Abstract

A challenge within the catalyst community is developing catalysts for gas-to-liquid (GTL) transformations with high activity, selectivity, and recyclability. One promising solution is a metal complex (i.e., a 3d transition metal such as Nickel(II)) anchored to a porous support since such materials feature well-defined, uniform, and isolated active-sites. Depending on the reaction environment, these supported metal complexes exhibit structural changes that affect catalytic performance. In this work, we use density functional theory (DFT) calculations and ab initio thermodynamic modeling to learn how the reaction environment influences Ni(II) complex catalysts supported on the metal-organic framework (MOF) NU-1000. We investigate more than 300 different structures and compositions in order to reveal those that are favorable at relevant activation and reaction conditions. The findings establish thermodynamically relevant models that require further computational catalytic investigations as well as showcasing how to tune structures using different reaction conditions.