To energetically evaluate our structures we use both ONETEP a linear-scaling Density functional theory (DFT) with the outlook of eventually scaling up to 'realistically' sized NPs in the future and Grimme et al.'s xTB to perform quick but reasonably accurate (c.f. figure ) energetic evaluations. We acknowledge that some assumptions have been made in order to create our ensembles of structures. Specifically we have not included noncollinear spin and spin-orbit coupling in our DFT calculations due to code limitations and computational effort. We aim for the methods and settings developed and optimised in this paper to be carried forward and used for larger more realistic catalytic systems in the future where we anticipate some of these effects will be less relevant.