Silanol Nest‐Anchored Oligomeric Vanadium Oxides for Highly Stable and Efficient Propane Dehydrogenation

ABSTRACT The controlled stabilization of non‐noble metal species for propane dehydrogenation (PDH) remains challenging due to their intrinsic tendency toward aggregation and oxidation‐state drift. Here, we demonstrate that silanol nests within dealuminated Beta zeolites act as defect‐engineered anchoring centers that regulate the polymerization of vanadium oxides (VO x ). Systematic manipulation of silanol density through dealumination, thermal condensation, and sodium passivation reveals a positive correlation among silanol‐nest population, vanadium dispersion, and PDH performance. The optimized V 1% /DeAlBeta catalyst achieves a high propylene formation rate of 1.93 mol C3H6 g V −1 h −1 , a low deactivation rate (0.0067 h −1 ) at 580°C, and excellent long‐term stability and regenerability across eight consecutive redox cycles. Comprehensive spectroscopic analyses identify cooperative silanol–VO x interactions that stabilize isolated and low‐polymerized vanadium species, whereas depletion of silanol nests triggers the formation of polymeric VO x domains with diminished activity. These results highlight a defect‐directed confinement strategy to stabilize earth‐abundant metal sites and offer conceptual guidelines for designing environmentally benign and cost‐effective PDH catalysts.