We conducted a thorough investigation into propylene oligomerization on the trimetallic MOF node Fe 2 M, employing two distinct strategies. In our first approach, we explored variations in the active metal M across 3d transition metals from Sc to Cu. Notably, among Fe 2 M configurations, we identified several cases (M=Sc, Mn, Co and Cu) with energy barriers lower or comparable to the experimentally observed Fe 2 Ni, thus presenting viable alternatives as catalysts for propylene oligomerization. In our second approach, we focused on varying the spectator atom, namely Fe in Fe 2 Ni, across the same range of transition metals. This exploration led to the discovery of configurations such as Cr 2 Ni, Mn 2 Ni, Co 2 Ni, and Ni 3 exhibiting lower energy barriers compared to the experimentally reported Fe 2 Ni. Our investigation also sheds light on the crucial role of spectators and electronic communication between the active metal center. This understanding provides a pathway to fine-tune the catalytic activity and selectivity, optimizing the reaction products. Specifically, we found an inverse correlation between the natural spin density of spectators and C-C coupling barriers. Moreover, NEVPT2 calculations successfully predicted the correct rate-determining step in cases where DFT initially misjudged the kinetically relevant step due to marginal energy differences between the two steps.