Carbonate mediated hole transfer boosting the photocatalytic degradation of organic pollutants over carbon nitride nanosheets

• A conceptual carbonate mediated hole transfer photocatalytic system is proposed. • carbonates can capture and transfer the photoinduced hole into solution in form of · CO 3 - • Efficient hole capture via carbonates oxidation boosts the charge separation. • The unique · CO 3 - /CO 3 2- shuttle boosting charge separation for enhanced · OH generation. • Enhanced · OH and · CO 3 - generation enables efficient organic pollutants degradation. Inspired by the important role of the manganese enzyme in photo-induced hole transfer of natural photosynthesis, we have developed an innovative carbonate-mediated-hole-transfer strategy for boosting the photocatalytic degradation of organic pollutants. We found that the carbonate species can effectively extract the photo-generated hole in the valence band of carbon nitride to generate · CO 3 - and leaves electron in the conduction band for oxygen reduction to generate · OH. The generated · CO 3 - can be returned to its pristine state of CO 3 2- via the oxidation of organic pollutants. The unique · CO 3 - /CO 3 2- shuttle could largely improve the charge separation via the fast hole extraction that leads to enhanced · OH generation for accelerating the photocatalytic degradation of organic pollutants. As expected, the as-prepared carbon nitride exhibits markedly enhanced photocatalytic performance toward formaldehyde, p-chlorophenol, and phenol degradation than the one without carbonate as additive. The conceptual study demonstrated here may offer new viewpoints in designing high-efficient photocatalytic systems for environmental applications.