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

Verma, Anand
Honkala, Karoliina
Melander, Marko

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

Fields of science: