The localized surface plasmon resonances (LSPR) effect makes W18O49 an effective visible and near‐infrared (NIR) light antenna to realize full‐spectrum solar‐light driven photocatalysis, yet the precise origin remains elusive. Here, the LSPR originates from the localized electron confinement around lattice W5+–W5+ pairs in the unique structure of W18O49 by density‐functional theory calculation, which gives W18O49 a broad absorption ranging from visible to NIR region, independent of the particle shape and size is confirmed. This unique periodic LSPR simplifies the design of W18O49‐sensitized photocatalytic composite into enhancing the light absorbance of W18O49 and screening photocatalytic semiconductors with suitable energy band potentials. To this end, hierarchical‐structure W18O49 microflowers with high absorbance have been coated with ZnIn2S4 nanosheets to achieve cocatalyst‐free photocatalytic composite, which presents an outstanding H2 production rate of 902.57 µmol within 3 h under simulated solar‐light. Comprehensive characterizations, including ultrafast transient absorption spectroscopy, prove the injection of hot electrons from W18O49 to ZnIn2S4 and the increase of long‐lived active electrons. This work clarifies the LSPR origin of oxygen‐deficient semiconductors and paves the way for the search of broad‐spectrum active photocatalyst.

W5+–W5+ Pair Induced LSPR of W18O49 to Sensitize ZnIn2S4 for Full‐Spectrum Solar‐Light‐Driven Photocatalytic Hydrogen Evolution

Construction of heterojunction is conventionally regarded as the prevailing technique to render effective solar-driven photocatalytic water splitting. Nonetheless, realization of p-n homojunction emerges to be an appealing scheme attributed to the non-defective layer coupling and minor charge transfer impedance. Herein, nitrogen-doped ZnIn2S4 (N-ZIS) with dual p-n charge properties was facilely synthesized via one-step in-situ solvothermal method. Systematic investigations unveil that the substituting phenomenon of hosting S by extrinsic N atom with dissimilar electronegativity and valence electron, which eventually ameliorates charge transfer rate and inhibits electron-hole pairs recombination. First-principle density functional theory calculations affirm the p-nature induced by N-doping imparting favorable charge redistribution in the ZIS framework and diminishing hydrogen (H2) evolution reaction kinetic barrier at the surface-active sites. Therein, optimal N-ZIS generated 1575.71 μmol∙g-1 of H2 under 6-hour visible-light irradiation (with an apparent quantum yield of 6.59% at 420 nm monochromatic light irradiation), which is 6.35-fold than the pristine counterpart. 

Non-metal doping induced dual p-n charge properties in a single ZnIn2S4 crystal structure provoking charge transfer behaviors and boosting photocatalytic hydrogen generation

Metal-sulfide nanostructures have piqued the interest of researchers for decades due to their intriguing optoelectronic properties. Indeed, significant advances and improvements have been made in various fundamental aspects for cutting-edge applications, such as water splitting and hydrogen production. Furthermore, rising demand for low-dimensional materials due to lower material consumption and improved performance due to quantum size effects has spurred research on semiconducting metal sulfides. Consequently, size-controllable nanostructures with diverse morphologies have been fabricated and studied for potential applications. However, the photocatalytic hydrogen evolution rate is still limited mainly by fast recombination rate, poor solar energy utilization and lack of surface-active sites for H2 reduction. This review will highlight particularly recent findings in metal-sulfide-based photocatalysts for hydrogen evolution reactions, considering the swift development and excellent research in this field. Following a brief overview of fundamental properties, we will explore state-of-the-art strategies for enhancing H2 generation efficiencies over the pristine, heterostructured and co-catalayzed metal-sulfide photocatalysts.

https://www.mdpi.com/2073-4344/12/11/1316/pdf?version=1667386496

Metal Sulfide Photocatalysts for Hydrogen Generation: A Review of Recent Advances

