Construction of a BC 3 -based TM single-atom catalyst for efficient reduction of CO 2 to CH 4 : a computational study.

The electrocatalytic conversion of CO 2 into fuels or chemicals presents an effective approach to mitigate greenhouse gas emissions and address the traditional fuel crisis. Based on density functional theory, we systematically investigate a series of transition metal atoms bound to a BC 3 monolayer as novel single-atom catalysts (SACs) for the CO 2 reduction reaction (CO 2 RR). Our results demonstrate that most of the constructed SACs exhibit superior selectivity for the CO 2 RR over the hydrogen evolution reaction, with CH 4 as the dominant product. Notably, the Pt@BC 3 monolayer emerges as the best CO 2 RR catalyst with a low limiting potential of -0.36 V, surpassing many previously reported catalysts. Additionally, we explore the correlations between the SAC's catalytic activity and both Δ G *OCHO and the structural descriptor φ , revealing volcano relationships. A catalyst with better performance is constructed with the aid of the volcano diagram. These findings are beneficial for understanding the CO 2 RR mechanism and designing efficient catalysts.