A1 Journal article (refereed)
Computational Screening of Doped Graphene Electrodes for Alkaline CO2 Reduction (2021)

Verma, A. M., Honkala, K., & Melander, M. M. (2021). Computational Screening of Doped Graphene Electrodes for Alkaline CO2 Reduction. Frontiers in Energy Research, 8, Article 606742. https://doi.org/10.3389/fenrg.2020.606742

JYU authors or editors

Publication details

All authors or editorsVerma, Anand M.; Honkala, Karoliina; Melander, Marko M.

Journal or seriesFrontiers in Energy Research


Publication year2021

Publication date02/02/2021


Article number606742

PublisherFrontiers Media SA

Publication countrySwitzerland

Publication languageEnglish


Publication open accessOpenly available

Publication channel open accessOpen Access channel

Publication is parallel published (JYX)https://jyx.jyu.fi/handle/123456789/74511

Web address of parallel published publication (pre-print)https://chemrxiv.org/articles/preprint/Computational_Screening_of_Doped_Graphene_Electrodes_for_Alkaline_CO2_Reduction/12958226


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.

Keywordselectrocatalysisgraphenedensity functional theory

Free keywordselectrosorption; proton-coupled electron transfer

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Ministry reportingYes

Reporting Year2021

JUFO rating1

Last updated on 2024-03-04 at 20:06