钨基非晶合金介导邻近铂原子全面增强宽pH析氢。

IF 26.8 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Advanced Materials Pub Date : 2025-09-29 DOI:10.1002/adma.202511276

Jianhua Zhang,Kai-Ling Zhou,Yongzheng Zhang,Hao Wang

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引用次数: 0

摘要

基于单原子催化剂（SACs）的电化学水分解为制氢提供了一条可持续的途径。然而，传统的sac在恶劣的电解质环境中协同效应较弱。在这里，我们报道了一种钨基非晶合金（FeNiWPB）支持邻近铂单原子催化剂（PtASSA@FeNiWPB）。光谱和计算分析表明，非晶w基合金基体提供了丰富的缺陷位点来锚定和介导相邻的Pt原子，从而通过金属-金属协同作用促进多次H转换。此外，催化剂的耐腐蚀性通过形成坚固的M─W键（M = Pt, Fe, Ni）而显著增强，这有效地抑制了金属在广泛的pH范围内的浸出。此外，通过pt -载体相互作用在合金表面形成Pt-W/Fe/Ni极化对，诱导电子重分配，加速H*/OH*吸附动力学，从而增强多种H2O*解离途径。因此，PtASSA@FeNiWPB在-10 mA cm-2下表现出17 mV（酸性）和18 mV（碱性）的超低过电位，其质量活性比商用Pt/C高5.8倍（酸性）和63.6倍（碱性）。值得注意的是，它在酸性和碱性环境下都能保持600小时的性能，远远超过无w的同类产品（<50小时）和之前的报道，使其处于HER性能的最前沿。这项工作建立了一个通用的战略工程耐用的电催化剂。基于单原子催化剂（SACs）的电化学水分解为制氢提供了一条可持续的途径。然而，传统的sac在恶劣的电解质环境中协同效应较弱。在这里，我们报道了一种钨基非晶合金（FeNiWPB）支持邻近铂单原子催化剂（PtASSA@FeNiWPB）。光谱和计算分析表明，非晶w基合金基体提供了丰富的缺陷位点来锚定和介导相邻的Pt原子，从而通过金属-金属协同作用促进多次H转换。此外，催化剂的耐腐蚀性通过形成坚固的M─W键（M = Pt, Fe, Ni）而显著增强，这有效地抑制了金属在广泛的pH范围内的浸出。此外，通过pt -载体相互作用在合金表面形成Pt-W/Fe/Ni极化对，诱导电子重分配，加速H*/OH*吸附动力学，从而增强多种H2O*解离途径。因此，PtASSA@FeNiWPB在-10 mA cm-2下表现出17 mV（酸性）和18 mV（碱性）的超低过电位，其质量活性比商用Pt/C高5.8倍（酸性）和63.6倍（碱性）。值得注意的是，它在酸性和碱性环境下都能保持600小时的性能，远远超过无w的同类产品（<50小时）和之前的报道，使其处于HER性能的最前沿。这项工作建立了一个通用的战略工程耐用的电催化剂。

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All-Round Enhancement of Wide pH Hydrogen Evolution Enabled by Tungsten-Based Amorphous Alloy-Mediated Adjacent Platinum Atoms.

Electrochemical water splitting based on single-atom catalysts (SACs) offers a sustainable route for hydrogen production. However, conventional SACs suffer from weak synergistic effects in harsh electrolytes. Here, we report a tungsten-based amorphous alloy (FeNiWPB) supported adjacent Platinum single-atom catalyst (PtASSA@FeNiWPB). Spectroscopic and computational analyses disclose that the amorphous W-based alloy matrix provides abundant defect sites to anchor and mediate adjacent Pt atoms, thereby boosting multiple H conversions via metal-metal synergy. Additionally, the catalyst's corrosion resistance is significantly enhanced through the formation of robust M─W bonds (M═Pt, Fe, Ni), which effectively suppress metal leaching across broad pH ranges. Furthermore, the formation of Pt-W/Fe/Ni polarized pairs at the alloy surface via Pt-support interactions induces electron redistribution and accelerates H*/OH* adsorption kinetics, thereby enhancing multiple H2O* dissociation pathways. Consequently, PtASSA@FeNiWPB exhibits ultralow overpotentials of 17 mV (acidic) and 18 mV (alkaline) at -10 mA cm-2, with mass activities 5.8 times (acidic) and 63.6 times (alkaline) higher than commercial Pt/C. Notably, it maintains performance for 600 h in both acidic and alkaline environments, far exceeding W-free counterparts (<50 h) and previous reports, positioning it at the forefront of HER performance. This work establishes a universal strategy for engineering durable electrocatalysts.Electrochemical water splitting based on single-atom catalysts (SACs) offers a sustainable route for hydrogen production. However, conventional SACs suffer from weak synergistic effects in harsh electrolytes. Here, we report a tungsten-based amorphous alloy (FeNiWPB) supported adjacent Platinum single-atom catalyst (PtASSA@FeNiWPB). Spectroscopic and computational analyses disclose that the amorphous W-based alloy matrix provides abundant defect sites to anchor and mediate adjacent Pt atoms, thereby boosting multiple H conversions via metal-metal synergy. Additionally, the catalyst's corrosion resistance is significantly enhanced through the formation of robust M─W bonds (M═Pt, Fe, Ni), which effectively suppress metal leaching across broad pH ranges. Furthermore, the formation of Pt-W/Fe/Ni polarized pairs at the alloy surface via Pt-support interactions induces electron redistribution and accelerates H*/OH* adsorption kinetics, thereby enhancing multiple H2O* dissociation pathways. Consequently, PtASSA@FeNiWPB exhibits ultralow overpotentials of 17 mV (acidic) and 18 mV (alkaline) at -10 mA cm-2, with mass activities 5.8 times (acidic) and 63.6 times (alkaline) higher than commercial Pt/C. Notably, it maintains performance for 600 h in both acidic and alkaline environments, far exceeding W-free counterparts (<50 h) and previous reports, positioning it at the forefront of HER performance. This work establishes a universal strategy for engineering durable electrocatalysts.

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来源期刊

Advanced Materials 工程技术-材料科学：综合

CiteScore

43.00

自引率

4.10%

发文量

2182

审稿时长

2 months

期刊介绍： Advanced Materials, one of the world's most prestigious journals and the foundation of the Advanced portfolio, is the home of choice for best-in-class materials science for more than 30 years. Following this fast-growing and interdisciplinary field, we are considering and publishing the most important discoveries on any and all materials from materials scientists, chemists, physicists, engineers as well as health and life scientists and bringing you the latest results and trends in modern materials-related research every week.