Homonuclear multi-atom catalysts for CO electroreduction: a comparison density functional theory study with their single-atom counterparts

• Published in: Journal of materials chemistry. A, Materials for energy and sustainability Vol. 11; no. 46; pp. 25662 - 2567
• Main Authors: Xiao, Jingjing, Liu, Ziyang, Wang, Xinshuang, Li, Fengyu, Zhao, Zhonglong
• Format: Journal Article
• Published: 28.11.2023
• ISSN: 2050-7488; 2050-7496
• DOI: 10.1039/d3ta05498e

The development of efficient electrocatalysts for the CO 2 reduction reaction (CO 2 RR) is essential to mitigate global energy and environmental problems. Single-atom catalysts (SACs) have become an emerging frontier in the CO 2 RR because of the high utilization of noble metals, but they suffer from poor selectivity toward high-order hydrocarbons. Herein, using density functional theory calculations, we predict that homonuclear double-atom and triple-atom catalysts supported by two-dimensional Mo 2 CO 2 exhibit superior catalytic performance for the CO 2 RR compared to their single-atom counterparts. We show that the multi-nuclear reaction centers on multi-atom catalysts boost the adsorption of key CO 2 RR intermediates, such as *HCOO and *CH, enabling selective reduction toward the CH 4 product at ultralow overpotentials. Besides, C-C coupling can also be facilitated on multi-nuclear sites, which enables an efficient production of the C 2 H 5 OH product. This work lays a foundation for the future development of multi-atom catalysts for the CO 2 RR. Multi-nuclear reaction centers on homonuclear multi-atom catalysts are designed to boost the CO 2 RR, outperforming their single-atom counterparts.