Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 58, Issue 51, Pages 18570-18576Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201912367
Keywords
hydrogen generation; rhodium; single-atom catalysts; tandem reactions; zeolites
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Funding
- National Key Research and Development Program of China [2016YFB0701100]
- National Natural Science Foundation of China [21835002, 21621001]
- 111 Project [B17020]
- SPST of ShanghaiTech University [EM02161943]
- NSFC [NFSC-21850410448]
- U.S. DOE [DE-AC02-06CH11357]
- Canadian Light Source
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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 H-2 reduction. C-s-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 H-2 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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