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局部无序诱导金属间化合物PtZn中实现超快H溢出用于优异的电催化析氢性能

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

作者信息

Wang Meiling, Shi Zhengju, Shi Wenwen, Jiang Jingyun, Lan Jianhong, Li Ruizhen, Yan Yuanyuan, Liu Zhenyu, Fu Longyi, Liu Xuguang, Sang Shengbo, Hu Yingjie, Zhou Jiadong

机构信息

College of Materials Science and Engineering, Taiyuan University of Technology, Taiyuan, 030024, China.

State Key Laboratory of Coal Conversion, Institute of Coal Chemistry, Chinese Academy of Sciences, Taiyuan, Shanxi, 030001, China.

出版信息

Adv Mater. 2025 Jan;37(3):e2409575. doi: 10.1002/adma.202409575. Epub 2024 Nov 28.

DOI:10.1002/adma.202409575
PMID:39610159
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 (η: 2.3 mV, η: 24 mV) than commercial Pt black catalyst. Furthermore, a 25 cm commercial proton exchange membrane (PEM) electrolyzer equipped with I-PtZn@NPC achieved stable operation at 1.60 V for 200 h at a current density of 1 A cm⁻. 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.

摘要

有序金属间化合物铂锌(PtZn)在析氢反应(HER)中显示出潜力,但由于锌(Zn)的氢排斥特性,在活性增强方面面临巨大挑战。在此,通过限域高温热解策略实现了限域在氮掺杂多孔碳(I-PtZn@NPC)中的有序金属间化合物PtZn纳米颗粒的局部无序,以提高HER性能。实验和计算表明,Pt原子对Zn原子的局部取代创造了一个超短的氢溢流通道(Pt位点→Pt-Zn桥位点→Zn位点)。受益于这种从Pt位点到Zn位点的超快氢迁移,I-PtZn@NPC表现出比商业铂黑催化剂更高的本征活性和超低过电位(η:2.3 mV,η:24 mV)。此外,配备I-PtZn@NPC的25厘米商业质子交换膜(PEM)电解槽在1 A cm⁻²的电流密度下于1.60 V稳定运行200小时。这种在有序金属间化合物PtZn中局部Zn无序的设计为高效锌基合金HER电催化剂的合理开发提供了新的思路。

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