Saturated Coordination LuN<sub>6</sub> Defect Sites for Highly Efficient Electroreduction of CO<sub>2</sub>
Luliang Liao, Guomin Xia, Fuqing Yu, Xian Liu, Minxing Shu, Guangyao Zhang, Xianshi Zeng, Hongming Wang
Abstract
Abstract Metal single‐atom and internal structural defects typically coexist in M–N–C materials obtained through the existing basic pyrolysis processes. Identifying a correlation between them to understand the structure–activity relationship and achieve efficient catalytic performance is important, particularly for the rare‐earth (RE) elements with rich electron orbitals and strong coordination capabilities. Herein, a novel single‐atom catalyst based on the RE element lutetium is successfully synthesized on a N–C support. Structural and simulation analyses demonstrate that the formation of a LuN 6 structural site with an individual defect because of pyrolysis is thermodynamically favorable in Lu–N–C. Using KHCO 3 ‐based electrolytes facilitates the fall of the K + cations into the defective sites of Lu–N–C, thus enabling improved CO 2 capture and activation, which increases the catalyst conductivity for Lu–N–C. In this study, the catalyst exhibits a Faradaic efficiency of 95.1% for CO at a current density of 18.2 mA cm −2 during carbon dioxide reduction reaction. This study thus provides new insights into understanding RE–N–C materials for energy utilization.