Abstract
Grain boundary (GB) segregation plays a pivotal role in maintaining and optimizing the remarkable catalytic or mechanical properties of nanocrystalline Pt by reducing the Gibbs free energy and thereby impeding structure degradation. The solute segregation behavior at the Pt GB, however, is not well understood at the atomic level. In this study, we employed first-principles calculations to elucidate the preferential segregation behavior of a single Au atom at the symmetrical tilt GB of Pt. For pure Pt, a linear relationship between the GB energy and excess volume is observed. Therefore, Au exhibits strong segregation tendencies towards GB to release excess energy and volume stored at the strained GB. Although the segregation energy is sensitive to various GB sites, it is interesting to note that the minimum one increases linearly with GB energy. This site-sensitivity of segregation energy can be attributed to mechanical, chemical, and interaction parts, which are quantitatively related to the atomic volume, coordination number, and average bond length, respectively. Finally, the interplay among different structural descriptors is revealed. These insights into the association between GB structures, segregation configuration and energy offers valuable atomic-scale quantitative insights into the segregation behavior of Au in Pt GBs, which holds significant implications for the design of Pt nanomaterials with enhanced thermal stability via GB engineering.
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