Nonlinear Viscoelasticity Raised at Low Temperatures by Intermolecular Cooperation of Bulk Amorphous Polymers

Ji-Ping Wang; Wen-Bing Hu

doi:10.1007/s10118-021-2624-x

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Nonlinear Viscoelasticity Raised at Low Temperatures by Intermolecular Cooperation of Bulk Amorphous Polymers

ARTICLE | Updated：2021-07-22

- Nonlinear Viscoelasticity Raised at Low Temperatures by Intermolecular Cooperation of Bulk Amorphous Polymers
- Chinese Journal of Polymer Science Vol. 39, Issue 11, Pages: 1496-1501(2021)
- Affiliations：
  
  Department of Polymer Science and Engineering, State Key Lab of Coordination Chemistry, School of Chemistry and Chemical Engineering, Nanjing University, Nanjing 210023, China
- Author bio：
  
  wbhu@nju.edu.cn
- Funds：
- DOI：10.1007/s10118-021-2624-x
  CLC：
- Received：12 May 2021，
  
  Revised：2021-6-6，
  
  Accepted：21 June 2021，
  
  Online First：22 July 2021，
  
  Published：18 September 2021
- Accepted：
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Wang, J. P.; Hu, W. B. Nonlinear viscoelasticity raised at low temperatures by intermolecular cooperation of bulk amorphous polymers. Chinese J. Polym. Sci. 2021, 39, 1496–1501

Ji-Ping Wang, Wen-Bing Hu. Nonlinear Viscoelasticity Raised at Low Temperatures by Intermolecular Cooperation of Bulk Amorphous Polymers[J]. Chinese Journal of Polymer Science, 2021, 39(11): 1496-1501.
Wang, J. P.; Hu, W. B. Nonlinear viscoelasticity raised at low temperatures by intermolecular cooperation of bulk amorphous polymers. Chinese J. Polym. Sci. 2021, 39, 1496–1501 DOI： 10.1007/s10118-021-2624-x.

Ji-Ping Wang, Wen-Bing Hu. Nonlinear Viscoelasticity Raised at Low Temperatures by Intermolecular Cooperation of Bulk Amorphous Polymers[J]. Chinese Journal of Polymer Science, 2021, 39(11): 1496-1501. DOI： 10.1007/s10118-021-2624-x.

摘要

Abstract

We performed dynamic Monte Carlo simulations of stress relaxation in parallel-aligned and uniaxially stretched bulk amorphous polymers at low temperatures. We observed an extra-slowing down in the early stage of stress relaxation

which causes nonlinear viscoelasticity as deviated from Debye relaxation and Arrhenius-fluid behaviors observed previously at high temperatures. Meanwhile

fluctuation analysis of stress relaxation revealed a substantial increase in the stretch fractions of polymers at the transient periods of high-temperature Debye relaxation. Structural analysis of free volume further revealed the scenario that

at low temperatures

the modulus of polymer entropy elasticity decreases with temperature and eventually loses its competition to the imposed modulus (Deborah number becomes larger than one)

and hence upon stress relaxation under constant strains

monomers are firstly accumulated nearby two stretching ends of polymers

resulting in tentative global jamming like physical cross-linking there

and thus retarding the coming transient state of stress relaxation. We concluded that intermolecular cooperation raises physical crosslinking for nonlinear viscoelasticity of polymer stress relaxation as well as the rubbery states unique to bulk amorphous polymers. The new microscopic mechanism of the fluid-rubbery transition of polymers may bring insights into the intermolecular cooperation mechanism of glass transition of small molecules

if the fluid-rubbery transition is regarded as an extrapolation of glass transition from low to high molecular weights.

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