Solar-driven hydrogen production from water using particulate photocatalysts is considered the most economical and effective approach to produce hydrogen fuel with little environmental concern. However, the efficiency of hydrogen production from water in particulate photocatalysis systems is still low. Here, we propose an efficient biphase photocatalytic system composed of integrated photothermal–photocatalytic materials that use charred wood substrates to convert liquid water to water steam, simultaneously splitting hydrogen under light illumination without additional energy. The photothermal–photocatalytic system exhibits biphase interfaces of photothermally-generated steam/photocatalyst/hydrogen, which significantly reduce the interface barrier and drastically lower the transport resistance of the hydrogen gas by nearly two orders of magnitude. In this work, an impressive hydrogen production rate up to 220.74 μmol h−1 cm−2 in the particulate photocatalytic systems has been achieved based on the wood/CoO system, demonstrating that the photothermal–photocatalytic biphase system is cost-effective and greatly advantageous for practical applications. The solar-driven H2 production from water by particulate photocatalysts is an effective approach to produce H2 fuel. Here, the authors propose an integrated photothermal–photocatalytic biphase system, which lowers the reaction barrier and the delivery resistance of the H2, boosting the catalytic H2 evolution rate.

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Boosting photocatalytic hydrogen production from water by photothermally induced biphase systems

Recently, semiconductor‐based photocatalytic water splitting has been extensively studied as a promising strategy for converting solar energy into carbon‐neutral and clean H2 fuel. However, the lack of sufficient active sites for surface redox reactions generally results in unsatisfactory photocatalytic water splitting performances over semiconductors. For this problem, cocatalyst provides an encouraging solution and is of great significance in improving photocatalytic performance. Noble metals and their derivatives are mostly utilized as efficient cocatalytic components, but their scarcity and expensiveness severely hamper large‐scale applications. Thereby, the utilization of noble‐metal‐free cocatalysts has aroused immense research attention. Owing to the facile availability, low cost, large abundance, high stability, and efficient performance, transition‐metal‐based materials have been developed as desirable candidates in the photocatalytic water splitting water splitting process. This review gives an outline of some recent advances in the active transition‐metal‐based water splitting cocatalysts. First, the fundamentals of transition‐metal‐based cocatalysts are presented, including the classification, function mechanisms, loading methods, modification strategies, and design considerations. Second, the various cases of depositing reduction cocatalysts, oxidation cocatalysts, and reduction–oxidation dual cocatalysts for water splitting are further discussed. Finally, the crucial challenges and possible research directions of transition‐metal‐based cocatalysts for photocatalytic water splitting are proposed.

Transition‐Metal‐Based Cocatalysts for Photocatalytic Water Splitting

The efficiency of photocatalytic water splitting, and CO2 conversion depend on the separation and transfer of charge carriers. Graphitic carbon components with decent conductivity can enhance the transport of the photoinduced charges in semiconductor heterostructures. As a typical visible-light-responsive photocatalyst, the application of graphitic carbon nitride (g-C3N4) is often limited by the relatively high recombination rate of photogenerated charge carriers. g-C3N4 has been a hot base material for constructing metals and semiconductors modified hetero- and homo-junctions for the application of solar-driven fuel production. Graphitic carbon components are the keys in enhancing the transport efficiency of photogenerated charge carriers in g-C3N4 based heterostructures. In this review, important aspects of the roles of graphitic carbon components in g-C3N4 based photocatalysts are discussed to provide paradigms for the advancement of these materials in photocatalytic water splitting and CO2 reduction. Moreover, graphitic carbon can serve as a coating material, or be in layer or nanotube forms, to be incorporated into heterostructure materials to affect the mobility of the charge carriers in Schottky junctions as well as in Z-scheme and S-scheme heterostructures. Important feature changes in g-C3N4 based photocatalysts after graphitic carbon incorporation as well as the progress and achievements in these composite photocatalyst materials in water splitting and CO2 reduction are summarized. 

Role of graphitic carbon in g-C3N4 nanoarchitectonics towards efficient photocatalytic reaction kinetics: A review

Scope and prospect of transition metal-based cocatalysts for visible light-driven photocatalytic hydrogen evolution with graphitic carbon nitride

A novel metal-free all-solid-state z-scheme g-C3N4/NCDs/WOx photocatalyst was fabricated using nitrogen-doped carbon dots (NCDs) as the electron mediator. As-prepared sandwich-structured composites...

Bifunctional Nitrogen-Doped Carbon Dots in g-C3N4/WOx Heterojunction for Enhanced Photocatalytic Water-Splitting Performance.

The development of earth-abundant cocatalysts with confined size on suitable conductive supports is of high importance for facilitating solar energy conversion using semiconductors. In this work, a green redox relay reaction between FeCl3 and a pyrrole (Py) monomer was developed for the synthesis of g-C3N4–PPy–FeP, in which FeCl3 realized the formation of PPy over graphitic carbon nitride, and the as-formed PPy confined and tightly supported Fe ions, which were then transformed into the nanosized FeP of diameter less than 5 nm. A highly porous morphology was obtained by inserting well-dispersed g-C3N4 into PPy, accompanied by conductive PPy and nanosized FeP acting as a mediator of charge carriers and high-performance cocatalyst, respectively. Consequently, optimal g-C3N4–PPy–FeP demonstrated a photocatalytic hydrogen evolution activity 6 and 20 times larger than that of g-C3N4 singly loaded separately with PPy and FeP, respectively, under visible light irradiation.

Conductive polymer supported and confined iron phosphide nanocrystals for boosting the photocatalytic hydrogen production of graphitic carbon nitride

The enhanced photocatalytic hydrogen evolution performance of g-C3N4–Co3O4 2D–1D Z-scheme heterojunctions was achieved by employing the cobalt ion redox and conductive polymers (polyaniline, PANi) for the first time. Specifically, a Co3O4 1D nanobelt acting as the Z-scheme heterostructure component could promote the separation of photo-excited charge carriers and increased the redox capacity, and the conductive PANi brought about the boosted transport efficiency of the charge carriers. Notably, cobalt ions were adopted as the intermediate of the electron transfer between two components for boosting the carrier transport and utilization efficiency. Consequently, the Co3O4 nanobelt, PANi and cobalt ions exhibited a synergistic effect on facilitating the photocatalytic HER performance of the g-C3N4-based heterostructure, and the optimal ternary heterostructure (g-C3N4–PANi–Co3O4) exhibited a photocatalytic H2-evolution rate of 4.61 μmol h−1 under visible light, which further increased to 9.95 μmol h−1 by adding Co2+ solution owing to the further facilitated transport of charge carriers through the redox reaction of cobalt ions. Moreover, even in the absence of sacrificial agents, this Z-scheme system exhibited a photocatalytic hydrogen production activity of 3.35 μmol h−1 in the Co2+ aqueous solution under UV-visible light.

Cobalt ion redox and conductive polymers boosted the photocatalytic activity of the graphite carbon nitride–Co3O4 Z-scheme heterostructure

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Conductive polymer supported and confined iron phosphide nanocrystals for boosting the photocatalytic hydrogen production of graphitic carbon nitride

Cobalt ion redox and conductive polymers boosted the photocatalytic activity of the graphite carbon nitride–Co3O4 Z-scheme heterostructure