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G‐C3N4‐SiC‐Pt for Enhanced Photocatalytic H2 Production from Water under Visible Light Irradiation
摘要： The g-C3N4 and SiC has drawn increasing attention for application to visible light photocatalytic hydrogen evolution from water splitting due to their unique band structure and high physicochemical stability. In this study, g-C3N4-SiC heterojunction with loaded noble metal was constructed. The g-C3N4-SiC-Pt composite photocatalysts were successfully prepared by the combination method of a bio-reduction, sol-deposition and calcination. The layers of g-C3N4 were thinned and the SiC and Pt nanoparticles simultaneously were tightly bound to g-C3N4 by calcination in the process of preparing the g-C3N4-SiC-Pt. The heterojunction formed in the interface of SiC and g-C3N4 enhances the separation efficiency of the photogenerated electron-hole pairs. These composite photocatalysts achieve a high hydrogen evolution rate of 595.3 μmol·h-1·g-1 with a 1wt% of deposited Pt, 3.7- and 2.07-fold higher than g-C3N4-bulk and g-C3N4-SiC under visible-light irradiation with a quantum efficiency of 2.76% at 420 nm, respectively.
关键词： visible light,g-C3N4-SiC-Pt photocatalysts,hydrogen evolution,photocatalysis
更新于2025-11-21 11:01:37
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Few-Layered 1T-MoS2-Modified ZnCoS Solid-Solution Hollow Dodecahedra for Enhanced Photocatalytic Hydrogen Evolution
摘要： Enhancing solar hydrogen production efficiency essentially relies on the modification of low-cost and highly stable photocatalysts with enhanced light-harvesting ability and promoted charge transfer kinetics. Herein, we report a facile synthetic route to modify the performance of a low-cost metal sulfide semiconductor, consisting of the bimetallic metal-organic frameworks (MOFs)-templating and the simultaneous sulfidation of the photocatalyst and loading of MoS2 co-catalyst. The mutual sulfur atom shared by all the transition metal sulfides allowed the formation of ZnCoS solid-solution structure and the stabilization of the metallic 1T-MoS2 phase, contributing to the photocatalytic activity enhancement from several aspects: i) extending the light absorption region from UV to visible and near-infrared light by the incorporation of another transition metal sulfide species, i.e., CoS; ii) achieving abundant catalytically active sites, and high electronic conductivity between the intimately contacted ZnCoS and MoS2 by loading few-layered 1T-MoS2; and iii) further increasing its capability of utilizing the single-photon with relatively higher energy in the UV-visible region by the involvement of a metal-free photosensitizer–Eosin Y (EY). As a consequence, the novel few-layered 1T MoS2-modified hollow Zn0.5Co0.5S rhombic dodecahedra exhibited a high photocatalytic H2 production activity of 15.47 mmol h-1 g-1 with an apparent quantum efficiency of 30.3% at 420 nm and stability with 90% H2 evolution retention even after seven consecutive runs for total 35 h irradiation. This novel approach to prepare advanced materials could be further extended to the phase-controllable preparation of MoS2 and the discovery of other transition metal chalcogenides with high activity and stability in various applications.
关键词： ZnCoS solid-solution,hollow dodecahedra,dye-sensitization,1T-MoS2,photocatalytic hydrogen evolution,MOF-templating
更新于2025-11-21 10:59:37
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Molybdenum Disulfide Catalytic Coatings via Atomic Layer Deposition for Solar Hydrogen Production from Copper Gallium Diselenide Photocathodes
摘要： We demonstrate that applying atomic layer deposition-derived molybdenum disulfide (MoS2) catalytic coatings on copper gallium diselenide (CGSe) thin film absorbers can lead to efficient wide band gap photocathodes for photoelectrochemical hydrogen production. We have prepared a device that is free of precious metals, employing a CGSe absorber and a cadmium sulfide (CdS) buffer layer, a titanium dioxide (TiO2) interfacial layer, and a MoS2 catalytic layer. The resulting MoS2/TiO2/CdS/CGSe photocathode exhibits a photocurrent onset of +0.53 V vs RHE and a saturation photocurrent density of ?10 mA cm?2, with stable operation for >5 h in acidic electrolyte. Spectroscopic investigations of this device architecture indicate that overlayer degradation occurs inhomogeneously, ultimately exposing the underlying CGSe absorber.
