Enhanced Cooperative Generalized Compressive Strain and Electronic Structure Engineering in W‐Ni₃N for Efficient Hydrazine Oxidation Facilitating H₂ Production

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

Published: Jan. 7, 2025

Abstract As promising bifunctional electrocatalysts, transition metal nitrides are expected to achieve an efficient hydrazine oxidation reaction (HzOR) by fine‐tuning electronic structure via strain engineering, thereby facilitating hydrogen production. However, understanding the correlation between strain‐induced atomic microenvironments and reactivity remains challenging. Herein, a generalized compressive strained W‐Ni 3 N catalyst is developed create surface with enriched states that optimize intermediate binding activate both water 2 H 4 . Multi‐dimensional characterizations reveal nearly linear evolution (HER) activity d‐band center of under state. Theoretically, enhances electron transfer capability at surface, increasing donation into antibonding orbitals adsorbed species, which accelerates HER HzOR. Leveraging modified from W incorporation, catalysts demonstrate outstanding performance, achieving overpotentials 46 mV for 10 mA cm −2 81 HzOR 100 Furthermore, achieves overall splitting low cell voltage 0.185 V 50 , maintaining stability ≈450 h. This work provides new insights dual engineering in design advanced catalysts.

Language: Английский

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Unlocking Efficient Alkaline Hydrogen Evolution Through Ru–Sn Dual Metal Sites and a Novel Hydroxyl Spillover Effect

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

Published: Sept. 28, 2024

Abstract Alkaline hydrogen evolution reaction (HER) has great potential in practical production but is still limited by the lack of active and stable electrocatalysts. Herein, efficient water dissociation process, fast transfer adsorbed hydroxyl optimized adsorption are first achieved on a cooperative electrocatalyst, named as Ru–Sn/SnO 2 NS, which Ru–Sn dual metal sites SnO heterojunction constructed based porous Ru nanosheet. The density functional theory (DFT) calculations situ infrared spectra suggest that can optimize process adsorption, while existence induce unique spillover effect, accelerating avoiding poison sites. As results, NS display remarkable alkaline HER performance with an extremely low overpotential (12 mV at 10 mA cm −2 ) robust stability (650 h), much superior to those (27 90 h stability) (16 120 stability). work sheds new light designing electrocatalyst.

Language: Английский

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Activity Enhancement of Molybdenum Carbide in Alkaline Hydrogen Evolution Reaction through Oxidation-Gradient Modulation

ACS Catalysis, Journal Year: 2024, Volume and Issue: 14(22), P. 16712 - 16722

Published: Oct. 30, 2024

Featured by their Pt-like electronic structure, molybdenum carbides have been widely developed for efficiently catalyzing the hydrogen evolution reaction (HER). It is noteworthy that oxophilicity of transition-metal atoms can give rise to inevitable surface oxidation carbides, which has a noticeable impact on HER activities. However, such significant detail was usually documented in theory simulations and rarely explored well-controlled experiments. Herein, advanced surface-science techniques using vacuum-connected setups are performed deliberately prepare oxidation-gradient carbide-oxide model electrocatalysts evaluate corresponding alkaline performance. The performance evaluations demonstrate minimal oxygen-modified Mo2C exhibits best activity among all electrocatalysts. In situ XPS combined with quasi under different applied negative potentials reveals tailoring decorated oxygen-containing species facilitate desorption produced OH* intermediates from water activation, thus avoiding deep issue catalyst accelerating regeneration active sites process. Moreover, comparable trend also observed synthetically practical powder catalysts, further proves our hypothesis deduced system. Our strategy oxygen-terminated utilization spectroscopy characterizations may pave an interesting route rational design low-cost but highly efficient carbide catalysts electrolysis.

Language: Английский

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Novel Ru‐O₃Se₄ Single Atoms Regulate the Charge Redistribution at Ni₃Se₂/FeSe₂ Interface for Improved Overall Water Splitting in Alkaline Media

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

Published: Dec. 4, 2024

Abstract Developing low‐cost, highly active, and stable bifunctional catalysts is of great significance for electrochemical water splitting. Herein, novel Ru‐O 3 Se 4 single atoms doped Ni 2 /FeSe interface catalyst fabricated by a two‐step method hydrogen evolution reaction (HER) oxygen (OER). Notably, Ru‐Ni nanosheets exhibit excellent HER (43 mV@10 mA cm −2 ) OER (283 mV@100 activities in alkaline solution. In particular, the mass activity 3593.61 mg Ru −1 at 200 mV 7073.80 400 OER, which 25.91 367.28 times commercial Pt/C RuO , respectively. situ spectroscopy techniques confirm facilitate adsorption intermediates H * OOH during processes, Further density functional theory calculations reveal introducing causes transfer electrons from to Fe atoms, leading redistribution charge interface, thus reducing energy barriers rate‐determining step −0.37 1.92 eV This work emphasizes significant role overall

