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Related Concept Videos

Radical Reactivity: Overview01:11

Radical Reactivity: Overview

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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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Radical Formation: Overview01:03

Radical Formation: Overview

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A bond can be broken either by heterolytic bond cleavage to form ions or homolytic bond cleavage to yield radicals. A fishhook arrow is used to represent the motion of a single electron in homolytic bond cleavage. There are two main sources from which radicals can be formed:
Radicals from spin-paired molecules:
Radicals can be obtained from spin-paired molecules either by homolysis or electron transfer. While two radicals are formed in the former, an electron is added in the...
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Valence Bond Theory02:42

Valence Bond Theory

10.2K
Coordination compounds and complexes exhibit different colors, geometries, and magnetic behavior, depending on the metal atom/ion and ligands from which they are composed. In an attempt to explain the bonding and structure of coordination complexes, Linus Pauling proposed the valence bond theory, or VBT, using the concepts of hybridization and the overlapping of the atomic orbitals. According to VBT, the central metal atom or ion (Lewis acid) hybridizes to provide empty orbitals of suitable...
10.2K
Radical Formation: Addition00:47

Radical Formation: Addition

2.0K
Radicals can be formed by adding a radical to a spin-paired molecule. This is typically observed with unsaturated species, where the addition of a radical across the π bond leads to the production of a new radical by dissolving the π bond. For example, the addition of a Br radical to an alkene yields a carbon-centered radical.
Similar to charge conservation in chemical reactions, spin conservation is implicit for radical reactions. Accordingly, the product formed must possess an...
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Colors and Magnetism03:02

Colors and Magnetism

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Color in Coordination Complexes
When atoms or molecules absorb light at the proper frequency, their electrons are excited to higher-energy orbitals. For many main group atoms and molecules, the absorbed photons are in the ultraviolet range of the electromagnetic spectrum, which cannot be detected by the human eye. For coordination compounds, the energy difference between the d orbitals often allows photons in the visible range to be absorbed and emitted, which is seen as colors by the human...
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Radical Reactivity: Steric Effects01:10

Radical Reactivity: Steric Effects

2.2K
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.
Along with electronic...
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Line Shape Analysis of Dynamic NMR Spectra for Characterizing Coordination Sphere Rearrangements at a Chiral Rhenium Polyhydride Complex
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TEMPO Radical-Functionalized Supramolecular Coordination Complexes with Controllable Spin-Spin Interactions.

Wei-Ling Jiang1, Zhiyong Peng1, Bin Huang1

  • 1Shanghai Key Laboratory of Green Chemistry and Chemical Processes, School of Chemistry and Molecular Engineering, East China Normal University, Shanghai 200062, P. R. China.

Journal of the American Chemical Society
|December 28, 2020
PubMed
Summary
This summary is machine-generated.

Researchers precisely controlled spins in radical-functionalized metallacycles and cages. They observed distinct spin-spin interactions, with metallacycle 3 showing the strongest due to proximity, and demonstrated switchable zero-field splitting in solid states.

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Site Directed Spin Labeling and EPR Spectroscopic Studies of Pentameric Ligand-Gated Ion Channels
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Area of Science:

  • Supramolecular Chemistry
  • Radical Chemistry
  • Materials Science

Background:

  • Noncovalent spin-spin interactions are crucial in supramolecular radical chemistry.
  • Controlling spin number, location, and distance is key for designing novel spin materials.
  • Understanding these interactions aids in developing advanced functional materials.

Purpose of the Study:

  • To construct and investigate spin-spin interactions in TEMPO-functionalized metallacycles and cages.
  • To precisely control the spin environment through coordination-driven self-assembly.
  • To explore the influence of molecular structure and solid-state packing on spin interactions.

Main Methods:

  • Coordination-driven self-assembly to synthesize TEMPO-functionalized metallacycles (1-4) and metallacages (5-6).
  • Electron Paramagnetic Resonance (EPR) spectroscopy to study spin-spin interactions.
  • X-ray crystallography to elucidate molecular structures and solid-state arrangements.
  • Mechanical grinding and solvent vapor stimuli to induce crystal-to-amorphous transformations.

Main Results:

  • Precisely controlled spin arrangements were achieved in metallacycles and cages.
  • Metallacycle 3 exhibited stronger spin-spin interaction in solution due to shorter spin-spin distance.
  • Significant spin-spin (dipole-dipole) interactions and large zero-field splitting (ZFS) were observed in the solid state, particularly in metallacycle 4 (D = 17.5 mT).
  • Reversible switching of ZFS was achieved in metallacycle 4 and its analog 4a via crystal-to-amorphous transformations.

Conclusions:

  • The study demonstrates precise control over inter- and intramolecular spin-spin interactions in metallosupramolecular assemblies.
  • Structural modifications and solid-state packing significantly influence spin interaction strength and ZFS.
  • The reversible switching of ZFS opens avenues for developing switchable organic spin materials.