Boosting photocatalytic hydrogen peroxide production by regulating electronic configuration of single Sb atoms via carbon vacancies in carbon nitrides.

Single Sb atoms on carbon vacancy-rich C 3 N 4 (Cv-C 3 N 4) with an electron-rich state tend to efficiently transfer electrons to pauling-type absorbed O 2 and boost the photocatalytic oxygen reduction reaction to H 2 O 2. [Display omitted] Single-atom catalysts supported on semiconductors can serve as active sites for efficient oxygen reduction to hydrogen peroxide (H 2 O 2). However, researchers have long been puzzled by the lack of guidance on optimizing the performance of single-atom photocatalysts. In this study, we propose a versatile strategy that utilizes carbon vacancies to regulate the electronic configuration of antimony (Sb) atoms on carbon nitrides (C 3 N 4). This strategy has been found to significantly enhance the photocatalytic production of H 2 O 2. The H 2 O 2 evolution rate of Sb single-atom on carbon vacancy-rich C 3 N 4 (designated as Sb 1 /Cv-C 3 N 4) is 5.369 mmol g-1h−1, which is 10.9 times higher than C 3 N 4 alone. By combining experimental characterizations and density functional theory simulations, we reveal the strong electronic interaction between Sb atoms and carbon vacancy-rich C 3 N 4. This interaction is capable for maintaining the electron-rich state of Sb atoms, facilitating efficient electron transfer to pauling-type absorbed oxygen, and ultimately enhancing the formation of *OOH intermediates. This innovative defect-engineering approach can manipulate the electronic configuration of single-atom catalysts, providing a new avenue to boost the photocatalytic oxygen reduction reaction towards H 2 O 2 production. [ABSTRACT FROM AUTHOR]