Lanthanide single-atom catalysts for efficient CO2-to-CO electroreduction

• Published in: Nature communications Vol. 16; no. 1; pp. 2985 - 10
• Main Authors: Wang, Qiyou, Luo, Tao, Cao, Xueying, Gong, Yujie, Liu, Yuxiang, Xiao, Yusen, Li, Hongmei, Gröbmeyer, Franz, Lu, Ying-Rui, Chan, Ting-Shan, Ma, Chao, Liu, Kang, Fu, Junwei, Zhang, Shiguo, Liu, Changxu, Lin, Zhang, Chai, Liyuan, Cortes, Emiliano, Liu, Min
• Format: Journal Article
• Language: English
• Published: London Nature Publishing Group UK 27.03.2025; Nature Publishing Group; Nature Portfolio
• Subjects: 119/118; 140/133; 140/146; 147/143; 639/301/299/886; 639/638/675; 639/638/77/885; 639/925/357/995; Absorption spectroscopy; Adsorption; Carbon dioxide; Carbon monoxide; Catalysts; Chemical reduction; Density functional theory; Efficiency; Electrowinning; Energy conversion efficiency; Energy efficiency; Erbium; Humanities and Social Sciences; multidisciplinary; Science; Science (multidisciplinary); Single atom catalysts; Spectrum analysis; X ray absorption; X-ray absorption spectroscopy
• ISSN: 2041-1723; 2041-1723
• DOI: 10.1038/s41467-025-57464-8

Single-atom catalysts (SACs) have received increasing attention due to their 100% atomic utilization efficiency. The electrochemical CO 2 reduction reaction (CO 2 RR) to CO using SAC offers a promising approach for CO 2 utilization, but achieving facile CO 2 adsorption and CO desorption remains challenging for traditional SACs. Instead of singling out specific atoms, we propose a strategy utilizing atoms from the entire lanthanide (Ln) group to facilitate the CO 2 RR. Density functional theory calculations, operando spectroscopy, and X-ray absorption spectroscopy elucidate the bridging adsorption mechanism for a representative erbium (Er) single-atom catalyst. As a result, we realize a series of Ln SACs spanning 14 elements that exhibit CO Faradaic efficiencies exceeding 90%. The Er catalyst achieves a high turnover frequency of ~130,000 h − 1 at 500 mA cm − 2 . Moreover, 34.7% full-cell energy efficiency and 70.4% single-pass CO 2 conversion efficiency are obtained at 200 mA cm − 2 with acidic electrolyte. This catalytic platform leverages the collective potential of the lanthanide group, introducing new possibilities for efficient CO 2 -to-CO conversion and beyond through the exploration of unique bonding motifs in single-atom catalysts. Single atom catalysts offer a promising approach for CO 2 electroreduction to CO, but achieving high efficiency remains challenging. Here, the authors report lanthanide single atom catalysts with the transition ability from bridge to linear adsorption that exhibit efficient CO production.