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author:

Liu, Hongling (Liu, Hongling.) [1] | Yu, Zhichao (Yu, Zhichao.) [2] | Zhao, Jia (Zhao, Jia.) [3] | Ip, Weng Fai (Ip, Weng Fai.) [4] | Lin, Sen (Lin, Sen.) [5] | Pan, Hui (Pan, Hui.) [6]

Indexed by:

SCIE

Abstract:

Dual-atom catalysts (DACs) embedded in nitrogen-doped graphene have been widely studied for electrochemical CO2 reduction (CO2R), primarily yielding CO. However, achieving selectivity for C1 hydrocarbons remains challenging. Here, 32 Janus DACs (J-M'M) are designed and investigated for CO2R using density functional theory (DFT) calculations, identifying 13 capable of producing methanol and methane. Notably, J-FeCo and J-CoNi exhibit favorable limiting potentials (-0.38 and -0.45 V vs. RHE) for CH3OH and CH4 production, respectively, based on constant-potential calculations. Compared to normal DACs (N-M'M), Janus DACs demonstrate enhanced initial CO2 hydrogenation and stronger CO adsorption. Oxygen coordination in J-FeCo and J-CoNi induces a downshift/upshift of majority-/minority-spin energy levels of d(z2), d(yz), and d(xz) orbitals toward the Fermi level relative to N-FeCo and N-CoNi, strengthening the bonding state and weakening the antibonding state, thereby improving CO adsorption. Furthermore, an effective descriptor based on atomic features is identified to evaluate *CO binding strength. This work highlights the critical role of partial oxygen coordination in DACs for C1 hydrocarbons production and proposes a robust descriptor to guide the design of related catalysts.

Keyword:

CO2 electroreduction density functional theory descriptor Janus dual-atom catalysts methane methanol

Community:

  • [ 1 ] [Liu, Hongling]Univ Macau, Inst Appl Phys & Mat Engn, Macau 999708, Peoples R China
  • [ 2 ] [Yu, Zhichao]Univ Macau, Inst Appl Phys & Mat Engn, Macau 999708, Peoples R China
  • [ 3 ] [Pan, Hui]Univ Macau, Inst Appl Phys & Mat Engn, Macau 999708, Peoples R China
  • [ 4 ] [Ip, Weng Fai]Univ Macau, Fac Sci & Technol, Dept Phys & Chem, Macau 999078, Peoples R China
  • [ 5 ] [Pan, Hui]Univ Macau, Fac Sci & Technol, Dept Phys & Chem, Macau 999078, Peoples R China
  • [ 6 ] [Zhao, Jia]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China
  • [ 7 ] [Lin, Sen]Fuzhou Univ, Coll Chem, State Key Lab Photocatalysis Energy & Environm, Fuzhou 350116, Peoples R China

Reprint 's Address:

  • [Pan, Hui]Univ Macau, Inst Appl Phys & Mat Engn, Macau 999708, Peoples R China;;[Ip, Weng Fai]Univ Macau, Fac Sci & Technol, Dept Phys & Chem, Macau 999078, Peoples R China;;[Pan, Hui]Univ Macau, Fac Sci & Technol, Dept Phys & Chem, Macau 999078, Peoples R China

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Source :

ADVANCED SCIENCE

Year: 2025

1 4 . 3 0 0

JCR@2023

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ESI Highly Cited Papers on the List: 0 Unfold All

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30 Days PV: 0

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