What Makes the Photocatalytic CO2 Reduction on N-Doped Ta2O5 Efficient: Insights from Nonadiabatic Molecular Dynamics.

摘要: Recent experimental studies demonstrated that photocatalytic CO2 reduction by Ru catalysts assembled on N-doped Ta2O5 surface is strongly dependent the nature of anchor group with which complexes are attached to substrate. We report a comprehensive atomistic analysis electron transfer dynamics in electroneutral Ru(di-X-bpy) (CO)2Cl2 X = COOH and PO3H2 N–Ta2O5 Nonadiabatic molecular simulations indicate faster anchors than groups, due larger nonadiabatic coupling. Quantum coherence counteracts this effect, however, small extent. The promotes significantly higher frequency modes PO3H2, both lighter atoms (C vs P) stronger bonds (double single). acceptor state delocalizes onto COOH, but not further favoring system. At same time, prone decom...