Photocatalytic production of hydrogen peroxide (H2O2) is an ideal pathway for obtaining solar fuels. Herein, an S-scheme heterojunction is constructed in hybrid TiO2/In2S3 photocatalyst, which greatly promotes the separation of photogenerated carriers to foster efficient H2O2 evolution. These composite photocatalysts show a high H2O2 yield of 376 µmol/(L·h). The mechanism of charge transfer and separation within the S-scheme heterojunction is well studied by computational methods and experiments. Density functional theory and in-situ irradiated X-ray photoelectron spectroscopy results reveal distinct features of the S-scheme heterojunction in the TiO2/In2S3 hybrids and demonstrate charge transfer mechanisms. The density functional theory calculation and electron paramagnetic resonance results suggest that O2 reduction to H2O2 follows stepwise one-electron processes. In2S3 shows a much stronger interaction with O2 than TiO2 as well as a higher reduction ability, serving as the active sites for H2O2 generation. The work provides a novel design of S-scheme photocatalyst with high H2O2 evolution efficiency and mechanistically demonstrates the improved separation of charge carriers.

TiO2/In2S3 S-scheme photocatalyst with enhanced H2O2-production activity

The high demand for hydrogen peroxide (H2O2) has been dominantly supplied by the anthraquinone process for various applications globally, including chemical synthesis and wastewater treatment. However, the centralized manufacturing and intensive energy input and waste output are significant challenges associated with this process. Accordingly, the on-site production of H2O2via electro- and photocatalytic water oxidation and oxygen reduction partially is greener and easier to handle and has recently emerged with extensive research aiming to seek active, selective and stable catalysts. Herein, we review the current status and future perspectives in this field focused on carbon-based catalysts and their hybrids, since they are relatively inexpensive, bio-friendly and flexible for structural modulation. We present state-of-the-art progress, typical strategies for catalyst engineering towards selective and active H2O2 production, discussion on electro- and photochemical mechanisms and H2O2 formation through both reductive and oxidative reaction pathways, and conclude with the key challenges to be overcome. We expect promising developments would be inspired in the near future towards practical decentralized H2O2 production and its direct use.

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Carbon-based materials for photo- and electrocatalytic synthesis of hydrogen peroxide

H2O2 plays an irreplaceable role in many aspects of human society, such as paper bleaching, medical disinfection, wastewater treatment, organic synthesis, hydrometallurgy and the electronic industry. However, the unsustainability of the current industrial production process of traditional anthraquinone has a serious conflict with the green sustainable development. The photo/electrocatalytic H2O2 production from renewable energy has the advantages of being more economical, low‐carbon and green, and in line with the requirements of energy economy. These catalytic methods of green H2O2 production have played a demonstrative role in the development of many small molecules, contributing to a fundamental understanding of general catalysis and providing a scientific perspective for future new energy cycles. In this review, the authors aim to integrate the reaction process and mechanism of photocatalytic and electrocatalytic H2O2 production, summarize the development and application of photocatalytic and electrocatalytic H2O2 production in recent years, and assess the modern technologies promoted in the process of H2O2 production research, including the development of flux production equipment and reaction coproduction, etc. This review intends to provide a clear logic profile and new directions for the development of H2O2 production, and calls for more researchers to provide more insights into the development of this field.

Versatile Photoelectrocatalysis Strategy Raising Up the Green Production of Hydrogen Peroxide

Emerging semiconductors and metal-organic-compounds-related photocatalysts for sustainable hydrogen peroxide production

Artificial photosynthesis offers a promising strategy for converting solar energy into environmental-friendly H2O2. Herein, robust photocatalytic H2O2 production through dioxygen reduction is achieved, reaching a high H2O2 yield of 873 μmol L−1 h−1. The photocatalyst was prepared by in-situ chemical vapor deposition of N, S co-doped graphene on TiO2 nanofibers. Thanks to the intimate interface with large area and Schottky junction, the H2O2 yield of the composite can be increased by eight times than that of pristine TiO2. Experimental results and density functional theory calculations clarify that the strong synergistic effect between the doped N and S atoms provides abundant active sites to facilitate the electron transfer, promote the adsorption of O2 molecules, and restrain the decomposition of formed H2O2 by suppressing H2O2 adsorption. This work not only provides a novel approach to build close contact between photocatalyst and co-catalyst, but also develops a highly efficient photocatalyst for H2O2 production. 

In-situ grown N, S co-doped graphene on TiO2 fiber for artificial photosynthesis of H2O2 and mechanism study

In this article, we demonstrate that TiO2@carbon core/shell (TiO2@C) nanocomposite photocatalysts prepared by carbonizing a single molecular layer of aromatic compounds adsorbed on the surface of T...

Formation of TiO2@Carbon Core/Shell Nanocomposites from a Single Molecular Layer of Aromatic Compounds for Photocatalytic Hydrogen Peroxide Generation.

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Formation of TiO2@Carbon Core/Shell Nanocomposites from a Single Molecular Layer of Aromatic Compounds for Photocatalytic Hydrogen Peroxide Generation.