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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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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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A comparative study on photocatalytic hydrogen evolution activity of synthesis methods of CDs/ZnIn2S4 photocatalysts
摘要： The introduction of carbon materials in photocatalytic systems can significantly enhance the photocatalytic hydrogen evolution activity. Here, we proposed and fabricated carbon nanodots/ZnIn2S4 (CDs/ZIS) samples via three methods. The morphology, chemical elements and valence, and photoelectric properties of CDs/ZIS samples were systematically characterized by SEM, TEM, XPS, UV and PL. The photocatalytic H2 production experiments indicate that the photocatalytic performance of all CDs/ZIS samples has been significantly improved, which could be attributed to the fact that serving as an excellent electron acceptor, CDs can accelerate the separation efficiency of photogenerated electrons and holes. The samples prepared via one-pot hydrothermal method exhibit the optimal photocatalytic activity and the corresponding H2 production rate of 4.15 mmol g?1 h?1 under visible light irradiation (λ > 420 nm), which is about 2.92 times higher than pure ZIS. Our work presented the influence of synthetic method on photoelectric performance and photocatalytic activity of CDs/ZIS nanocomposites, and provided a reliable idea for improving the photocatalytic performance of photocatalyst toward practical applications.
关键词： Synthesis methods,ZnIn2S4,Photocatalytic hydrogen evolution,Carbon dots
更新于2025-11-14 15:29:11
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Construction of dual defect mediated Z-scheme photocatalysts for enhanced photocatalytic hydrogen evolution
摘要： The construction of Z-scheme system is a promising approach for photocatalytic hydrogen evolution (PHE). In this study, we fabricated a direct Z-scheme system consisting of defect-rich g-C3N4 nanosheets (DR-CNNS) crumpled nanosheets with defect-rich TiO2 (DR-TiO2) nanoparticles via a dual defective strategy. The optimized dual-defective rich TiO2/CNNS composite showed a superior PHE rate of ?651.79 μmol/h with a turnover frequency of ?419.3 h?1 as well as high stability and recyclability, which presented the highest value in single defective TiO2 or g-C3N4-based photocatalysts families reported previously. Furthermore, this protocol could also be extended to synthesize other dual defective g-C3N4/oxides (ZnO, SnO2, etc.) heterostructures. The improved photocatalytic performances could be ascribed to the following aspects: (1) rich dual defect, narrowing the band gap and providing more reactive sites for PHE; (2) intimate interface, facilitating interfacial migration and utilization of photogenerated charges; (3) Z-scheme structure, accelerating photogenerated electron-hole pair separation and thus leading to more e?cient PHE. Our work highlights the critical role of defects in construction of Z-scheme system and provides the possibility of utilizing dual defective g-C3N4-based systems for other photocatalytic applications including CO2 reduction and water puri?cation.
关键词： Photocatalytic hydrogen evolution,Dual defect,Oxides/g-C3N4,Heterojunction,Direct Z-scheme
更新于2025-11-14 15:27:09
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Zinc ions modified InP quantum dots for enhanced photocatalytic hydrogen evolution from hydrogen sulfide
摘要： Through direct addition of inorganic zinc ions into the solution of indium phosphide quantum dots (InP QDs) at ambient environment, we here present a facile but effective method to modify InP QDs for photocatalytic hydrogen evolution from hydrogen sulfide (H2S). X-ray diffraction patterns and transmission electron microscopic images demonstrate that zinc ions have no significant influence on the crystal structure and morphology of InP QDs, while X-ray photoemission spectra and UV–Vis diffuse and reflectance spectra indicate that zinc ions mainly adsorbed on the surface of InP QDs. Photocatalytic results show the average hydrogen evolution rate has been enhanced to 2.9 times after modification and H2S has indeed involves in the hydrogen evolution process. Steady-state and transient photoluminescence spectra prove that zinc ions could effectively eliminate the surface traps on InP QDs, which is crucial to suppress the recombination of charge carriers. In addition, the electrostatic interaction between zinc ions and the surface sulfide from InP QDs could mitigate the repulsion between QDs and sulfide/hydrosulfide, which may promote the surface oxidative reaction during photocatalysis. This work avoids the traditional harsh and complicated operations required for surface passivation of QDs, which offers a convenient way for optimization of QDs in photocatalysis.
