Controllable Cu<sup>0</sup>‐Cu<sup>+</sup> Sites for Electrocatalytic Reduction of Carbon Dioxide
Xintong Yuan, Sai Chen, Dongfang Cheng, Lulu Li, Wenjin Zhu, Dazhong Zhong, Zhi‐Jian Zhao, Jingkun Li, Tuo Wang, Jinlong Gong
Abstract
Abstract Cu‐based electrocatalysts facilitate CO 2 electrochemical reduction (CO 2 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 CO 2 ER performance. 20 % Cu/CuSiO 3 shows the superior CO 2 ER performance with 51.8 % C 2 H 4 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 CO 2 ER activity is mainly attributed to the synergism of Cu 0 ‐Cu + pairs: Cu 0 activates CO 2 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 CO 2 ER.