Aluminum‐Rich Molecular Sieve Interface Regulating Electron‐Enriched Mn‐O‐Ce Active Sites for Environmental Catalysis

Abstract The improvement of low‐temperature catalytic activity still remains a paramount scientific challenge in environmental catalysis. To address this issue, an aluminum‐rich molecular sieve interface regulating electron‐enriched Mn‐O‐Ce active sites for highly efficient environmental catalysis has been demonstrated. Specifically, the surface aluminum‐rich hollow ZSM‐5 zeolites are constructed through dissolution‐recrystallization and coupled with MnCeO x composites owning strong redox properties to amplify contact between acidic and active sites that manipulate effective environmental catalytic reactions. Taking the selective catalytic reduction of nitrogen oxide (NO x ) as a probing reaction, the engineered Al‐rich interface significantly facilitates the electron transfer from ZSM‐5 zeolite to MnCeO x composite, creating electron‐enriched Mn‐O‐Ce active sites that artfully establish adjacent centers for reactant molecules adsorption and activation: Mn‐end of Mn‐O‐Ce sites for NO x coordination and Ce‐end of Mn‐O‐Ce sites for partial ammonia (NH 3 ) adsorption to achieve superior catalytic activity and selectivity below 150 °C. Concurrently, the modulated zeolite‐metal oxide interface with electron‐enriched Mn‐O‐Ce active sites and sufficient Brønsted acid sites also demonstrates exceptional efficiency in synergistic removal of nitrogen oxide with representative volatile organic compounds. Beyond superior multifunctional catalytic performance, this work pioneers interfacial electron engineering as a universal strategy to design advanced functional materials for efficient environmental catalysis.