Classical Strong Metal‐Support Interactions Induced by Calcination in Argon Atmosphere

Supported noble‑metal catalysts are central to heterogeneous catalysts, yet stabilizing highly dispersed metal nanoparticles against sintering and deactivation remains challenging. Strong metal–support interactions (SMSI) can effectively stabilize metal nanoparticles, but classical SMSI typically requires harsh reductive treatments and is widely considered inaccessible on nonreducible oxides such as ZrO 2 . Here, we demonstrate a breakthrough strategy to achieve classical SMSI on the non‐reducible substrate like ZrO 2 with Pt by a calcination process in inert argon. Argon calcination generates oxygen vacancies in ZrO 2 , which thermodynamically promotes support migration and the formation of a ZrO x overlayer that partially encapsulates Pt nanoparticles. Molecular dynamics simulations further reveal that increasing surface oxygen‐vacancy concentrations facilitate ZrO 2 migration and encapsulation. Explicit electron transfer from the substrate ZrO 2 to Pt is observed to induce an explicit SMSI. The SMSI formed in Pt/ZrO 2 substantially improves catalyst stability, allowing efficient and durable CO oxidation for over 100 h without noticeable degradation, whereas fresh Pt/ZrO 2 continuously deactivates. This argon calcination strategy is further extendable to multiple catalytic systems, establishing a general and operationally simple paradigm to construct classical SMSI on non‐reducible oxide supports.