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关联单原子催化类芬顿反应中的活性位点与氧化物种。

Correlating active sites and oxidative species in single-atom catalyzed Fenton-like reactions.

作者信息

Miao Jie, Jiang Yunyao, Wang Xixi, Li Xue, Zhu Yuan, Shao Zongping, Long Mingce

机构信息

School of Environmental Science and Engineering, Nanjing Tech University Nanjing 211816 China.

State Key Laboratory of Materials-Oriented Chemical Engineering, College of Chemical Engineering, Nanjing Tech University Nanjing 210009 China.

出版信息

Chem Sci. 2024 Jul 3;15(30):11699-11718. doi: 10.1039/d4sc02621g. eCollection 2024 Jul 31.

Abstract

Single-atom catalysts (SACs) have gained widespread popularity in heterogeneous catalysis-based advanced oxidation processes (AOPs), owing to their optimal metal atom utilization efficiency and excellent recyclability by triggering reactive oxidative species (ROS) for target pollutant oxidation in water. Systematic summaries regarding the correlation between the active sites, catalytic activity, and reactive species of SACs have rarely been reported. This review provides an overview of the catalytic performance of carbon- and metal oxide-supported SACs in Fenton-like reactions, as well as the different oxidation pathways induced by the metal and non-metal active sites, including radical-based pathways (, ·OH and SO˙) and nonradical-based pathways ( O, high-valent metal-oxo species, and direct electron transfer). Thereafter, we discuss the effects of metal types, coordination environments, and spin states on the overall catalytic performance and the generated ROS in Fenton-like reactions. Additionally, we provide a perspective on the future challenges and prospects for SACs in water purification.

摘要

单原子催化剂(SACs)因其最佳的金属原子利用效率以及通过触发活性氧化物种(ROS)对水中目标污染物进行氧化而具有出色的可回收性,在基于多相催化的高级氧化过程(AOPs)中受到广泛关注。关于SACs的活性位点、催化活性和反应物种之间的相关性的系统总结鲜有报道。本综述概述了碳基和金属氧化物负载的SACs在类芬顿反应中的催化性能,以及金属和非金属活性位点诱导的不同氧化途径,包括基于自由基的途径(·OH和SO˙)和非自由基途径(O、高价金属氧物种和直接电子转移)。此后,我们讨论了金属类型、配位环境和自旋态对类芬顿反应中整体催化性能和产生的ROS的影响。此外,我们还展望了SACs在水净化方面未来面临的挑战和前景。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/772f/11290428/f47af3db6fa6/d4sc02621g-f1.jpg

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