Photothermal-enabled single-atom catalysts for high-efficiency hydrogen peroxide photosynthesis from natural seawater

Abstract

AbstractHydrogen peroxide (H2O2) is a powerful industrial oxidant and potential carbon-neutral liquid energy carrier. Sunlight-driven synthesis of H2O2from the most earth-abundant O2and seawater is highly desirable. However, the solar-to-chemical efficiency of H2O2synthesis in particulate photocatalysis systems is low. Here, we present a cooperative sunlight-driven photothermal-photocatalytic system based on cobalt single-atom supported on sulfur doped graphitic carbon nitride/reduced graphene oxide heterostructure (Co–CN@G) to boost H2O2photosynthesis from natural seawater. By virtue of the photothermal effect and synergy between Co single atoms and the heterostructure, Co–CN@G enables a solar-to-chemical efficiency of more than 0.7% under simulated sunlight irradiation. Theoretical calculations verify that the single atoms combined with heterostructure significantly promote the charge separation, facilitate O2absorption and reduce the energy barriers for O2reduction and water oxidation, eventually boosting H2O2photoproduction. The single-atom photothermal-photocatalytic materials may provide possibility of large-scale H2O2production from inexhaustible seawater in a sustainable way.