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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.
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Journal of Materials Engineering
ISSN: 1001-4381
CN: 11-1800/TB
Year: 2020
Issue: 10
Volume: 48
Page: 169-175
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JCR@2022
Cited Count:
SCOPUS Cited Count: 3
ESI Highly Cited Papers on the List: 0 Unfold All
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30 Days PV: 2
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