In this paper we will provide a review of our recent studies on the general stability of the Pt-3d-Pt (3d = Ti, V, Cr, Mn, Fe, Co and Ni) subsurface structures, which are the desirable structural configurations in several applications in heterogeneous catalysis and electrocatalysis. We will first provide a review of density functional theory (DFT) predictions of the thermodynamic stability of Pt-3d-Pt(111) and Pt-3d-Pt(100) in vacuum and with adsorbed hydrogen and oxygen. The DFT results predict that the Pt-3d-Pt subsurface structures are stable in vacuum and with adsorbed hydrogen, while with adsorbed oxygen the 3d atoms should segregate to the surface to produce the 3d-Pt-Pt surface structures. The DFT predictions are verified experimentally on selected Pt-3d-Pt(111) systems. The experimental efforts are further expanded by bridging the materials gap form single crystal Pt(111) to polycrystalline Pt to incorporate multiple crystal facets and to determine their effects on the kinetic barriers for the segregation of the subsurface 3d atoms. In order to further correlate DFT calculations with experimental results, a Brønsted-Evans-Polanyi relationship is derived to correlate thermodynamic stability from DFT calculations with kinetic barriers from experimental measurements for the Pt-3d-Pt systems. Finally, empirical equations have been developed for predicting the thermodynamic stability of other bimetallic systems both in vacuum and with adsorbed hydrogen and oxygen.