Activation of Nitrogen-Doped Carbon Materials on the C–N Bond and C–O Bond: Modeling Study Toward Enhanced Pyrolysis Products

The present study investigated the effects of doped nitrogen atoms in carbon materials on the hydrodeoxygenation (HDO) and hydrodenitrogenation (HDN) processes. Density functional theory was used to evaluate the structural stability and catalytic activity of different nitrogen-doped carbon cluster models for HDO and HDN reactions. The results showed that the carbon atom near the nitrogen in graphite is the active center of nitrogen-doped carbon catalytic activation of hydrogen. In the H2-rich system, N@C catalysts can not only activate hydrogen molecules but also directly break the C–O/C–N bond. Results confirmed that the nitrogen assembly structure can affect the performance of C–O/C–N bond activation, and meta-doping nitrogen sites have the highest catalytic activity. This study provides theoretical guidance and views for the development of high-performance carbon catalysts that can replace conventional metal catalysts.