用17O固态NMR光谱和DFT计算揭示了Pt1/CeO2的结构-活性关系
Yujie Wen1, Fang Wang1, Jie Zhu2,3
1Key Laboratory of Mesoscopic Chemistry of MOE, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing, China.
单原子催化剂 (SACs) 在上使用正方形平面,显示了增强的CO氧化. 这种精确的结构洞察力有助于开发先进的催化剂.
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) 通过各种协调环境提供可调节的性能.
- 精确地描述活跃地点对于结构-活动关系至关重要,但仍然具有挑战性.
- 在SAC中活跃地点的各种局部结构阻碍了详细分析.
研究的目的:
- 为了阐明在 (Pt/CeO2) SACs上的详细结构信息.
- 为了研究不同 Pt/CeO2 SAC 结构的催化行为.
- 为氧化物支持的SAC建立结构-活性关系.
主要方法:
- 使用了17O固态核磁共振 (NMR) 光谱.
- 用人密度函数理论 (DFT) 计算用于结构和能量分析.
- 研究了CO氧化催化性能.
主要成果:
- 确定了嵌入CeO2 (111) 表面的正方形平面几何体的单个Pt原子,通过从集群中的水蒸气分散形成.
- 与原始Pt集群和其他传统合成的SAC相比,观察到明显的结构差异.
- 与八面体对应物相比,方形平面Pt/CeO2 SAC的CO氧化性能得到了改善.
结论:
- 方形平面Pt/CeO2 SAC表现出优越的CO氧化,这是由于最佳的CO吸附和低能量的障碍.
- 结合的NMR和DFT方法使SACs的精确,空间分辨的特征成为可能.
- 这种方法可以扩展到其他氧化物支持的SAC,用于全面的结构-活性关系研究.
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