The interaction between adjacent active sites is crucial to balance the efficiency and utilization of functional atoms in single-atom catalysts. Herein, the catalytic activity of hydrogen evolution reaction at different site (nitrogen coordinated transition metal centers embedded in graphene) distances was comprehensively investigated by density functional theory calculations. The results show that a proximity effect of reactivity and site spacing can be identified in the Co-series single-atom catalysts. Although the proximity effect is more linearly responded with the site spacing along x direction, an optimal distance of ∼0.8 and ∼2.8 nm are found for Co and Rh, Ir atoms, respectively. An in-depth analysis of the electronic property reveals that the proximity effect is caused by the distinct net charge of the active site, which is affected by the position relative to EF. Subsequently, an excess electron nodal channel in x direction was found to serve as a communication pathway between the active sites. Through the finding in this work, an optimal Fe-N2C2 structure was deliberately designed and has shown prominent proximity effect as Co-series do. The results reported in this work provide a simple and effective tuning method for the reactivity of a single-atom catalyst.
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7 September 2023
Research Article|
September 01 2023
Proximity effects in graphene‐supported single-atom catalysts for hydrogen evolution reaction
Weijie Lin
;
Weijie Lin
(Investigation, Validation, Visualization, Writing – original draft)
1
School of Physics and Electronics, Henan University
, Kaifeng 475004, China
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Wen-Jin Yin
;
Wen-Jin Yin
(Formal analysis, Supervision, Writing – review & editing)
2
School of Physics and Electronic Science, Hunan University of Science and Technology
, Xiangtan 411201, China
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Bo Wen
Bo Wen
a)
(Conceptualization, Formal analysis, Supervision, Writing – review & editing)
1
School of Physics and Electronics, Henan University
, Kaifeng 475004, China
a)Author to whom correspondence should be addressed: [email protected]
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a)Author to whom correspondence should be addressed: [email protected]
J. Chem. Phys. 159, 094703 (2023)
Article history
Received:
June 29 2023
Accepted:
August 09 2023
Citation
Weijie Lin, Wen-Jin Yin, Bo Wen; Proximity effects in graphene‐supported single-atom catalysts for hydrogen evolution reaction. J. Chem. Phys. 7 September 2023; 159 (9): 094703. https://doi.org/10.1063/5.0165695
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