Abstract
Pt nanoclusters (PtC) on the surface of ceria-zirconia solid solutions exhibit superior low-temperature CO oxidation activity compared to Pt single atoms (Pt1). However, the redispersion behavior of the PtC to Pt1 lowers the efficiency of CO Oxidation. In this work, the stable surface hydroxyl groups were constructed by high-temperature hydrothermal aging treatment. Specifically, the Pt1 catalyst (Pt/CZOe-SA) prepared by atom trapping was subjected to high-temperature hydrothermal treatment to obtain the stable PtC catalyst (Pt/CZOe-HT) with in-situ formed PtC. The experimental results showed that PtC with 2–3 nm size could achieve excellent low-temperature activity and thermal stability. In addition, the ab initio molecular dynamics and density functional theory calculations revealed the specific evolution process of dynamic dispersion for PtC with or without hydroxyl groups from the femtosecond scale, suggesting that the hydroxyl groups limited the dispersion of PtC in the form of “energy fence”. The hydrothermal treatment not only introduced high-temperature stable hydroxyl groups to improve the stability of the in-situ formed PtC, but also optimized the ratio of Pt1 and PtC, and then enhanced the low-temperature activity by the synergistic effect between Pt1 and PtC. The present work can provide theoretical guidance for developing high-performance and high-stability Pt-based catalysts.
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