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Nano Research 2023, 16(2): 2199-2208 https://doi.org/10.1007/s12274-022-4982-2
Research Article | Issue | Published: 29 September 2022

Dynamics of non-metal-regulated FeCo bimetal microenvironment on oxygen reduction reaction activity and intrinsic mechanism

Show Author's Information Hong Cui1,2,§( ),  Tong Liu1,2,§( ),  Yunjian Chen1,2,  Pengyue Shan1,2,  Qi Jiang1,2,  Xue Bai1,2,  Yazhou Wang1,2,  Zhiyong Liang1,2,  Rong Feng1,2,  Qin Kang1,2,  Hongkuan Yuan3
School of Mechanical Engineering, Shaanxi University of Technology, Hanzhong 723001, China
Shaanxi Key Laboratory of Industrial Automation, Shaanxi University of Technology, Hanzhong 723001, China
School of Physical Science and Technology, Southwest University, Chongqing 400715, China

§ Hong Cui and Tong Liu contributed equally to this work.

Keywords:
charge transfer, coordination environment, dynamic distribution of charges, orbital energy levels
Topics:
Oxygen reduction reaction
Cite this article:
Cui H, Liu T, Chen Y, et al. Dynamics of non-metal-regulated FeCo bimetal microenvironment on oxygen reduction reaction activity and intrinsic mechanism. Nano Research, 2023, 16(2): 2199-2208. https://doi.org/10.1007/s12274-022-4982-2
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Abstract Full text Electronic supplementary material About this article

The change in the coordination environment of the active sites of a fuel cell cathode catalyst provides a new modulation strategy for stimulating the catalyst’s oxygen reduction reaction activity. The thermodynamic and electronic properties of the FeCoN5A and FeCoN6A catalyst structures with nonmetallic A-doped (A = B, N, O, P, and S) coordination were calculated and analyzed based on density functional theory. The modulation order of G*OH by different A-doped FeCo bimetal pairs (BMPs) was as follows: S > P > O > N/C > B. There was a dynamic distribution of charges in the coordination environment during the adsorption of OH, which resulted in inversely proportional relationship with the charge transfer between the adsorbate OH, active site, first coordination layer, and second coordination layer in turn. Descriptors of the orbital energy levels of neighboring nonmetal atoms were constructed based on the p-electron number and electronegativity of the doped nonmetal A. The change of the orbital energy levels of the first coordination atom during the adsorption process caused the structure to exhibit different adsorption energies. This study provides new insights on the non-metallic modulation of the M-N-C coordination environment to improve the oxygen reduction reaction activity.


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About this article

Dynamics of non-metal-regulated FeCo bimetal microenvironment on oxygen reduction reaction activity and intrinsic mechanism

Show Author's information Hong Cui1,2,§( ), Tong Liu1,2,§( ), Yunjian Chen1,2, Pengyue Shan1,2, Qi Jiang1,2, Xue Bai1,2, Yazhou Wang1,2, Zhiyong Liang1,2, Rong Feng1,2, Qin Kang1,2, Hongkuan Yuan3
School of Mechanical Engineering, Shaanxi University of Technology, Hanzhong 723001, China
Shaanxi Key Laboratory of Industrial Automation, Shaanxi University of Technology, Hanzhong 723001, China
School of Physical Science and Technology, Southwest University, Chongqing 400715, China

§ Hong Cui and Tong Liu contributed equally to this work.

Abstract

The change in the coordination environment of the active sites of a fuel cell cathode catalyst provides a new modulation strategy for stimulating the catalyst’s oxygen reduction reaction activity. The thermodynamic and electronic properties of the FeCoN5A and FeCoN6A catalyst structures with nonmetallic A-doped (A = B, N, O, P, and S) coordination were calculated and analyzed based on density functional theory. The modulation order of G*OH by different A-doped FeCo bimetal pairs (BMPs) was as follows: S > P > O > N/C > B. There was a dynamic distribution of charges in the coordination environment during the adsorption of OH, which resulted in inversely proportional relationship with the charge transfer between the adsorbate OH, active site, first coordination layer, and second coordination layer in turn. Descriptors of the orbital energy levels of neighboring nonmetal atoms were constructed based on the p-electron number and electronegativity of the doped nonmetal A. The change of the orbital energy levels of the first coordination atom during the adsorption process caused the structure to exhibit different adsorption energies. This study provides new insights on the non-metallic modulation of the M-N-C coordination environment to improve the oxygen reduction reaction activity.

Keywords: charge transfer, coordination environment, dynamic distribution of charges, orbital energy levels

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Publication history
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Acknowledgements

Publication history

Received: 30 June 2022
Revised: 17 August 2022
Accepted: 29 August 2022
Published: 29 September 2022
Issue date: February 2023

Copyright

© Tsinghua University Press 2022

Acknowledgements

Acknowledgements

This research was funded by the National Natural Science Foundation of China (Nos. 61701288 and 51706128), the basic research plan of natural science in Shaanxi province (No. 2021JM-485), and the key scientific research project of Shaanxi provincial education department (No. 20JS019).

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