Solar-driven water splitting provides a leading approach to store the abundant yet intermittent solar energy and produce hydrogen as a clean and sustainable energy carrier. A straightforward route to light-driven water splitting is to apply self-supported particulate photocatalysts, which is expected to allow solar hydrogen to be competitive with fossil-fuel-derived hydrogen on a levelized cost basis. More importantly, the powder-based systems can lend themselves to making functional panels on a large scale while retaining the intrinsic activity of the photocatalyst. However, all attempts to generate hydrogen via powder-based solar water-splitting systems to date have unfortunately fallen short of the efficiency values required for practical applications. Photocatalysis on photocatalyst particles involves three sequential steps: (i) absorption of photons with higher energies than the bandgap of the photocatalysts, leading to the excitation of electron-hole pairs in the particles, (ii) charge separation and migration of these photoexcited carriers, and (iii) surface chemical reactions based on these carriers. In this review, we focus on the challenges of each step and summarize material design strategies to overcome the obstacles and limitations. This review illustrates that it is possible to employ the fundamental principles underlying photosynthesis and the tools of chemical and materials science to design and prepare photocatalysts for overall water splitting.

Particulate Photocatalysts for Light-Driven Water Splitting: Mechanisms, Challenges, and Design Strategies

Two-dimensional (2D) heterostructures with the Z-scheme can significantly improve the recombination of the photogenerated charge pairs and increase the overpotential compared with the corresponding monolayers. Based on first-principles calculations, we demonstrate the photocatalytic performance with the Z-scheme of three 2D AuSe/SnS heterostructures identified from nine stacking types of AuSe and SnS monolayers using their formation energies. The thermal stabilities of the chosen heterostructures are assured by molecular dynamics simulations. The band alignment and built-in electric field support the heterostructures to drive the photocatalytic hydrogen and oxidation evolution reactions with the direct Z-scheme. Moreover, the optical absorption of both AuSe and SnS monolayers is obviously observed in the visible light and UV ranges, indicating their excellent response to solar light. The highest solar-to-hydrogen energy conversion efficiency of the heterostructures can reach 23.96%. The change in Gibbs free energy in the hydrogen evolution reaction with the heterostructures is in the range of 0.63–0.97 eV, indicating that these reactions are not difficult to carry out. Therefore, the present AuSe/SnS heterostructures could be promising candidates for producing hydrogen from photocatalytic water splitting with the Z-scheme driven by solar light.

Two-dimensional heterostructures of AuSe/SnS for the photocatalytic hydrogen evolution reaction with a Z-scheme

Plasmonic metal@semiconductor core–shell nanoparticles (CSNPs) are considered as promising candidates for artificial photosynthesis. Herein, Au@CeO2 CSNPs are hydrothermally fabricated for photocatalytic hydrogen evolution reaction (HER). CSNPs deliver superior HER performance compared to free CeO2. In particular, Au@CeO2-18 model (shell thickness of 18 nm) produces an HER rate of 4.05 μmol mg–1 h–1, which is ∼10 times higher than that of pure CeO2 (0.40 μmol mg–1 h–1) under visible-light. Additionally, Au@CeO2-18 photocatalyst demonstrates long-term stability after five repetitive runs, at which point it only loses approximately 5% of the activity, while core-free CeO2 decreases by 37.5 %. Such improvements are attributed to the electronic interactions between Au and CeO2, which not only enriches Ce3+ active sites to narrow bandgap of ceria toward visible, but also increases the affinity for hydrogen ions on the CSNPs surface. Moreover, localized surface plasmon resonance is light-excited and decays to efficiently produce hot-carrier to drive catalytic reactions.

Insightful understanding of hot-carrier generation and transfer in plasmonic Au@CeO2 core–shell photocatalysts for light-driven hydrogen evolution improvement

The design and application of semiconductor-based photocatalytic technology has a significant impact on addressing the world’s energy crisis and environmental degradation by transforming solar energy into chemicals and fuels. Semiconductor-based photocatalyst, ceria (CeO2), which possesses unique 4f electrons, is superior to other metal oxide semiconductors owing to its defect-rich structure, multivalence state, surface oxygen vacancy, photostability, and eco-friendly properties. This critical review is taken up to report the basic mechanistic details of CeO2-based photocatalysis as well as several methods for boosting the activity and stability of this group of photocatalysts. Additionally, numerous photocatalytic applications of CeO2, such as H2 generation by water splitting and CO2 reduction to alcohols and hydrocarbon fuels, are introduced and summarized. In the end, a concise summary of the challenges and potential areas for future research in the synthesis of CeO2-based photocatalysts are also provided. This review is anticipated to provide directions for developing innovative CeO2-based photocatalysts with low-cost and high efficiency, which have the promising application possibilities to fulfill the pressing needs of alternative fuels. 

Ceria-based photocatalysts in water-splitting for hydrogen production and carbon dioxide reduction

Effect of conduction band potential on cocatalyst-free plasmonic H2 evolution over Au loaded on Sr2+-doped CeO2

Photocatalytic overall water splitting into hydrogen and oxygen on RuO2-loaded Sm3+-doped CeO2 was examined. Pure CeO2 showed a negligible small activity, however Sm3+ doped CeO2 with heterogeneous...

Photocatalytic Overall Water Splitting on RuO2-loaded Sm3+-doped CeO2 with Heterogenous Doping Structure

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Photocatalytic Overall Water Splitting on RuO2-loaded Sm3+-doped CeO2 with Heterogenous Doping Structure