Exploring the computational aspects of propylene oligomerization catalysis using Fe2M type trimetallic MOF nodes

Metal-organic frameworks (MOFs) have emerged as promising materials in the field of catalysis. They offer an optimal ground for screening catalysts and tailoring their catalytic properties. In this work, we investigate the catalytic activity of the propylene oligomerization reaction on the trimetallic MOF nodes, Fe2Ni, by varying the active metal Ni with other 3d-transition metals ranging from Sc to Cu, aiming to grasp the impact of altering the active atoms on the catalyst’s activity. Additionally, we examined how substituting the spectator atom, Fe, in Fe2Ni with other transition metals, i.e., from Sc to Cu, affects these energy barriers. In addition, we found a correlative relationship between spin-density from natural population analysis and energy barriers in the realm of C-C bond formation, whereby an elevation in spin density is found to be inversely proportional to the magnitude of energy barriers. Moreover, we calculated the energy barriers for C-C coupling and β-hydride elimination using multireference NEVPT2 calculations on top of the CASSCF wavefunction to validate the rate-determining step of the reaction.