Mechanistic insights into PtN/MoS2 catalyzed CO2 hydrogenation to methanol: A first-principles study

The exploration and development of suitable catalysts for selective hydrogenation of CO2 to chemicals with industrial value has great significance for CO2 conversion and utilization. Herein, Pt-N/MoS2 (N = 1-12) is used as a typical example to establish a catalyst model that CO2 gas is efficiently catalyzed to industrial CH3OH by first-principles calculations. The highly selective catalysis for CO2 to CH3OH is attributed to the dynamic evolution of the geometry and the effective transfer of charge between Pt-N/MoS2 and reactant. The rate-determining step in the whole reaction process is formation of CH3OH by CH2OH & lowast; hydrogenation, the highest barrier to be overcome is only 0.55 eV. The important conclusions in this paper can provide a theoretical basis for the design and development of highly efficient supported metal cluster catalysts for CO2 hydrogenation.