A theoretical study on molybdenum and sulfur co-doped graphene for electrocatalytic nitrogen reduction

Yanyang Qin; Shishi Zhang; Guoxin Gao; Shujiang Ding; Yaqiong Su

doi:10.1016/j.mcat.2021.112048

A theoretical study on molybdenum and sulfur co-doped graphene for electrocatalytic nitrogen reduction

Yanyang Qin, Shishi Zhang, Guoxin Gao, Shujiang Ding, Yaqiong Su (Corresponding author)

Inorganic Materials & Catalysis

Onderzoeksoutput: Bijdrage aan tijdschrift › Tijdschriftartikel › Academic › peer review

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The electrocatalytic nitrogen reduction reaction (NRR) is a promising strategy to generate NH₃ in mild condition. Herein, we designed four NRR single-atom catalysts to mimic the structures of FeMo-cofactor in nitrogenase, in which a Mo or Fe atom is anchored to sulfur doped graphene carbon nanosheets (Mo/Fe@S-gCNS). Density functional theory calculations were performed to investigate the stability of Mo/Fe@S-gCNS, as well as their NRR activity. The results suggest that Mo@S-gCNS coordinated with three S (Mo-S₃) displays the best NRR catalytic activity among the four catalysts, and the NRR prefers to proceed through the enzymatic pathway with an overpotential as low as 0.24 V. The outstanding performance is mainly attribute to the appropriate coordination environment together with the intrinsic electronic structure of the embedded Mo atom. These findings contribute to designing the NRR single-atom catalysts and understanding the potential active sites of the FeMo-cofactor.

Originele taal-2	Engels
Artikelnummer	112048
Aantal pagina's	7
Tijdschrift	Molecular Catalysis
Volume	517
DOI's	https://doi.org/10.1016/j.mcat.2021.112048
Status	Gepubliceerd - jan. 2022

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© 2021 Elsevier B.V.

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Y. Su Acknowledge the “Young Talent Support Plan” of Xi'an Jiaotong University and the Open Funds of State Key Laboratory of Physical Chemistry of Solid Surfaces (Xiamen University No. 202018 ). Supercomputing facilities were provided by Hefei Advanced Computing Center. Y. Su Acknowledge the ?Young Talent Support Plan? of Xi'an Jiaotong University and the Open Funds of State Key Laboratory of Physical Chemistry of Solid Surfaces (Xiamen University No. 202018). Supercomputing facilities were provided by Hefei Advanced Computing Center.

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published versionDefinitieve gepubliceerde versie, 4,3 MBLicentie: TAVERNE

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title = "A theoretical study on molybdenum and sulfur co-doped graphene for electrocatalytic nitrogen reduction",

abstract = "The electrocatalytic nitrogen reduction reaction (NRR) is a promising strategy to generate NH3 in mild condition. Herein, we designed four NRR single-atom catalysts to mimic the structures of FeMo-cofactor in nitrogenase, in which a Mo or Fe atom is anchored to sulfur doped graphene carbon nanosheets (Mo/Fe@S-gCNS). Density functional theory calculations were performed to investigate the stability of Mo/Fe@S-gCNS, as well as their NRR activity. The results suggest that Mo@S-gCNS coordinated with three S (Mo-S3) displays the best NRR catalytic activity among the four catalysts, and the NRR prefers to proceed through the enzymatic pathway with an overpotential as low as 0.24 V. The outstanding performance is mainly attribute to the appropriate coordination environment together with the intrinsic electronic structure of the embedded Mo atom. These findings contribute to designing the NRR single-atom catalysts and understanding the potential active sites of the FeMo-cofactor.",

keywords = "DFT, Graphene, Nitrogen reduction, Nitrogenase, Single-atom catalysts",

author = "Yanyang Qin and Shishi Zhang and Guoxin Gao and Shujiang Ding and Yaqiong Su",

note = "Funding Information: Y. Su Acknowledge the “Young Talent Support Plan” of Xi'an Jiaotong University and the Open Funds of State Key Laboratory of Physical Chemistry of Solid Surfaces (Xiamen University No. 202018 ). Supercomputing facilities were provided by Hefei Advanced Computing Center. ",

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doi = "10.1016/j.mcat.2021.112048",

language = "English",

volume = "517",

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AU - Zhang, Shishi

AU - Gao, Guoxin

AU - Ding, Shujiang

AU - Su, Yaqiong

N1 - Funding Information: Y. Su Acknowledge the “Young Talent Support Plan” of Xi'an Jiaotong University and the Open Funds of State Key Laboratory of Physical Chemistry of Solid Surfaces (Xiamen University No. 202018 ). Supercomputing facilities were provided by Hefei Advanced Computing Center.

PY - 2022/1

Y1 - 2022/1

N2 - The electrocatalytic nitrogen reduction reaction (NRR) is a promising strategy to generate NH3 in mild condition. Herein, we designed four NRR single-atom catalysts to mimic the structures of FeMo-cofactor in nitrogenase, in which a Mo or Fe atom is anchored to sulfur doped graphene carbon nanosheets (Mo/Fe@S-gCNS). Density functional theory calculations were performed to investigate the stability of Mo/Fe@S-gCNS, as well as their NRR activity. The results suggest that Mo@S-gCNS coordinated with three S (Mo-S3) displays the best NRR catalytic activity among the four catalysts, and the NRR prefers to proceed through the enzymatic pathway with an overpotential as low as 0.24 V. The outstanding performance is mainly attribute to the appropriate coordination environment together with the intrinsic electronic structure of the embedded Mo atom. These findings contribute to designing the NRR single-atom catalysts and understanding the potential active sites of the FeMo-cofactor.

AB - The electrocatalytic nitrogen reduction reaction (NRR) is a promising strategy to generate NH3 in mild condition. Herein, we designed four NRR single-atom catalysts to mimic the structures of FeMo-cofactor in nitrogenase, in which a Mo or Fe atom is anchored to sulfur doped graphene carbon nanosheets (Mo/Fe@S-gCNS). Density functional theory calculations were performed to investigate the stability of Mo/Fe@S-gCNS, as well as their NRR activity. The results suggest that Mo@S-gCNS coordinated with three S (Mo-S3) displays the best NRR catalytic activity among the four catalysts, and the NRR prefers to proceed through the enzymatic pathway with an overpotential as low as 0.24 V. The outstanding performance is mainly attribute to the appropriate coordination environment together with the intrinsic electronic structure of the embedded Mo atom. These findings contribute to designing the NRR single-atom catalysts and understanding the potential active sites of the FeMo-cofactor.

KW - DFT

KW - Graphene

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KW - Nitrogenase

KW - Single-atom catalysts

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A theoretical study on molybdenum and sulfur co-doped graphene for electrocatalytic nitrogen reduction

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