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Hydrogen is readily obtained from renewable and non‐renewable resources via water splitting by using thermal, electrical, photonic and biochemical energy. The major hydrogen production is generated from thermal energy through steam reforming/gasification of fossil fuel. As the commonly used non‐renewable resources will be depleted in the long run, there is great demand to utilize renewable energy resources for hydrogen production. Most of the renewable resources may be used to produce electricity for driving water splitting while challenges remain to improve cost‐effectiveness. As the most abundant energy resource, the direct conversion of solar energy to hydrogen is considered the most sustainable energy production method without causing pollutions to the environment. In overall, this review briefly summarizes thermolytic, electrolytic, photolytic and biolytic water splitting. It highlights photonic and electrical driven water splitting together with photovoltaic‐integrated solar‐driven water electrolysis. Energy‐driven hydrogen production via water splitting with thermal, electrical, photonic and biochemical energy and their combined forms such as thermoelectrolysis, biophotolysis, and photoelectrolysis are summarized in this review. There are focuses on recent advances in water splitting with the use of renewable energy for photocatalytic and electrocatalytic hydrogen production such as photovoltaic‐integrated solar driven water electrolysis.

Clean water and the increased use of renewable energy are considered to be two of the main goals in the effort to achieve a sustainable living environment. The fulfillment of these goals may include the use of solar-driven photocatalytic processes that are found to be quite effective in water purification, as well as hydrogen generation. H2 production by water splitting and photocatalytic degradation of organic pollutants in water both rely on the formation of electron/hole (e−/h+) pairs at a semiconducting material upon its excitation by light with sufficient photon energy. Most of the photocatalytic studies involve the use of TiO2 and well-suited model compounds, either as sacrificial agents or pollutants. However, the wider application of this technology requires the harvesting of a broader spectrum of solar irradiation and the suppression of the recombination of photogenerated charge carriers. These limitations can be overcome by the use of different strategies, among which the focus is put on the creation of heterojunctions with another narrow bandgap semiconductor, which can provide high response in the visible light region. In this review paper, we report the most recent advances in the application of TiO2 based heterojunction (semiconductor-semiconductor) composites for photocatalytic water treatment and water splitting. This review article is subdivided into two major parts, namely Photocatalytic water treatment and Photocatalytic water splitting, to give a thorough examination of all achieved progress. The first part provides an overview on photocatalytic degradation mechanism principles, followed by the most recent applications for photocatalytic degradation and mineralization of contaminants of emerging concern (CEC), such as pharmaceuticals and pesticides with a critical insight into removal mechanism, while the second part focuses on fabrication of TiO2-based heterojunctions with carbon-based materials, transition metal oxides, transition metal chalcogenides, and multiple composites that were made of three or more semiconductor materials for photocatalytic water splitting.

Janus two-dimensional (2D) materials, referring to the layers with different surfaces, have attracted intensive research interest due to the unique properties induced by symmetry breaking, and promising applications in energy conversion. Based on the successful experimental synthesis of Janus transition metal dichalcogenides (TMDC), here we present a review on their potential application in photocatalytic overall water splitting, from the perspectives of the latest theoretical and experimental progress. Four aspects which are related to photocatalytic reaction, including the adsorption of water molecules, utilization of sunlight, charge separation and transport, and surface chemical reactions have been discussed, and it is concluded that the Janus structures have better performances than symmetric TMDCs. At the end of this review, we raise further challenges and possible future research directions for Janus 2D materials as water-splitting photocatalysts.

Heterostructure catalysts are highly anticipated in the field of photocatalytic water splitting. AlN/Sc2CF2 and GaN/Sc2CF2 heterostructures are proposed in this work, and the electronic structures were revealed with the first-principles method to explore their photocatalytic properties for water splitting. The results found that the thermodynamically stable AlN/Sc2CF2 and GaN/Sc2CF2 heterostructures are indirect semiconductors with reduced band gaps of 1.75 eV and 1.84 eV, respectively. These two heterostructures have been confirmed to have type-Ⅰ band alignments, with both VBM and CBM contributed to by the Sc2CF2 layer. AlN/Sc2CF2 and GaN/Sc2CF2 heterostructures exhibit the potential for photocatalytic water splitting as their VBM and CBM stride over the redox potential of water. Gibbs free energy changes in HER occurring on AlN/Sc2CF2 and GaN/Sc2CF2 heterostructures are as low as −0.31 eV and −0.59 eV, respectively. The Gibbs free energy change in HER on the AlN (GaN) layer is much lower than that on the Sc2CF2 surface, owing to the stronger adsorption of H on AlN (GaN). The AlN/Sc2CF2 and GaN/Sc2CF2 heterostructures possess significant improvements in absorption range and intensity compared to monolayered AlN, GaN, and Sc2CF2. In addition, the band gaps, edge positions, and absorption properties of AlN/Sc2CF2 and GaN/Sc2CF2 heterostructures can be effectively tuned with strains. All the results indicate that AlN/Sc2CF2 and GaN/Sc2CF2 heterostructures are suitable catalysts for photocatalytic water splitting.

