Boosting CO2 Electroreduction over a Cadmium Single‐Atom Catalyst by Tuning of the Axial Coordination Structure. (16th August 2021)

• Record Type: Journal Article
• Authors: Wu, Yahui; Chen, Chunjun; Yan, Xupeng; Sun, Xiaofu; Zhu, Qinggong; Li, Pengsong; Li, Yiming; Liu, Shoujie; Ma, Jingyuan; Huang, Yuying; Han, Buxing
• Is Part Of: Angewandte Chemie. Volume 133:Number 38(2021)
• Page Start: 20971
• Page End: 20978
• Publication Date: 2021-08-16
• Subjects: carbon dioxide -- electrocatalysis -- green chemistry -- ionic liquids -- single-atom catalysts; Chemistry -- Periodicals; 540
• DOI: 10.1002/ange.202105263
• Languages: English
• ISSNs: 0044-8249

Abstract

Abstract: Guided by first‐principles calculations, it was found that Cd single‐atom catalysts (SACs) have excellent performance in activating CO2, and the introduction of axial coordination structure to Cd SACs cannot only further decrease the free energy barrier of CO2 reduction, but also suppress the hydrogen evolution reaction (HER). Based on the above discovery, we designed and synthesized a novel Cd SAC that comprises an optimized CdN4 S1 moiety incorporated in a carbon matrix. It was shown that the catalyst exhibited outstanding performance in CO2 electroreduction to CO. The faradaic efficiency (FE) of CO could reach up to 99.7 % with a current density of 182.2 mA cm −2 in a H‐type electrolysis cell, and the turnover frequency (TOF) value could achieve 73000 h −1, which was much higher than that reported to date. This work shows a successful example of how to design highly efficient catalysts guided by theoretical calculations. Abstract : Cd single‐atom catalysts (SACs) with an optimized CdN4 S1 moiety were designed and prepared. The faradaic efficiency (FE) of CO reached 99.7 % with a current density of 182.2 mA cm −2, and the TOF of CO production was as high as 73000 h −1 . Cd SACs are effective for reduction of CO2 to CO. Introduction of an axial coordination structure boosts the activity of CO2 RR and also enhances the selectivity of CO2 RR by suppressing the adsorption of *H.