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Computational Screening of Doped Graphene Electrodes for Alkaline CO2 Reduction

preprint
submitted on 15.09.2020 and posted on 17.09.2020 by Anand Mohan Verma, Karoliina Honkala, Marko Melander
The electrocatalytic CO2 reduction reaction (CO2RR) is considered as one of the most promising approaches to synthesizing carbonaceous fuels and chemicals without utilizing fossil resources. However, current technologies are still in the early phase focusing primarily on identifying optimal electrode materials and reaction conditions. Doped graphene-based materials are among the best CO2RR electrocatalysts and in the present work we have performed a computational screening study to identify suitable graphene catalysts for CO2RR to CO under alkaline conditions. Several types of modified-graphene frameworks doped with metallic and non-metallic elements were considered. After establishing thermodynamically stable electrodes, the electrochemical CO2RR to CO is studied in the alkaline media. Both concerted proton-coupled electron transfer (PCET) and decoupled proton and electron transfer (ETPT) mechanisms were considered by developing and using a generalization of the computational hydrogen electrode approach. It is established that the CO2 electrosorption and associated charge transfer along the ETPT pathway are of utmost importance and significantly impact the electrochemical thermodynamics of CO2RR. Our study suggests an exceptional performance of metal-doped nitrogen-coordinated graphene electrodes, especially 3N-coordinated graphene electrodes.

Funding

Koctails - Kinetics of charge-transfer at liquid-solid interfaces: Basic mechanisms in electrochemical energy production and storage

Academy of Finland

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Catalytic and electrocatalytic oxidation of biomass-derived polyols at the liquid-solid interfaces

Academy of Finland

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History

Email Address of Submitting Author

marko.m.melander@jyu.fi

Institution

Nanoscience Center, Department of Chemistry, University of Jyväskylä

Country

Finland

ORCID For Submitting Author

0000-0001-7111-1603

Declaration of Conflict of Interest

None

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