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.
Original language | English |
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Pages (from-to) | 18570-18576 |
Number of pages | 7 |
Journal | Angewandte Chemie - International Edition |
Volume | 58 |
Issue number | 51 |
DOIs | |
Publication status | Published - 16 Dec 2019 |
Externally published | Yes |
Keywords
- hydrogen generation
- rhodium
- single-atom catalysts
- tandem reactions
- zeolites