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The presence of electron-donating, electron-withdrawing, or conjugating groups adjacent to a radical center, imparts electronic stabilization to the radicals. Examples of such electronically-stabilized radicals are triphenylmethyl, tetramethylpiperidine‐N‐oxide, and 2,2‐diphenyl‐1‐picrylhydrazyl. These radicals are remarkably stable and are known as persistent radicals. Some of the persistent radicals can even be isolated and purified.
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The absorption of UV–visible light by conjugated systems causes the promotion of an electron from the ground state to the excited state. Consequently, photochemical electrocyclic reactions proceed via the excited-state HOMO rather than the ground-state HOMO. Since the ground- and excited-state HOMOs have different symmetries, the stereochemical outcome of electrocyclic reactions depends on the mode of activation; i.e., thermal or photochemical.
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Radicals, the highly reactive species, gain stability by undergoing three different reactions. The first reaction involves a radical-radical coupling, in which a radical combines with another radical, forming a spin‐paired molecule. The second reaction is between a radical and a spin‐paired molecule, generating a new radical and a new spin‐paired molecule. The third reaction is radical decomposition in a unimolecular reaction, forming a new radical and a spin‐paired...
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A Technical Guide for Performing Spectroscopic Measurements on Metal-Organic Frameworks
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Chaotropic Effect Stabilized Radical-Containing Supramolecular Organic Frameworks for Photothermal Therapy.

Wen-Zhen Li1, Hao Chen2, Meng-Na Shen1

  • 1The State Key Laboratory of Refractories and Metallurgy, School of Chemistry and Chemical Engineering, Wuhan University of Science and Technology, Wuhan, 430081, P. R. China.

Small (Weinheim an Der Bergstrasse, Germany)
|March 7, 2022
PubMed
Summary

New radical-containing supramolecular organic frameworks (SOFs) were synthesized using a chaotropic effect. These photochromic SOFs generate stable radicals upon irradiation and show potential as photothermal agents for antibacterial applications.

Keywords:
chaotropic effectsdodecaborate clustersphotothermal therapyradical-containing frameworkssupramolecular organic frameworks

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Area of Science:

  • Materials Science
  • Supramolecular Chemistry
  • Nanotechnology

Background:

  • Radical-containing frameworks (RCFs) combine ordered structures with organic radical properties.
  • Organic radicals offer unique electronic and magnetic characteristics for advanced materials.
  • Supramolecular chemistry enables the construction of complex architectures through self-assembly.

Purpose of the Study:

  • To report the first example of radical-containing supramolecular organic frameworks (SOFs).
  • To investigate the photochromic and radical-generating properties of these novel SOFs.
  • To explore the potential of these SOFs as photothermal agents for antibacterial applications.

Main Methods:

  • Fabrication of SOFs via the chaotropic effect between closo-dodecaborate clusters (B12H122-) and 2,4,6-tri(4-pyridyl)-1,3,5-triazine (TPT3+).
  • Synthesis through self-assembly in aqueous solution.
  • Characterization using light irradiation, electron paramagnetic resonance spectroscopy, and powder X-ray diffraction.

Main Results:

  • SOFs were synthesized through facile self-assembly.
  • Photochromic behavior observed upon 435 nm light irradiation, changing from yellow to dark purple.
  • Stable radicals generated in situ after irradiation, confirmed by electron paramagnetic resonance spectroscopy.
  • Maintained structural stability under light irradiation.
  • Demonstrated efficient photothermal effect under 660 nm light irradiation.

Conclusions:

  • Successfully constructed radical-containing SOFs using supramolecular self-assembly.
  • These SOFs exhibit photochromism, in situ radical generation, and structural stability.
  • The developed SOFs show promise as photothermal agents for antibacterial applications.
  • Highlights potential applications in energy, catalysis, photoluminescence, and biomedical fields.