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共价有机框架@ZIF-67 衍生的新型纳米复合材料催化剂有效激活过一硫酸盐来降解有机污染物。

Covalent organic frameworks@ZIF-67 derived novel nanocomposite catalyst effectively activated peroxymonosulfate to degrade organic pollutants.

机构信息

Key Laboratory for Environmental Pollution Prediction and Control, College of Earth and Environmental Sciences, Lanzhou University, Lanzhou, 730000, Gansu Province, PR China.

Department of Electrical and Electronic Engineering, Southern University of Science and Technology, Shenzhen, 518055, Guangdong Province, PR China.

出版信息

Chemosphere. 2023 Jan;311(Pt 1):137038. doi: 10.1016/j.chemosphere.2022.137038. Epub 2022 Oct 30.

DOI:10.1016/j.chemosphere.2022.137038
PMID:36323385
Abstract

Metal organic frameworks-Covalent organic frameworks (MOFs-COFs) nanocomposites could improve the catalytic performance. Herein, a novel nanocomposite catalyst (CC@CoO) derived from MOFs-COFs (COF@ZIF-67) was prepared on peroxymonosulfate (PMS) activation for bisphenol A (BPA) and rhodamine B (RhB) degradation. Owing to the Co species, oxygen vacancy (O), surface hydroxyl (-OH), graphite N and ketone groups (C=O), the CC@CoO exhibited higher catalytic degradation performance and total organic carbon (TOC) for BPA (93.8% and 22.3%) and RhB (98.2% and 82.5%) with a small quantity of catalyst (0.10 g/L) and low concentration of PMS (0.20 g/L) even without pH adjustment. Sulfate radicals (•SO), hydroxyl radicals (•OH), single oxygen (O), superoxide radicals (•O) and electron transfer process were all involved in the degradation of BPA and RhB. Among them, the degradation of BPA and RhB mainly depended on •O and O, respectively. Meanwhile, the degradation pathways of BPA and RhB were proposed, and the biotoxicity of the degradation products was evaluated by freshwater chlorella. The results illustrated that the degradation products were environmentally friendly to organisms. In addition, the role of COF in the nanocomposites was also studied. The addition of COF remarkably improved the catalytic performance of CC@CoO due to the faster electron transfer, more graphite N and C=O. Overall, this work may open the door to the development of COF-based catalysts in the field of water pollutant remediation.

摘要

金属有机骨架-共价有机骨架(MOFs-COFs)纳米复合材料可以提高催化性能。本文通过过一硫酸盐(PMS)活化制备了一种新型的 MOFs-COFs(COF@ZIF-67)衍生的纳米复合材料催化剂(CC@CoO),用于双酚 A(BPA)和罗丹明 B(RhB)的降解。由于 Co 物种、氧空位(O)、表面羟基(-OH)、石墨 N 和酮基(C=O)的存在,CC@CoO 表现出更高的催化降解性能和总有机碳(TOC)去除率,对于 BPA(93.8%和 22.3%)和 RhB(98.2%和 82.5%),只需少量催化剂(0.10 g/L)和低浓度的 PMS(0.20 g/L),甚至无需调节 pH 值。硫酸盐自由基(•SO)、羟基自由基(•OH)、单线态氧(O)、超氧自由基(•O)和电子转移过程都参与了 BPA 和 RhB 的降解。其中,BPA 和 RhB 的降解主要依赖于•O 和 O。同时,提出了 BPA 和 RhB 的降解途径,并通过淡水小球藻评价了降解产物的生物毒性。结果表明,降解产物对生物是友好的。此外,还研究了 COF 在纳米复合材料中的作用。COF 的添加由于更快的电子转移、更多的石墨 N 和 C=O,显著提高了 CC@CoO 的催化性能。总的来说,这项工作可能为 COF 基催化剂在水污染修复领域的发展开辟了道路。

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