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一种通过双金属分段配位反应中心促进不锈钢基催化剂上析氧动力学以实现高效碱性水分解的激光合成策略。

A Laser Synthesis Strategy to Boost Oxygen Evolution Kinetics on Stainless Steel-Based Catalyst via Dual-Metal Segmentally Coordinated Reaction Centers for Efficient Alkaline Water Splitting.

作者信息

Xu Jiayi, Pan Rui, Li Haotian, Wang Lizhong, Yang Zicong, Zhang Shuye, Sun Xin, Li Hongyi, Chen Shujun

机构信息

College of Mechanical and Energy Engineering, Beijing University of Technology, Beijing, 100124, China.

School of Materials Science and Engineering, Tsinghua University, Beijing, 100084, China.

出版信息

Small. 2025 Aug;21(32):e2410421. doi: 10.1002/smll.202410421. Epub 2025 Jun 13.

DOI:10.1002/smll.202410421
PMID:40511673
Abstract

The fabrication of efficient, stable, and noble-metal-free electrocatalysts for the hydrogen energy field has been of great interest, but still faces numerous challenges, especially in the development of fast and convenient strategies. This study reports a state-of-the-art strategy for the ultrafast preparation of spinel-type oxide self-supporting catalysts on stainless steel by ultrafast two-step laser synthesis. The self-supporting catalytic electrode not only possesses remarkable superhydrophilic/superaerophobic properties but also the constructed (Ni, Fe, Co)(Fe, Cr)O·(OH)@SS304 microcone array catalyst also demonstrates a superior oxygen evolution reaction (OER) performance with a low overpotential of 130 mV at 10 mA cm, a Tafel slope of 34.0 mV dec, and outstanding long-term stability (a negligible overpotential decay of ≈5% at 10 mA cm for over 88 h). The laser-fabricated catalysts exhibit optimal performances, surpassing that of the best previously reported stainless steel-based OER catalysts. First-principles calculations also reveal that the reaction mechanism of the as-prepared catalyst is affiliated with the oxide path mechanism dominated by the exposed (220) crystal facet, and dual-metal segmentally coordinated reaction centers effectively reduce the oxygen evolution energy barriers, boosting the OER kinetics. This work may open up a new path to design multi-metal-based self-supporting catalysts for hydrogen energy applications.

摘要

在氢能领域制备高效、稳定且无贵金属的电催化剂备受关注,但仍面临诸多挑战,尤其是在开发快速便捷的策略方面。本研究报告了一种通过超快两步激光合成在不锈钢上超快制备尖晶石型氧化物自支撑催化剂的先进策略。该自支撑催化电极不仅具有显著的超亲水/超疏气性能,而且构建的(Ni, Fe, Co)(Fe, Cr)O·(OH)@SS304微锥阵列催化剂在10 mA cm时具有130 mV的低过电位、34.0 mV dec的塔菲尔斜率以及出色的长期稳定性(在10 mA cm下超过88小时,过电位衰减可忽略不计,约为5%),展现出优异的析氧反应(OER)性能。激光制备的催化剂表现出最佳性能,超过了此前报道的最好的不锈钢基OER催化剂。第一性原理计算还表明,所制备催化剂的反应机理与以暴露的(220)晶面为主导的氧化物路径机理相关,双金属分段配位反应中心有效降低了析氧能垒,促进了OER动力学。这项工作可能为设计用于氢能应用的多金属基自支撑催化剂开辟一条新途径。

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