Asymmetrically coordinated main group atomic In-S1N3 interface sites for promoting electrochemical CO2 reduction
Yan Gao, Jinlong Ge, Jingqiao Zhang, Ting Cao, Zhiyi Sun, Wensheng Yan, Yu Wang, Jie Lin, Wenxing Chen, Zheng Liu
Abstract
Designing catalysts with highly active, selectivity, and stability for electrocatalytic CO 2 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 CO 2 reduction reaction. As expected, atomically dispersed In-based catalysts with In-S 1 N 3 atomic interface with asymmetrically coordinated exhibited high efficiency for CO 2 reduction reaction (CO 2 RR) 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-S 2 N 2 and In-N 4 atomic interface. And at a potential of −1.10 V vs. RHE, In-S 1 N 3 achieves an impressive Faradaic efficiency of 93.7% in flow cell. The catalytic performance of In-S 1 N 3 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 CO 2 RR at atomic scale.