Application of atomic-scale mechanistic insights into carbon-catalyzed N2O reduction for kinetic modeling construction

To achieve the collaborative elimination of N 2 O and carbon of potent greenhouse pollutants from automotive mobile sources, a chemical kinetic model is developed to accurately track the heterogeneous process of carboncatalyzed N 2 O reduction based on density functional theory, with experimental data used to validate the model ' s reliability. The influence of carbon structure, site density, and surface chemical properties on N 2 O catalytic reduction can be analyzed within this system. Results reveal that the free -edge site of carbon accurately describes the catalytic reduction process of N 2 O. Adsorption of N 2 O to carbon edges in O -down, N -down, or parallel orientations exhibits an exothermic process with energy barriers. The N 2 O with O -down reduction pathway predominates due to the limitations imposed by the unitary carbon site. As the number of active carbon atoms at carbon edges increases, the N 2 O reaction mode tends towards parallel and N -down pathways, resulting in a significant enhancement of N 2 O conversion rates and a reduction in catalytic temperatures, with the lowest achievable temperature being 300 K. Furthermore, the triplet carbon structure exhibits higher efficiency in N 2 O catalytic reduction compared to the singlet carbon structure, achieving a remarkable N 2 O conversion rate of 93.8 % within the typical temperature exhaust window of diesel engines. This study supplies a breakthrough for carbon materials as catalysts for achieving high N 2 O conversion rates at low cost, which is important for the collaborative catalytic elimination of N 2 O and carbon black pollutants.