在CO氧化过程中解开支单原子的电荷状态
Xiong Zhou1,2, Qian Shen1,2, Kaidi Yuan2
1BNLMS, College of Chemistry and Molecular Engineering, Peking University , Beijing 100871, China.
Journal of the American Chemical Society
|January 3, 2018
概括
在氧化铜上稳定的单个金原子有效催化一氧化碳. 支持器中的电荷转移和氧气空缺是这种催化活动的关键,这种催化活动可以通过氧气暴露恢复.
科学领域:
- 不同质的催化
- 表面科学
- 纳米材料
背景情况:
- 单原子催化剂提供高原子利用效率.
- 调节催化剂活动需要了解金属支相互作用.
- 铜氧化物 (CuO) 是一种有前途的催化支持材料.
研究的目的:
- 在单层CuO上制备和描述热稳定的黄金单原子.
- 研究电荷转移和支结构在CO氧化中的作用.
- 阐明反应机制和失活/恢复途径.
主要方法:
- 通过原子层沉积在单层CuO/Cu110上合成Au单原子.
- 在现场表征技术研究电荷转移和表面物种.
- 动力学研究和理论计算以了解反应机制.
主要成果:
- 在单层CuO的支持下成功合成了热稳定的Au单原子.
- 证实了从CuO支到Au单原子的显著电荷转移.
- 证明负电荷的Au原子对CO氧化具有活性,从而产生氧气空缺.
- 在氧气暴露时观察到催化剂的失活和恢复.
结论:
- 从CuO到Au单原子的电荷转移对于CO氧化活动至关重要.
- 催化循环包括氧空位的形成和CuO支的愈合.
- 通过控制充电状态和支缺陷,可以调节Au SAC的稳定性和活动.
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