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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 Reactivity: Steric Effects01:10

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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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Radical Chain-Growth Polymerization: Overview01:10

Radical Chain-Growth Polymerization: Overview

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Chain-growth or addition polymerization is successive addition reactions of monomers with a polymer chain. In radical chain-growth polymerization, the reaction proceeds via a free-radical intermediate. The free radical is formed from radical initiators, which spontaneously generate free radicals by homolytic fission. Organic peroxides (such as dibenzoyl peroxide, as shown in Figure 1) or azo compounds are popular radical initiators. A low concentration ratio of radical initiator to monomer is...
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Radical Chain-Growth Polymerization: Mechanism01:09

Radical Chain-Growth Polymerization: Mechanism

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The radical chain-growth polymerization mechanism consists of three steps: initiation, propagation, and termination of polymerization. The polymerization initiates when a free radical generated from the radical initiator adds to the unsaturated bond in the monomer. The unpaired electron of the free radical and one π electron in the unsaturated bond creates a σ bond between the free radical and the monomer. As a result, the other π electron in the unsaturated bond converts this...
2.6K
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...
2.1K
Radical Formation: Elimination00:51

Radical Formation: Elimination

1.8K
Another method of radical formation is the elimination process. It is the opposite of the addition route and is driven by the instability of the radical. For example, as depicted in Figure 1, dibenzoyl peroxide yields a pair of unstable radicals upon homolysis. Given its instability, this radical spontaneously undergoes elimination via a C–C bond cleavage to form a relatively more stable phenyl radical. The mechanism involves cleavage of the bond between the α and β positions...
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Fabrication of Large-area Free-standing Ultrathin Polymer Films
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Long-Term Degradation Mechanisms in Application-Implemented Radical Thin Films.

Ewa Malgorzata Nowik-Boltyk1, Tobias Junghoefer1, Mathias Glaser1

  • 1Institute of Physical and Theoretical Chemistry, University of Tübingen, 72076 Tübingen, Germany.

ACS Applied Materials & Interfaces
|June 15, 2023
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Blatter radical thin films degrade due to contaminants like atomic hydrogen and molecular water. Water specifically impacts diradical films, shortening their lifespan in air.

Keywords:
Blatter radicalsab initio simulationsdegradationorganic radicalsphotoemissionthin films

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Area of Science:

  • Organic radical chemistry
  • Materials science
  • Thin film degradation

Background:

  • Blatter radical derivatives show promise for applications in batteries and quantum technologies.
  • Understanding the long-term stability of radical thin films is crucial for their practical implementation.

Purpose of the Study:

  • To investigate the fundamental degradation mechanisms of Blatter radical thin films.
  • To compare the effects of various contaminants on two different Blatter radical derivatives.
  • To elucidate the role of contaminant interaction sites on film properties.

Main Methods:

  • Thin film preparation of two Blatter radical derivatives.
  • Exposure of films to various atomic and molecular contaminants (H, Ar, N, O, H2, N2, O2, H2O, NH2).
  • Analysis of chemical and magnetic property changes upon air exposure.

Main Results:

  • Contaminant interactions significantly alter the chemical and magnetic properties of Blatter radical thin films.
  • Atomic hydrogen and ammonia (NH2) negatively impact the magnetic properties of Blatter radicals.
  • Molecular water specifically affects the magnetic properties of diradical thin films, contributing to their reduced lifetime.

Conclusions:

  • The degradation of Blatter radical thin films is influenced by specific contaminant interactions.
  • Molecular water is identified as a primary factor limiting the stability of diradical thin films in air.
  • Site-specific interactions between contaminants and radicals dictate the degradation pathways and resulting film properties.