通过双核站点建设登上ORR火山地块的顶峰:电子和几何工程
Meiling Xiao1, Yongting Chen2, Jianbing Zhu1
1State Key Laboratory of Electroanalytical Chemistry, Jilin Province Key Laboratory of Low Carbon Chemical Power , Changchun Institute of Applied Chemistry Chinese Academy of Sciences , Changchun 130022 , China.
Journal of the American Chemical Society
|October 12, 2019
概括
我们开发了一种新的Fe-Co双原子催化剂, 这种新的催化剂通过优化中间脱离和O-O键裂变,显著提高ORR性能,优于单原子催化剂.
科学领域:
- 电化学
- 材料科学
- 催化剂
背景情况:
- 具有M-NX中心的单原子催化剂 (SAC) 对氧降解反应 (ORR) 是有前途的.
- 目前ORR的SAC表现低于基于的催化剂,因为吸附-脱附动力学不理想.
- 针对最佳的能量水平和几何形状来定制活动场地配置对于改进SAC至关重要.
研究的目的:
- 设计和合成一种具有增强ORR活性的新型二原子催化剂.
- 研究电子结构修饰和协调几何学在ORR催化中的作用.
- 为ORR电催化提供对二原子位点的基本见解.
主要方法:
- 构建一个Fe-Co双原子中心位点 (FeCoN5-OH).
- 加入一个吸收电子的OH连接体来改变能量水平并促进中间溶解.
- 电化学表征以评估ORR性能,包括开始和半波潜力.
主要成果:
- 在FeCoN5-OH位点表现出优异的ORR活性,发射和半波电位分别为1. 02V和0. 86V (vs RHE).
- FeCoN5-OH位点的内在活性是单原子FeN4位点的20倍以上.
- OH配体有效地改变了电子结构,促进了中间脱离和O-O键裂变.
结论:
- 一个新的策略使用二原子站点与定制的电子结构已成功为ORR开发.
- 具有OH联体的Fe-Co双原子位点为设计高性能ORR电催化剂提供了有前途的途径.
- 这项工作促进了对二原子位点的理解,并为催化剂设计提供了新的途径.
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