Asymmetrically coordinated main group atomic In-S1N3 interface sites for promoting electrochemical CO2 reduction

作者：Yan Gao, Jinlong Ge, Jingqiao Zhang, Ting Cao, Zhiyi Sun, Wensheng Yan, Yu Wang, Jie Lin, Wenxing Chen, Zheng Liu · 发表于：Nano Research · 年份：2024 · DOI：10.1007/s12274-024-6513-9 · 被引用次数：16 · 研究领域：CO2 Reduction Techniques and Catalysts、Advanced Photocatalysis Techniques、Electrocatalysts for Energy Conversion

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.