Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2018-07-31 , DOI: 10.1016/j.cej.2018.07.210 Hui Lin , Junfeng Niu , Shangtao Liang , Chong Wang , Yujuan Wang , Fangyuan Jin , Qi Luo , Qingguo Huang
Magnéli phase Ti4O7 ceramic materials having extensive interconnecting macropores with an average pore size of 2.6 μm and 21.6% porosity were fabricated using a high-temperature sintering method, and then tested as an anode in a batch mode for electrooxidative mineralization of environmentally persistent poly- and perfluoroalkyl substances (PFASs) such as perfluorooctanoate (PFOA) and perfluorooctanesulfonate (PFOS). Tests were also conducted with other “non-active” electrodes for comparison, including Ce-doped PbO2 and Ti/BDD electrodes. The results showed that the porous Ti4O7 ceramic anode exhibited greater PFOA/PFOS oxidation rates than those of the other electrodes. Only trace amounts of perfluorocarboxylic acid (PFCAs) with shortened chain lengths were observed as intermediates during PFOA mineralization. SO42− and F− were recovered as the mineralization products of PFOS electrooxidation, while no organofluorine compounds such as shorter-chain PFCAs were detected in the solution by high-resolution mass spectrometry (HRMS). Possible mechanisms for PFOA/PFOS mineralization over porous Ti4O7 ceramic electrode were proposed on the basis of reaction products analysis. In addition, the developed porous Ti4O7 ceramic anode was successfully applied to treatment of the still bottom liquid waste containing high concentrations of poly- and perfluoroalkyl substances (PFASs) as well as high chloride and organic content concentrations from the regeneration of ion-exchange resin that had been used for remediation of PFASs-impacted groundwater. The results illustrate the promise of the macroporous Magnéli phase Ti4O7 ceramic materials for electrochemical treatment of PFASs in water.
中文翻译:
大孔Magnéli相Ti 4 O 7陶瓷材料的开发:作为有效的阳极,用于多聚和全氟烷基物质的矿化
使用高温烧结方法制造了具有广泛的互连大孔,平均孔径为2.6μm,孔隙率为21.6%的Magnéli相Ti 4 O 7陶瓷材料,然后以分批方式作为阳极进行测试,以进行环境持久性的电氧化矿化聚和全氟烷基物质(PFAS),例如全氟辛酸酯(PFOA)和全氟辛烷磺酸(PFOS)。还使用其他“非活性”电极(包括Ce掺杂的PbO 2和Ti / BDD电极)进行了测试以进行比较。结果表明,多孔Ti 4 O 7陶瓷阳极表现出比其他电极更高的PFOA / PFOS氧化速率。在PFOA矿化过程中,仅观察到痕量的具有较短链长的全氟羧酸(PFCA)作为中间体。SO 4 2-和F -回收作为PFOS电氧化的矿化产品,而作为短链全氟羧酸是在通过高分辨率质谱(HRMS)的溶液检测不到有机氟化合物等。在反应产物分析的基础上,提出了多孔Ti 4 O 7陶瓷电极上PFOA / PFOS矿化的可能机理。另外,开发了多孔Ti 4 O 7陶瓷阳极已成功地用于处理釜底废液,该废液中含有高浓度的多氟烷基和全氟烷基物质(PFAS),以及来自离子交换树脂再生的高氯化物和有机物浓度,这些离子交换树脂已用于PFAS的修复-受到影响的地下水。结果表明,大孔的Magnéli相Ti 4 O 7陶瓷材料有望用于水中PFAS的电化学处理。