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Charge Transfer Engineering via Multiple Heteroatom Doping in Dual Carbon-Coupled Cobalt Phosphides for Highly Efficient Overall Water Splitting
摘要： The exploration of non-noble-metal bifunctional electrocatalysts with high activity and stability for overall water splitting is crucial, but remains challenging for hydrogen fuel production. Herein, tuning of the charge transfer ability and catalytic performance of zeolitic imidazolate framework-derived porous carbon/reduced graphene oxide-coupled CoP composites (CoP@C@rGO) was achieved by incorporating multiple heteroatoms. The combined experimental investigation and density functional theory calculations revealed that the electronic interaction within the composites caused by B, N, and S tri-doped heteroatoms effectively induced interfacial charge transfer, which improved the active site accessibility and reduced the energy barriers of the evolution reaction; water splitting intermediates. From the synergetic effects of the components, the overall water splitting electrolyzer assembled using the newly prepared B,N,S-CoP@C@rGO catalyst required only 1.50 V to drive a current density of 10 mA cm–2, which is superior to the commercial Pt/C and IrO2/C couple (1.56 V).
关键词： hydrogen evolution reaction,oxygen evolution reaction,multiple doping,overall water splitting,charge transfer
更新于2025-09-12 10:27:22
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Laser Synthesis of Iridium Nanospheres for Overall Water Splitting
摘要： Engineering surface structure of catalysts is an efficient way towards high catalytic performance. Here, we report on the synthesis of regular iridium nanospheres (Ir NSs), with abundant atomic steps prepared by a laser ablation technique. Atomic steps, consisting of one-atom level covering the surface of such Ir NSs, were observed by aberration-corrected high-angle annular dark-field scanning transmission electron microscopy (HAADF-STEM). The prepared Ir NSs exhibited remarkably enhanced activity both for oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) in acidic medium. As a bifunctional catalyst for overall water splitting, they achieved a cell voltage of 1.535 V @ 10 mA/cm2, which is much lower than that of Pt/C-Ir/C couple (1.630 V @ 10 mA/cm2).
关键词： overall water splitting,laser ablated nanoparticles,bifunctional catalyst,Ir nanoparticles
更新于2025-09-12 10:27:22
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A Three-Dimensional ZnO/CdS/NiFe Layered Double Hydroxide Photoanode Coupled with a Cu <sub/>2</sub> O Photocathode in a Tandem Cell for Overall Solar Water Splitting
摘要： An integrated tandem photoelectrochemical (PEC) cell, composed of a three-dimensional (3D) ZnO/CdS/NiFe layered double hydroxide (LDH) core/shell/hierarchical nanowire arrays (NWAs) photoanode and a p-Cu2O photocathode, was designed for unassisted overall solar water splitting in this study. The optical and photoelectrochemical characteristics of ZnO-based photoanodes and Cu2O photocathode were investigated. The results show that ZnO/CdS/NiFe LDH nanostructures offer significantly enhanced performances with a photocurrent density reaching 5.8 mA cm?2 at 0.9 V and an onset potential as early as 0.1 V (versus RHE). The enhancement can be attributed to the existence of CdS nanoparticles (NPs) which boosts the light absorption in visible region and enhances charge separation. Moreover, the introduction of NiFe LDH nanoplates, with unique hierarchical mesoporous architecture, promotes electrochemical reactions by providing more active sites as co-catalyst. On the above basis, the ZnO/CdS/NiFe LDH–Cu2O two-electrode tandem cell system was established. At zero bias, the device shows a photocurrent density of 0.4 mA cm?2 along with the corresponding solar-to-hydrogen (STH) conversion efficiency reaching 0.50%. Our results indicate that the tandem PEC cells consisting of metal–oxide–semiconductor photoelectrodes based on Earth-abundant and low-cost materials hold promising application potential for overall solar water splitting.
