Journal
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
Volume 57, Issue 27, Pages 8007-8011Publisher
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.201801998
Keywords
covalent organic frameworks; materials science; oxygen reduction reaction; radicals; structure elucidation
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Funding
- NRF CRP grant [NRF-CRP16-2015-02]
- MOE Tier 3 programme [MOE2014-T3-1-004]
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Reported is the synthesis, characterization, and material properties of the first pi-conjugated two-dimensional covalent organic radical framework (CORF), PTM-CORF, based on the stable polychlorotriphenylmethyl (PTM) radical. The covalent organic framework (COF) precursor (PTM-H-COF) was first synthesized by liquid/liquid interfacial acetylenic homocoupling of a triethynylpolychlorotriphenylmethane monomer, and showed crystalline features with a hexagonal diffraction pattern matching that of A-B-C stacking. Subsequent deprotonation and oxidation of the PTM units in PTM-H-COF gave PTM-CORF. Magnetic measurements revealed that the neighboring PTM radicals in the PTM-CORF are anti-ferromagnetically coupled each other, with a moderate exchange interaction (J = -375 cm(-1)). The PTM-CORF has a small energy gap (ca. 0.88 eV) and a low-lying LUMO energy level (-4.72 eV), and exhibits high electrocatalytic activity and durability toward the oxygen reduction reaction.
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