Axially coordinated dual-atomic-site catalysts for nearly 100% peroxymonosulfate conversion to 1O2 in membrane filtration

Abstract

Reactive membrane filtration, integrating membrane technology with catalytic processes, offers a promising avenue for efficiently generating and utilizing active species in environmental remediation. Herein, a dual-atom Co-Mn site achieved through axial coordination on N-doped graphene catalyst (sp-CoMn@NG) has been developed and applied in membrane filtration for the targeted removal of specific pollutants. Experimental investigations, alongside density functional theory (DFT) calculations, have substantiated that axial coordination can effectively reduce the adsorption energy and activation barrier of PMS, thereby facilitating nearly 100% conversion of PMS to 1O2 and enhancing catalytic performance. Mechanistic studies further elucidate the 1O2 production mechanism through a superoxide-mediated chain reaction at the axially coordinated Co-Mn center, as well as the inactivation mechanism of catalytic membranes via the addition reaction of 1O2 and phenolic-hydroxyl compounds. This research underscores the intelligent prefabrication of axial coordination in dual-atomic-site catalysts, offering an efficient approach for scalable 1O2 production in reactive membrane filtration.