关键词： ZnO,PEC tandem cell,CdS,solar hydrogen,self-driven water splitting,NiFe LDH
更新于2025-09-12 10:27:22
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Enhanced PEC performance of hematite photoanode coupled with bimetallic oxyhydroxide NiFeOOH through a simple electroless method
摘要： The oxygen evolution reaction (OER) is one important bottleneck in the development of economical photoelectrodes. Herein, we firstly prepared bimetallic oxyhydroxide NiFeOOH layer on Fe2O3 photoanode through a simple electroless ligand-regulated oxidation method in order to build highly-matched semiconductor/cocatalyst interface. Benefited from the accelerated OER kinetics and low overpotential of bimetallic oxyhydroxide NiFeOOH, the resultant Fe2O3/NiFeOOH core-shell with strongly-bound heterojunction interface possesses better visible light absorption, enhanced photocurrent density (1.83 mA/cm2 at 1.23 VRHE) and good stability than bare Fe2O3 and semi-FeOOH and NiOOH decorated Fe2O3 photoanodes. We believe this work provides a new pathway for designing high-quality contact interface of various photoelectrode/catalyst.
关键词： electroless ligand-regulated oxidation,photoelectrochemical water splitting,Fe2O3,core-shell nanorod arrays,NiFeOOH
更新于2025-09-12 10:27:22
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Black/red phosphorus quantum dots for photocatalytic water splitting: from a type I heterostructure to a Z-scheme system
摘要： By virtue of the quantum confinement effect, the junction between black phosphorus and red phosphorus changes from a type I heterostructure for bulk materials to a Z-scheme system for quantum dots. The Z-scheme system of black/red phosphorus quantum dots (BP/RP-QD) achieves H2 evolution from water splitting in the absence of sacrificial agents.
关键词： red phosphorus,black phosphorus,quantum dots,photocatalytic water splitting,Z-scheme system
更新于2025-09-12 10:27:22
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A high-efficiency and stable cupric oxide photocathode coupled with Al surface plasmon resonance and Al <sub/>2</sub> O <sub/>3</sub> self-passivation
摘要： The key to achieving high performance in photoelectrochemical (PEC) water splitting is the design of e?cient and stable photoelectrode structures. Herein, we firstly synthesized a novel and high-photoactivity CuO/Al photocathode and then the Al2O3 passivation layer was further introduced through a spontaneous oxidation process in air to protect the photocathode against photocorrosion. On account of the localized surface plasmon resonance (LSPR) of Al nanoparticles (NPs) in conjunction with surface passivation of the Al2O3 layer, the obtained CuO/Al/Al2O3 photocathode exhibits a high photocurrent density of (cid:2)0.95 mA cm(cid:2)2 at (cid:2)0.55 V vs. Ag/AgCl and photocorrosion stability of 89.5% after 1 h.
关键词： water splitting,localized surface plasmon resonance,CuO,Al2O3 passivation layer,photoelectrochemical,Al nanoparticles
更新于2025-09-12 10:27:22
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Plasmonic Bi nanoparticle decorated BiVO4/rGO as an efficient photoanode for photoelectrochemical water splitting
摘要： We report the application of plasmonic Bi nanoparticles supported rGO/BiVO4 anode for photoelectrochemical (PEC) water splitting. Nearly, 2.5 times higher activity was observed for Bi-rGO/BiVO4 composite than pristine BiVO4. Typical results indicated that Bi-rGO/BiVO4 exhibits the highest current density of 6.05 mA/cm2 at 1.23 V, whereas BieBiVO4 showed the current density of only 3.56 mA/cm2. This enhancement in PEC activity on introduction of Bi-rGO is due to the surface plasmonic behavior of BiNPs, which improves the absorption of radiation thereby reduces the charge recombination. Further, the composite electrode showed good solar to hydrogen conversion efficiency, appreciable incident photon-to-current efficiency and low charge transfer resistance. Hence, Bi-rGO/BiVO4 provides an opportunity to realize PEC water splitting.
