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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

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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...
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Radical Formation: Addition00:47

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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

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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

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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.
Along with electronic...
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Complejos de coordinación supramoleculares funcionalizados con radicales TEMPO con interacciones espín-espín

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
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Resumen

Los investigadores controlaron con precisión los giros en celdas y metales funcionalizados por radicales. Observaron distintas interacciones espín-espín, con el ciclo metálico 3 mostrando el más fuerte debido a la proximidad, y demostraron la división de campo cero conmutable en estados sólidos.

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Área de la Ciencia:

  • Química supramolecular
  • La Química Radical
  • Ciencias de los materiales

Sus antecedentes:

  • Las interacciones espín-espín no covalentes son cruciales en la química radical supramolecular.
  • Controlar el número de espín, la ubicación y la distancia es clave para diseñar nuevos materiales de espín.
  • La comprensión de estas interacciones ayuda en el desarrollo de materiales funcionales avanzados.

Objetivo del estudio:

  • Construir e investigar las interacciones espín-espín en los metalciclos y las jaulas funcionalizadas por TEMPO.
  • Para controlar con precisión el entorno de giro a través del autoensamblaje impulsado por la coordinación.
  • Para explorar la influencia de la estructura molecular y el embalaje en estado sólido en las interacciones de espín.

Principales métodos:

  • Autoensamblaje impulsado por la coordinación para la síntesis de metales funcionalizados con TEMPO (1-4) y metales envasados (5-6).
  • Espectroscopia de resonancia paramagnética de electrones (EPR) para el estudio de las interacciones espín-espín.
  • Cristalografía de rayos X para dilucidar las estructuras moleculares y los arreglos en estado sólido.
  • Moldeo mecánico y estímulos de vapor de disolvente para inducir transformaciones de cristal a amorfo.

Principales resultados:

  • Se lograron arreglos de giro controlados con precisión en metaciclos y jaulas.
  • Metallacycle 3 exhibió una mayor interacción espín-espín en solución debido a la menor distancia espín-espín.
  • Se observaron importantes interacciones espín-espín (dipolo-dipolo) y una gran división de campo cero (ZFS) en estado sólido, particularmente en el ciclo metálico 4 (D = 17,5 mT).
  • La conmutación reversible de ZFS se logró en el ciclo metálico 4 y su análogo 4a a través de transformaciones de cristal a amorfo.

Conclusiones:

  • El estudio demuestra un control preciso de las interacciones espín-espín intermoleculares e intramoleculares en conjuntos metalosupramoleculares.
  • Las modificaciones estructurales y el embalaje en estado sólido influyen significativamente en la resistencia a la interacción de espín y el ZFS.
  • La conmutación reversible de ZFS abre vías para el desarrollo de materiales de espín orgánicos conmutables.