Heterostructures are highly promising photocatalyst candidates for water splitting due to their advanced properties than those of pristine components. The ZnO/Sc2CF2 heterostructure was designed in this work, and its electronic structure was investigated to explore its potential for water splitting. The assessments of binding energy, phonon spectrum, ab initio molecular dynamics, and elastic constants provide strong evidence for its stability. The ZnO/Sc2CF2 heterostructure has an indirect band gap of 1.93 eV with a type-Ⅰ band alignment. The electronic structure can be modified with strain, leading to a transition in band alignment from type-Ⅰ to type-Ⅱ. The heterostructure is suitable for water splitting since its VBM and CBM stride over the redox potential. The energy barrier and built-in electric field, resulting from the charge transfer, facilitate the spatial separation of photogenerated carriers, enhancing their utilization efficiency for redox processes. The photogenerated carriers in the heterostructures with lattice compression greater than 6% follow the direct-Z transfer mechanism. The ZnO/Sc2CF2 heterostructure is confirmed with high photocatalytic activity by a Gibbs free energy change of HER, which is 0.89 eV and decreases to −0.52 eV under an 8% compressive strain. The heterostructure exhibits a remarkable enhancement in both absorption range and intensity, which can be further improved with strains. All these findings suggest that the ZnO/Sc2CF2 heterostructure is an appreciated catalyst for efficient photocatalytic water splitting.

Single-atom photocatalysts exhibit outstanding performance in energy and environmental photocatalysis, due to their exceptional capabilities in enhancing light-harvesting, charge transfer dynamics, and surface reactions. The key to preparing single-atom photocatalysts lies in developing an appropriate metal-support that can prevent aggregation or sintering during synthetic procedures. In this work, a Co(II)-urea complexe in-situ formed in melamine was employed as single-atom Co precursors to synthesize an efficient single-atom Co decorated P doped g-C 3 N 4 (Co/PCN) photocatalyst. The high-angle annular dark field transmission electron microscope (HAADF-TEM) results indicated abundant Co single atoms were immobilized in the g-C 3 N 4 matrix. Under visible-light irradiation, the as-prepared photocatalysts show remarkably enhanced photocatalytic performance. Especially, loaded with 1.5 wt% single atoms Co, the optimized Co/PCN exhibits H 2 evolution of 892.5 µmol g −1  h −1 , which is 33 times higher than that of PCN, and even twice as much as that of Pt-loaded g-C 3 N 4 (Pt/PCN). The enhanced photocatalytic activity is ascribed to the synergistic effect between single-atom Co and P doping, which facilitates efficient light harvesting, charge separation, and migration. It is believed that this study paves a new avenue for developing high-efficiency single-atom photocatalysts. Graphical Abstract

Renewable hydrogen production is a sustainable method for the development of next-generation energy technologies. Utilising solar energy and photocatalysts to split water is an ideal method to produce hydrogen. In this review, the fundamental principles and recent progress of hydrogen production by artificial photosynthesis are reviewed, focusing on hydrogen production from photocatalytic water splitting using organic-inorganic composite-based photocatalysts.

Solar water splitting (SWS) has been researched for about five decades, but despite successes there has not been a big breakthrough advancement. While the three fundamental steps, light absorption, charge carrier separation and diffusion, and charge utilization at redox sites are given a great deal of attention either separately or simultaneously, practical considerations that can help to increase efficiency are rarely discussed or put into practice. Nevertheless, it is possible to increase the generation of solar hydrogen by making a few little but important adjustments. In this review, we talk about various methods for photocatalytic water splitting that have been documented in the literature and importance of the thin film approach to move closer to the large-scale photocatalytic hydrogen production. For instance, when comparing the film form of the identical catalyst to the particulate form, it was found that the solar hydrogen production increased by up to two orders of magnitude. The major topic of this review with thin-film forms is, discussion on several methods of increased hydrogen generation under direct solar and one-sun circumstances. The advantages and disadvantages of thin film and particle technologies are extensively discussed. In the current assessment, potential approaches and scalable success factors are also covered. As demonstrated by a film-based approach, the local charge utilization at a zero applied potential is an appealing characteristic for SWS. Furthermore, we compare the PEC-WS and SWS for solar hydrogen generation and discuss how far we are from producing solar hydrogen on an industrial scale. We believe that the currently employed variety of attempts may be condensed to fewer strategies such as film-based evaluation, which will create a path to address the SWS issue and achieve sustainable solar hydrogen generation.

Photocatalytic water splitting is an environmentally friendly hydrogen production method that uses abundant renewable resources such as water and sunlight. While Titanium dioxide (TiO2) photocatalyst exhibits excellent properties, its high band gap limits absorption to ultraviolet (UV) irradiation, resulting in low photo conversion efficiency. This review explores various modification techniques aimed at enhancing the efficiency of TiO2 under visible light irradiation. Factors influencing the photocatalytic water splitting reaction, such as catalyst structure, morphology, band gap, sacrificial reagents, light intensity, temperature, and potential of Hydrogen (pH) are examined. This review also summarizes different catalyst synthesis methods, and types of photocatalytic reactors, and provides insights into quantum yield. Finally, the review addresses the challenges and future outlook of photocatalytic water splitting. Solar and water are critical in addressing the global challenge of energy. Photocatalytic production of hydrogen is a step toward a truly reliable renewable energy source. The paper dwells into the roles of TiO2 as a catalyst in the production of hydrogen. Challenges and prospects facing this promising process are also discussed.

In this work we have narrowed the band gap of orthorhombic sodium tantalate by doping the perovskite structure with 5 and 10% of iron. The hydrothermal method was used in the preparation of the samples. Moreover, the evolution of hydrogen by photocatalytic water splitting is reported for first time for orthorhombic NaTaO 3 mono-doped with Fe. The band gap was reduced from 4.08 to 3.24 eV for sodium tantalate doped with 5% of Fe, and up to 2.05 eV for the perovskite doped with 10% of Fe. The highest photocatalytic activity was obtained with the semiconductor that had 5% of Fe. Which was attributable to its smaller particle size, larger specific surface area and lower recombination of electron–hole pairs in contrast with the sample that had 10% of Fe. X-ray diffraction, energy dispersive X-ray spectroscopy, transmission electron microscopy, nitrogen physisorption, ultraviolet–visible diffuse reflectance and photoluminescence spectroscopies were used to analyze the perovskite materials. Graphical Abstract