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Defect engineering within clusters to enhance cluster-support interaction boosts catalytic performance
Jiankang Chen1, Yangping Wang1, Yu Zhang1
1Institutes of Physical Science and Information Technology, Department of Chemistry and Centre for Atomic Engineering of Advanced Materials, Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education, Anhui Province Key Laboratory of Chemistry for Inorganic/Organic Hybrid Functionalized Materials, Anhui University Hefei Anhui 230601 China gaoguiqi1@126.com yangshac@ahu.edu.cn.
None:
Supported cluster catalysts effectively optimize mass transfer and electron transfer efficiency, synergistically boosting catalytic performance. However, the regular morphology of clusters hinders adsorption on the support. Therefore, strengthening the metal-support surface interaction remains a critical challenge requiring urgent solutions. In this study, we constructed the Au40 cluster by modifying the Au44 cluster with phosphine, and the resulting Au40 cluster exhibits features similar to those of the parent Au44 cluster, albeit with three gold atoms missing from its core as defects. Furthermore, we loaded the two clusters onto various support materials to evaluate the interaction strength between the clusters and their supports. The results of experiments as well as DFT calculations showed that the defects enhanced the interaction between the Au40 clusters and their supports. Using the hydrogenation of 4-nitrophenol as a model, the catalytic activity of supported catalysts was investigated. The catalytic activity of the Au40 system was much higher than that of the Au44 system, with a catalytic time ratio of approximately 1 : 4. This work reveals that constructing surface defects on clusters serves as an effective method to enhance the interaction between clusters and supports, providing a novel approach for developing cluster-based heterogeneous catalysts.
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