A General Dual-Metal Nanocrystal Dissociation Strategy to Generate Robust High-Temperature-Stable Alumina-Supported...

Designing new synthesis routes to fabricate highly thermally durable precious metal single-atom catalysts (SACs) is challenging in industrial applications. Herein, a general strategy is presented that starts from dual-metal nanocrystals (NCs), using bimetallic NCs as a facilitator to spontaneously convert a series of noble metals to single atoms on aluminum oxide. The metal single atoms are captured by cation defects in situ formed on the surface of the inverse spinel (AB₂O₄) structure, which process provides numerous anchoring sites, thus facilitating generation of the isolated metal atoms that contributes to the extraordinary thermodynamic stability. The Pd₁/AlCo₂O₄-Al₂O₃ shows not only improved low-temperature activity but also unprecedented (hydro)thermal stability for CO and propane oxidation under harsh aging conditions. Furthermore, our strategy exhibits a small scaling-up effect by the simple physical mixing of commercial metal oxide aggregates with Al₂O₃. The good regeneration between oxidative and reductive atmospheres of these ionic palladium species makes this catalyst system of potential interest for emissions control.