Abstract
Single-atom alloys (SAAs) are emerging materials containing isolated metal atoms dispersed on host metal surfaces, exhibiting unique reactivity compared with the corresponding monometallic counterparts. However, the stability of the isolated atoms in the host metal has hardly been studied, although, metal segregation has been commonly observed in bimetallic nanoparticles under reaction conditions. In this work we focus on single-atom Pt anchored on various metallic support surfaces. Density Functional Theory (DFT) calculations coupled with environmental segregation energy analysis are performed to map the segregation trends of 22 different Pt-SAA surfaces under various hydrogen conditions. The results show the high stability of single-atom Pt in Ni, Co, Rh and Ir host metallic surfaces while no stability is predicted on Au and Ag surfaces. For Pd and Cu host supports, the single-atom Pt is found to be stable on specific surface facets and within definite temperature and pressure conditions. This work brings an important understanding of SAA systems through the prediction of of surface atomic ordering changes under operating conditions which related to the reactivity will ultimately allow the design of more efficient catalysts.