关键词： Hydrogen sulfide,Photocatalytic hydrogen evolution,InP quantum dots,Surface modification
更新于2025-10-22 19:38:57
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Carbon Nanotube-Supported Cu <sub/>3</sub> P as High-Efficiency and Low-Cost Cocatalysts for Exceptional Semiconductor-Free Photocatalytic H <sub/>2</sub> Evolution
摘要： Developing an inexpensive and high-efficiency hydrogen-production cocatalyst to replace the noble metal Pt remains a big challenge in the fields of sustainable photocatalytic hydrogen evolution. Herein, we report the exploration of a high-efficient binary noble metal free Cu3P-CNT H2-evolution cocatalyst by direct high-temperature phosphatizing of Cu(OH)2-CNT. Impressively, combining the advantages of noble metal free Cu3P and carbon nanotube (CNT), the binary Cu3P-CNT cocatalysts show high-efficient photocatalytic H2 evolution in Eosin Y(EY)-contained semiconductor-free photocatalytic systems. The maximum visible-light H2-generation rate for promising EY-Cu3P-CNT systems was 17.22 mmolg-1h-1. The highest apparent quantum efficiency (AQE) could reach 10.23% at 500 nm. More importantly, we found that the separation of photogenerated electrons and holes in the Eosin Y, the efficiency of electron transfer from EY to the active edge sites of Cu3P, and the electrocatalytic H2-evolution activity of Cu3P, could be simultaneously boosted via readily adding the conductive CNT, thus achieving the significantly improved photocatalytic H2 evolution. This work provides a simple and facile strategy to design highly efficient semiconductor-free photocatalytic proton-reduction systems using high-activity transition metal phosphides (TMPs) and inexpensive carbon nanomaterials.
关键词： Photocatalytic Hydrogen Evolution,noble metal-free Cu3P Co-catalysts,Solar Fuel,Carbon nanotube (CNT),Dye sensitization
更新于2025-09-23 15:23:52
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Unique 1D Cd <sub/>1?</sub><i> <sub/>x</sub></i> Zn <i> <sub/>x</sub></i> S@O-MoS <sub/>2</sub> /NiO <i> <sub/>x</sub></i> Nanohybrids: Highly Efficient Visible-Light-Driven Photocatalytic Hydrogen Evolution via Integrated Structural Regulation
摘要： Development of noble-metal-free photocatalysts for highly efficient sunlight-driven water splitting is of great interest. Nevertheless, for the photocatalytic H2 evolution reaction (HER), the integrated regulation study on morphology, electronic band structures, and surface active sites of catalyst is still minimal up to now. Herein, well-defined 1D Cd1?xZnxS@O-MoS2/NiOx hybrid nanostructures with enhanced activity and stability for photocatalytic HER are prepared. Interestingly, the band alignments, exposure of active sites, and interfacial charge separation of Cd1?xZnxS@O-MoS2/NiOx are optimized by tuning the Zn-doping content as well as the growth of defect-rich O-MoS2 layer and NiOx nanoparticles, which endow the hybrids with excellent HER performances. Specifically, the visible-light-driven (>420 nm) HER activity of Cd1?xZnxS@O-MoS2/NiOx with 15% Zn-doping and 0.2 wt% O-MoS2 (CZ0.15S-0.2M-NiOx) in lactic acid solution (66.08 mmol h?1 g?1) is about 25 times that of Pt loaded CZ0.15S, which is further increased to 223.17 mmol h?1 g?1 when using Na2S/Na2SO3 as the sacrificial agent. Meanwhile, in Na2S/Na2SO3 solution, the CZ0.15S-0.2M-NiOx sample demonstrates an apparent quantum yield of 64.1% at 420 nm and a good stability for HER under long-time illumination. The results presented in this work can be valuable inspirations for the exploitation of advanced materials for energy-related applications.
