College of Chemistry and Chemical Engineering, Hubei Key Laboratory of Mine Environmental Pollution Control & Remediation, Hubei Polytechnic University, Huangshi, 435003, China; Hubei Key Laboratory of Coal Conversion and New Carbon Material, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan, 430081, China.
College of Chemistry and Chemical Engineering, Hubei Key Laboratory of Mine Environmental Pollution Control & Remediation, Hubei Polytechnic University, Huangshi, 435003, China.
Environ Res. 2023 Jul 1;228:115847. doi: 10.1016/j.envres.2023.115847. Epub 2023 Apr 6.
A novel CuO-FeO encapsulated in the carbon framework with abundant oxygen vacancies (CuO-FeO@C) was successfully prepared by thermal conversion of Cu(OAc)/Fe-metal organic framework. The as-prepared catalyst exhibited excellent peroxymonosulfate (PMS) activation performance, good recyclability and fast magnetic separation. Under optimal conditions, the added BPA (60 mg/L) could be completely removed by CuO-FeO@C/PMS system within 15 min with the degradation rate constant (k) of 0.32 min, being 10.3 and 246.2 times that in CuO/PMS (0.031min) and FeO/PMS (0.0013 min) system. A deep mineralization rate of BPA (＞80%) was achieved within 60 min. The results demonstrated the synergistic effect of bimetallic clusters, oxygen vacancies and carbon framework was a key benefit for the exposure of more active sites, the electron donor capacity and the mass transfer of substrates, thereby promoting the decomposition of BPA. Capture experiments and EPR indicated that O was the predominant reactive oxygen species (ROSs). The degradation routes of BPA and the activation mechanism of PMS were proposed. This study offers an opportunity to develop promising MOFs-derived hybrid catalysts with tailored structures and properties for the practical application of SR-AOPs.
一种新型的氧化铜-氧化亚铁封装在富含氧空位的碳框架中（CuO-FeO@C），是通过热转化 Cu(OAc)/Fe-金属有机骨架制备而成。所制备的催化剂表现出优异的过一硫酸盐（PMS）活化性能、良好的可回收性和快速的磁分离性能。在最佳条件下，加入的 BPA（60mg/L）可以在 15min 内被 CuO-FeO@C/PMS 体系完全去除，降解速率常数（k）为 0.32min，是 CuO/PMS（0.031min）和 FeO/PMS（0.0013 min）体系的 10.3 和 246.2 倍。在 60min 内实现了 BPA 的深度矿化率（＞80%）。结果表明，双金属簇、氧空位和碳框架的协同效应是暴露更多活性位点、电子供体能力和底物传质的关键优势，从而促进了 BPA 的分解。捕获实验和 EPR 表明 O 是主要的活性氧物种（ROSs）。提出了 BPA 的降解途径和 PMS 的活化机制。本研究为开发具有定制结构和性能的有前途的 MOFs 衍生混合催化剂提供了机会，以用于实际的 SR-AOPs。
