Hydrogen (H2) production via photocatalytic water splitting is one of the most promising technologies for clean solar energy conversion to emerge in recent decades. The achievement of energy production from water splitting would mean that we could use water as a fuel for future energy need. Among the various photocatalytic materials, titanium dioxide (TiO2) is the dominant and most widely studied because of its exceptional physico-chemical characteristics. Surface decoration of metal/non-metal on TiO2 nanoparticles is an outstanding technique to revamp its electronic properties and enrich the H2 production efficiency. Metal dopants play a vital role in separation of electron-hole pairs on the TiO2 surface during UV/visible/simulated solar light irradiation. In this paper, the basic principles, photocatalytic-reactor design, kinetics, key findings, and the mechanism of metal-doped TiO2 are comprehensively reviewed. We found that Langmuir-Hinshelwood kinetic model is commonly employed by the researchers to demonstrate the rate of H2 production. Copper (Cu), gold (Au) and platinum (Pt) are the most widely studied dopants for TiO2, owing to their superior work function. The metal dopants can amplify the H2 production efficiency of TiO2 through Schottky barrier formation, surface plasmon resonance (SPR), generation of gap states by interaction with TiO2 VB states. The recent advances and important consequences of 2D materials, perovskites, and other novel photocatalysts for H2 generation have also been reviewed.

Photocatalytic hydrogen production using metal doped TiO2: A review of recent advances

Photoelectrochemical (PEC) water splitting is a promising approach for solar-driven hydrogen production with zero emissions, and it has been intensively studied over the past decades. However, the solar-to-hydrogen (STH) efficiencies of the current PEC systems are still far from the 10% target needed for practical application. The development of efficient photoelectrodes in PEC systems holds the key to achieving high STH efficiencies. In recent years, crystal facet engineering has emerged as an important strategy in designing efficient photoelectrodes for PEC water splitting, which has yet to be comprehensively reviewed and is the main focus of this article. After the Introduction, the second section of this review concisely introduces the mechanisms of crystal facet engineering. The subsequent section provides a snapshot of the unique facet-dependent properties of some semiconductor crystals including surface electronic structures, redox reaction sites, surface built-in electric fields, molecular adsorption, photoreaction activity, photocorrosion resistance, and electrical conductivity. Then, the methods for fabricating photoelectrodes with faceted semiconductor crystals are reviewed, with a focus on the preparation processes. In addition, the notable advantages of the crystal facet engineering of photoelectrodes in terms of light harvesting, charge separation and transfer, and surface reactions are critically discussed. This is followed by a systematic overview of the modification strategies of faceted photoelectrodes to further enhance the PEC performance. The last section summarizes the major challenges and some invigorating perspectives for future research on crystal facet engineered photoelectrodes, which are believed to play a vital role in promoting the development of this important research field.

Crystal facet engineering of photoelectrodes for photoelectrochemical water splitting

Rutile titanium dioxide (TiO2 ) is a promising photocatalyst due to its high thermodynamic stability and few intragrain defects. However, it has not yet achieved photocatalytic activity comparable to that of anatase TiO2 owing to its higher recombination rate of electron-hole pairs. To effectively separate the electron-hole pairs in rutile TiO2 , a facet heterojunction (FH) structure to prolong the lifetime of the photogenerated electrons is proposed. Ultrathin TiO2 nanosheets with different facets are coated in situ onto TiO2 nanorod (NR) substrates, where FHs are built among the nanosheets as well as between the nanosheets and NR substrates. The as-prepared rutile TiO2 , with an FH structure (FH-TiO2 ), serves as an effective photocatalyst for water splitting. More than 45 and 18 times higher photogenerated current density and H2 production rate, respectively, are obtained compared to those of pure rutile TiO2 NRs. Moreover, FH-TiO2 delivers a 0.566 mmol g-1 h-1 H2 production rate even in pure water. This study offers important insights into the rational design of rutile TiO2 structures for highly efficient photocatalytic reactions.

A Photoresponsive Rutile TiO2 Heterojunction with Enhanced Electron-Hole Separation for High-Performance Hydrogen Evolution.

