A DFT study of carbon dioxide reduction catalyzed by group 3 metal complexes of silylamides

Abstract

The catalytic conversion of carbon dioxide into clean fuel and value-added chemicals is one of best ways to resolve the issues of greenhouse-gas emission and worldwide energy shortage and to benefit sustainable development of society. Our DFT calculations demonstrate that group 3 metal silylamides are able to accomplish the CO2 reduction reaction, where the scandium one bears the best catalytic activity. It requires very small positive free energy to capture CO2. The subsequent hydrogenation reactions are thermodynamically and kinetically favored, where the transition state (*CO2H2)# costs 4.7 kcal/mol energy. Comparatively, the water elimination requires to absorb less energy.