Proceedings of nanoGe Fall Meeting 2021 (NFM21)
DOI: https://doi.org/10.29363/nanoge.nfm.2021.086
Publication date: 23rd September 2021
Recently, carbon-based catalyst materials doped with nitrogen and transition metals (MNC) have emerged as a selective and cost-efficient alternative to metal catalysts for the of CO2 electrochemical reduction (CO2RR). [1] Usually, these solid catalysts are prepared using heat treatment of a carbon precursor, nitrogen containing compounds and inorganic salts to form different nitrogen functionalities, which coordinated to the metal centers resulting catalytically active MNx single sites.These different functionalities tend to be non uniformly distributed making it challenging to establish the correlations between the structure and the catalytic activity
To address these challenges, we have prepared polyanilline derived MNC catalysts and observed that the catalytic performance of MNCs toward the CO2RR is affected by the structure and composition of the catalyst and by the conditions of the catalytic process. In particular, we observe that the metal center plays a crucial role in activity and selectivity of the process. While N functionalities do have some activity, MNx moieties play a predominant role and a higher concentration of FeNx correlates with higher partial current densities towards CO production. [2]
In addition to the catalyst structure and composition the reaction conditions also play a crucial role in determining the reaction’s selectivity. In particular, the pH can be used to tune the ratio of the different products. [3] For a polyaniline derived FeNC catalyst it was observed that hydrogen formation was strongly dependent on pH, while the CO production was not affected, resulting in high selectivities toward CO at high local pH values. Nevertheless, working in the absence of protons (in a non-protic electrolyte) resulted in the suppression of both the HER and the CO2RR, as both reactions require protons. We found that adding small amounts of water enhances the CO2RR while keeping the HER low, showing that there is an optimal proton concentration to ensure a high activity and selectivity.
This work was supported by the Mexican council of Science and Technology (SEP-CONACyT) through the project No 282552
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