Revealing the Phase Separation Behavior of Thermodynamically Immiscible Elements in a Nanoparticle

Nano Lett. 2021 Aug 11;21(15):6684-6689. doi: 10.1021/acs.nanolett.1c02225. Epub 2021 Jul 20.

Abstract

Phase-separation is commonly observed in multimetallic nanomaterials, yet it is not well understood how immiscible elements distribute in a thermodynamically stable nanoparticle. Herein, we studied the phase-separation of Au and Rh in nanoparticles using electron microscopy and tomography techniques. The nanoparticles were thermally annealed to form thermodynamically stable structures. HAADF-STEM and EDS characterizations reveal that Au and Rh segregate into two domains while their miscibility is increased. Using aberration-corrected HAADF-STEM and atomic electron tomography, we show that the increased solubility of Au in Rh is achieved by forming Au clusters and single atoms inside the Rh domains and on the Rh surface. Furthermore, based on the three-dimensional reconstruction of a AuRh nanoparticle, we can visualize the uneven interface that is embedded in the nanoparticle. The results advance our understanding on the nanoscale thermodynamic behavior of metal mixtures, which is crucial for the optimization of multimetallic nanostructures for many applications.

Keywords: Heterostructured nanoparticle; electron tomography; phase separation; thermodynamics.

Publication types

  • Research Support, Non-U.S. Gov't
  • Research Support, U.S. Gov't, Non-P.H.S.

MeSH terms

  • Microscopy, Electron
  • Nanoparticles*
  • Nanostructures*
  • Solubility
  • Thermodynamics