含有Fe的氧化物中的晶格O-O连接物增强了水氧化电催化作用
Guoshuai Shi1, Jili Li1, Tingyu Lu1
1Department of Chemistry, State Key Laboratory of Porous Materials for Separation and Conversion, Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) and Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials, Fudan University, Shanghai, China.
研究人员在Ni-Fe催化剂中发现了一种新的超氧-氧化物阶段,揭示了格子O-O连接物如何激活铁位点以实现高效的氧进化电催化.
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:
- 在反应条件下,理解触媒中心的配体动力学对于催化剂设计至关重要.
- 催化剂在运行过程中的结构变化往往难以阐明.
研究的目的:
- 在氧化演化电催化过程中研究Ni-Fe氧化催化剂的现场结构动力学.
- 确定特定的连接体构成在激活催化中心中的作用.
主要方法:
- 使用Operando 18O标记光谱电化学来追踪同位素的结合.
- 机器学习辅助的全球优化用于分析结构数据.
- 第一原则计算验证了实验发现.
主要成果:
- 观察到Ni-Fe氧化物转化为稳定的超氧氧化物阶段.
- 格子O-O (Olatt-Olatt) 连接体的形成被确定为一个关键的中间体.
- 奥拉特-奥拉特度与氧气进化过程中Fe位点的内在活性直接相关.
结论:
- 格子O-O干激活超氧-氧化物结构中的铁位点,增强氧的进化电催化.
- 氧气的生产是通过一种吸附剂演化机制进行的,Fe位点的激活能量降低.
- 这项研究提供了一个设计高性能Fe-incorporated电催化剂的框架,通过控制连接体动力学.
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