Design of compositionally complex catalysts

Abstract

Besides revealing excellent mechanical properties, compositionally complex alloys are also very promising candidates for applications in heterogeneous catalysis. The opportunity provided by the tremendously large composition phase space to explore new materials and tune the materials properties in the materials design cycle is, however, intrinsically coupled with the challenge of controlling surface segregation, which is generally more severe in multicomponent alloys as compared to simpler systems. We demonstrate this by computing the surface phase diagram of two candidate compositionally complex catalysts. Significant surface segregation is found even at very high temperature and this can strongly affect the catalytic properties of these alloys. We explain the observed phase stabilities in terms of segregation energies and rationalize the segregation trends with canonical models. Finally, we propose a set of descriptors accessible with first-principles calculations that allows to quickly incorporate the evaluation of the segregation during the alloy design process.