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The skeletal structure of polymers synthesized via radical polymerization is always branched. For example, the polymerization of ethylene by radical polymerization results in a low-density grade of polyethylene with a heavily branched skeletal structure. Here, the radical site abstracts hydrogen from the growing chain, and the radical site shifts from the end (a primary carbon center) to anywhere within the growing chain (a secondary carbon center). Consequently, the part of the chain from the...
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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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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 species into...
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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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Slip-spring simulations of different constraint release environments for linear polymer chains.

Teng Ma1, Guochang Lin1,2, Huifeng Tan1,2

  • 1Centre for Composite Materials and Structures, Harbin Institute of Technology, Harbin 150080, People's Republic of China.

Royal Society Open Science
|April 10, 2020
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Constraint release (CR) accelerates polymer relaxation, particularly viscoelastic relaxation. Simulations using the slip-spring model validate these findings and demonstrate flexibility in modeling diverse CR environments.

Keywords:
constraint releasepolymer chainsslip-spring model

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Area of Science:

  • Polymer Physics
  • Rheology
  • Computational Materials Science

Background:

  • Constraint release (CR) significantly influences polymer chain dynamics and relaxation behavior.
  • Previous studies demonstrated CR accelerates both dielectric and viscoelastic relaxation in linear polyisoprene (PI) chains.
  • Understanding CR effects is crucial for predicting polymer melt properties in various topological environments.

Purpose of the Study:

  • To validate the accelerating effects of CR on dielectric and viscoelastic relaxation using simulations.
  • To reproduce experimental data from Matsumiya et al. (2013) with the single slip-spring (SSp) model.
  • To develop and test a flexible SSp model capable of simulating diverse CR environments.

Main Methods:

  • Utilized the single slip-spring (SSp) model to simulate polymer relaxation dynamics.
  • Employed a probe version of the SSp model to analyze end-to-end and viscoelastic relaxation coincidence.
  • Developed a variant SSp model incorporating characteristic lifetimes for entanglements to simulate various CR environments.

Main Results:

  • Simulations confirmed that CR accelerates both dielectric and viscoelastic relaxation, with a more pronounced effect on viscoelastic relaxation.
  • The SSp model successfully reproduced experimental data for monodisperse and bidisperse polymer melts.
  • The lifetime version SSp model accurately described relaxation functions and CR environments.

Conclusions:

  • The single slip-spring model effectively validates the CR mechanism's accelerating impact on polymer relaxation.
  • The proposed lifetime version SSp model offers a flexible and accurate approach to simulating polymer dynamics in complex CR environments.
  • This work provides strong computational evidence supporting experimental observations of CR effects in polymer melts.