The goal of this experiment is to study the structural and catalytic properties of single alloyed Ni-Fe crystals using Bragg Coherent X-ray Diffraction Imaging (BCDI) under catalytic in situ and operando conditions. The 3D intensity distribution in reciprocal space in the vicinity of a selected Bragg reflection contains information about the shape and strain states of the nanostructure, thus revealing insight to the nature of nanoscale deformation following chemical stimuli, such as adsorption of gases or changes in adsorbate structure. Here, we aim at imaging the strain evolution of pure Ni and alloyed Ni-Fe particles and evaluating the impact of alloying and support/substrate during CO2 hydrogenation. Ni-Fe particles have been demonstrated as the best candidates for an “all-inclusive” material of choice for the reaction.