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

Photoreduction of CO2 into sustainable and green solar fuels is generally believed to be an appealing solution to simultaneously overcome both environmental problems and energy crisis. The low selectivity of challenging multi-electron CO2 photoreduction reactions makes it one of the holy grails in heterogeneous photocatalysis. This Review highlights the important roles of cocatalysts in selective photocatalytic CO2 reduction into solar fuels using semiconductor catalysts. A special emphasis in this review is placed on the key role, design considerations and modification strategies of cocatalysts for CO2 photoreduction. Various cocatalysts, such as the biomimetic, metal-based, metal-free, and multifunctional ones, and their selectivity for CO2 photoreduction are summarized and discussed, along with the recent advances in this area. This Review provides useful information for the design of highly selective cocatalysts for photo(electro)reduction and electroreduction of CO2 and complements the existing reviews on various semiconductor photocatalysts.

Cocatalysts for Selective Photoreduction of CO2 into Solar Fuels.

Spinels with the formula of AB2O4 (where A and B are metal ions) and the properties of magnetism, optics, electricity, and catalysis have taken significant roles in applications of data storage, biotechnology, electronics, laser, sensor, conversion reaction, and energy storage/conversion, which largely depend on their precise structures and compositions. In this review, various spinels with controlled preparations and their applications in oxygen reduction/evolution reaction (ORR/OER) and beyond are summarized. First, the composition and structure of spinels are introduced. Then, recent advances in the preparation of spinels with solid-, solution-, and vapor-phase methods are summarized, and new methods are particularly highlighted. The physicochemical characteristics of spinels such as their compositions, structures, morphologies, defects, and substrates have been rationally regulated through various approaches. This regulation can yield spinels with improved ORR/OER catalytic activities, which can furth...

Spinels: Controlled Preparation, Oxygen Reduction/Evolution Reaction Application, and Beyond

Microwave-assisted preparation of inorganic nanostructures in liquid phase.

Multiferroic bismuth ferrite-based materials for multifunctional applications: Ceramic bulks, thin films and nanostructures

Water oxidation reaction (i.e., OER) is the one of most challenging reaction steps in the photocatalytic overall CO2 reduction, especially on metal sulfide photocatalysts. Herein, we first demonstrate that the...

Boosting Water Decomposition by Sulfur Vacancy for Efficient CO2 Photoreduction

Self-doping by Ti3+ is a useful method to expand the light response of TiO2 into the visible light region. However, to obtain a stable Ti3+-doped TiO2 seems to be a challenge due to the easy oxidation of Ti3+ during the heterogeneous reaction. Here, we propose a simple carbon coating route to stabilize the Ti3+-doped TiO2, in which both the Ti3+ and precursor of the carbon coating layer were in situ formed from the hydrothermal hydrolysis of titanium isopropoxide. The carbon coated Ti3+-doped TiO2 exhibited excellent stability for photocatalytic hydrogen production. Based on electron paramagnetic resonance (EPR) analysis, the proposed stabilizing mechanism is that the conductive carbon coating layer as a barrier layer prevents the H2O and O2 from diffusing into the surface of the photocatalyst, which can oxidize the surface O vacancies and Ti3+ in TiO2. Our findings offer a simple route to prepare a highly stable TiO2-based photocatalyst with visible light response.

Carbon coating stabilized Ti3+-doped TiO2 for photocatalytic hydrogen generation under visible light irradiation

Accelerating electron transfer kinetics is an efficient strategy to tackle sluggish oxygen evolution reaction (OER). Herein, Ni3Fe1-xVx/Ni3Fe1-xVxN heterojunctions were elaborately constructed to demonstrate that the coupling of variable-valence metal doping...

Variable-valence ion and heterointerface accelerated electron transfer kinetics of electrochemical water splitting

Herein, we report highly efficient carbon supported Ni-MoO2 heterostructured catalysts for the electrochemical hydrogenation (ECH) of phenol in 0.10 M aqueous sulfuric acid (pH = 0.7) at 60 °C. Highest yields for cyclohexanol and cyclohexanone of 95% and 86% with faradaic efficiencies of ~50% are obtained with catalysts bearing high and low densities of oxygen vacancy (Ov) sites, respectively. In situ diffuse reflectance infrared spectroscopy and density functional theory calculations reveal that the enhanced phenol adsorption strength is responsible for the superior catalytic efficiency. Furthermore, 1-cyclohexene-1ol is an important intermediate. Its hydrogenation route and hence the final product are affected by the Ov density. This work opens a promising avenue to the rational design of advanced electrocatalysts for the upgrading of phenolic compounds.

Selective Electrochemical Hydrogenation of Phenol with Earth-abundant Ni-MoO2 Heterostructured Catalysts: Effect of Oxygen Vacancy on Product Selectivity.

Photocathodes consisting of semiconductors and cocatalysts have demonstrated promising performances for the solar-driven CO2 reduction reaction (CO2 RR) and the H2 evolution reaction. However, the performance of cocatalyst materials has been limited due to the degradation of semiconductors during the loading processes. Hence, a photocathode that withstands harsh reaction conditions can broaden the selection of cocatalyst materials and improve catalytic activity. Here, we have developed Ag halide (AgX, X = Cl, Br, I) cocatalysts, which are transformed by anodization of Ag on GaN nanowires (NWs)/n+–p Si heterojunction photocathodes, for CO2 RR to syngas with superior performance. N-terminated GaN NWs are chemically robust modifiers to load the cocatalysts of AgCl and AgBr. As a result, the photocathodes showed a superior faradaic efficiency of CO >80% at −0.4 VRHE and an onset potential of ∼0.2 VRHE because the halogen elements reduce the energy barrier for forming a *COOH intermediate from CO2. Moreover, a record high photocurrent density of ∼92 mA/cm2 was achieved under concentrated solar light (300 mW/cm2) without any noticeable change in the CO/H2 syngas ratio for 12 h operation. The present findings offer critical insights into the design and development of photocathodes for selective, productive, and stable solar fuel generation. 

Silver Halide Catalysts on GaN Nanowires/Si Heterojunction Photocathodes for CO2 Reduction to Syngas at High Current Density

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