Thesis (Ph.D. (Physics)) --University of Limpopo, 2013 / The intention of the current study is to investigate structure, ion transport and reactivity of various forms of the cobalt pentlandite, Co9S8, at different temperatures using atomistic simulation methods with the support of electronic structure calculations. The first interatomic potentials of Co9S8 were derived with input data as structure and elastic properties from experiment and electronic structure calculations respectively. The potentials were validated by running energy minimization and molecular dynamics calculations. Structure, elastic properties and phonon spectra were well reproduced, together with the complex high temperature transformations and melting of Co9S8 as deduced from crystal structure, radial distribution functions, density profiles and diffusion coefficients. Amongst the high symmetry surfaces {111}, {101} and {101} atomistic surface energy calculations proposed the {111} surface of Co9S8 as the most stable in agreement with experimental morphologies, and water adsorption energies on the such surfaces which mostly agreed with those from electronic structure calculations. The structural and ion transport variations with temperature were investigated and predicted surface melting at lower temperatures than the bulk. The effects of hydration on the surfaces at low and high temperatures were also studied. The structural and ion transport properties of Co9S8 nanoparticles of varying sizes, covered by high symmetry surfaces {111}, {101} and {100} were predicted using molecular dynamics method based on our derived interatomic potentials. The structural and ion transport properties of Co9S8 nanoparticles of varying sizes, covered by high symmetry surfaces {111}, {101} and {100} were predicted using molecular dynamics method based on our derived interatomic potentials. Generally for {111}, {101} nanoparticles, high temperature transitions were abrupt for smaller nanoparticles and these tended to disintegrate and form voids. However, for larger nanoparticles the transitions were more gradual. Transitions in the {100} bound nanoparticles were less dramatic for all sizes and the formation of voids was reduced at high temperatures. Generally, the melting temperatures of different sizes of nanoparticles increases with the particle size hence approach the bulk limit. The interaction of nanoparticles with water was investigated. / Anglo Platinum, National Research Foundation (South Africa), and The Royal Society (UK)