关键词： charge separation,1D hybrid nanostructures,photocatalytic hydrogen evolution,band alignments,active sites
更新于2025-09-23 15:22:29
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Enhanced Photocatalytic Hydrogen Evolution with TiO <sub/>2</sub> -TiN Nanoparticle Composites
摘要： Metal nitrides have potential in energy applications due to their physical and optical properties. Nanoparticle composites of titanium nitride (TiN) and titanium dioxide (TiO2) were investigated for their photocatalytic hydrogen (H2) activity via methanol reformation. Physical mixing of the nanoparticulate TiO2 and TiN was employed to prevent the oxy-nitride formation and particle aggregation observed in thermal preparations. This convenient combination of TiO2 and TiN demonstrated a substantial synergistic effect with enhanced activity (9.4 μmol/h TiO2-TiN vs 1.8 μmol/h TiO2) under combined UV/Vis light. Irradiation under only UV light resulted in a similar enhancement factor compared to using combined UV/Vis light, demonstrating that the enhanced activity of the composites occurs essentially for UV-driven photocatalysis. No activity/enhancement was observed with only visible light irradiation, however, minor enhancement was observed when switching between UV and UV/Vis irradiation, suggesting a contribution from the TiN plasmon. We propose that the plasmonic contribution is dependent on the band gap excitation of TiO2, which reduces the degree of band bending at the TiO2/TiN interface. This promotes the migration of hot electrons from TiN away from the TiO2/TiN interface to be used for H2 evolution.
关键词： TiO2-TiN Nanoparticle Composites,Plasmonics,Optical,Magnetic,and Hybrid Materials,Photocatalytic Hydrogen Evolution
更新于2025-09-23 15:22:29
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Single Nickel Atoms Anchored on Nitrogen-Doped Graphene as a Highly Active Co-Catalyst for Photocatalytic H2 Evolution
摘要： Earth abundant nickel is a typical non-noble-metal cocatalyst used for photocatalytic hydrogen evolution (PHE). Ni nanoparticles, however, tend to aggregate during the hydrogen production process, significantly lowering their PHE activity. In this research, we report single nickel atoms anchored on nitrogen-doped graphene (Ni-NG) as a cocatalyst for PHE. We have demonstrated that Ni-NG is a robust and highly active cocatalyst for PHE from water. With only 0.0013 wt.% of Ni loading, the PHE activity of composite Ni-NG/CdS photocatalyst is 3.4 times greater than that of NG/CdS. The quantum efficiency of Ni-NG/CdS for PHE reaches 48.2% at 420 nm, one of the highest efficiencies for non-noble-metal based cocatalysts reported in literature. Photoluminescence spectral analyses and electrochemical examinations have indicated that Ni-NG coupled to CdS can serve not only as an electron storage medium to suppress electron-hole recombination, but also as an active catalyst for proton reduction reaction. Density functional theory calculation shows that the high activity of Ni-NG/CdS composite results from the single Ni atoms trapped in NG vacancies, which significantly reduces the activation energy barrier of the hydrogen evolution reaction. This approach may be valuable for developing robust and highly active noble-metal free cocatalysts for solar hydrogen production.
关键词： Non-noble Metal Cocatalyst,CdS,Photocatalytic Hydrogen Evolution,Nitrogen-Doped Graphene,Single Ni Atom Catalysts
更新于2025-09-23 15:21:21
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Simultaneously engineering K-doping and exfoliation into graphitic carbon nitride (g-C3N4) for enhanced photocatalytic hydrogen production
摘要： Doping and exfoliation are effective strategies to improve the photocatalytic activity of bulk graphitic carbon nitride (g-C3N4). Therefore, it can be inferred that engineering element-doping and exfoliation into g-C3N4 would further enhance the photocatalytic performance. Herein, we demonstrated a KOH-assisted hydrothermal-reformed melamine strategy for achieving the simultaneous K-doping and exfoliation of g-C3N4. The as-synthesized K-doped g-C3N4 ultrathin nanosheets displayed much enhanced photocatalytic hydrogen evolution rate (HER) of about 13.1 times higher than that of the bulk g-C3N4 under visible-light irradiation, achieving an apparent quantum efficiency of 6.98% at 420 nm. The improved photocatalytic HER can be attributed to the high surface area offering numerous photocatalytic active sites, enlarged conductive band edge optimizing photoreduction potential, and K-doping promoting charge generation and separation as well as the long life-time of photogenerated carriers. This work would provide a promising way to integrate co-doping and exfoliation into new g-C3N4-based materials.
关键词： Graphitic carbon nitride,Exfoliation,Photocatalytic hydrogen evolution,Nanosheet,K-doping
更新于2025-09-23 15:21:21