Zeolite-Encaged Single-Atom Rhodium Catalysts: Highly-Efficient Hydrogen Generation and Shape-Selective Tandem
Qiming Sun1, Ning Wang1, Tianjun Zhang1
1State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012, P. R. China.
Abstract:
Single-atom catalysts are emerging as a new frontier in heterogeneous catalysis because of their maximum atom utilization efficiency, but they usually suffer from inferior stability. Herein, we synthesized single-atom Rh catalysts embedded in MFI-type zeolites under hydrothermal conditions and subsequent ligand-protected direct H2 reduction. Cs -corrected scanning transmission electron microscopy and extended X-ray absorption analyses revealed that single Rh atoms were encapsulated within 5-membered rings and stabilized by zeolite framework oxygen atoms. The resultant catalysts exhibited excellent H2 generation rates from ammonia borane (AB) hydrolysis, up to 699 min-1 at 298 K, representing the top level among heterogeneous catalysts for AB hydrolysis. The catalysts also showed superior catalytic performance in shape-selective tandem hydrogenation of various nitroarenes by coupling with AB hydrolysis, giving >99 % yield of corresponding amine products.
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