Aher Ashish, Thompson Samuel, Nickerson Trisha, Ormsbee Lindell, Bhattacharyya Dibakar
Chemicals and Materials Engineering Department, University of Kentucky, 177 FPAT Bldg, Lexington, KY, 40506, USA.
Civil Engineering Department, University of Kentucky, Lexington, KY, 40506, USA.
RSC Adv. 2019;9(66):38547-38557. doi: 10.1039/c9ra08178j. Epub 2019 Nov 26.
This study explores the integration of separation performance of rGO membrane with heterogeneous oxidation reactions for remediation of organic contaminants from water. Herein, an approach was introduced based on layer-by-layer assembly for functionalizing rGO membranes with polyacrylic acid and then by synthesis of Fe based reactive nanoparticles. TEM characterization of the cross-section lamella of the membranes showed a high density of nanoparticles (12% Fe) in the functionalized domain, signifying the importance of polyacrylic acid for synthesis of nanoparticles. The membranes exhibited a pure water permeability of 1.9 LMH bar. The membranes had low to moderate salt retention, and more than 90% neutral red retention (organic probe molecule, size: 1.2 nm). The membranes also exhibited high retention of humic acids (80%), preventing these organics from entering the reactive domain, and thus potentially reducing the formation of undesired by-products. A persulfate mediated oxidative pathway was employed to demonstrate the reactive removal of organic contaminants. The membranes achieved >95% conversion by convectively passing 2 mM persulfate feed at a transmembrane pressure of 0.4 bar. Successful degradation of TCE (up to 61%) was achieved in a single pass by convective flowing of the feed solution through the membrane, generating up to 80% of the theoretical maximum chloride as one of the byproducts. Elevated temperatures significantly enhanced persulfate mediated TCE oxidation extent from 24% at 23 oC to 54% at 40 o C under batch operating conditions.
本研究探索了还原氧化石墨烯(rGO)膜的分离性能与非均相氧化反应相结合用于去除水中有机污染物的方法。在此,介绍了一种基于层层组装的方法,先用聚丙烯酸对rGO膜进行功能化,然后合成铁基反应性纳米颗粒。对膜的横截面薄片进行透射电子显微镜(TEM)表征,结果表明在功能化区域纳米颗粒(铁含量为12%)密度很高,这表明聚丙烯酸对纳米颗粒合成的重要性。这些膜的纯水渗透率为1.9 LMH·bar。膜对盐的截留率低至中等,对中性红(有机探针分子,尺寸:1.2 nm)的截留率超过90%。膜对腐殖酸的截留率也很高(80%),可防止这些有机物进入反应区域,从而有可能减少不需要的副产物的形成。采用过硫酸盐介导的氧化途径来证明对有机污染物的反应性去除。通过在0.4 bar的跨膜压力下对流通过2 mM过硫酸盐进料,这些膜实现了>95%的转化率。通过使进料溶液对流通过膜,一次通过即可成功降解三氯乙烯(TCE,降解率高达61%),产生高达理论最大氯化物量80%的氯化物作为副产物之一。在间歇操作条件下,升高温度可显著提高过硫酸盐介导的TCE氧化程度,从23℃时的24%提高到40℃时的54%。