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Zeolite‐Encaged Single‐Atom Rhodium Catalysts: Highly‐Efficient Hydrogen Generation and Shape‐Selective Tandem Hydrogenation of Nitroarenes
Author(s) -
Sun Qiming,
Wang Ning,
Zhang Tianjun,
Bai Risheng,
Mayoral Alvaro,
Zhang Peng,
Zhang Qinghong,
Terasaki Osamu,
Yu Jihong
Publication year - 2019
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201912367
Subject(s) - catalysis , chemistry , zeolite , ammonia borane , rhodium , hydrolysis , inorganic chemistry , hydrogen production , organic chemistry
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.