原子尺度催化剂上的C3H8氧化:对活性氧物种和反应途径的洞察
Qifeng Zhang1, Yuchun Song1, Aijie Xu1
1State Key Laboratory of Green Chemical Engineering and Industrial Catalysis, Research Institute of Industrial Catalysis, School of Chemistry and Molecular Engineering, East China University of Science and Technology, Shanghai 200237, PR China.
Journal of hazardous materials
|June 3, 2025
概括
与双原子或集群催化剂相比,在 (Ru/CeO2-SA) 上的单原子催化剂显著增强了氧化. 原子级催化剂的这一突破为更清洁的能源应用提供了卓越的效率.
科学领域:
- 不同质的催化剂.
- 纳米材料科学科学 纳米材料科学
- 表面化学 表面化学
背景情况:
- 原子级分散催化剂比纳米催化剂更深入地了解催化反应机制.
- 了解超低金属负载效应对于开发高效和成本效益的催化剂至关重要.
研究的目的:
- 研究单原子 (Ru/CeO2-SA),双对 (Ru2/CeO2) 和四原子集群 (Ru4/CeO2) 催化剂对C3H8氧化的影响.
- 阐明催化剂结构和负荷对氧激活,反应中间体和氧化途径的作用.
主要方法:
- 合成Ru/CeO2催化剂具有不同的Ru原子排列 (单原子,双对,四原子集群) 在超低负载 (0.1重量%) 时.
- 在和无水条件下对C3H8氧化中的催化性能的评估.
- 使用光谱和动力学方法 (隐含) 分析反应中间体和途径.
主要成果:
- Ru/CeO2-SA和Ru4/CeO2表现出比Ru2/CeO2.2更优越的氧化性能.
- Ru/CeO2-SA实现了 43.7 × 10^-2 s^-1 的高周转频率 (TOF),以及 267 °C 的低 T50.
- 在Ru/CeO2-SA中增强的活性与由表面晶格氧和Ru的接近促进的烯酸中间体形成有关.
结论:
- 在CeO2上单原子的配置显著提高了氧化效率.
- 催化剂结构,特别是单原子分散,极大地影响氧气激活和反应途径.
- 形成特定的中间体,如烯酸,是原子级催化剂优越性能的关键.
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