关键词： hydrogen evolution,molybdenum disulfide,photoelectrochemical water splitting,atomic layer deposition,copper gallium diselenide
更新于2025-11-19 16:56:35
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Colloidally synthesized defect-rich $$\hbox {MoSe}_{2}$$ MoSe 2 nanosheets for superior catalytic activity
摘要： Transition metal dichalcogenide (TMD) nanosheets (NSs) with defect-rich and vertically aligned edges are highly advantageous for various catalytic applications. However, colloidal synthesis of defect-rich NSs with thickness variation has been a challenging task. Here, we report a colloidal synthesis of 2H-MoSe2 NSs having a large number of defects and vertically aligned edges, where the thickness is varied by changing the amount of coordinating solvent. The Se-vacancies in these NSs have introduced defect sites which are corroborated by the presence of additional vibration modes in Raman spectra. These NSs exhibit electrocatalytic hydrogen evolution reaction performances with a low overpotential (210–225 mV) at 10 mA cm?2 current density and a small Tafel slope (54–68 mV per decade). Moreover, these MoSe2 NSs are also employed as counter electrodes (CEs) for the fabrication of dye sensitized solar cells via a cost-effective and simplified procedure. The power conversion efficiencies of 7.02 ± 0.18%, comparable with Pt CE (7.84 ± 0.10%) could be routinely achieved. These results demonstrate a novel synthetic strategy to prepare layered TMDs with superior catalytic applications.
关键词： counter electrode,Transition metal dichalcogenides,dye sensitized solar cells,MoSe2 nanosheets,hydrogen evolution reaction
更新于2025-11-19 16:56:35
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A novel photocatalyst, Y2SiO5:Pr3+,Li/Pt-NaNbxTa1?xO3, for highly efficient photocatalytic hydrogen evolution under visible-light irradiation
摘要： In this work, Y2SiO5:Pr3+,Li, as an excellent up-conversion luminescence agent from visible-light to ultraviolet-light, is synthesized by using sol-gel method. And then, a series of Y2SiO5:Pr3+,Li/NaNbxTa1?xO3 (x = 0.00, 0.25 and 0.50) with different amounts of Y2SiO5:Pr3+,Li are prepared by using hydrothermal method. The prepared samples are characterized by X-ray diffractometer (XRD), scanning electron microscopy (SEM), energy dispersive X-ray spectroscopy (EDX), X-ray photoelectron spectroscopy (XPS), UV–vis absorption spectroscopy and photoluminescence spectroscopy (PL). The activities of Y2SiO5:Pr3+,Li/Pt-NaNbxTa1?xO3 are investigated through photocatalytic hydrogen evolution in 10 vol% methanol solution under visible-light irradiation. The influences of Nb content in NaNbxTa1?xO3, mass ratio of Y2SiO5:Pr3+,Li and NaNb0.5Ta0.5O3, visible-light irradiation time and reuse-times are examined on the visible-light photocatalytic hydrogen evolution. The experimental results showed that the prepared Y2SiO5:Pr3+,Li/Pt-NaNb0.5Ta0.5O3 with 0.4:1.0 mass ratio of Y2SiO5:Pr3+,Li and NaNb0.5Ta0.5O3 and 0.25 wt% Pt loading displayed a highest evolved hydrogen activity under visible-light irradiation. This study may provide some significant references for large scale photocatalytic hydrogen evolution utilizing solar energy.
