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Design of platinum single-atom doped metal nanoclusters as efficient oxygen reduction electrocatalysts by coupling electronic descriptor

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Abstract

Inspired by the single-atom catalysts (SACs) concept, we rationally design a series of Pt single atom catalysts embedded in different transition metal nanoclusters through first-principles calculations. In these so-called “crown-jewel” (CJ) structures, Pt atoms (jewels) occupy the vertex sites of the metal nanocluster (crown) surface. We investigated the thermal stability and oxygen reduction reaction (ORR) catalytic activity of these catalysts. The results reveal that CJ-structured PtCu nanoclusters are stable and possess a comparable or even better ORR activity compared to Pt catalyst, making it a promising candidate for low-cost ORR catalysts. The effect of cluster size on the adsorption strength of ORR intermediates and catalytic property has also been studied. Furthermore, the overall ORR catalytic activity trend of these SACs is explained based on analysis of their electronic properties. A descriptor Ψ was established to provide further insight into the correlation between the electronic structure and catalytic activity, which provides a design strategy for new ORR catalysts. More importantly, we reveal that this electronic descriptor can be extended to predict other CJ-structured nanoclusters.

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Acknowledgements

This work was financially supported by the National Key Research and Development Program of China (No. 2018YFB0704300) and partially by the Ministry of Education, Singapore, under its MOE AcRF Tier 3 Award MOE2018-T3-1-002. Q. L. thanks the China Scholarship Council (CSC) for financial support (No. 202006460065). We acknowledge Centre for Advanced 2D Materials, National University of Singapore, and National Supercomputing Center Singapore for providing highperformance computing facilities.

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Authors and Affiliations

  1. Beijing Advanced Innovation Center for Materials Genome Engineering, University of Science and Technology Beijing, Beijing, 100083, China

    Qing Liu, Lu Li, Keke Song & Ping Qian

  2. Department of Physics, Faculty of Science, National University of Singapore, Singapore, 117551, Singapore

    Qing Liu & Yuan Ping Feng

  3. DP Technology, Beijing, 100080, China

    Xiaoxu Wang

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  1. Qing Liu
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  2. Xiaoxu Wang
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  3. Lu Li
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Correspondence to Ping Qian or Yuan Ping Feng.

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Design of platinum single-atom doped metal nanoclusters as efficient oxygen reduction electrocatalysts by coupling electronic descriptor

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Liu, Q., Wang, X., Li, L. et al. Design of platinum single-atom doped metal nanoclusters as efficient oxygen reduction electrocatalysts by coupling electronic descriptor. Nano Res. 15, 7016–7025 (2022). https://doi.org/10.1007/s12274-022-4343-1

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