese).Chinese Journal of Environmental Engineering,2016,10(9):4887-4894
[10]Fang C,Zhang T,Li P,et al.Application of magnesium modified corn biochar for phosphorus removal and recovery from swine wastewater.International Journal of Environmental Research&Public Health,2014,11(9):9217-9237
[11]李婷,孟昭福,张斌.两性修饰膨润土对苯酚的吸附及热力学特征.环境科学,2012,33(5):1632-1638Li T,Meng Z F,Zhang B.Adsorption of amphoteric midified bentonites to phenol and its thermodynamics(In Chinese).Environmental Science,2012,33(5):1632-1638
[12]任爽,孟昭福,刘伟,等.两性修饰磁性膨润土的表征及其对苯酚的吸附.农业环境科学学报,2017,36(1):108-115Ren S,Meng Z F,Liu W,et al.Characterization and adsorption performance of phenol on amphoteric modified magnetic bentonite(In Chinese).Journal of Agro-Environment Science,2017,36(1):108-115
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[14]余璐,孟昭福,李文斌,等.CTMAB对BS-12修饰膨润土的复配修饰模式.土壤学报,2016,53(2):543-551Yu L,Meng Z F,Li W B,et al.Mechanism of CTMABmodifying BS-12 modified bentonite(In Chinese).Acta Pedologica Sinica,2016,53(2):543-551
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