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使用铁包覆颗粒活性炭吸附剂从水中吸附去除亚硒酸盐

Adsorptive selenite removal from water using iron-coated GAC adsorbents.

作者信息

Zhang Ning, Lin Lian-Shin, Gang Dianchen

机构信息

Department of Civil and Environmental Engineering, West Virginia University, Morgantown, WV 26506, USA.

出版信息

Water Res. 2008 Aug;42(14):3809-16. doi: 10.1016/j.watres.2008.07.025. Epub 2008 Jul 25.

Abstract

Removal of selenite from aqueous phase using iron-coated granular activated carbons (GAC) was investigated in this study. Five different types of GAC were used for iron coating by oxidizing ferrous chloride with sodium hypochlorite and the iron-coated GAC (Fe-GAC) were tested for selenite removal. Nitrogen adsorption-desorption analyses indicated that Brunauer-Emmett-Teller (BET) specific surface area, pore size, and pore volume decreased with the iron coating. The Darco 12x20 GAC was shown to be the most effective adsorbent among the five tested GACs after iron coating. Among the different concentrations used for iron coating, the Darco 12x20 GAC coated with 0.1M ferrous chloride achieved the highest selenite removal (97.3%). High removal efficiency of selenite occurred in a wide range of pH (i.e., 2-8), but the efficiency decreased when pH was higher than 8. Adsorption kinetics showed that selenite removal efficiency reached more than 90% after 6-h adsorption for initial selenium concentration of 2mg/L and equilibrium was obtained after 48h. A pseudo-second-order kinetic model was found to characterize the adsorption kinetics well for all the initial selenium concentrations and temperatures tested (R(2)> or =0.9969). Three temperatures (25, 35, 45 degrees C) were used to examine temperature effect on the adsorption behavior of the Fe-GAC with initial selenium concentration of 1mg/L. Activation energy was calculated to be 30.42kJ/mol. Adsorption isotherms for initial selenium concentration of 2mg/L at various temperatures and ionic strengths were developed and the data generally fit the Langmuir model well (R(2)> or =0.994). The adsorption capacity reached as high as 2.50mg-Se/g-adsorbent at equilibrium for initial concentration of 2mg/L at 25 degrees C. The Gibbs free energy was determined to be negative, indicating the spontaneous nature of the adsorption reaction. Oxyanion competitive adsorption showed that sulfate (0.1-5mM) barely affected selenite adsorption. Other anions (phosphate, silicate and carbonate) impact selenite adsorption to various degrees with phosphate completely excluded selenite adsorption at 5mM. The possible adsorption mechanisms were discussed.

摘要

本研究考察了用铁负载颗粒活性炭(GAC)从水相中去除亚硒酸盐的效果。通过用次氯酸钠氧化氯化亚铁,使用五种不同类型的GAC进行铁负载,并测试了铁负载GAC(Fe-GAC)对亚硒酸盐的去除效果。氮气吸附-脱附分析表明,随着铁负载,Brunauer-Emmett-Teller(BET)比表面积、孔径和孔体积均减小。结果表明,在五种测试的GAC中,Darco 12x20 GAC负载铁后是最有效的吸附剂。在用于铁负载的不同浓度中,负载0.1M氯化亚铁的Darco 12x20 GAC对亚硒酸盐的去除率最高(97.3%)。在较宽的pH范围(即2-8)内,亚硒酸盐的去除效率较高,但当pH高于8时,效率降低。吸附动力学表明,对于初始硒浓度为2mg/L的情况,吸附6小时后亚硒酸盐去除效率达到90%以上,48小时后达到平衡。发现伪二级动力学模型能很好地表征所有测试的初始硒浓度和温度下的吸附动力学(R²≥0.9969)。使用三个温度(25、35、45℃)考察了温度对初始硒浓度为1mg/L的Fe-GAC吸附行为的影响。计算得到活化能为30.42kJ/mol。建立了不同温度和离子强度下初始硒浓度为2mg/L的吸附等温线,数据总体上很好地拟合了Langmuir模型(R²≥0.994)。在25℃下,对于初始浓度为2mg/L的情况,平衡时吸附容量高达2.50mg-Se/g吸附剂。吉布斯自由能为负,表明吸附反应是自发的。含氧阴离子竞争吸附表明,硫酸盐(0.1-5mM)对亚硒酸盐吸附几乎没有影响。其他阴离子(磷酸盐、硅酸盐和碳酸盐)对亚硒酸盐吸附有不同程度的影响,其中磷酸盐在5mM时完全抑制亚硒酸盐吸附。文中讨论了可能的吸附机制。

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