The catalytic conversion of propylene, a key intermediate in the petrochemical industry, holds significant importance in the synthesis of valuable chemical products. The oligomerization of propylene to obtain higher olefins demonstrates promising applications in fragrances, gasoline additives, and agrochemicals while also serving as valuable feedstocks for producing polymer films and thermoplastic resins. Among various catalytic systems, metal-organic frameworks (MOFs) have emerged as highly versatile materials, gaining significant attention for their wide-ranging potential in various catalytic applications. Their modular structure, characterized by nodes and linkers with specific structure and composition, positions them as ideal platforms for catalyst screening and the customization of their catalytic properties. Numerous categories of MOFs like MIL-88(Fe 3 , Cr 3 , Fe 2 Ni), MIL-127/PCN-250 (Fe 2 M, M = Fe 2+,3+ , Co 2+ , Ni 2+ , Mn 2+ , Zn 2+ ), MIL-100 (M) (M = Cr, Fe, Sc, Al, V), and MIL-101 (M) (M=Fe, Cr, Ni, Cu) feature open transition-metal sites, incorporating metal oxo-trimer nodes described by the chemical composition (M 3+ ) 2 (M' 2+/3+ )(µ 3 -O)(RCOO) 6 (X) as secondary building units (SBUs). Here, M and M' denote transition metals and X is a counter-anion which is present only when M' is trivalent to maintain the charge neutrality in the system and RCOO -are the carboxylate linkers. The crystallographic structure of MIL-127 (Fe 3 ) is shown in Figure that comprises of the trimetallic MOF nodes (Figure ) linked by ABTC (3,3',5,5'-azobenzenetetracarboxylate) linkers (Figure ). An intriguing aspect of MOFs is the presence of structural defects, often resulting from the absence of linkers in their framework. Figure shows one missing carboxylate linker that is obtained upon heating thereby creating a structural defect in the oxo-trimer. These defects create unique active sites, increase surface area, and improve accessibility to the MOFs' internal structure, making them exceedingly effective for catalysis. Their remarkable versatility is underscored by their success in facilitating numerous complex reactions. These include C-H bond activation, partial oxidation of methane into methanol, dimerization, and oligomerization of ethylene and propylene, among others. Computational calculations serve as a useful tool for contributing to mechanistic understanding of catalysis through molecular and periodic simulations. The knowledge gained from computational analyses can then be leveraged for the rational design of catalysts. Density Functional Theory (DFT) is the most widely utilized electronic structure method for modeling catalytic processes owing to its optimal balance between computational cost and accuracy. However, in the case of open-shell catalysts, such as transition metals with nearly degenerate ground states, the accuracy of DFT can be notably compromised. Therefore, to validate the trends obtained from DFT calculations, multiref-erence methods are required to ensure reliability. Lyu et al. computationally investigated the trimetallic building unit for CO 2 reduction to methanol by the systematic variation of M in Fe 2 M with various transition metals to explore its catalytic activity. The oxidative dehydrogenation of alkanes was systematically explored by varying the divalent metal, M in Fe 2 M MOF nodes by Snurr and co-workers. The trimetallic MOF node exhibits remarkable activity in the oxidation of methane to methanol. Vitillo et al.