关键词： Visible-light photocatalyst (Y2SiO5:Pr3+,Li/Pt-NaNb0.5Ta0.5O3),Photocatalytic hydrogen evolution,Pt loading,Nb-substituted NaTaO3,Up-conversion luminescence agent (Y2SiO5:Pr3+,Li)
更新于2025-11-19 16:51:07
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Poly(1,4-di(2-thienyl))benzene Facilitating Complete Light-Driven Water Splitting under Visible Light at High pH
摘要： The recent discovery that metal-free polyterthiophene (PTTh) prepared by iodine-vapor-assisted polymerization (IVP) can catalyze the hydrogen evolution reaction (HER) when illuminated, and this light-enhanced electrolysis expresses a non-Nernstian relation with pH, provides the foundation for further improvement of the photovoltage of the reaction by engineering the band structure of the light-absorbing polymer. Deviating from an all-thiophene backbone, using poly(1,4-di(2-thienyl))benzene (PDTB) lowers the highest occupied molecular orbital level by ≈0.3 eV compared with polythiophene, and PDTB simultaneously maintains the photoelectrocatalytic properties without an all-thiophene backbone, resulting in very high conversion rate of 600 mmol(H2) h?1 g?1 at 0 V versus the reversible hydrogen electrode (RHE) at pH 11. PDTB shows the same non-Nernstian behavior as PTTh with increasing onset potential (versus RHE) at higher pH, and the open circuit potential on PDTB under visible light reaches 1.4 V versus RHE at pH 12. The PDTB photocathode thus produces a photovoltage above the theoretical potential for the complete water-splitting (1.229 V) and is indeed able to produce hydrogen in a one-photon-per-electron light-driven water splitting setup with MnOx as the anode at a rate of 6.4 mmol h?1 gPDTB?1.
关键词： high pH,photocathodes,water splitting,hydrogen evolution,poly(1,4-di(2-thienyl))benzene
更新于2025-11-19 16:51:07
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Effect of conduction band potential on cocatalyst-free plasmonic H <sub/>2</sub> evolution over Au loaded on Sr <sup>2+</sup> -doped CeO <sub/>2</sub>
摘要： There is little information on the effect of the conduction band (CB) position on plasmonic hydrogen (H2) formation under visible light irradiation over gold (Au) nanoparticles supported on semiconductors because there were no appropriate materials for which the CB position gradually changes. In this study, we analyzed the flatband potential of strontium ion (Sr2+)-doped cerium(IV) oxide (CeO2:Sr) and found that the CB position gradually shifted negatively from +0.031 V to ?1.49 V vs. NHE with an increase in the Sr2+ mole fraction. Plasmonic photocatalysts consisting of Au nanoparticles, CeO2:Sr and a platinum (Pt) cocatalyst were prepared and characterized by using X-ray diffraction, UV-vis spectroscopy, and transmission electron spectroscopy. Photocatalytic reaction under visible light irradiation revealed that H2 was produced over Au nanoparticles supported on CeO2:Sr having the CB potential of ?0.61 V vs. NHE and that the negative limit of the CB position for electron injection from Au nanoparticles existed between ?0.61 V and ?1.49 V vs. NHE. We found that Au/CeO2:Sr plasmonic photocatalysts also produced H2 without the aid of a Pt cocatalyst due to the sufficiently negative potential of electrons injected into the CB of CeO2:Sr.
关键词： hydrogen evolution,visible light irradiation,gold nanoparticles,plasmonic photocatalysts,strontium-doped cerium oxide
更新于2025-11-19 16:51:07
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Dual Function of Graphene Oxide for Assisted Exfoliation of Black Phosphorus and Electron Shuttle in Promoting Visible and Near-Infrared Photocatalytic H2 Evolution
摘要： The search for suitable photocatalysts with broadband absorption in visible and near-infrared (NIR) region is recognized as one of the most challenging issues on solar energy utilization. Black phosphorous (BP) is demonstrated as an effective visible and NIR activated material in solar energy conversion. However, traditional liquid exfoliation yield is low and the rigid structure and insoluble properties of pristine BP hinder its high-yield of hybridization. Herein, a new and stable noble-metal-free ternary photocatalyst molybdenum disulfide (MoS2)-BP/graphene oxide (GO) was constructed for splitting water to H2, showing dual functions of GO in synthetic and photocatalytic processes. Under visible-NIR light irradiation, the H2 evolution rates of MoS2-BP/GO was enhanced to 3.47 μmol h-1. Rapid electron injection efficiency from excited BP to GO and to MoS2 was confirmed by femtosecond transient absorption spectroscopy. This study provides new insight into the design of nanomaterials, and offers a noble-metal-free protocol with noble-metal-free.
