Effective photocatalytic H2O2 production under visible light irradiation at g-C3N4 modulated by carbon vacancies

Abstract Hydrogen peroxide (H2O2) is of great significance in biological and environmental processes as well as in chemical industry. Even though anthraquinone autoxidation (AO) process has been the major artificial way to produce H2O2, its energy cost and non-green nature have been motivating people to develop more efficient, economic and green technologies as alternatives. Here we demonstrated that photocatalytic H2O2 production at g-C3N4 could be improved by as much as 14 times in the absence of organic scavenger through a carbon vacancy-based strategy. Both the experimental and theoretical calculation results indicated that the creation of carbon vacancies could reduce the symmetry of g-C3N4 and produce the effect of electron delocalization. This will allow g-C3N4 to possess more excitable electrons and a narrower band gap. On the other hand, carbon vacancies provided more sites to adsorb molecular oxygen and thereby help electrons transfer from g-C3N4 to the surface adsorbed O2. More interestingly, the presence of carbon vacancies changed the H2O2 generation pathway from a two-step single-electron indirect reduction to an one-step two-electron direct reduction. This study could not only develop a novel strategy to improve the H2O2 production activity of semiconductors, but also shed light on the deep understanding of the role played by surface defect structure on photocatalytic activity of semiconductor photocatalysts.

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