Construction of a BC3-based TM single-atom catalyst for efficient reduction of CO2 to CH4: a computational study†
Abstract
The electrocatalytic conversion of CO2 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 BC3 monolayer as novel single-atom catalysts (SACs) for the CO2 reduction reaction (CO2RR). Our results demonstrate that most of the constructed SACs exhibit superior selectivity for the CO2RR over the hydrogen evolution reaction, with CH4 as the dominant product. Notably, the Pt@BC3 monolayer emerges as the best CO2RR 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 ΔG*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 CO2RR mechanism and designing efficient catalysts.