关键词： visible and NIR,hydrogen evolution,graphene oxide,black phosphorous,noble-metal-free
更新于2025-11-19 16:51:07
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Self-generating CeVO4 as conductive channel within CeO2/CeVO4/V2O5 to induce Z-scheme-charge-transfer driven photocatalytic degradation coupled with hydrogen production
摘要： The construction of highly efficient Z-scheme photocatalytic system is regarded as a hot research topic in the fields of environmental remediation and renewable energy production. In this work, a novel Z-scheme CeO2/CeVO4/V2O5 photocatalyst is successfully prepared by using solid phase reaction method. The photocatalytic degradation of organic pollutant (Methylene Blue) with simultaneous hydrogen production is efficiently realized over the prepared Z-scheme CeO2/CeVO4/V2O5 photocatalysts under visible-light irradiation. The effects of treatment temperatures and treatment times of CeO2/V2O5 composite on the photocatalytic performance of Z-scheme CeO2/CeVO4/V2O5 photocatalyst are studied. The as-prepared Z-scheme CeO2/CeVO4/V2O5 (550-3) photocatalyst heat-treated at 550 °C for 3.0 h exhibits the highest photocatalytic performance. It can be ascribed to a moderate amount of CeVO4 nanoparticles generated between CeO2 and V2O5. The generated CeVO4 nanoparticles can be used as effective conductive channel to transfer the photo-generated carriers. At the same time, as redox reaction centers it can further accelerate the transfer of photo-generated electrons, effectively enhancing the separation efficiency of photo-generated electron and hole pairs. Furthermore, cyclic test demonstrates that the as-prepared Z-scheme CeO2/CeVO4/V2O5 (550-3) photocatalyst still maintains a high level of photocatalytic activity within five periods under the same conditions. Moreover, the related photocatalytic mechanism for degradation of organic pollutants with simultaneous hydrogen evolution over the Z-scheme CeO2/CeVO4/V2O5 (550-3) photocatalyst is proposed. Perhaps, this study affords a simple and novel method to design and develop next generation of highly efficient Z-scheme photocatalysts.
关键词： Conductive channel,Z-scheme CeO2/CeVO4/V2O5 photocatalyst,Solid phase reaction method,Simultaneous hydrogen evolution,Visible-light photocatalytic degradation
更新于2025-11-19 16:51:07
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An anti-symmetric dual (ASD) Z-scheme photocatalytic system: (ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4) for organic pollutants degradation with simultaneous hydrogen evolution
摘要： An anti-symmetric dual (ASD) Z-scheme ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4 photocatalyst was prepared by isoelectric point and calcination methods. The photocatalytic activity is estimated via degradation of Acid Orange II as a target organic contaminant with simultaneous hydrogen evolution under simulated solar-light irradiation. The prepared ASD Z-scheme ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4 photocatalyst has a high photocatalytic activity, which can be assigned to the enlarged photoresponse range, increased reduction surface and enhanced separation efficiency of photo-induced carriers. Furthermore, the cyclic experiment proves that the prepared ASD Z-scheme ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4 photocatalyst still maintains a high photocatalytic activity within five repetitive cycles. Moreover, the mechanism on photocatalytic degradation of organic pollutants with simultaneous hydrogen evolution caused by ASD Z-scheme ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4 photocatalyst is proposed. It is wished that this study could provide a promising pathway for effective degradation and rapid hydrogen production.
关键词： Simultaneous hydrogen evolution,Organic contaminants,Anti-symmetric dual (ASD) Z-scheme photocatalytic system,ZnIn2S4/Er3+:Y3Al5O12@ZnTiO3/CaIn2S4 composite,Up-conversion luminescence agent,Photocatalytic degradation
更新于2025-11-19 16:51:07