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在以为基础的氧气进化催化剂中通过前体多态工程识别有益和有害的Co⁴⁺物种

Zhongheng Li¹, Zheng Shu¹, Lun Li¹

¹Institute of Applied Physics and Materials Engineering, University of Macau, Taipa, Macau SAR, 999078, China.

Advanced science (Weinheim, Baden-Wurttemberg, Germany)

|September 29, 2025

概括

氧化物相 (CoO2) 显著影响水电解效率. 该研究表明,γ-CoO2阶段通过稳定关键中间体来增强氧演化反应 (OER),从而导致更好的生产催化剂.

科学领域:

电化学电化学电化学
材料科学材料科学材料科学
催化剂是一种催化剂.

背景情况:

氧化演化反应 (OER) 对于通过水电解产生至关重要,但通常受到催化剂效率和成本的限制.
基于的材料是高贵金属催化剂的有希望的替代品,但CO4+物种在OER过程中的确切作用尚不清楚.
现有的研究提出了相互矛盾的观点,即CoO2是活性阶段,还是Co4+物种抑制反应.

研究的目的:

系统地调查CO4+物种对OER活动的影响.
了解不同的氧化物相 (γ-CoO2和β-CoO2) 如何影响催化性能.
为先进的过渡金属催化剂提供合理的设计策略.

主要方法:

通过热定制多态氧硫化物的重建,以稳定特定的CO2相.
使用结构分析来将格子灵活性和协调与OER条件下的相稳定性相关联.
进行机制研究以阐明反应通路 (氧气通路机制与吸附物进化机制).

主要成果:

H2O/OH−的间隙促进了格子扩张,有利于形成γ-CoO2阶段.
在β-CoO2中的刚性CO−O键限制了结构灵活性.
γ-CoO2阶段通过氧通路机制 (OPM) 促进超氧化中间体的产生,其性能优于遵循吸附物进化机制 (AEM) 的β-CoO2阶段.

结论:

γ-CoO2阶段表现出优越的OER催化性能,其特点是较低的超电位和更好的长期稳定性.
Co4+物种的微环境极大地影响了OER的表现.
这些发现为优化基催化剂提供了一个框架,用于高效的水电解和生产.

关键词:

Co4+物种的种类.氧气进化反应反应氧气进化反应工程的先驱工程的前体.反应机制的反应机制.表面重建重建的重建.

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