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author:

Zhuang, J.-L. (Zhuang, J.-L..) [1] | Liu, X.-Y. (Liu, X.-Y..) [2] | Du, X. (Du, X..) [3]

Indexed by:

Scopus PKU CSCD

Abstract:

A strategy based on grafting organocatalytic units as side-chain on the organic linkers, a TEMPO radical decorated terphenyl-dicarboxylic acid linker was synthesized. By employing acetic acid as modulator, TEMPO radical decorated UiO-68-TEMPO nanocrystals were synthesized by using H2tpdc-TEMPO as organic linker and ZrOCl2 as metal source under solvothermal conditions. UiO-68-TEMPO are monodispersed nanocrystals with side in the range of 800-1200 nm, with high BET areas (up to 1320 m2/g), and contain a large number of TEMPO radicals as evidenced by solid-state EPR spectrum. UiO-68-TEMPO nanocrystals enable selective oxidation of a broad range of alcohols, including primary aromatic alcohols, secondary aromatic alcohols, and heterogeneous atomic alcohols, with high efficiency and selectivity. The catalytic activity of UiO-68-TEMPO nanocrystals remains 75% after catalysis for four cycles. Finally, a plausible catalytic mechanism for the oxidation of benzyl alcohol by UiO-68-TEMPO was proposed, that is the TBN co-catalyst produces NO2/NO redox mediator, which enables the oxidation of TEMPO radicals to oxoammonium cations by O2, and finally oxidize benzyl alcohol to benzaldehyde. © 2020, Journal of Materials Engineering. All right reserved.

Keyword:

Alcohol oxida-tion; Organocatalyst; Porous material; Radical; Zr-based metal-organic framework

Community:

  • [ 1 ] [Zhuang, J.-L.]Key Laboratory of Functional Materials and Chemistry of Guizhou Province, School of Chemistry and Materials, Guizhou Normal University, Guiyang, 550001, China
  • [ 2 ] [Liu, X.-Y.]Key Laboratory of Functional Materials and Chemistry of Guizhou Province, School of Chemistry and Materials, Guizhou Normal University, Guiyang, 550001, China
  • [ 3 ] [Liu, X.-Y.]College of Chemistry, Fuzhou University, Fuzhou, 350108, China
  • [ 4 ] [Du, X.]Key Laboratory of Green Process and Engineering, CAS, Institute of Process Engineering, Beijing, 100190, China

Reprint 's Address:

  • [Zhuang, J.-L.]Key Laboratory of Functional Materials and Chemistry of Guizhou Province, School of Chemistry and Materials, Guizhou Normal UniversityChina

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Source :

Journal of Materials Engineering

ISSN: 1001-4381

Year: 2020

Issue: 10

Volume: 48

Page: 169-175

0 . 6 0 0

JCR@2023

Cited Count:

WoS CC Cited Count:

SCOPUS Cited Count: 3

ESI Highly Cited Papers on the List: 0 Unfold All

WanFang Cited Count:

Chinese Cited Count:

30 Days PV: 1

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