Design of a CO Oxidation Catalyst Based on Two-Dimensional MnO₂

Two-dimensional (2D) MnO 2 monolayer can be prepared by delamination of a layered manganese oxide. Herein, for the first time, we design a 2D MnO 2 -based catalyst for CO oxidation reaction through density functional theory calculations. We found that pristine MnO 2 sheet does not exhibit high catalytic activity for CO oxidation, while active sites can be created by doping MnO 2 with transition metal elements. We examined the effects of substitutional doping of MnO 2 with Ru, Rh, Pd, Pt, and Au. The calculated energetic profiles of CO oxidation suggest that the reaction proceed very facile with a Mars–van Krevelen mechanism on Ru-doped MnO 2 monolayer, while it is less likely to occur for other doped systems including Rh, Pd, Pt, and Au as well as the pristine MnO 2 . The discrepancy of catalytic activities is rationalized by electronic structure calculations. We expect this study can shed light on the development of low-temperature CO oxidation catalysts.