期刊
NANO RESEARCH
卷 15, 期 2, 页码 1338-1346出版社
TSINGHUA UNIV PRESS
DOI: 10.1007/s12274-021-3662-y
关键词
heterogeneous catalysis; palladium single atom catalyst; porous ceria nanorod; hydrodehalogenation; catalytic activity
类别
资金
- China Postdoctoral Science Foundation [2019M661247, 2020T130091]
- Postdoctoral Science Foundation of Heilongjiang Province [LBH-Z19047]
- Program for Overseas Talents Introduction of Northeast Petroleum University [15041260303]
- Scientific Research Foundation for Returned Scholars of Heilongjiang Province of China [719900091]
The study describes a simple and efficient approach to create atomically dispersed palladium catalysts, which exhibit excellent catalytic activity and recyclability. Density functional theory calculations reveal that the high activity stems from the spatial isolation of palladium atoms and the modified electronic structure in defect-containing ceria nanorods.
Tuning the electronic properties of single atom catalysts (SACs) between the central metal and the neighboring surface atoms has emerged as an efficient strategy to boost catalytic efficiency and metal utilization. Here we describe a simple and efficient approach to create atomically dispersed palladium atoms supported over defect-containing porous ceria nanorod containing palladium up to 0.26 wt.%. The existence of singly dispersed palladium atoms is confirmed by spherical aberration correction electron microscopy and extended X-ray absorption fine structure measurements. This catalyst shows excellent efficiency in hydrodehalogenation reactions at low H-2 pressure under mild conditions, along with satisfactory recyclability and scalability. Density functional theory (DFT) calculations reveal that the high activity stems from the spatial isolation of palladium atoms and the modified electronic structure of palladium confined in defect-containing ceria nanorod. This work may lay the foundation for the facile creation of single atom catalysts within the synthetic community and shed light on the possibility for scale-up production.
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