Precision Chemistry (Feb 2023)
Three-Dimensional Welded Mn1 Site Catalysts with nearly 100% Singlet Oxygen Fabrication for Contaminant Elimination
Abstract
Reactive oxygen species (ROS) have a significant part in the elimination of recalcitrant organic pollutants and commonly coexist in one advanced oxidation system. It is difficult for us to make clear the effect of the co-instantaneous generation of radicals and nonradicals, which would cover and obscure the transformation pathway. Herein, a coordinate welding process is presented for fabricating accessible Mn1 site catalysts (Mn SSCs) in order to clarify the nonradical (singlet oxygen/1O2) generated pathway and transformation in oxidative removal of contaminants. The Mn SSCs achieve nearly 100% 1O2 fabrication by activating peroxymonosulfate, which displays an excellent sulfamethoxazole elimination performance, super anti-anion interference, and extraordinary stability. As revealed by density functional theory calculations, the Mn SSCs with a special welded three-dimensional nanostructure could significantly boost the activation process by oxidizing the peroxymonosulfate at the interlayer of Mn SSCs and reducing dissolved oxygen on the surface of Mn SSCs. This design of Mn SSCs with a three-dimensional welded nanostructure might offer a potential approach for employing single site catalysts for environmental remediation.