Simultaneously Utilizing Excited Holes and Electrons for Piezoelectric-Enhanced Photoproduction of H2O2 from S-Scheme 2D S-Doped VOx/g-C3N4 Nanostructures.

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.

Revisiting the roles of dopants in g-C3N4 nanostructures for piezo-photocatalytic production of H2O2: a case study of selenium and sulfur.

The sustainable production of hydrogen peroxide (H2O2) from oxygen and water has become an exciting research hotspot in the scientific community due to the importance of this fine chemical in various fields. Besides, piezo-photocatalysis is an emerging star for generating H2O2 from these green reagents. For developing catalysts for this specific application, doping heteroatoms into carbon-based materials such as graphitic carbon nitrides (g-C3N4) is a growing fascination among worldwide scientists. However, systematic study on the effects of doping precursors on the catalytic results is still rare. Herein, we fabricated sulfur (S) and selenium (Se) doped g-C3N4 with various doping precursors to evaluate the effects of these agents on the production of H2O2 under light and ultrasound irradiation. Based on the results, Se-doped g-C3N4 gave an outstanding catalytic performance compared to S-doped g-C3N4, even in a significantly low quantity of Se. In order to fully understand the chemical, physical, optical, and electronic properties of pristine g-C3N4 and its derivatives, the as-prepared materials were thoroughly analyzed with various tools. Thus, this study would give more profound insights into doping techniques for carbon-based materials and encourage further research on the design and development of piezo-photocatalysts for practical applications.