Self‐Reconstructed Spinel with Enhanced SO₄²⁻ Adsorption and Highly Exposed Co³⁺ From Heterostructure Boosts Activity and Stability at High Current Density for Overall Water Splitting

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

Published: Jan. 10, 2025

Abstract Developing overall water splitting non‐noble metal electrocatalysts achieving long‐term stability with high activity at industrial‐grade current density remains challenging. Herein, a self‐reconstruction strategy of Co 9 S 8 ‐Ni 3 2 /NCF is employed to fabricate Ni x 3‐x O 4 ‐Ov‐ in which partial replaced by the structure. The reconstructed ‐Ov can enhance adsorbing ability leached from initial phase compared spinel, exceeding 1000‐h oxygen evolution reaction (OER) and 600‐h 1000 mA cm −2 excellent activity. In situ Raman X‐ray photoelectron spectroscopy (XPS) results indicate that substitution for atoms enhances adsorption capacity on ‐Ov, facilitating formation high‐density 3+ active sites (400) expedited interfacial electron transfer densities. Density functional theory (DFT) calculations reveal stabilizes surface vacancies optimizes energy intermediates, thereby improving both catalytic performance. findings provide new insights into overcoming activity‐stability trade‐off contribute design

Language: Английский

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Differentiated Modulating the Electronic Structure of NiFe@Ni/Fe‐MnOx via Phase Transformation Engineering to Synergy Promote Bifunctional Water Splitting Reactions

Small, Journal Year: 2025, Volume and Issue: 21(7)

Published: Jan. 7, 2025

Abstract Modulating electronic structure to balance the requirement of both hydrogen evolution reaction (HER) and oxygen (OER) is crucial for developing bifunctional catalysts. Herein, phase transformation engineering utilized separately regulate catalyst structure, designed NiFe@Ni/Fe‐MnOOH schottky heterojunction exhibits remarkable electrocatalytic activity with low overpotentials 19 230 mV at 10 mA cm −2 HER OER in 1M KOH, respectively. Meanwhile, an anion‐exchange membrane water electrolyzer employing as electrodes shows voltages 1.487/1.953 V 10/1000 , operating over 200 h 1000 . Combining theoretical calculations experiments reveal that can differentially active phases HER/OER. In HER, Ni/Fe‐MnOOH metallic NiFe act *OH *H acceptors respectively accelerates dissociation subsequent Heyrovsky/Tafel step. While OER, significant Jahn‐Teller effect Mn 3+ induces surface reconstruction from Ni/Fe‐MnO 2 The formative high value 4+ modify M‐O hybridization activate lattice mechanism, which pivotal breaking restriction volcanic relationship reducing overpotential. These findings provide valuable design guidelines high‐performance multi‐functional electrocatalysts via engineering.

Language: Английский

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Interface engineering of hollow Janus-structured NiCoP/P-MoS2 heterojunction as self-supported electrode enables boosted alkaline hydrogen evolution reaction

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: 684, P. 668 - 677

Published: Jan. 11, 2025

Language: Английский

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Tunable Ferroelectric Polarization in BaTiO₃ Coupled with Zn_0.5Cd_0.5S Quantum Dots for Efficient Solar‐Driven Hydrogen Evolution

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

Published: Feb. 23, 2025

Abstract Integrating ferroelectric materials with semiconductor photocatalysts offers a groundbreaking strategy to enhance solar‐driven hydrogen production by improving charge separation and transfer efficiency. Herein, synergistic system is developed coupling the tunable polarization of BaTiO 3 (BTO) Z‐scheme heterojunction in Zn 0.5 Cd S quantum dots (ZCS QDs). The strong adjustable built‐in electric field generated BTO effectively drives carrier separation, enhances interfacial band bending, mitigates excitonic effects commonly observed QDs, facilitating directional transfer. Mechanistic insights, validated situ X‐ray photoelectron spectroscopy (XPS) Kelvin Probe Force Microscopy (KPFM), highlight pivotal role modulating dynamics interactions. These attributes, resulting from heterojunction, enable ZCS QDs/BTO composite achieve an outstanding evolution rate 0.83 mmol g −1 h , surpassing pure QDs factors 20.8 1.7, respectively. Notably, external further amplifies 1.19 representing remarkable 143% increase compared pristine showcasing polarization‐enhanced fields photocatalysis. This work presents novel pathway for designing advanced photocatalysts, providing promising prospects sustainable production.

