ClAg<sub>14</sub>(C≡C<sup>t</sup>Bu)<sub>12</sub> Nanoclusters as Efficient and Selective Electrocatalysts Toward Industrially Relevant CO<sub>2</sub> Conversion
Hoeun Seong, Kiyoung Chang, Fang Sun, Sojung Lee, Sang Myeong Han, Yujin Kim, Chang Hyuck Choi, Qing Tang, Dongil Lee
Abstract
Abstract Atomically precise metal nanoclusters (NCs) have emerged as a promising frontier in the field of electrochemical CO 2 reduction reactions (CO 2 RR) because of their distinctive catalytic properties. Although numerous metal NCs are developed for CO 2 RR, their use in practical applications has suffered from their low‐yield synthesis and insufficient catalytic activity. In this study, the large‐scale synthesis and electrocatalytic performance of ClAg 14 (C≡C t Bu) 12 + NCs, which exhibit remarkable efficiency in catalyzing CO 2 ‐to‐CO electroreduction with a CO selectivity of over 99% are reported. The underlying mechanisms behind this extraordinary CO 2 RR activity of ClAg 14 (C≡C t Bu) 12 + NCs are investigated by a combination of electrokinetic and theoretical studies. These analyses reveal that different active sites, generated through electrochemical activation, have unique adsorption properties for the reaction intermediates, leading to enhanced CO 2 RR and suppressed hydrogen production. Furthermore, industrially relevant CO 2 ‐to‐CO electroreduction using ClAg 14 (C≡C t Bu) 12 + NCs in a zero‐gap CO 2 electrolyzer, achieving high energy efficiency of 51% and catalyst activity of over 1400 A g −1 at a current density of 400 mA cm −2 is demonstrated.