Periodic Defect Engineering of Iron–Nitrogen–Carbon Catalysts for Nitrate Electroreduction to Ammonia

Runxi Zhu; Yanyang Qin; Tiantian Wu; Shujiang Ding; Yaqiong Su

doi:10.1002/smll.202307315

Periodic Defect Engineering of Iron–Nitrogen–Carbon Catalysts for Nitrate Electroreduction to Ammonia

Runxi Zhu, Yanyang Qin, Tiantian Wu, Shujiang Ding, Yaqiong Su (Corresponding author)

Inorganic Materials & Catalysis

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

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Iron–nitrogen–carbon single atom catalyst (SAC) is regarded as one of the promising electrocatalysts for NO₃⁻ reduction reaction (NO₃RR) to NH₃ due to its high activity and selectivity. However, synergistic effects of topological defects and FeN₄ active moiety in Fe–N–C SAC have rarely been investigated. By performing density functional theory (DFT) calculations, 13 defective graphene FeN₄ with 585, 484, and 5775 topological line defects are constructed, yielding 585-68-FeN₄ with optimal NO₃RR catalytic activity, high selectivity, as well as robust anti-dissolution stability. The high NO₃RR activity on 585-68-FeN₄ is well explained by the high valence state of Fe center as well as asymmetric charge distribution on FeN₄ moiety influenced by 5- and 8-member rings. This DFT work provides theoretical guidance for engineering NO₃RR performance of iron–nitrogen–carbon catalysts by modulating periodic topological defects.

Originele taal-2	Engels
Artikelnummer	2307315
Aantal pagina's	9
Tijdschrift	Small
Volume	20
Nummer van het tijdschrift	8
Vroegere onlinedatum	12 okt. 2023
DOI's	https://doi.org/10.1002/smll.202307315
Status	Gepubliceerd - 22 feb. 2024

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

Financiers	Financiernummer
Xi’an Jiaotong University

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title = "Periodic Defect Engineering of Iron–Nitrogen–Carbon Catalysts for Nitrate Electroreduction to Ammonia",

abstract = "Iron–nitrogen–carbon single atom catalyst (SAC) is regarded as one of the promising electrocatalysts for NO3− reduction reaction (NO3RR) to NH3 due to its high activity and selectivity. However, synergistic effects of topological defects and FeN4 active moiety in Fe–N–C SAC have rarely been investigated. By performing density functional theory (DFT) calculations, 13 defective graphene FeN4 with 585, 484, and 5775 topological line defects are constructed, yielding 585-68-FeN4 with optimal NO3RR catalytic activity, high selectivity, as well as robust anti-dissolution stability. The high NO3RR activity on 585-68-FeN4 is well explained by the high valence state of Fe center as well as asymmetric charge distribution on FeN4 moiety influenced by 5- and 8-member rings. This DFT work provides theoretical guidance for engineering NO3RR performance of iron–nitrogen–carbon catalysts by modulating periodic topological defects.",

keywords = "density functional theory, electrocatalysts, iron–nitrogen–carbon, nitrate reduction reaction, periodic topological defects",

author = "Runxi Zhu and Yanyang Qin and Tiantian Wu and Shujiang Ding and Yaqiong Su",

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AU - Zhu, Runxi

AU - Qin, Yanyang

AU - Wu, Tiantian

AU - Ding, Shujiang

AU - Su, Yaqiong

PY - 2024/2/22

Y1 - 2024/2/22

N2 - Iron–nitrogen–carbon single atom catalyst (SAC) is regarded as one of the promising electrocatalysts for NO3− reduction reaction (NO3RR) to NH3 due to its high activity and selectivity. However, synergistic effects of topological defects and FeN4 active moiety in Fe–N–C SAC have rarely been investigated. By performing density functional theory (DFT) calculations, 13 defective graphene FeN4 with 585, 484, and 5775 topological line defects are constructed, yielding 585-68-FeN4 with optimal NO3RR catalytic activity, high selectivity, as well as robust anti-dissolution stability. The high NO3RR activity on 585-68-FeN4 is well explained by the high valence state of Fe center as well as asymmetric charge distribution on FeN4 moiety influenced by 5- and 8-member rings. This DFT work provides theoretical guidance for engineering NO3RR performance of iron–nitrogen–carbon catalysts by modulating periodic topological defects.

AB - Iron–nitrogen–carbon single atom catalyst (SAC) is regarded as one of the promising electrocatalysts for NO3− reduction reaction (NO3RR) to NH3 due to its high activity and selectivity. However, synergistic effects of topological defects and FeN4 active moiety in Fe–N–C SAC have rarely been investigated. By performing density functional theory (DFT) calculations, 13 defective graphene FeN4 with 585, 484, and 5775 topological line defects are constructed, yielding 585-68-FeN4 with optimal NO3RR catalytic activity, high selectivity, as well as robust anti-dissolution stability. The high NO3RR activity on 585-68-FeN4 is well explained by the high valence state of Fe center as well as asymmetric charge distribution on FeN4 moiety influenced by 5- and 8-member rings. This DFT work provides theoretical guidance for engineering NO3RR performance of iron–nitrogen–carbon catalysts by modulating periodic topological defects.

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Periodic Defect Engineering of Iron–Nitrogen–Carbon Catalysts for Nitrate Electroreduction to Ammonia

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