Language: Английский

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Machine learning‐accelerated computational screening of CrNiCu ternary alloy as superior cocatalyst for photocatalytic hydrogen evolution

Materials Genome Engineering Advances, Journal Year: 2025, Volume and Issue: unknown

Published: May 12, 2025

Abstract The development of cost‐effective noble‐metal‐free cocatalysts with exceptional hydrogen evolution reaction (HER) activity is critical for advancing scalable and sustainable photocatalytic production. Although platinum (Pt) remains a benchmark HER catalyst, its scarcity high cost stimulates the search viable alternatives. In this work, machine learning (ML)‐accelerated strategy presented to screen highly active ternary CrNiCu alloys. Combining density functional theory calculations, XGBoost regression models were trained predict adsorption energies water dissociation energy barriers on alloy surfaces. Consequently, theoretical exchange current densities predicted all possible compositions alloys, enabling identification catalysts composition 10∼30 at.% Cr, 30–50 Ni, 20–60 Cu that exhibits superior than Pt. Stability assessment optimal alloys further confirms their excellent resistance element segregation hydroxyl poisoning under operational conditions. This work not only identifies promising non‐noble but also establishes an efficient ML‐accelerated computational framework discovery durable high‐activity renewable applications.

Language: Английский

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Balanced Adsorption Ability of NiFeP by Nonmetal Doping for Enhanced Water Dissociation Kinetics and Stability

Small Methods, Journal Year: 2025, Volume and Issue: unknown

Published: May 15, 2025

Abstract Hydrogen evolution reaction (HER) under alkaline conditions is determined by the water dissociation process. Strengthening adsorption ability of electrocatalyst crucial to promoting in HER, whereas too‐intense will poison active sites. Herein, NiFeP modulated nonmetal F doping for an efficient and durable HER. incorporation (NiFePF) tailors electronic structure Ni, Fe, P, optimizing * OH/ H on The balanced facilitates hydrogen NiFePF, exhibiting smaller overpotential 233 mV at 100 mA cm −2 . Furthermore, NiFePF achieves 1 A only 231 30 wt% KOH. desorption OH alleviates poisoning center, limiting surface hydroxylation a few nanometers. This enables remain stable 360 h, demonstrating its commercial potential.

Language: Английский

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Spontaneous Alkaline Water Electrolysis Driven by the “OH‐Baton”

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

Published: May 27, 2025

Abstract Nano‐metal particles integrating with single‐atom catalysts (NMP‐SACs) have been constructed recently for accelerated alkaline hydrogen evolution reaction (HER). However, the design of NMP‐SACs primarily aims at separate adsorption *OH and H*, while neglecting desorption, causing blockage slow kinetics. To address this, Mo 2 C is introduced to (e.g., Pt nanoparticles‐Pt atom, n ‐Pt 1 ) by a “one‐step dual‐confinement pyrolysis” strategy 1@Mo2C , where precisely confined remaining adjacent @Mo C. Experiments calculations demonstrate that acting as an “OH‐baton” helps overcome on accelerating separation H* thus promoting spontaneous water dissociation. Thus, supported achieves significantly lower overpotential ( η 10 = 24 mV) more than seven times higher mass activity (MA 100 4.33 mA µg Pt⁻ in alkaline. The anion‐exchange membrane electrolyzer (AEMWE) delivers low cell voltage 1.91 V durable 120 h electrolysis 1.0 A cm −2 . This work proposes new insight introducing dual‐site catalyst system achieve

Language: Английский

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Tailoring electronic environments of dispersed Ru sites for efficient alkaline hydrogen evolution

Inorganic Chemistry Frontiers, Journal Year: 2024, Volume and Issue: 11(18), P. 5884 - 5893

Published: Jan. 1, 2024

Benefiting from the metal-support interactions, prepared Ru-NiCoO 2 /CC exhibits excellent alkaline HER activity. Importantly, two-electrode electrolyzer with demonstrates potential for integration intermittent energy systems.

Language: Английский

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Analysis of the OH coverage on low-coordinated Pt sites at low potentials

Published: Aug. 6, 2024

In a previous study, we demonstrated the presence of OH species adsorbed on low-coordinated Pt sites (or steps) at low potentials using spectroscopy and electrochemical experiments. This investigation was specifically conducted Pt(311) surface in an electrolyte with pH=1. this work, extend our study to other surfaces featuring (111) terraces but varying step geometry density. Additionally, explored influence pH these systems. Our findings reveal that coverage steps is independent sensitive structure. Specifically, observed approximately 0.5 (110) 0.33 (100) steps. Furthermore, potential zero total charge aligns local for predominantly influenced by sites.

Language: Английский

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Au,Ag,Cu Doped Niwo4 Hetergeneous with Exceptional Hydrogen Evolution Capability and Stability in Alkaline Media Under Large Current Density Exceeding 100 Ma Cm-2

Published: Jan. 1, 2024

Language: Английский

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