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构建从原子簇到单原子的氢迁移通道,实现超低铂负载下的高效电催化析氢
作者:小柯机器人 发布时间:2026/1/4 16:44:18


近日,天津大学邹吉军团队报道了构建从原子簇到单原子的氢迁移通道,实现超低铂负载下的高效电催化析氢。2025年12月29日出版的《德国应用化学》杂志发表了这项成果。

在质子交换膜水电解槽中,如何以极低贵金属用量开发高活性、长寿命的阴极催化剂仍是一项重大挑战。

研究组设计了一种锚定在硫掺杂碳基底上的铂基亚纳米催化剂,其特点是同时存在单原子与原子簇的双活性位点。这种双活性位点构型能够分别优化活性氢中间体的生成动力学与随后的重组动力学,从而突破萨巴蒂尔原则的限制。具体而言,通过引入锰等第二过渡金属,调控了铂原子簇的界面电荷分布与功函数,同步促进了氢中间体的生成与迁移;而邻近的缺电子铂单原子则加速了氢中间体的重组动力学。

该催化剂在铂负载量仅为3.6 wt%的条件下,于15 mV过电位下实现了创纪录的14.48 A mg-1质量活性,超过商用40 wt%铂碳催化剂41倍。在集成电解槽测试中,该催化剂仅需对标商用催化剂10%的铂负载量即展现出卓越的活性与稳定性,标志着向实用化绿氢生产迈出关键一步。研究还通过原位实验与理论计算首次证实了氢中间体"生成-迁移-重组"全过程的直接证据,为析氢反应的解耦研究与催化剂理性设计提供了新范式。

附:英文原文

Title: Constructing Hydrogen Migration Channel from Atomic Clusters to Single Atom for Superior Electrocatalytic Hydrogen Evolution with Ultralow Pt Loading

Author: Zexing He, Xiaokang Liu, Minghui Zhang, Yajun Wang, Zhen-Feng Huang, Chengxiang Shi, Ruijie Gao, Lun Pan, Chong Peng, Wanliang Mi, Xiangwen Zhang, Jinlong Gong, Ji-Jun Zou

Issue&Volume: 2025-12-29

Abstract: Developing highly active and durable cathode catalysts using minimal use of noble metal remains a grand challenge for proton exchange membrane water electrolyzer. Herein we design a Pt-based sub-nanometric catalysts featuring coexisting single atoms and atomic clusters anchored on sulfur-doped carbon. This dual-active-site architecture enables independent optimization of active hydrogen (H*) formation and subsequent recombination kinetics, thus breaking the limitation of Sabatier principle. Specially, by introducing a secondary transition metal such as Mn, the interfacial charge distribution and work function of Pt clusters is regulated, promoting both H* formation and migration. Meanwhile, the neighboring electron-deficient Pt single atoms facilitate H* recombination kinetics. The catalyst with 3.6 wt% Pt loading achieves a recorded mass activity of 14.48 A mg1 at 15 mV, exceeding commercial 40wt% Pt/C by 41-fold. When integrated into an electrolyzer, the catalyst demonstrates exceptional activity and stability with only 10% Pt loading relative to commercial benchmark, representing a critical advancement toward practical green hydrogen production. Also, the direct evidences of H* formation, migration and recombination process are confirmed by operando experiments and theoretical calculations for the first time, which offers new concept for decoupling of HER reaction and rational design of catalysts.

DOI: 10.1002/anie.202523933

Source: https://onlinelibrary.wiley.com/doi/10.1002/anie.202523933

期刊信息

Angewandte Chemie:《德国应用化学》,创刊于1887年。隶属于德国化学会,最新IF:16.823
官方网址:https://onlinelibrary.wiley.com/journal/15213773
投稿链接:https://www.editorialmanager.com/anie/default.aspx