关键词： Water splitting,Photoelectrochemical cell,Reduced graphene oxide,Charge transportation,Bismuth nanoparticles,Surface plasmon resonance
更新于2025-09-12 10:27:22
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Controlled Synthesis of Ni‐doped MoS2 Hybrid Electrode for Synergistically Enhanced Water‐Splitting Process
摘要： The development of high-efficiency, low cost, and earth abundant electrocatalysts for overall water splitting remains challengeable. In this work, we present the nickel (Ni) modified MoS2 hybrid catalysts grown on carbon cloth (Ni-Mo-S@CC) through a one-step hydrothermal treatment. The optimized Ni-Mo-S@CC catalyst shows excellent HER activity with low overpotentials of 168 mV at a current density of 10 mA cm?2 in 1.0 M KOH, which is lower than those of Ni-Mo-S@CC (1:1), Ni-Mo-S@CC (3:1) and pure MoS2. Significantly, the Ni-Mo-S@CC hybrid catalyst also displays outstanding OER activity with a low overpotential of 320 mV at a current density of 10 mA cm?2, and the remarkable long-term stability for 30 hours at a constant current density of 10 mA cm-2. Experimental and theoretical analysis based on density functional theory demonstrate that the excellent electrocatalytic performance is mainly attributed to remarkable conductivity, abundant active sites and synergistic effect of Ni-doped MoS2. This work sheds light on a unique strategy to design high performance and stable electrocatalysts for water splitting electrolyzers.
关键词： MoS2,nanocomposite,electrocatalysis,doping,water splitting
更新于2025-09-11 14:15:04
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Highly-efficient overall water splitting in 2D Janus group-III chalcogenide multilayers: the roles of intrinsic electric filed and vacancy defects
摘要： Two-dimensional (2D) van der Waals materials have been widely adopted as photocatalysts for water splitting, but the energy conversion efficiency remains low. On the basis of first-principles calculations, we demonstrate that the 2D Janus group-III chalcogenide multilayers: InGaXY, M2XY and InGaX2 (M = In/Ga; X, Y = S/Se/Te), are promising photocatalysts for highly-efficient overall water splitting. The intrinsic electric field enhances the spatial separations of photogenerated carriers and alters the band alignment, which is more pronounced compared with the Janus monolayers. High solar-to-hydrogen (STH) efficiency with the upper limit of 38.5% was predicted in the Janus multilayers. More excitingly, the Ga vacancy of InGaSSe bilayer effectively lowers the overpotentials of hydrogen evolution reaction (HER) and oxygen evolution reaction (OER) to the levels provided solely by the photogenerated carriers. Our theoretical results suggest that the 2D Janus group-III chalcogenide multilayers could be utilized as highly efficient photocatalysts for overall water splitting without the needs of sacrificial reagents.
关键词： Photocatalytic water splitting,Janus group-III chalcogenides,Intrinsic electric fields,First-principle calculation,Solar-to-hydrogen efficiency
更新于2025-09-11 14:15:04
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Mesoporous Tungsten Trioxide Photoanodes Modified with Nitrogen-Doped Carbon Quantum Dots for Enhanced Oxygen Evolution Photo-Reaction
摘要： Nanostructured photoanodes are attractive materials for hydrogen production via water photo-electrolysis process. This study focused on the incorporation of carbon quantum dots doped with nitrogen as a photosensitizer into mesoporous tungsten trioxide photoanodes (N-CQD/meso-WO3) using a surfactant self-assembly template approach. The crystal structure, composition, and morphology of pure and N-CQD- modi?ed mesoporous WO3 photoanodes were investigated using scanning electron and transmission microscopy, X-ray di?raction, and X-ray photoelectron spectroscopy. Due to their high surface area, enhanced optical absorption, and charge-carrier separation and transfer, the resulting N-CQD/meso-WO3 photoanodes exhibited a signi?cantly enhanced photocurrent density of 1.45 mA cm?2 at 1.23 V vs. RHE under AM 1.5 G illumination in 0.5 M Na2SO4 without any co-catalysts or sacri?cial reagent, which was about 2.23 times greater than its corresponding pure meso-WO3. Moreover, the oxygen evolution onset potential of the N-CQD/meso-WO3 photoanodes exhibited a negative shift of 95 mV, signifying that both the charge-carrier separation and transfer processes were promoted.
关键词： tungsten,dots,trioxide,photo-electrochemical,mesoporous,quantum,carbon,water splitting
更新于2025-09-11 14:15:04