Solvent-free synthesis of foam board-like CoSe2 alloy to selectively generate singlet oxygen via peroxymonosulfate activation for sulfadiazine degradation

Abstract

Singlet oxygen (1O2) is a highly effective reactive species in selectively oxidizing organic pollutants. However, it is still challenging to rationally design robust catalysts for the selective generation of 1O2. Herein, the coordination and engineering architecture of the foam board-like CoSe2 alloy were facilely constructed through a green solvent-free method and displayed almost 100% 1O2 production selectivity. The CoSe2 alloy showed excellent catalytic ability for the efficient and fast removal of organic pollutants via peroxymonosulfate (PMS) activation compared with previously reported cobalt-based catalysts. The CoSe2/PMS system exhibited strong resistance for a broad pH range (3.0–11.0) and various coexisting inorganic ions owing to the advantage of the strong bonding of Co-Se in CoSe2 alloy. Mechanism studies revealed that 1O2 was the only reactive oxygen species in the CoSe2/PMS system. Theoretical calculations demonstrated that Co was the dominant adsorption site for PMS in CoSe2, and the production pathway of 1O2 was PMS* → *OH → *O → 1O2. In addition, it was proved that *OH and *O served as the rate-determining steps for the formation of 1O2 by PMS activation on CoSe2 alloy. These findings provide a rational strategy for preparing a series of low-cost transition metal-based alloy catalysts for PMS activation to achieve high-efficiency 1O2 production in the elimination of organic pollutants.