缺陷工程LaFeO3 稳定氧化Pt单原子位点用于低温CO氧化
Tao Gan1,2, Lei Tao3, Zedong Zhang2
1Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai 201204, China.
Journal of the American Chemical Society
|September 2, 2025
概括
在有缺陷的矿支上安装的工程单原子催化剂 (SAC) 显示了氧化反应的增强稳定性和活性. 这种缺陷工程策略优化了催化剂性能,而不需要减少预处理.
科学领域:
- 材料科学
- 催化剂
- 表面化学
背景情况:
- 单原子催化剂 (SAC) 在氧化反应中面临着活性和稳定性之间的权衡.
- 高协调点是稳定的,但不活跃;低协调点是活跃的,但不稳定的.
- 过度氧化和聚合限制了SAC的实际应用.
研究的目的:
- 制定一个缺陷工程策略,以克服白金SAC中的活动稳定性困境.
- 将氧化单个原子固定在空置工程矿支上 (v-LaFeO3).
- 为了提高氧化反应的催化性能.
主要方法:
- 通过引入La-空隙来对LaFeO3矿进行缺陷工程.
- 在v-LaFeO3支上固定氧化单个原子 (Pt4+).
- 使用结构分析和现场实验进行表征.
- 密度函数理论 (DFT) 计算以验证结构和机制.
主要成果:
- 该v-LaFeO3支增强了晶格氧的移动性,并保持了结构完整性.
- 固定Pt单个原子表现出最佳的协调和高氧化状态 (Pt4+).
- 在没有减少预处理的情况下,催化剂表现出高稳定的CO氧化活性.
- 空隙调节接口电子结构,激活晶格氧气和加速O2激活.
结论:
- 精确控制支缺陷可以同时优化电子状态和SAC的稳定性.
- 这种缺陷工程策略为设计强大的氧化催化剂提供了通用范式.
- 开发的催化剂对长期高温氧化反应具有前景.
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