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Replacing fossil fuels with fuel cells is a feasible way to reduce global energy shortages and environmental pollution. However, the oxygen reduction reaction (ORR) at the cathode has sluggish kinetics, which limits the development of fuel cells. It is significant to develop catalysts with high catalytic activity of ORR. The single-atom catalysts (SACs) of Pt supported on heteroatom-doped graphene are potential candidates for ORR. Here we studied the SACs of Pt with different heteroatoms doping and screened out Pt-C4 and Pt-C3O1 structures with only 0.13 V overpotential for ORR. Meanwhile, it is found that B atoms doping could weaken the adsorption capacity of Pt, while N or O atoms doping could enhance it. This regularity was verified on Fe SACs. Through the electronic interaction analysis between Pt and adsorbate, we explained the mechanism of this regularity and further proposed a new descriptor named corrected d-band center (εd-corr) to describe it. This descriptor is an appropriate reflection of the number of free electrons of the SACs, which could evaluate its adsorption capacity. Our work provides a purposeful regulatory strategy for the design of ORR catalysts.

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Publication history
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Acknowledgements

Publication history

Received: 29 March 2023
Revised: 22 May 2023
Accepted: 05 June 2023
Published: 24 July 2023
Issue date: February 2024

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

This work was supported by the National Key R&D Program of China (Nos. 2022YFA1503100 and 2022YFA1503102), the National Natural Science Foundation of China (No. 22273050), and the Natural Science Foundation of Shandong Province (Nos. YDZX2021001 and ZR2022MB098).

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