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Regulating the Oxygen Affinity of Single Atom Catalysts by Dual-atom Design for Enhanced Oxygen Reduction Reaction Activity

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Abstract

This work chooses Cu/Fe single-atom catalysts(SACs) with weak/strong oxygen affinity to clarify the effect of dual-atom configuration on oxygen reduction reaction(ORR) performance based on density functional theory(DFT) calculations. The stability and ORR activity of single or dual Cu/Fe atomic sites anchored on nitrogen-doped graphene sheets(Cu-N4-C, Cu2-N6-C, Fe-N4-C, and Fe2-N6-C) are investigated, and the results indicate the dual-atom catalysts(Cu2-N6-C and Fe2-N6-C) are thermodynamically stable enough to avoid sintering and aggregation. Compared with single-atom active sites of Cu-N4-C, which show weak oxygen affinity and poor ORR performance with a limiting potential of 0.58 V, the dual-Cu active sites of Cu2-N6-C exhibit enhanced ORR activity with a limiting potential up to 0.87 V due to strengthened oxygen affinity. Interestingly, for Fe SACs with strong oxygen affinity, the DFT results show that the dual-Fe sites stabilize the two OH* ligands structure[Fe2(OH)2-N6-C], which act as the active sites during ORR process, resulting in greatly improved ORR performance with a limiting potential of 0.90 V. This study suggests that the dual-atom design is a potential strategy to improve the ORR performance of SACs, in which the activity of the single atom active sites is limited with weak or strong oxygen affinity.

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Acknowledgements

This work was supported by the National Key R&D Program of China(No. 2021YFA1600800) and the National Natural Science Foundation of China(No. 22022508).

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Authors and Affiliations

  1. College of Materials Science and Engineering, Shenzhen University, Shenzhen, 518071, P. R. China

    Meng Zheng & Jin Wang

  2. College of Physics and Optoelectronic Engineering, Shenzhen University, Shenzhen, 518060, P. R. China

    Meng Zheng

Authors
  1. Meng Zheng
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  2. Jin Wang
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Correspondence to Jin Wang.

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The authors declare no conflicts of interest.

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40242_2022_2241_MOESM1_ESM.pdf

Special Issue of Single-atom Catalysis: Regulating the Oxygen Affinity of Single Atom Catalysts by Dual-Atom Design for Enhanced Oxygen Reduction Reaction Activity

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Zheng, M., Wang, J. Regulating the Oxygen Affinity of Single Atom Catalysts by Dual-atom Design for Enhanced Oxygen Reduction Reaction Activity. Chem. Res. Chin. Univ. 38, 1275–1281 (2022). https://doi.org/10.1007/s40242-022-2241-4

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  • DOI: https://doi.org/10.1007/s40242-022-2241-4

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