Controllable Cu0‐Cu+ Sites for Electrocatalytic Reduction of Carbon Dioxide. Issue 28 (9th June 2021)

• Record Type: Journal Article
• Authors: Yuan, Xintong; Chen, Sai; Cheng, Dongfang; Li, Lulu; Zhu, Wenjin; Zhong, Dazhong; Zhao, Zhi‐Jian; Li, Jingkun; Wang, Tuo; Gong, Jinlong
• Is Part Of: Angewandte Chemie international edition. Volume 60:Issue 28(2021)
• Page Start: 15344
• Page End: 15347
• Publication Date: 2021-06-09
• Subjects: C−C coupling -- CO2 activation -- CO2 electrochemical reduction -- Cu0-Cu+ pairs -- synergistic effect; Chemistry -- Periodicals; 540
• DOI: 10.1002/anie.202105118
• Languages: English
• ISSNs: 1433-7851

Abstract

Abstract: Cu‐based electrocatalysts facilitate CO2 electrochemical reduction (CO2 ER) to produce multi‐carbon products. However, the roles of Cu 0 and Cu + and the mechanistic understanding remain elusive. This paper describes the controllable construction of Cu 0 ‐Cu + sites derived from the well‐dispersed cupric oxide particles supported on copper phyllosilicate lamella to enhance CO2 ER performance. 20 % Cu/CuSiO3 shows the superior CO2 ER performance with 51.8 % C2 H4 Faraday efficiency at −1.1 V vs reversible hydrogen electrode during the 6 hour test. In situ attenuated total reflection infrared spectra and density functional theory (DFT) calculations were employed to elucidate the reaction mechanism. The enhancement in CO2 ER activity is mainly attributed to the synergism of Cu 0 ‐Cu + pairs: Cu 0 activates CO2 and facilitates the following electron transfers; Cu + strengthens *CO adsorption to further boost C−C coupling. We provide a strategy to rationally design Cu‐based catalysts with viable valence states to boost CO2 ER. Abstract : Controllable Cu 0 ‐Cu + pairs derived from the well‐dispersed cupric oxide supported on copper phyllosilicate lamella can break thermodynamic and kinetic limitations of CO2 reduction reaction and achieve the superior CO2 electroreduction performance.