Advancing highly selective low-temperature ammonia oxidation: Hydrophobic silicalite-1 shell confining silver nanoparticles on Cu/ZSM-5 core

Abstract

A judiciously devised core–shell NH3-SCO catalyst featuring a Cu/ZSM-5 core enveloped by an Ag/silicalite-1 shell (Cu/ZSM-5@Ag/S-1) was rationally constructed. Integrating the silicalite-1 shell effectively suppresses the migration of Ag into Cu/ZSM-5 core, conserving the active Cu2+ sites for the catalytical conversion of byproducts NOx. Concurrently, the shell averts the formation of positively charged Ag species, facilitating the generation of abundant Ag0 nanoparticles encapsulated in the S-1 shell. Comprehensive characterizations reveal abundant Ag0 species within the core–shell Cu/ZSM-5@Ag/S-1 catalyst, boosting O2 activation and NH3 dehydrogenation and thereby contributing to superior low-temperature activity in NH3-SCO reactions. Furthermore, the hydrophobic S-1 shell effectively reinforces the hydrothermal stability of the core–shell Cu/ZSM-5@Ag/S-1. DRIFTS coupled with DFT studies elucidate that the core–shell sample follows the imide mechanism, while the shell-free sample adheres to the hydrazine mechanism. This work advances our understanding of catalyst design and presents a promising solution with practical implications for ammonia oxidation processes.