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 editors: Verma, Anand M.; Honkala, Karoliina; Melander, Marko M.
Journal or series: Frontiers in Energy Research
eISSN: 2296-598X
Publication year: 2021
Publication date: 02/02/2021
Volume: 8
Article number: 606742
Publisher: Frontiers Media SA
Publication country: Switzerland
Publication language: English
DOI: https://doi.org/10.3389/fenrg.2020.606742
Publication open access: Openly available
Publication channel open access: Open 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
Abstract
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.
Keywords: electrocatalysis; graphene; density functional theory
Free keywords: electrosorption; proton-coupled electron transfer
Contributing organizations
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Ministry reporting: Yes
VIRTA submission year: 2021
JUFO rating: 1