通过表面增强红外吸收光谱解开单原子催化剂的动态结构演变
Jie Ding1, Lingyue Liu2, Jian Zhang3
1Department of Materials Science and Engineering, City University of Hong Kong, Hong Kong SAR 999077, China.
Journal of the American Chemical Society
|March 7, 2025
概括
金属--碳单原子催化剂 (SAC) 在电化学CO降解过程中通过基攻击降解. 由于更强的Cu-N键,Cu1/Npyri-C表现出比Cu1/Npyrr-C优越的稳定性,指导了未来耐用的催化剂设计.
科学领域:
- 材料科学
- 电化学
- 催化剂
背景情况:
- 金属--碳 (M-N-C) 单原子催化剂 (SAC) 对电化学反应具有前景.
- 它们的实际应用受到有限的长期催化稳定性的阻碍.
- 了解禁用机制对于设计持久性SAC至关重要.
研究的目的:
- 在电化学CO降解反应 (CORR) 中研究两个模型Cu-N-C SACs (Cu1/Npyri-C和Cu1/Npyrr-C) 的动态演变和失活机制.
- 将不同Cu-N协调环境的SAC的催化稳定性进行比较.
- 为开发具有更强耐久性的下一代SAC提供见解.
主要方法:
- 在现场表征:减弱的总反射面增强红外吸收光谱,X射线吸收光谱,电子磁共振光谱和紫外线可见光谱.
- 电化学CO降解反应 (CORR) 测试
- 理论计算和运动分析.
主要成果:
- 在CORR过程中,Cu1/Npyrr-C的纳米粒子形成速度超过Cu1/Npyri-C的6倍.
- 在CORR过程中产生的基攻击Cu-N键,导致Cu出和纳米粒子形成.
- 由于强的Cu-Npyri键,Cu1/Npyri-C的催化稳定性明显优于Cu1/Npyrr-C.
结论:
- 在电化学CORR中Cu-N-C SAC的失活主要是由基诱导的Cu-N键的降解引起的.
- 的协调环境显著影响SAC的稳定性,更强的键带来更强的耐用性.
- 本研究为电化学应用中强大的SAC提供了基本的理解和设计原则.
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