Surface segregation is a phenomenon common to all multicomponent materials and one that plays a critical role in determining their surface properties such a catalysis. Comprehensive studies of surface segregation versus bulk composition in ternary alloys have been prohibitive because of the need to study many different compositions. In this work, high-throughput low-energy He+ ion scattering spectra (LEIS) and energy dispersive X-ray spectra (EDX) were collected from a CuxAuyPd1-x-y composition spread alloy film (CSAF) under ultra-high vacuum conditions. These have been used to quantify surface segregation across the entire CuxAuyPd1-x-y composition space (x = 0→1 and y = 0→1-x). Surface compositions at 164 different bulk compositions were measured at 500 K and 600 K. At both temperatures, Au shows the greatest tendency for segregation to the topmost surface while Pd is always depleted from surface. Higher temperatures enhance the Au segregation. Segregation at most of the binary alloy bulk compositions matches observations previously reported in the literature. However, surface compositions in the CuPd B2 composition region reveal segregation profiles that are non-monotonic in bulk alloy composition. These were not observable in prior studies due to their limited resolution of composition space. An extended Langmuir-MacLean model, which describes ternary alloy segregation, has been used to analyze experimental data from the ternary alloys, and to estimate pair-wise segregation free energies and segregation equilibrium constants. The ability to study surface segregation across ternary alloy composition space with high throughput methods has been validated, and the impact of bulk alloy phase on surface segregation is demonstrated and discussed.

Surface segregation across ternary alloy composition space

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