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高耐用的Rh单原子催化剂通过表面缺陷调节Fe-Ce氧化物固体溶液上的表面缺陷

Gunjoo Kim¹, Seokhyun Choung², Jae-Eon Hwang¹

¹Department of Chemical and Biomolecular Engineering, Korea Advanced Institute of Science and Technology, Daejeon, 34141, South Korea.

Angewandte Chemie (International ed. in English)

|January 8, 2025

概括

具有在铁氧化物支上固定的单原子催化剂在选择性催化降解氧化物 (NOx) 与一氧化碳 (CO) 中表现出更好的性能. 这种持久的催化剂设计提供了卓越的活性和稳定性.

科学领域:

材料科学材料科学材料科学
催化剂是一种催化剂.
表面化学表面化学

背景情况:

单原子催化剂 (SAC) 对于高效的化学转换至关重要.
催化剂支上的缺陷点可以固定单个金属原子以提高反应性.
铁 (Fe-Ce) 氧化物固体溶液为催化剂设计提供独特的表面特性.

研究的目的:

准备和表征单个原子 (Rh ₁) 在一个Fe-Ce氧化物支 (FC).
评估Rh₁/FC在氧化物与一氧化碳 (CO-SCR) 的选择性催化还原中的性能.
在反应条件下研究SAC的结构稳定性和反应机制.

主要方法:

在Fe-Ce氧化物支上使用缺陷点合成Rh₁/FC.
使用先进的光谱和理论方法对催化剂进行表征.
评估CO-SCR活动和耐用性在高温下.
在现场进行DRIFTS和DFT计算,以研究反应中间体和机制.

主要成果:

与对照组相比,Rh₁/FC降低到500°C显示出更高的CO-SCR活性和耐久性.
单原子结构在400°C下保持稳定超过100小时.
DFT计算显示,Fe位稳定Rh原子,而NO和CO优先吸附于Rh.
Fe促进了氧气的转移,提高了催化性能.

结论:

氧化铁支是有效的固定稳定和活跃的单个Rh原子.
优化降低条件 (500°C) 产生高活性和持久的SAC,用于CO-SCR.
铁和Rh位点之间的协同作用是提高催化性能和稳定性的关键.

关键词:

耐久性耐久性耐久性是的元素之一.选择性催化还原选择性催化还原单个原子催化剂的催化剂.表面缺陷表面缺陷

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