采用超声搅拌法,制备十二烷基三甲基氯化铵(DTAC)改性的凹凸棒土,探讨了改性后的DTAC-凹凸棒土对水中苯酚的吸附行为。对比了超声搅拌和机械搅拌这两种工艺在DTAC改性凹凸棒土过程中的作用;优化超声搅拌时间和DTAC/凹凸棒土的用量配比,通过正交试验得到其最佳值分别为9min和40mmol/100g。采用优化改性的DTAC-凹凸棒土对水中苯酚进行吸附研究,结果表明,超声改性的DTAC-凹凸棒土比未改性凹凸棒土的吸附量最多可提高近12倍;碱性条件有利于苯酚的吸附;DTAC-凹凸棒土对苯酚的吸附是一个快速过程,5min即可达到最大吸附容量的80%,动力学过程符合准二级动力学模型,线性相关系数R2=0.9999;吸附等温线符合Langmiur等温吸附模型(R2>0.98),说明该吸附以单层吸附为主;热力学结果表明,该行为是一个自发的、放热的、熵减少的吸附过程。
Dodecyl trimethyl ammonium chloride (DTAC) modified attapulgite was prepared via ultrasonic agitation method,and the adsorption behavior of DTAC-attapulgite for phenol in water was discussed.As comparison,mechanical mixing method was investigated as well.The ultrasonic time and dosage ratio of DTAC/attapulgite were also optimized by orthogonal experiment,which were 9min and 40mmol/100g respectively.The results showed that the adsorption capacity of DTAC-attapulgite could be improved twelve times compared with the natural attapulgite.The adsorption process was proved to be a fast process,and the adsorption capacity could reach 80% of maximum adsorption capacity within 5 minutes.Besides,the adsorption process could be well described by the pseudo-second order kinetic model (R2=0.9999).And Langmuir model was found to be applicable to the prediction of isothermal adsorption (R2>0.98),revealing the adsorption was monolayer.The thermodynamic experimental results showed that the adsorption was a spontaneous,exothermic and entropy-reduction process.
[1] Kakavandi B,Jahangiri-Rad M,Rafiee M,et al.Development of response surface methodology for optimization of phenol and p-chlorophenol adsorption on magnetic recoverable carbon[J].Microporous and Mesoporous Materials,2016,231(1):192-206.
[2] Yang G,Chen H L,Qin H D,et al.Amination of activated carbon for enhancing phenol adsorption:effect of nitrogen-containing functional groups[J].Applied Surface Science,2014,293(28):299-305.
[3] Zhang D F,Huo P L,Liu W.Behavior of phenol adsorption on thermal modified activated carbon[J].Chinese Journal of Chemical Engineering,2016,24(4):446-452.
[4] Jiang J,Gao Y,Pang S Y,et al.Understanding the role of manganese dioxide in the oxidation of phenolic compounds by aqueous permanganate[J].Environmental Science & Technology,2015,49(1):520-528.
[5] Sharma N K,Philip L.Effect of cyanide on phenolics and aromatic hydrocarbons biodegradation under anaerobic and anoxic conditions[J].Chemical Engineering Journal,2014,256(15):255-267.
[6] Wu X P,Gao P,Zhang X L,et al.Synthesis of clay/carbon adsorbent through hydrothermal carbonization of cellulose on palygorskite[J].Applied Clay Science,2014,95(3):60-66.
[7] Zhang X L,Cheng L P,Wu X P,et al.Activated carbon coated palygorskite as adsorbent by activation and its adsorption for methylene blue[J].Journal of Environmental Sciences,2015,33(1):97-105.
[8] 高丽丽,李雪莲,于晶.有机膨润土/酸改性粉煤灰复合材料处理含Cr(Ⅵ)废水[J].太原理工大学学报,2014,45(5):674-678.
[9] 王素青,陈静,陈田田,等.改性凹凸棒土处理含苯酚水的技术[J].工业水处理,2012,32(4):55-58.
[10] 宋燕,王海玲,朱兆连,等.有机改性凹凸棒土的制备表征及其对4-氯苯酚的吸附[J].环境工程学报,2012,6(12):4481-4486.
[11] 包军杰,余贵芬,牛牧晨.邻硝基苯酚在有机改性凹凸棒土上的吸附行为[J].环境化学,2007,26(3):339-342.
[12] Chen L,Wang Y W,He M Y,et al.Facile synthesis of 5A zeolite from attapulgite clay for adsorption of n-paraffins[J].Adsorption-Journal of the International Adsorption Society,2016,3(22):309-314.
[13] 薛广海,高芒来,罗忠新.新型双子表面活性剂改性膨润土对苯酚的吸附特性[J].材料研究学报,2014,28(12):925-933.
[14] 刘宛宜,杨璐泽,于萌,等.聚丙烯酸盐-丙烯酰胺水凝胶的制备及对重金属离子吸附性能的研究[J].分析化学,2016,44(5):707-715.
[15] 史艳婷,张金利,杨庆.白陶土对Pb(Ⅱ)吸附特性[J].大连理工大学学报,2016,56(4):396-405.
基金资助
国家自然科学基金(51408397);山西省自然科学基金(201601D102013)