在氧化物演化反应过程中,TM-N4-C单原子催化剂的活性部位演化
Shaojie Jing1,2, Zhouhao Zhu2, Yang Wang3
1Donghai Laboratory, Zhoushan, Zhejiang 316021, China.
The journal of physical chemistry letters
|July 17, 2025
概括
单原子催化剂 (SACs) 对氧演化反应 (OER) 显示出希望. 这项研究揭示了Fe,Co和Ni催化剂在工作条件下的活性位点是如何演变的,澄清了它们的催化机制.
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
- 计算化学计算化学
背景情况:
- 单原子催化剂 (SAC) 具有过渡金属原子在N-合碳 (TM-N4-C) 中,对氧演化反应 (OER) 是有前途的.
- 在工作条件下,SAC中活跃站点的确切性质仍然不明确.
研究的目的:
- 在OER期间调查Fe,Co和Ni SACs活性位点的演变.
- 阐明金属d波段轨道位置与活性点组成之间的关系.
- 提供关于在应用潜力下活跃地点的稳定性的见解.
主要方法:
- 第一原则计算.第一原则计算.
- 热力学和动力学模拟.
主要成果:
- 活性部位的组成强烈依赖于金属d波段的轨道位置,以Fe > Co > Ni的顺序下降.
- 铁SACs被*OH或*O覆盖;Co SACs被*OH覆盖.
- Ni SAC 具有具有 *OH 轴协调和相邻的 *O 覆盖的组合活性位点.
结论:
- 鉴定到的活性位点配置在应用电极电位下是稳定的.
- 这项工作提供了对TM-N4-C SAC中的OER路径和活跃中心的详细了解.
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