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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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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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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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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Analysis of the OH Coverage on Low-Coordinated Pt Sites at Low Potentials

ACS electrochemistry., Journal Year: 2024, Volume and Issue: 1(3), P. 351 - 359

Published: Nov. 18, 2024

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

Language: Английский

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Fe‐Rich Medium‐Entropy Core‐Shell Electrocatalyst for Hydrogen Evolution Reaction Under Large Current Density

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

Published: Dec. 10, 2024

Abstract In response to the low stability of expensive Pt under large current, exploring stable, efficient and cost‐competitive electrocatalyst for hydrogen evolution reaction is crucial advancing green production. Here, a strategy relating constructing core‐shell structure with near‐zero‐resistance homogeneous interface applied synthesize new Fe‐rich medium‐entropy alloy (MEA) catalyst. This low‐cost sample presents both outstanding durability catalytic activity an overpotential 343.6 mV at 1,000 mA cm −2 as well Tafel slope 67.6 dec −1 , respectively much lower than benchmark catalyst 20%Pt/C (416.9 mV, 156.8 ) in 1.0 m KOH solution. Such properties are attributed enhanced reactivity surface active sites electrons easy injection from MEA metallic core MEO (medium entropy oxide) shell via their highly conductive interface. layer, Fe/Ni/Co identified centres high oxidation shift themselves toward deep energy, weakening Metal─H bonding thereby accelerating evolution. work not only exploits one novel suitable industrial high‐current environments but also provides broad application prospects utilization.

Language: Английский

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