Electrochemical reduction of CO2 (CO2RR) using renewable electricity has emerged as an attractive approach to synthesize hydrocarbons and mitigate atmospheric CO2 concentration. Carbon-based materials have recently attracted a particular attention as electrocatalysts for CO2RR due to their extraordinary properties such as low cost and flexibility in tuning the morphology and electronic structure. A wide range of different N-doped carbon materials have been experimentally tested and reported for CO2RR. The performance map for CO2RR over these materials presents diverse activities and in most cases the major product of the CO2 reduction is found to be CO. Using density functional theory (DFT) calculations we study a wide range of different possible active motifs in the defective carbon materials to rationalize the associated trends in their intrinsic activities. We investigate both CO2RR and hydrogen evolution reaction (HER) activity and identify several active motifs that are expected to exhibit a comparable or even better activity to the state-of-the-art gold catalyst. Several configurations are suggested to be selective for CO2RR over HER. This study provides insights in the nature of active and selective motifs for CO2RR and rationalizes a number of reports in the literature.2 We also show that in the presence of metal impurities activity and selectivity can be significantly improved.

Designing carbon-based materials for effective electrochemical reduction of CO2

255th National Meeting (2018)

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