Ultrafast H-Spillover in Intermetallic PtZn Induced by the Local Disorder for Excellent Electrocatalytic Hydrogen Evolution Performance

IF 26.8 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY Advanced Materials Pub Date : 2024-11-28 DOI:10.1002/adma.202409575
Meiling Wang, Zhengju Shi, Wenwen Shi, Jingyun Jiang, Jianhong Lan, Ruizhen Li, Yuanyuan Yan, Zhenyu Liu, Longyi Fu, Xuguang Liu, Shengbo Sang, Yingjie Hu, Jiadong Zhou
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Abstract

Ordered intermetallic Platinum-Zinc (PtZn) shows potential in hydrogen evolution reaction (HER), but faces a huge challenge in activity enhancement due to the H-repulsion properties of Zinc (Zn). Here, local disorder in ordered intermetallic PtZn nanoparticles confined in N-doped porous carbon (I-PtZn@NPC) via a confinement-high-temperature pyrolysis strategy is realized to boost the HER performance. Experiments and calculations demonstrate that the local substitution of Pt atoms for Zn atoms creates an ultra-short H-spillover channel (Pt site→Pt-Zn bridge site →Zn site). Benefiting from such an ultra-fast H-migration from Pt site to Zn site, I-PtZn@NPC exhibits enhanced intrinsic activity with an ultralow overpotential (η10: 2.3 mV, η100: 24 mV) than commercial Pt black catalyst. Furthermore, a 25 cm2 commercial proton exchange membrane (PEM) electrolyzer equipped with I-PtZn@NPC achieved stable operation at 1.60 Vcell for 200 h at a current density of 1 A cm⁻2. This design of local Zn disorder in the ordered intermetallic PtZn sheds new light on the rational development of efficient Zn-based alloy HER electrocatalysts.

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金属间PtZn中由局部无序引起的超快h溢出,以获得优异的电催化析氢性能。
有序金属间铂锌(PtZn)在析氢反应(HER)中表现出潜力,但由于锌(Zn)的h排斥特性,其活性增强面临巨大挑战。通过约束-高温热解策略,将有序金属间PtZn纳米颗粒限制在n掺杂多孔碳(I-PtZn@NPC)中,实现了局部无序,从而提高了HER性能。实验和计算表明,Pt原子局部取代Zn原子形成了一个超短的h -溢出通道(Pt位→Pt-Zn桥位→Zn位)。得益于这种从Pt位到Zn位的超快h迁移,I-PtZn@NPC具有比商业Pt黑催化剂更强的固有活性和超低过电位(η为10.2.3 mV, η为100:24 mV)。此外,一个25平方厘米的商业质子交换膜(PEM)电解槽配备I-PtZn@NPC,在1 a cm⁻2的电流密度下,以1.60 v的电压稳定运行200小时。有序金属间PtZn中局部Zn无序的设计为合理开发高效的Zn基合金HER电催化剂提供了新的思路。
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来源期刊
Advanced Materials
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.
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