ABSTRACT
2D/2D step-scheme (S-scheme) piezo-photocatalysts for the production of fine chemicals, such as hydrogen peroxide (H2O2), have attracted significant attention of global scientists owing to the efficiency in utilizing surface piezoelectric effects from 2D materials to overcome rapid charge recombination in photocatalytic processes. In this research, we reported the fabrication of 2D S-doped VOx deposited on 2D g-C3N4 to produce H2O2 via the piezo-photocatalytic process with high production yields at 20.19 mmol g-1 h-1, which was 1.75 and 4.87 times higher than that from solely piezo-catalytic and photocatalytic H2O2 generation. The finding pointed out that adding sulfur (S) to VOx can help to improve the catalytic outcomes by modifying the electronic properties of pristine VOx. In addition, when coupled with g-C3N4, the presence of S limits the formation of graphene in the VOx/g-C3N4 composites, causing shielding effects and pushing the cascade reactions toward water generation in the materials. Besides, the research also sheds light on the charge transport between g-C3N4 and S-VOx under irradiation and how the composites work to trigger the formation of H2O2. The presence of S in the composite systems enhances charge transfer between two semiconductors by strengthening the internal electric fields (IEF) to drive electrons moving in one direction, as demonstrated by density functional theory (DFT) calculations. Moreover, the formation of H2O2 significantly relies on the reduction of oxygen to generate oxygenic radical species at the g-C3N4 sites. Meanwhile, S-VOx provides oxidative sites in the composites to oxidize water molecules to directly or indirectly generate H2O2 or O2, which will further participate in the reactions to produce the final products. This study confirms the validation of S-scheme piezo-photocatalysts, thus encouraging further research on developing heterojunction materials with high catalytic efficiency, which can be used in practical conditions.
