Zeolite-Encaged Single-Atom Rhodium Catalysts: Highly-Efficient Hydrogen Generation and Shape-Selective Tandem Hydrogenation of Nitroarenes

Qiming Sun, Ning Wang, Tianjun Zhang, Risheng Bai, Alvaro Mayoral*, Peng Zhang, Qinghong Zhang, Osamu Terasaki, Jihong Yu

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

371 Citations (Scopus)

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 languageEnglish
Pages (from-to)18570-18576
Number of pages7
JournalAngewandte Chemie - International Edition
Volume58
Issue number51
DOIs
Publication statusPublished - 16 Dec 2019
Externally publishedYes

Keywords

  • hydrogen generation
  • rhodium
  • single-atom catalysts
  • tandem reactions
  • zeolites

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