Affiliation:
1. School of Environmental Science and Engineering Key Laboratory of Thin Film and Microfabrication Technology (Ministry of Education) Shanghai Jiao Tong University Shanghai 200240 P. R. China
Abstract
AbstractTuning the electronic distribution of the single‐atom sites in single‐atom catalysts (SACs) is crucial for unlocking their catalytic potential. The four‐nitrogen‐coordinated transitional metal (M−N4) configuration has been widely investigated in peroxymonosulfate (PMS)‐based advanced oxidation processes (PMS‐AOPs), but restricted by the sluggish electron transfer from PMS to generate the high‐valent metal‐oxo (HVMO), reactive species with high redox potentials and long half‐lives, for the degradation of organic pollutants in water due to its symmetric structure. Recently, the SACs with asymmetric coordination configurations are found to break the symmetric electronic distribution of M−N4, which facilitates the O−H and O−O bond breaking in PMS, thus promoting HVMO formation. Asymmetric coordination has emerged as a novel and effective strategy for single‐atom coordination modulation. In this paper, two strategies for breaking the symmetry of nitrogen‐coordinated SACs by planar heteroatom doping and axial optimization engineering are outlined, and the reaction mechanisms on the formation of HVMO species over asymmetrically coordinated SACs via PMS activation are highlighted. Finally, we prospect the development of asymmetrically coordinated SACs in water purification.
Funder
National Natural Science Foundation of China
Subject
Inorganic Chemistry,Organic Chemistry,Physical and Theoretical Chemistry,Catalysis