Tailoring p‐Orbital Electron Delocalization Induced by Sulfur Defect Engineering for Enhancing Photoelectrochemical Water Splitting Performance

Advanced Energy Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 4, 2025

Abstract Indium sulfide (In 2 S 3 ) as water splitting photocatalyst has been broadly investigated due to its narrow bandgap (2.0–2.3 eV) and optimized opto‐electronic properties. However, In still suffers from a rapid photogenerated charge carrier recombination rate. addition, the main group metals (such In) lack active d ‐orbital electrons for catalysis, thus limits activation of intermediates during catalytic reaction. Herein, overcome above limitations , /TiO heterojunction with sulfur defects are constructed by temperature control strategy. The vacancy (Sv) can induce electron density transformation 5 p localized states delocalized states, which efficiently enhances chemical affinity * OOH. Thus, interaction between O atoms greatly facilitates rate‐determining step ( OOH → +O ), realizing high yield rate 10.00 µmol cm −2 h −1 at 1.23 V versus RHE. Furthermore, heterogeneous structure also enhance interfacial electric field (IEF) stability promoting oxygen generation. This work provides an efficient pathway improve photoelectrochemical (PEC) activity manipulating delocalization through defect engineering.

Language: Английский

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Synergetic Oxidized Mg and Mo Sites on Amorphous Ru Metallene Boost Hydrogen Evolution Electrocatalysis

Advanced Materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 21, 2025

Ruthenium (Ru) is considered as a promising catalyst for the alkaline hydrogen evolution reaction (HER), yet its weak water adsorption ability hinders splitting efficiency. Herein, concept of introducing oxygenophilic MgOx and MoOy species onto amorphous Ru metallene demonstrated through simple one-pot salt-templating method synergic promotion to greatly enhance HER electrocatalysis. The atomically thin on (MgOx/MoOy-Ru) show 15.3-fold increase in mass activity at potential 100 mV than that an ultralow overpotential 8.5 current density 10 mA cm-2. It further MgOx/MoOy-Ru-based anion exchange membrane electrolyzer can achieve high cm-2 remarkably low cell voltage 1.55 V, exhibit excellent durability over 60 h 500 In situ spectroscopy theoretical simulations reveal co-introduction enhances interfacial by promoting oxidized Mg sites lowering dissociation energy barrier Mo sites.

Language: Английский

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Regulating Reconstruction‐Engineered Active Sites of CoP Electrocatalyst by Br Ions During the Oxygen and Hydrogen Evolution Reaction

Energy & environment materials, Journal Year: 2025, Volume and Issue: unknown

Published: March 23, 2025

An in‐depth understanding of the catalyst surface evolution is crucial for precise control active sites, yet this aspect has often been overlooked. This study reveals spontaneous anion regulation mechanism Br‐doped CoP electrocatalysts in alkaline hydrogen reaction (HER) and oxygen (OER). The introduction Br modulates electronic structure Co site, endowing Br‐CoP with a more metallic character. In addition, P ion leaching promotes situ reconstruction Br‐CoOOH, which real site OER reaction. Meanwhile, HER situation different. On basis leaching, ions formation CoP‐Co(OH) 2 species. doping enhances adsorption *H, showing excellent H free energy, thereby greatly improving activity. Simultaneously, it also OOH*, effectively facilitating occurrence reactions. only needs 261 76 mV overpotential to drive current density 20 mA cm −2 10 , can be maintained unchanged 100 h. provides new insights into strategies mechanisms.

Language: Английский

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Lamellar Nanoporous Intermetallic Cobalt-Titanium Multisite Electrocatalyst with Extraordinary Activity and Durability for the Hydrogen Evolution Reaction

Nano Letters, Journal Year: 2025, Volume and Issue: unknown

Published: April 1, 2025

Constructing well-defined multisites with high activity and durability is crucial for the development of highly efficient electrocatalysts toward multiple-intermediate reactions. Here we report negative mixing enthalpy caused intermetallic cobalt-titanium (Co3Ti) nanoprecipitates on a lamellar hierarchical nanoporous cobalt skeleton as high-performance nonprecious multisite electrocatalyst an alkaline hydrogen evolution reaction. The Co3Ti robust substantially boosts reaction kinetics water dissociation adsorption/combination by unisonous adsorptions hydroxyl intermediates proper binding energies. By virtue bicontinuous that enables sufficiently accessible facilitates electron transfer ion/molecule transportation, self-supported heterogeneous electrode exhibits extraordinary electrocatalytic in 1 M KOH. It reaches current density ∼3.31 A cm–2 at low overpotential 200 mV maintains exceptional stability ∼1.33 >1000 h.

Language: Английский

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Embedding Tandem Built‐in Electric Fields within Hollow Architectures for Enhanced Photothermal Effect in Alcohol Oxidation Coupled with H₂ Production

Advanced Functional Materials, Journal Year: 2025, Volume and Issue: unknown

Published: April 1, 2025

Abstract Rationally designing nanostructures based on a comprehensive understanding of structure‐property relationships is instrumental in enhancing the photothermal effect. Here, general two‐stage morphology‐structure‐control strategy presented to construct tandem built‐in electric fields (BIEFs) embedded hollow bifunctional photocatalysts (Sv‐chalcogenide nanocage/NiCo 2 S 4 heterojunctions, Sv represents sulfur vacancies, chalcogenides include ZnIn , CdS, CdIn ). This involves fabricating polyhedral cages via constraint epitaxy and embedding BIEFs (consisting intra‐component inter‐component BIEF) within nanocages through defect‐mediated heterocomponent anchorage. The resulting nanoreactors synergize multilight scattering/reflection with directional charge‐transfer boost photocarrier dynamics by stimulating plentiful carrier generation driving continuous localization delocalized‐electron transportation. Subsequently, localized surface plasmon resonance (LSPR)‐induced photogenerated electron excitation continuously collaborates intrinsic for hot generation, thus improving Heterojunctions efficient regulation optimize pivotal intermediate adsorption/activation selective alcohol oxidation coupled H evolution, delivering unprecedented reactivity broad substrate compatibility. study provides programmable framework structurally architectures, elucidating substantial impact morphology‐structure control molecular catalytic behavior.

Language: Английский

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