Abstract: | Bimetallic nanoparticle encapsulation in microporous zeolite crystals is a promising route for producing catalysts with unprecedented reaction selectivities. Herein, a novel synthetic approach was developed to produce PtZnx nanoclusters encapsulated inside zeolite micropores by introducing Pt2+ cations into a zincosilicate framework via ion exchange, and subsequent controlled demetallation and alloying with framework Zn. The resulting zeolites featured nanoclusters with sizes of approximately 1 nm, having an interatomic structure corresponding to a PtZnx alloy as confirmed by pair distribution function (PDF) analysis. These materials featured simultaneous shape and substrate specificity demonstrated by the selective production of p‐chloroaniline from the competitive hydrogenation of p‐chloronitrobenzene and 1,3‐dimethyl‐5‐nitrobenzene. |