The non-equilibrium phase diagram approach uses thermodynamic principles to predict the formation of various solid phases under reaction conditions. This approach attempts to systematically control the phases in-situ by controlling the gas-phase potentials and has been applied successfully to investigating carbon deposition over Fe, Co, and Ni. In order to maintain the same gas-phase composition and driving force for carbon deposition over the solid phases, this approach is extended to binary alloys of these metals. The thermodynamic metal activities are determined using excess Gibbs free energy of mixing for the [NiCo], [FeNi], and [CoFe] alloy systems and the lattice stability parameters for Fe, Co, and Ni reported by Kaufman and co-workers. The non-equilibrium phase diagrams for the [NiCo], [FeNi], and [CoFe] alloy systems have been generated. By varying the alloy composition, the catalytic activity of the various thermodynamically favored solid phases can be studied under identical gas phase conditions.