Executive Summary : | The transformation of CO2 into a reduced form, leading to value-added products, is crucial for economic and environmental reasons. However, activating CO2 towards hydrogenation is challenging due to its kinetic inertness and thermodynamic stability. Transition metal catalysts have shown promising results in reducing CO2, but high temperature and pressure conditions are needed for the reaction. Researchers are working on designing an efficient catalyst that can activate CO2 towards hydrogenation at ambient conditions. Uncertainty remains regarding the reaction mechanism due to the lack of experimental evidence on the isolation and characterization of key intermediates involved in the CO2 hydrogenation reaction in the condensed phase. Recent experimental efforts have focused on understanding the reactivity of CO2 with gas-phase transition metal clusters, such as PtH3-, FeH-, Cu1,2H2, PdCuH4-, and PdH-. However, there is a lack of computational studies on the dynamics and kinetics associated with the CO2 hydrogenation reaction mediated by transition metal clusters. State-of-the-art computer simulation studies are needed to shed light on the atomistic details of the reaction mechanism. Additionally, understanding the role of the fluxional character of metal clusters in dictating reactivity towards CO2 is essential. Furthermore, understanding the intra-molecular vibrational energy redistribution (IVR) process during the title reaction is crucial for identifying key normal modes facilitating the title reaction and enhancing the efficiency of the catalyst. It is also important to verify whether the kinetics of the title reaction can be described within the Rice-Ramsperger-Kassel-Marcus (RRKM) theory. |