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High-throughput screening of carbon-supported single metal atom catalysts for oxygen reduction reaction

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Abstract

Carbon-supported transition metal single atoms are promising oxygen reduction reaction (ORR) electrocatalyst. Since there are many types of carbon supports and transition metals, the accurate prediction of the components with high activity through theoretical calculations can greatly save experimental time and costs. In this work, the ORR catalytic properties of 180 types single-atom catalysts (SACs) composed of the eight representative carbon-based substrates (graphdiyne, C2N, C3N4, phthalocyanine, C-coordination graphene, N-coordination graphene, covalent organic frameworks and metal-organic frameworks) and 3d, 4d, and 5d transition metal elements are investigated by density functional theory (DFT). The adsorption free energy of OH* is proved a universal descriptor capable of accurately prediction of the ORR catalytic activity. It is found that the oxygen reduction reaction overpotentials of all the researched SACs follow one volcano shape very well with the adsorption free energy of OH*. Phthalocyanine, N-coordination graphene and metal-organic frameworks stand out as the promising supports for single metal atom due to the relatively lower overpotentials. Notably, the Co-doped metal-organic frameworks, Ir-doped phthalocyanine, Co-doped N-coordination graphene, Co-doped graphdiyne and Rh-doped phthalocyanine show extremely low overpotentials comparable to that of Pt (111). The study provides a guideline for design and selection of carbon-supported SACs toward oxygen reduction reaction.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (No. 51371017). This research was supported by the high-performance computing (HPC) resources at Beihang University.

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Authors and Affiliations

  1. School of Materials Science and Engineering, Beihang University, Beijing, 100191, China

    Yiran Wang, Riming Hu, Jiaxiang Shang & Jianglan Shui

  2. Qinghai Provincial Key Laboratory of New Light Alloys, Qinghai Provincial Engineering Research Center of High-Performance Light Metal Alloys and Forming, Qinghai University, Xining, 810016, China

    Yongcheng Li

  3. Center for Condensed Matter Physics Department of Physics, Capital Normal University, Beijing, 100048, China

    Fuhe Wang

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  1. Yiran Wang
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Wang, Y., Hu, R., Li, Y. et al. High-throughput screening of carbon-supported single metal atom catalysts for oxygen reduction reaction. Nano Res. 15, 1054–1060 (2022). https://doi.org/10.1007/s12274-021-3598-2

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