Language: Английский

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Engineering Mn-doped Co-based heterostructures with oxygen vacancies toward efficient industrial-scale water oxidation catalysis

Journal of Colloid and Interface Science, Journal Year: 2025, Volume and Issue: 690, P. 137314 - 137314

Published: March 12, 2025

Language: Английский

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Hollow Fe‐Doped Ni(OH)₂–NiS@Ni(OH)₂ Nanorod Array with Regulated Heterostructural Interface and Band Structure for Expediting Alkaline Electrocatalytic Overall Water Splitting

Advanced Functional Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Aug. 2, 2024

Abstract Aiming to efficiently expedite alkaline overall water splitting (OWS) by addressing challenges such as sluggish kinetics and limited stability, a hollow Fe‐doped Ni(OH) 2 ‐NiS@Ni(OH) nanorod array with surface nanosheets is devised, featuring high‐index (101)‐NiS(211) heterostructural interface an upshifted d ‐band center. This nanoarchitecture intensifies the adsorption interaction of H O OH − reactants on electrocatalyst surface, suitably bonds * intermediate in hydrogen evolution reaction (HER) accelerates electron movement H, minimizes energy requirement rate‐limiting phase ( → O) oxygen (OER) facilitating O─H cleavage optimally adsorbs O, amplifies exposure surface‐active centers, ultimately reduces apparent activation energy. Consequently, overpotentials are low 66.4 mV 254.9 at 10 mA cm −2 , alongside high turnover frequencies 142 s −1 (H ) 279 (O 100 300 mV, respectively, markedly outperforming direct‐electrodeposited analogues. When functioning bifunctional electrode OWS, this material merely requires 1.57 V sustains operation for 168 h, approaching Pt/C||RuO benchmark.

Language: Английский

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In Situ Investigation of Interfacial Water in the Hydrogen Evolution Reaction: A Comparative Study Unraveling the Impact of Oxide Impurity

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(20), P. 15665 - 15674

Published: Oct. 7, 2024

Understanding the sluggish kinetics of hydrogen evolution reaction (HER) in neutral media is a grand challenge. The correlation between interfacial water structure and HER activity has yet to be determined, particularly for catalysts with complex chemical compositions. Herein, we used situ electrochemical spectroscopic methods (e.g., surface-enhanced infrared absorption shell-isolated nanoparticle-enhanced Raman spectroscopy) investigate bonding network molecules typical Pt/C NiCo-phosphide, -sulfide, -hybrid with/without oxide impurity) under potential bias media. cathodic potentials always influenced composition water, rendering records distinct nominal tuning rates among different catalysts. Interestingly, found that suitable amount surface impurity, inert phase, can drastically alter dynamic behaviors promoting transition from ice-like liquid-like free while leading an improved performance (j0 > 0.7 mA cm–2; η = 101.7 mV@10 cm–2). Such effect was presumably correlated hydrophilic moieties, as evidenced by studies pure hydroxide controls. This work provides insights understanding media, paving way rational design electrocatalysts.

Language: Английский

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Self‐Supported Metallic Alkaline Hydrogen Evolution Electrocatalysts Tolerant for Ampere‐Level Current Densities

Advanced Energy Materials, Journal Year: 2024, Volume and Issue: unknown

Published: Nov. 19, 2024

Abstract Electrocatalytic water splitting is an attractive approach for large‐scale hydrogen generation, critical global carbon neutrality. However, the prevalent commercialized alkaline electrolysis generally conducted at low current densities due to sluggish kinetics and high overpotential, severely hampering high‐efficiency production. Exploration of evolution reaction (HER) electrocatalysts that can reliably operate ampere‐level under overpotentials thus a primary challenge. In contrast extensive studies using powdery electrocatalysts, self‐supported metallic catalytic cathode has become burgeoning direction toward densities, owing their integrated design with intensive interfacial binding, conductivity mechanical stability industrial tolerance/adaption. Recent years have witnessed tremendous research advances in designing electrocatalysts. Therefore, this flourishing area specially summarized. Beginning introduction theory mechanism HER, engineering strategies on electrodes are systematically summarized, including metal alloy construction, heterostructure engineering, doping manipulation, surface design. Meanwhile, particular emphasis focused relationship between structure, activity, HER. Finally, existing challenges, requirements industrial‐scale application, future aiming provide better solution electrolysis.

Language: Английский

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Preparation of dendritic CuNi@CF catalysts by one-step electrodeposition: Achieve efficient hydrogen evolution reaction from seawater

Separation and Purification Technology, Journal Year: 2024, Volume and Issue: 354, P. 129171 - 129171

Published: Aug. 10, 2024

Language: Английский

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Lanthanides in the water electrolysis

EcoMat, Journal Year: 2024, Volume and Issue: unknown

Published: Sept. 12, 2024

Abstract The most feasible technique for producing green hydrogen is water electrolysis. In recent years, there has been significant study conducted on the use of transition metal compounds as electrocatalysts both anodes and cathodes. Peoples have attempted several strategies to improve electrocatalytic activity their original structure. One such involves introducing rare earth metals or creating heterostructures with based metals. incorporation significantly enhances by many folds, while offer structural stability ability manipulate electronic properties system. These factors led a boom in investigations metal‐based electrocatalysts. There currently pressing demand review article that can provide comprehensive overview scientific advancements elucidate mechanistic aspects impact lanthanide doping. This begins explaining structure lanthanides. We next examine aspects, followed doping heterostructure formation electrolysis applications. It expected this particular effort will benefit broad audience stimulate more research area interest. image

Language: Английский

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