Initiating photocatalytic degradation of organic pollutants under ultra-low light intensity via oxygen-centered organic radicals

Abstract

Photocatalysis, as a promising method for in-situ water pollution remediation but faces challenges due to the limited natural light intensity. Herein, we achieve highly-efficient photocatalytic removal of organic pollutants even under ultra-low light intensities of only 0.1 mW·cm⁻². This was accomplished by developing and effectively stabilizing a novel reactive species - oxygen-centered organic radicals (OCORs), which has an impressive half-life of up to seven minutes in water. With lifetimes 8 to 11 orders of magnitude longer than traditional transient radicals, OCORs can effectively wait for pollutants to diffuse, enabling them to remove organic pollutants through polymerization and degradation pathways. The mechanism behind the stability of OCORs lies in the enhanced electron-withdrawing ability of the electron acceptor and the extended conjugation of the catalyst, which effectively prevent back electron transfer. This study provides a theoretical foundation for practical applications of photochemistry in pollution remediation.