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

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 subse...

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Published inAngewandte Chemie International Edition Vol. 58; no. 51; pp. 18570 - 18576
Main Authors Sun, Qiming, Wang, Ning, Zhang, Tianjun, Bai, Risheng, Mayoral, Alvaro, Zhang, Peng, Zhang, Qinghong, Terasaki, Osamu, Yu, Jihong
Format Journal Article
LanguageEnglish
Published WEINHEIM Wiley 16.12.2019
Wiley Subscription Services, Inc
EditionInternational ed. in English
Subjects
Ammonia
Catalysis
Catalysts
Chemical synthesis
Chemistry
Chemistry, Multidisciplinary
hydrogen generation
Hydrogen production
Hydrogen storage
Hydrogenation
Hydrolysis
Oxygen atoms
Physical Sciences
Rhodium
Scanning transmission electron microscopy
Science & Technology
Single atom catalysts
tandem reactions
Transmission electron microscopy
Zeolites
single-atom catalysts
OXIDATION
TRANSFORMATION
STORAGE
HYDROLYTIC DEHYDROGENATION
PLATINUM
AMMONIA-BORANE
CO
NANOPARTICLES
zeolites
CLUSTERS
hydrogen generation
SITES
tandem reactions
rhodium
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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. Together alone: Single Rh atoms were encapsulated within MFI zeolites under in situ hydrothermal conditions and a ligand‐protected direct H2 reduction. The catalyst gave a high turnover frequency of 699 molH2  (molRh)−1 min−1 at 298 K for ammonia borane (AB) hydrolysis and exhibited superior catalytic efficiency in shape‐selective tandem hydrogenation of nitroarenes by coupling with the hydrolysis of AB.
AbstractList 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.
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.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.
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 reduction. C -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 generation rates from ammonia borane (AB) hydrolysis, up to 699 min 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.
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.
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. Together alone: Single Rh atoms were encapsulated within MFI zeolites under in situ hydrothermal conditions and a ligand‐protected direct H2 reduction. The catalyst gave a high turnover frequency of 699 molH2  (molRh)−1 min−1 at 298 K for ammonia borane (AB) hydrolysis and exhibited superior catalytic efficiency in shape‐selective tandem hydrogenation of nitroarenes by coupling with the hydrolysis of AB.
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.
Author Sun, Qiming
Zhang, Tianjun
Zhang, Peng
Yu, Jihong
Wang, Ning
Bai, Risheng
Zhang, Qinghong
Mayoral, Alvaro
Terasaki, Osamu
Author_xml – sequence: 1
  givenname: Qiming
  orcidid: 0000-0002-8895-5703
  surname: Sun
  fullname: Sun, Qiming
  organization: Jilin University
– sequence: 2
  givenname: Ning
  surname: Wang
  fullname: Wang, Ning
  organization: Jilin University
– sequence: 3
  givenname: Tianjun
  surname: Zhang
  fullname: Zhang, Tianjun
  organization: Jilin University
– sequence: 4
  givenname: Risheng
  surname: Bai
  fullname: Bai, Risheng
  organization: Jilin University
– sequence: 5
  givenname: Alvaro
  orcidid: 0000-0002-5229-2717
  surname: Mayoral
  fullname: Mayoral, Alvaro
  email: amayoral@shanghaitech.edu.cn
  organization: ShanghaiTech University
– sequence: 6
  givenname: Peng
  surname: Zhang
  fullname: Zhang, Peng
  organization: Dalhousie University
– sequence: 7
  givenname: Qinghong
  surname: Zhang
  fullname: Zhang, Qinghong
  organization: Xiamen University
– sequence: 8
  givenname: Osamu
  surname: Terasaki
  fullname: Terasaki, Osamu
  organization: ShanghaiTech University
– sequence: 9
  givenname: Jihong
  orcidid: 0000-0003-1615-5034
  surname: Yu
  fullname: Yu, Jihong
  email: jihong@jlu.edu.cn
  organization: Jilin University
BackLink https://www.ncbi.nlm.nih.gov/pubmed/31657875$$D View this record in MEDLINE/PubMed
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Issue 51
Keywords single-atom catalysts
OXIDATION
TRANSFORMATION
STORAGE
HYDROLYTIC DEHYDROGENATION
PLATINUM
AMMONIA-BORANE
CO
NANOPARTICLES
zeolites
CLUSTERS
hydrogen generation
SITES
tandem reactions
rhodium
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Snippet Single‐atom catalysts are emerging as a new frontier in heterogeneous catalysis because of their maximum atom utilization efficiency, but they usually suffer...
Single-atom catalysts are emerging as a new frontier in heterogeneous catalysis because of their maximum atom utilization efficiency, but they usually suffer...
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StartPage 18570
SubjectTerms Ammonia
Catalysis
Catalysts
Chemical synthesis
Chemistry
Chemistry, Multidisciplinary
hydrogen generation
Hydrogen production
Hydrogen storage
Hydrogenation
Hydrolysis
Oxygen atoms
Physical Sciences
Rhodium
Scanning transmission electron microscopy
Science & Technology
Single atom catalysts
tandem reactions
Transmission electron microscopy
Zeolites
Title Zeolite‐Encaged Single‐Atom Rhodium Catalysts: Highly‐Efficient Hydrogen Generation and Shape‐Selective Tandem Hydrogenation of Nitroarenes
URI https://onlinelibrary.wiley.com/doi/abs/10.1002%2Fanie.201912367
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https://www.ncbi.nlm.nih.gov/pubmed/31657875
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https://www.proquest.com/docview/2309815124
Volume 58
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