Wang Yumeng, Lyu Lai, Wang Di, Yu Han-Qing, Li Tong, Gao Yaowen, Li Fan, Crittenden John C, Zhang Lili, Hu Chun
Key Laboratory for Water Quality and Conservation of the Pearl River Delta, Ministry of Education, Institute of Environmental Research at Greater Bay, Guangzhou University, Guangzhou 510006, China.
CAS Key Laboratory of Urban Pollutant Conversion, Department of Applied Chemistry, University of Science and Technology of China, Hefei 230026, China.
iScience. 2021 Jul 16;24(8):102874. doi: 10.1016/j.isci.2021.102874. eCollection 2021 Aug 20.
High energy consumption is impedimental for eliminating refractory organic pollutants in water by applying advanced oxidation processes (AOPs). Herein, we develop a novel process for destructing these organics in chemical conjuncted Fe-FeC/Fe, graphited ZIF-8, and rGO air-saturated aqueous suspension without additional energy. In this process, a strong Fe-π interaction occurs on the composite surface, causing the surface potential energy ∼310.97 to 663.96 kJ/mol. The electrons for the adsorbed group of pollutants are found to delocalize to around the iron species and could be trapped by O in aqueous suspension producing OH, H, and adsorbed organic cation radicals, which are hydrolyzed or hydrogenated to intermediate. The target pollutants undergo surface cleavage and convert HO to OH, consuming chemical adsorption energy (∼2.852-9.793 kJ/mol), much lower than that of AOPs. Our findings provide a novel technology for water purification and bring new insights into pollutant oxidation chemistry.
高能耗不利于通过应用高级氧化工艺(AOPs)去除水中的难降解有机污染物。在此,我们开发了一种新型工艺,可在不额外耗能的情况下,在化学结合的Fe-FeC/Fe、石墨化ZIF-8和rGO空气饱和水悬浮液中破坏这些有机物。在该工艺中,复合材料表面发生强烈的Fe-π相互作用,导致表面势能约为310.97至663.96 kJ/mol。发现吸附的污染物基团的电子离域到铁物种周围,并可被水悬浮液中的O捕获,生成OH、H和吸附的有机阳离子自由基,这些自由基水解或氢化生成中间体。目标污染物发生表面裂解并将HO转化为OH,消耗的化学吸附能量(约2.852-9.793 kJ/mol)远低于AOPs。我们的研究结果为水净化提供了一种新技术,并为污染物氧化化学带来了新的见解。