We summarise current state-of-the-art efficient visible-light driven heterojunction water splitting photo(electro)catalysts and describe how theoretical modelling of electronic structures at interfaces can explain their functionality.
It is widely accepted within the community that to achieve a sustainable society with an energy mix primarily based on solar energy we need an efficient strategy to convert and store sunlight into chemical fuels. A photoelectrochemical (PEC) device would therefore play a key role in offering the possibility of carbon-neutral solar fuel production through artificial photosynthesis. The past five years have seen a surge in the development of promising semiconductor materials. In addition, low-cost earth-abundant co-catalysts are ubiquitous in their employment in water splitting cells due to the sluggish kinetics of the oxygen evolution reaction (OER). This review commences with a fundamental understanding of semiconductor properties and charge transfer processes in a PEC device. We then describe various configurations of PEC devices, including single light-absorber cells and multi light-absorber devices (PEC, PV-PEC and PV/electrolyser tandem cell). Recent progress on both photoelectrode materials (light absorbers) and electrocatalysts is summarized, and important factors which dominate photoelectrode performance, including light absorption, charge separation and transport, surface chemical reaction rate and the stability of the photoanode, are discussed. Controlling semiconductor properties is the primary concern in developing materials for solar water splitting. Accordingly, strategies to address the challenges for materials development in this area, such as the adoption of smart architectures, innovative device configuration design, co-catalyst loading, and surface protection layer deposition, are outlined throughout the text, to deliver a highly efficient and stable PEC device for water splitting.
The use of hydrogen as a fuel, when generated from water using semiconductor photocatalysts and driven by sunlight, is a sustainable alternative to fossil fuels. Polymeric photocatalysts are based on earth-abundant elements and have the advantage over their inorganic counterparts that their electronic properties are easily tuneable through molecular engineering. Polymeric photocatalysts have developed rapidly over the last decade, resulting in the discovery of many active materials. However, our understanding of the key properties underlying their photoinitiated redox processes has not kept pace, and this impedes further progress to generate cost-competitive technologies. Here, we discuss state of the art polymeric photocatalysts and our microscopic understanding of their activities. We conclude with a discussion of five outstanding challenges in this field: nonstandardized reporting of activities, limited photochemical stability, insufficient knowledge of reaction mechanisms, balancing charge carrier lifetimes with catalysis timescales, and the use of unsustainable sacrificial reagents.
For the first time, it is demonstrated that the robust organic semiconductor g-C3N4 can be integrated into a nature-inspired water splitting system, analogous to PSII and PSI in natural photosynthesis. Two parallel systems have been developed for overall water splitting under visible light involving graphitic carbon nitride with two different metal oxides, BiVO4 and WO3. Consequently, both hydrogen and oxygen can be evolved in an ideal ratio of 2:1, and evolution rates in both systems have been found to be dependent on pH, redox mediator concentration, and mass ratio between the two photocatalysts, leading to a stable and reproducible H2 and O2 evolution rate at 36 and 18 μmol h(-1) g(-1) from water over 14 h. Our findings demonstrate g-C3N4 can serve as a multifunctional robust photocatalyst, which could also be used in other systems such as PEC cells or coupled solar cell systems.
Photocatalysis is a promising technology that can contribute to renewable energy production from water and water purification. In order to further develop the field and meet industrial requirements, it is imperative to focus on advancing high efficiency visible light photocatalysts, such as silver phosphate (Ag3PO4). This review aims to highlight the recent progress made in the field, focusing on oxygen production from water, and organic contaminant decomposition using Ag3PO4. The most important advances are discussed and explained in detail, including semiconductor-semiconductor junctions, metal-semiconductor junctions, exposing facet control, and fundamental understanding using advanced spectroscopies and computational chemistry. The review then concludes by critically summarising both findings and current perspectives, and ultimately how the field might best advance in the near future.
We report the synthesis and photoelectrochemical assessment of phase pure tetragonal matlockite structured BiOX (where X = Cl, Br, I) films.
aWater oxidation is a rate-determining step in solar driven H 2 fuel synthesis and is technically challenging to promote. Despite decades of effort, only a few inorganic catalysts are effective and even fewer are effective under visible light. Recently, attention has been paid to synthetic semiconducting polymers, mainly on graphitic C 3 N 4 , with encouraging hydrogen evolution performance but lower activity for water oxidation. Here, a highly ordered covalent triazine-based framework, CTF-1 (C 8 N 2 H 4 ), is synthesised by a very mild microwave-assisted polymerisation approach. It demonstrates extremely high activity for oxygen evolution under visible light irradiation, leading to an apparent quantum efficiency (AQE) of nearly 4% at 420 nm. Furthermore, the polymer can also efficiently evolve H 2 from water. A high AQE of 6% at 420 nm for H 2 production has also been achieved. The polymer holds great potential for overall water splitting. This exceptional performance is attributed to its well-defined and ordered structure, low carbonisation, and superior band positions. Broader contextSplitting water by sunlight is an attractive renewable approach to generate clean hydrogen for producing chemicals or powering vehicles. This ultra-pure hydrogen also avoids the dreaded catalyst poisoning, which occurs even with very low levels of CO residuals from fossil-fuel generated hydrogen. The key challenge to sustain continued hydrogen generation from this artificial photosynthesis process is to speed up the water oxidation reaction, which is hard to proceed due to multiple electron transfer steps. Oxidation catalysts based on polymeric semiconductors are particularly promising for this purpose because of their abundance leading to low cost, tunable band structure to match the solar spectrum and variable degree of conjugation to impact on the p-p* excitation for efficient electron transfer. With a moderate microwave assisted strategy, we are able to control the degree of conjugation and minimise the undesirable structural carbonisation of a new type of polymeric photocatalyst-covalent triazine-based framework. The optimised catalyst shows advantageous band positions, to capture a wide spectrum of visible light and enhance the charge separation efficiency, leading to very high water oxidation and hydrogen evolution capabilities. The overall discovery paves the way for the development of efficient and continuous clean hydrogen production from the renewable visible-light water splitting process.
A linker-controlled strategy has been demonstrated to synthesize polymeric photocatalysts for efficient H2 evolution by UV-Vis-IR with benchmark quantum yields.
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