Graphical Abstract
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Designing catalysts with highly active, selectivity, and stability for electrocatalytic CO2 to formate is currently a severe challenge. Herein, we developed an electronic structure engineering on carbon nano frameworks embedded with nitrogen and sulfur asymmetrically dual-coordinated indium active sites toward the efficient electrocatalytic CO2 reduction reaction. As expected, atomically dispersed In-based catalysts with In-S1N3 atomic interface with asymmetrically coordinated exhibited high efficiency for CO2 reduction reaction (CO2RR) to formate. It achieved a maximum Faradaic efficiency (FE) of 94.3% towards formate generation at −0.8 V vs. reversible hydrogen electrode (RHE), outperforming that of catalysts with In-S2N2 and In-N4 atomic interface. And at a potential of −1.10 V vs. RHE, In-S1N3 achieves an impressive Faradaic efficiency of 93.7% in flow cell. The catalytic performance of In-S1N3 sites was confirmed to be enhanced through in-situ X-ray absorption near-edge structure (XANES) measurements under electrochemical conditions. Our discovery provides the guidance for performance regulation of main group metal catalysts toward CO2RR at atomic scale.
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