A Versatile Cucurbituril‐Anchored Platform for Atomically Dispersed Metal Catalysts on Oxide Supports

Atomically dispersed metal catalysts maximize metal utilization and can deliver exceptional activity and selectivity in challenging reactions that are often inaccessible to nanoparticle‐based catalysts. However, frequent aggregation during catalyst preparation and activation drives growth of the target metal species into nanometer‐scale particles, which has conventionally forced the use of very low metal loadings to suppress sintering. Herein, a general strategy is proposed to generate atomically dispersed metal species on oxide supports by using the partially negatively charged carbonyl portals of cucurbituril (CB) as anchoring sites for single cationic metal ions. Cucurbituril enabled effective functionalization of common oxide supports, and even highly mobile Ag was stabilized in a single‐atomic form on CB‐functionalized TiO 2 after calcination. When applied to CO 2 hydrogenation, the resulting atomically dispersed Ni/TiO 2 catalyst selectively produced CO with over 95% selectivity, suppressing the methane formation pathway typically observed for Ni catalysts. The activated catalyst after H 2 treatment at 400°C also remained atomically dispersed, consistent with strong Ni‐support interactions that stabilize isolated Ni species under reductive conditions. This CB‐mediated approach is expected to provide a versatile platform for deploying densely stabilized, atomically dispersed metal catalysts in demanding reactions that are otherwise difficult to realize.