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Flagship Article

Modulating the electronic spin state by constructing dual-metal atomic pairs for activating the dynamic site of oxygen reduction reaction

Shenghua Ye1,3,§, Shuhua Xie1,§, Yaqi Lei1,§, Xiuyuan Yang1, Jing Hu1, Lirong Zheng4, Zhida Chen1, Yonghuan Fu1, Xiangzhong Ren1, Yongliang Li1, Xiaoping Ouyang5, Qianling Zhang1 ( ), Jianhong Liu1,3( ), Xueliang Sun2 ( )
College of Chemistry and Environmental Engineering, Graphene Composite Research Center, Shenzhen University, Shenzhen 518060, China
Department of Mechanical and Materials Engineering, University of Western Ontario, London, Ontario N6A 5B9, Canada
Shenzhen Eigen-Equation Graphene Technology Co. Ltd., Shenzhen 518000, China
Institute of High Energy Physics Chinese Academy of Sciences, Beijing 100049, China
School of Materials Science and Engineering, Xiangtan University, Xiangtan 411105, China

§ Shenghua Ye, Shuhua Xie, and Yaqi Lei contributed equally to this work.

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Abstract

In this study, dual-metal atomic pairs of manganese (Mn)-iron (Fe) binuclear sites (BNSs) with two conjoint MnN4 and FeN4 moieties (MnFeN8) anchored onto a graphite-like structure (GLS) (Mn-Fe BNSs/GLS) were constructed. The binuclear MnFeN8 structure was verified experimentally and theoretically. Magnetic measurements and Gaussian calculations reveal that this unique Mn-Fe BNSs exhibit strong short-range electronic interaction between Mn and Fe sites, which decouples two paired d electrons in Fe sites, thereby transforming Fe sites from an intermediate to a high spin state. The optimal electronic configuration of Fe sites and their binuclear structure facilitate an oxygen reduction reaction (ORR) thermodynamically and dynamically, respectively, endowing Mn-Fe BNSs with improved ORR performance.

Graphical Abstract

The binuclear MnFeN8 moiety anchored onto a graphite-like structure (GLS) (Mn-Fe BNSs/GLS) was constructed by pyrolysis for oxygen reduction reaction (ORR). Unique short-range electronic interaction between Mn and Fe sites renders Fe sites transform from intermediate to a high spin state facilitates the cleavage of O–O and endows Mn-Fe BNSs/GLS with excellent ORR activity.

Keywords

manganese (Mn)-iron (Fe) binuclear sitessynergistic effectspin stateoxygen reduction reaction

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Nano Research
Volume 16 Issue 2,
February 2023
Pages 1869-1877
DOI: 10.1007/s12274-022-4979-x

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Cite this article:
Ye S, Xie S, Lei Y, et al. Modulating the electronic spin state by constructing dual-metal atomic pairs for activating the dynamic site of oxygen reduction reaction. Nano Research, 2023, 16(2): 1869-1877. https://doi.org/10.1007/s12274-022-4979-x
Topics:
Oxygen reduction reaction

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Received: 05 August 2022
Revised: 26 August 2022
Accepted: 27 August 2022
Published: 04 November 2022
© Tsinghua University Press 2022