Well-defined asymmetric nitrogen/carbon-coordinated single metal sites for carbon dioxide conversion
Journal of colloid and interface science(2024)
Abstract
Asymmetric nitrogen/carbon-coordinated single metal sites (M-NxC4-x) outperform symmetric M-N4 sites in carbon dioxide (CO2) electroreduction. However, the challenge of crafting well-defined M-NxC4-x sites complicates the understanding of their structure-catalytic performance relationship. In this study, we employ metallized N-confused tetraphenylporphyrin (M-NCTPP) to investigate CO2 conversion on M-N3C1 sites using both density functional theory and experimental methods. The optimal cobalt (Co)-N3C1 site (Co-NCTPP) achieves a current density of 500 mA cm−2 and a carbon monoxide Faraday efficiency exceeding 90 % at −1.25 V vs. the reversible hydrogen electrode, surpassing the performance of Co-N4 (Co-TPP). This research introduces a novel approach for designing and synthesizing high-activity heteroatom-anchored single metal sites, advancing fundamental understanding in the field.
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Key words
Nitrogen/carbon-coordinated single metal sites,Nitrogen-confused tetraphenylporphyrin,Carbon dioxide electroreduction,Density functional theory calculations,Structure-property relationship
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