Constructing hollow multi-shelled structures (HoMSs) has a significant effect on promoting light absorption property of catalysts and enhancing their performance in solar energy conversion applications. A facile hydrothermal method is used to design the SrTiO3 -TiO2 heterogeneous HoMSs by hydrothermal crystallization of SrTiO3 on the surface of the TiO2 HoMSs, which will realize a full coverage of SrTiO3 on the TiO2 surface and construct the SrTiO3 /TiO2 junctions. The broccoli-like SrTiO3 -TiO2 heterogeneous HoMSs exhibited a fourfold higher overall water splitting performance of 10.6 μmol h-1 for H2 production and 5.1 μmol h-1 for O2 evolution than that of SrTiO3 nanoparticles and the apparent quantum efficiency (AQE) of 8.6 % at 365 nm, which can be mainly attributed to 1) HoMS increased the light absorption ability of the constructed photocatalysts and 2) the SrTiO3 -TiO2 junctions boosted the separation efficiency of the photogenerated charge carriers.

Constructing SrTiO 3 -TiO 2 Heterogeneous Hollow Multi-shelled Structures for Enhanced Solar Water Splitting

Construction of internal electric fields (IEFs) is crucial to realize efficient charge separation for charge-induced redox reactions, such as water splitting and CO2 reduction. However, a quantitative understanding of the charge transfer dynamics modulated by IEFs remains elusive. Here, electron microscopy study unveils that the non-equilibrium photo-excited electrons are collectively steered by two contiguous IEFs within binary (001)/(200) facet junctions of BiOBr platelets, and they exhibit characteristic Gaussian distribution profiles on reduction facets by using metal co-catalysts as probes. An analytical model justifies the Gaussian curve and allows us to measure the diffusion length and drift distance of electrons. The charge separation efficiency, as well as photocatalytic performances, are maximized when the platelet size is about twice the drift distance, either by tailoring particle dimensions or tuning IEF-dependent drift distances. The work offers great flexibility for precisely constructing high-performance particulate photocatalysts by understanding charge transfer dynamics. 

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Unveiling the charge transfer dynamics steered by built-in electric fields in BiOBr photocatalysts

Metal oxide semiconductors with surface homojunctions characteristic of continuous band bending and well-defined epitaxial interfaces show amazing potential for photocatalytic applications. Herein, a new concept of facet junctions is proposed and validated according to the synergy between the co-exposed crystal facets of shape-tailored anatase TiO2 single crystals. By considering the atomic and electronic interactions between the co-exposed facets, our density functional theory calculations reveal the existence of type-II band alignment between the co-exposed {001} and {101} facets. This band alignment results in in situ construction of a facet junction to allow built-in facet-mediated carrier transfer. The self-constructed {101}/{001} facet junction, due to the effective carrier separation between different exposed facets, exhibits a significantly enhanced quantum efficiency and catalytic performance in photochemical hydrogen generation compared to TiO2 poly-crystals. These findings open a new horizon of facet junction-engineered nano-catalysts for more robust and efficient energy and environmental applications.

Epitaxial facet junctions on TiO2 single crystals for efficient photocatalytic water splitting

316L stainless steel samples were prepared by selective laser melting (SLM) and annealed at 1000 °C for durations of between 1 and 6 h to investigate both the kinetics of microstructural evolution during heat treatment and the effect of annealing on mechanical properties. The as-printed materials contain a high density of oxide particles and dislocations, forming a dislocation cell substructure that shows high thermal stability during heat treatment. Moreover, coarsened oxide particles act as pinning barriers for moving dislocations and grain boundaries, thus extending the recovery and recrystallization process. The process of recrystallization can be effectively tracked by measuring the density of the low-angle misorientation boundaries associated with the oxide particles and dislocations, as characterized by high-resolution EBSD. The evolution of mechanical properties during annealing shows a strong relationship with the observed microstructural changes, suggesting possible optimization of strength and ductility of SLM-prepared metal samples by use of appropriate heat treatments.

/pdf/effect-of-heat-treatment-on-microstructural-evolution-in-2h87ptah.pdf

Effect of Heat Treatment on Microstructural Evolution in Additively Manufactured 316L Stainless Steel

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Epitaxial facet junctions on TiO2 single crystals for efficient photocatalytic water splitting

Effect of Heat Treatment on Microstructural Evolution in Additively Manufactured 316L Stainless Steel