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    Effect of Polymer Chemistry on the Linear Viscoelasticity of Complex Coacervates
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    • Yalin Liu
      Yalin Liu
      Department of Chemical Engineering, University of Massachusetts Amherst, Amherst, Massachusetts 01003, United States
      More by Yalin Liu
    • Cristiam F. Santa Chalarca
      Cristiam F. Santa Chalarca
      Department of Polymer Science & Engineering, University of Massachusetts Amherst, Amherst, Massachusetts 01003, United States
      More by Cristiam F. Santa Chalarca
    • R. Nicholas Carmean
      R. Nicholas Carmean
      George & Josephine Butler Polymer Research Laboratory, Center for Macromolecular Science & Engineering, Department of Chemistry, University of Florida, Gainesville, Florida 32611, United States
      More by R. Nicholas Carmean
    • Rebecca A. Olson
      Rebecca A. Olson
      George & Josephine Butler Polymer Research Laboratory, Center for Macromolecular Science & Engineering, Department of Chemistry, University of Florida, Gainesville, Florida 32611, United States
      More by Rebecca A. Olson
    • Jason Madinya
      Jason Madinya
      Department of Chemical and Biomolecular Engineering, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States
      More by Jason Madinya
    • Brent S. Sumerlin
      Brent S. Sumerlin
      George & Josephine Butler Polymer Research Laboratory, Center for Macromolecular Science & Engineering, Department of Chemistry, University of Florida, Gainesville, Florida 32611, United States
      More by Brent S. Sumerlin
      Orcidhttp://orcid.org/0000-0001-5749-5444
    • Charles E. Sing
      Charles E. Sing
      Department of Chemical and Biomolecular Engineering, University of Illinois at Urbana-Champaign, Urbana, Illinois 61801, United States
      More by Charles E. Sing
      Orcidhttp://orcid.org/0000-0001-7231-2685
    • Todd Emrick
      Todd Emrick
      Department of Polymer Science & Engineering, University of Massachusetts Amherst, Amherst, Massachusetts 01003, United States
      More by Todd Emrick
      Orcidhttp://orcid.org/0000-0003-0460-1797
    • Sarah L. Perry*
      Sarah L. Perry
      Department of Chemical Engineering, University of Massachusetts Amherst, Amherst, Massachusetts 01003, United States
      *Email: [email protected]
      More by Sarah L. Perry
      Orcidhttp://orcid.org/0000-0003-2301-6710
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    Macromolecules

    Cite this: Macromolecules 2020, 53, 18, 7851–7864
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    https://doi.org/10.1021/acs.macromol.0c00758
    Published September 10, 2020
    Copyright © 2020 American Chemical Society
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    Abstract

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    Complex coacervates can form through the electrostatic complexation of oppositely charged polymers. The material properties of the resulting coacervates can change based on the polymer chemistry and the complex interplay between electrostatic interactions and water structure, controlled by salt. We examined the effect of varying the polymer backbone chemistry using methacryloyl- and acryloyl-based complex coacervates over a range of polymer chain lengths and salt conditions. We simultaneously quantified the coacervate phase behavior and the linear viscoelasticity of the resulting coacervates to understand the interplay between polymer chain length, backbone chemistry, polymer concentration, and salt concentration. Time-salt superposition analysis was used to facilitate a broader characterization and comparison of the stress relaxation behavior between different coacervate samples. Samples with mismatched polymer chain lengths highlighted the ways in which the shortest polymer chain can dominate the resulting coacervate properties. A comparison between coacervates formed from methacryloyl vs acryloyl polymers demonstrated that the presence of a backbone methyl group affects the phase behavior, and thus the rheology in such a way that coacervates formed from methacryloyl polymers have a similar phase behavior to those of acryloyl polymers with ∼10× longer polymer chains.

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    • Details on the synthesis and characterization of monomers; polymer characterization; calibration curves for salt concentration as a function of solution conductivity; propagation of error analysis; tabulated binodal curve data including uncertainty and potential systematic errors; individual and comparison binodal curve plots with error bars; plots of salt partitioning trends; Cole–Cole plots; individual and comparison plots of horizontal and vertical shift factors as a function of salt and polymer concentration; tabulated parameters describing fits to shift factor data; and additional rheology comparison graphs (PDF)

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    Macromolecules

    Cite this: Macromolecules 2020, 53, 18, 7851–7864
    Click to copy citationCitation copied!
    https://doi.org/10.1021/acs.macromol.0c00758
    Published September 10, 2020
    Copyright © 2020 American Chemical Society
    Request reuse permissions

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