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Dynamics of Associative Polymers with High Density of Reversible Bonds

Shifeng Nian, Shalin Patil, Siteng Zhang, Myoeum Kim, Quan Chen, Mikhail Zhernenkov, Ting Ge, Shiwang Cheng, and Li-Heng Cai (蔡历恒)
Phys. Rev. Lett. 130, 228101 – Published 31 May 2023
Physics logo See synopsis: Bond Density Not Strength Controls Polymer Stickiness
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Abstract

An associative polymer carries many stickers that can form reversible associations. For more than 30 years, the understanding has been that reversible associations change the shape of linear viscoelastic spectra by adding a rubbery plateau in the intermediate frequency range, at which associations have not yet relaxed and thus effectively act as crosslinks. Here, we design and synthesize new classes of unentangled associative polymers carrying unprecedentedly high fractions of stickers, up to eight per Kuhn segment, that can form strong pairwise hydrogen bonding of 20kBT without microphase separation. We experimentally show that reversible bonds significantly slow down the polymer dynamics but nearly do not change the shape of linear viscoelastic spectra. This behavior can be explained by a renormalized Rouse model that highlights an unexpected influence of reversible bonds on the structural relaxation of associative polymers.

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  • Received 3 May 2022
  • Revised 2 February 2023
  • Accepted 19 April 2023

DOI:https://doi.org/10.1103/PhysRevLett.130.228101

© 2023 American Physical Society

Physics Subject Headings (PhySH)

Polymers & Soft Matter

synopsis

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Bond Density Not Strength Controls Polymer Stickiness

Published 31 May 2023

Experiments show that the sticky behavior of so-called associative polymers is controlled by the density of bonding structures, contradicting theoretical predictions.

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Authors & Affiliations

Shifeng Nian1,*, Shalin Patil4,*, Siteng Zhang5, Myoeum Kim1, Quan Chen6, Mikhail Zhernenkov7, Ting Ge5, Shiwang Cheng4,‡, and Li-Heng Cai (蔡历恒)1,2,3,†

  • 1Soft Biomatter Laboratory, Department of Materials Science and Engineering, University of Virginia, Charlottesville, Virginia 22904, USA
  • 2Department of Chemical Engineering, University of Virginia, Charlottesville, Virginia 22904, USA
  • 3Department of Biomedical Engineering, University of Virginia, Charlottesville, Virginia 22904, USA
  • 4Department of Chemical Engineering and Materials Science, Michigan State University, East Lansing, Michigan 48824, USA
  • 5Department of Chemistry and Biochemistry, University of South Carolina, Columbia, South Carolina 29208, USA
  • 6State Key Lab Polymer Physics and Chemistry, Changchun Institute of Applied Chemistry, Renmin St. 5625, Changchun 130022, Jilin, People’s Republic of China
  • 7National Synchrotron Light Source-II, Brookhaven National Laboratory, Upton, New York 11973, USA

  • *These authors contributed equally to this work.
  • Corresponding author. liheng.cai@virginia.edu
  • chengsh9@msu.edu

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Issue

Vol. 130, Iss. 22 — 2 June 2023

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