1. Advancing highly selective low-temperature ammonia oxidation: Hydrophobic silicalite-1 shell confining silver nanoparticles on Cu/ZSM-5 core.
- Author
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Chen, Xiaoxin, Qiu, Ziyi, Wang, Xiaolin, Li, Yulei, Hou, Changmin, Li, Lin, Zhang, Jing, Nan, Maiyan, and Yang, Guoju
- Subjects
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AMMONIA , *OXIDATION , *SILVER nanoparticles , *NANOPARTICLES , *HYDRAZINE , *CATALYSTS , *SILVER ions - Abstract
[Display omitted] • Cu/ZSM-5 core enveloped by S-1 shell with confined Ag0 nanoparticles. • Core-shell architecture fosters the generation of abundant active Ag0 nanoparticles. • Silicalite-1 shell hinders Ag0 migration and preserves active Cu2+ sites. • Discretely distributed Cu2+ and Ag0 centers underpin a catalytically robust system. • Cu/ZSM-5@Ag/S-1 exhibits superior hydrothermal stability and NH 3 -SCO activity. A judiciously devised core–shell NH 3 -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 NO x. 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 O 2 activation and NH 3 dehydrogenation and thereby contributing to superior low-temperature activity in NH 3 -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. [ABSTRACT FROM AUTHOR]
- Published
- 2024
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