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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...
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Radical Formation: Homolysis00:54

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A bond is formed between two atoms by sharing two electrons. When this bond is broken by supplying sufficient energy, either two electrons can be taken up by one atom forming ions by the cleavage called heterolysis, or the two electrons are shared by two atoms, with one each creating radicals by the cleavage called homolysis.
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Radical Chain-Growth Polymerization: Overview01:10

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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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Step-Growth Polymerization: Overview01:03

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Step-growth or condensation polymerization is a stepwise reaction of bi or multifunctional monomers to form long-chain polymers. As all the monomers are reactive, most of the monomers are consumed at the early stages of the reaction to form small chains of reactive oligomers, which then combine to form long polymer chains in the late stages. Hence, the reaction has to proceed for a long time to achieve high molecular weight polymers.
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Formation of Halohydrin from Alkenes02:41

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An alkene, such as propene, reacts with bromine in the presence of water to yield a halohydrin. Halohydrins contain a halogen and a hydroxyl group attached to adjacent carbons. When the halogen is bromine, it is called a bromohydrin, while a chlorohydrin has chlorine as the halogen.
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Electrophilic Addition to Alkynes: Hydrohalogenation02:35

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Electrophilic addition of hydrogen halides, HX (X = Cl, Br or I) to alkenes forms alkyl halides as per Markovnikov's rule, where the hydrogen gets added to the less substituted carbon of the double bond. Hydrohalogenation of alkynes takes place in a similar manner, with the first addition of HX forming a vinyl halide and the second giving a geminal dihalide.
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Fabricating Degradable Thermoresponsive Hydrogels on Multiple Length Scales via Reactive Extrusion, Microfluidics, Self-assembly, and Electrospinning
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Dual Temperature- and pH-Responsive Layered Hydrogels Synthesized via Halogen Bond-Based Solid Phase Radical

Lyly Hui Ting Leow1, Hong Tho Le1, Atsushi Goto1

  • 1School of Chemistry, Chemical Engineering and Biotechnology, Nanyang Technological University, 62 Nanyang Drive, Singapore 637459, Singapore.

ACS Applied Materials & Interfaces
|February 3, 2025
PubMed
Summary

Researchers developed novel stimuli-responsive hydrogels using solid-phase polymerization. These layered hydrogel sheets exhibit tunable shape changes in response to temperature and pH, offering versatile material fabrication.

Keywords:
bendingconvex-concave-trapezoid shape changedual temperature- and pH-responsive layered hydrogel sheetshalogen bondingsolid phase polymerization

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Area of Science:

  • Materials Science
  • Polymer Chemistry
  • Supramolecular Chemistry

Background:

  • Stimuli-responsive hydrogels are crucial for advanced applications.
  • Fabricating complex layered hydrogel structures with controlled shape-changing properties remains challenging.

Purpose of the Study:

  • To develop a facile and versatile method for preparing stimuli-responsive shape-changing layered hydrogels.
  • To demonstrate dual-responsive (temperature and pH) shape-changing behaviors in bilayer and trilayer hydrogel sheets.

Main Methods:

  • Utilized halogen bond-based solid-phase radical polymerization to create layered hydrogel sheets.
  • Assembled monomer cocrystals into predetermined layered structures prior to polymerization.
  • Prepared AB bilayer and ABA/ABC trilayer hydrogel sheets with temperature- and pH-responsive layers.

Main Results:

  • Achieved dual responsiveness to temperature (5-65 °C) and pH (2.0-11.0) in layered hydrogel sheets.
  • Demonstrated tunable bending in bilayer sheets with switchable directionality.
  • Exhibited unprecedented switchable concave, trapezoid, and convex shape changes in trilayer sheets.

Conclusions:

  • The solid-phase polymerization method provides a facile and versatile approach for fabricating stimuli-responsive shape-changing hydrogel materials.
  • The developed hydrogels exhibit unique and controllable shape-morphing capabilities.
  • This technique offers broad applicability due to its wide monomer scope and ease of operation.