Abstract Metal sulfide‐based homojunction photocatalysts are extensively explored with improved photocatalytic performance. However, the construction of metal sulfide‐based S‐scheme homojunction remains a challenge. Herein, the fabrication of 2D CdIn2S4 nanosheets coated 3D CdIn2S4 octahedra (referred to as 2D/3D n‐CIS/o‐CIS) S‐scheme homojunction photocatalyst is reported by simply adjustment of polyvinyl pyrrolidone amount during the solvothermal synthesis. The formation of S‐scheme homojunction within n‐CIS/o‐CIS is systematically investigated via a series of characterizations, which can generate an internal electric field to facilitate the separation and migration of photogenerated electron‐hole pairs. The 2D/3D n‐CIS/o‐CIS composite exhibits significantly improved photocatalytic activity and stability in the selective oxidation of phenylcarbinol (PhCH2OH) to benzaldehyde (PhCHO) when compared to pure n‐CIS and o‐CIS samples under visible light irradiation. It is hoped that this work can contribute novel insights into the development of metal sulfides S‐scheme homojunction photocatalysts for solar energy conversion.

Metal Sulfide S-Scheme Homojunction for Photocatalytic Selective Phenylcarbinol Oxidation.

S-scheme regulated Ni2P-NiS/twinned Mn0.5Cd0.5S hetero-homojunctions for efficient photocatalytic H2 evolution

Recent Advances in Nanoscale Engineering of Ternary Metal Sulfide-Based Heterostructures for Photocatalytic Water Splitting Applications

Abstract Engineering an efficient semiconductor to sustainably produce green hydrogen via solar-driven water splitting is one of the cutting-edge strategies for carbon-neutral energy ecosystem. Herein, a superhydrophilic green hollow ZnIn 2 S 4 (gZIS) was fabricated to realize unassisted photocatalytic overall water splitting. The hollow hierarchical framework benefits exposure of intrinsically active facets and activates inert basal planes. The superhydrophilic nature of gZIS promotes intense surface water molecule interactions. The presence of vacancies within gZIS facilitates photon energy utilization and charge transfer. Systematic theoretical computations signify the defect-induced charge redistribution of gZIS enhancing water activation and reducing surface kinetic barriers. Ultimately, the gZIS could drive photocatalytic pure water splitting by retaining close-to-unity stability for a full daytime reaction with performance comparable to other complex sulfide-based materials. This work reports a self-activated, single-component cocatalyst-free gZIS with great exploration value, potentially providing a state-of-the-art design and innovative aperture for efficient solar-driven hydrogen production to achieve carbon-neutrality. 

Self-activated superhydrophilic green ZnIn2S4 realizing solar-driven overall water splitting: close-to-unity stability for a full daytime

Abstract ZnIn 2 S 4 (ZIS) is an efficient photocatalyst for solar hydrogen (H 2 ) generation from water splitting owing to its suitable band gap, excellent photocatalytic behaviour and high stability. Nevertheless, modifications are still necessary to further enhance the photocatalytic performance of ZIS for practical applications. This has led to our interest in exploring phosphorus doping on ZIS for photocatalytic water splitting, which has not been studied till date. Herein, phosphorus-doped ZnIn 2 S 4 (P-ZIS) was modelled via Density Functional Theory to investigate the effects of doping phosphorus on the structural and electronics properties of ZIS as well as its performance toward photocatalytic water splitting. This work revealed that the replacement of S3 atom by substitutional phosphorus gave rise to the most stable P-ZIS structure. In addition, P-ZIS was observed to experience a reduction in band gap energy, an upshift of valence band maximum (VBM), an increase in electron density near VBM and a reduction of H* adsorption–desorption barrier, all of which are essential for the enhancement of the hydrogen evolution reaction. In overall, detailed theoretical analysis carried out in this work could provide critical insights towards the development of P-ZIS-based photocatalysts for efficient H 2 generation via solar water splitting. 

/pdf/insights-from-density-functional-theory-calculations-on-2efx6bxd.pdf

Insights from density functional theory calculations on heteroatom P-doped ZnIn2S4 bilayer nanosheets with atomic-level charge steering for photocatalytic water splitting

Bismuth-rich Bi12O17Cl2 nanorods engineered with oxygen vacancy defects for enhanced photocatalytic nitrogen fixation

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