Linear and nonlinear viscoelasticity of concentrated thermoresponsive microgel suspensions

Chaudhary, Gaurav; Ghosh, Ashesh; Kang, Jin Gu; Braun, Paul V.; Ewoldt, Randy H.; Schweizer, Kenneth S.

doi:10.1016/j.jcis.2021.05.111

Linear and nonlinear viscoelasticity of concentrated thermoresponsive microgel suspensions

Journal Article · Sun May 23 00:00:00 EDT 2021 · Journal of Colloid and Interface Science

DOI:https://doi.org/10.1016/j.jcis.2021.05.111· OSTI ID:1875532

^[1]; ^[2]; Kang, Jin Gu ^[3]; ^[4]; ^[4]; Schweizer, Kenneth S. ^[4]

Univ. of Illinois at Urbana-Champaign, IL (United States); Harvard Univ., Cambridge, MA (United States); University of Illinois
Univ. of Illinois at Urbana-Champaign, IL (United States); Stanford Univ., CA (United States)
Univ. of Illinois at Urbana-Champaign, IL (United States); Korea Inst. of Science and Technology, Seoul (South Korea)
Univ. of Illinois at Urbana-Champaign, IL (United States)

We present an integrated experimental and theoretical study of the dynamics and rheology of self-crosslinked, slightly charged, temperature responsive soft poly(N-isopropylacrylamide) (pNIPAM) microgels over a wide range of concentration and temperature spanning the sharp change in particle size and intermolecular interactions across the lower critical solution temperature (LCST). Dramatic, non-monotonic changes in viscoelasticity are observed as a function of temperature, with distinct concentration dependence in the dense fluid, glassy, and soft-jammed regimes. Motivated by our experimental observations, we formulate a minimalistic model for the size dependence of a single microgel particle and the change of the interparticle interaction from purely repulsive to attractive upon heating. Using microscopic equilibrium and time-dependent statistical mechanical theories, theoretical predictions are quantitatively compared with experimental measurements of the shear modulus. Good agreement is found for the nonmonotonic temperature behavior that originates as a consequence of the competition between reduced microgel packing fraction and increasing interparticle attractions. Furthermore, testable predictions are made for nonlinear rheological properties such as the yield stress and strain. To our knowledge, this is the first attempt to quantitatively understand in a unified manner the viscoelasticity of dense, temperature-responsive microgel suspensions spanning a wide range of temperatures and concentrations.

View Accepted Manuscript (DOE)

Research Organization:: Univ. of Illinois at Urbana-Champaign, IL (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE Office of Science (SC), Basic Energy Sciences (BES). Materials Sciences & Engineering Division

Grant/Contract Number:: FG02-07ER46471; SC0020858

OSTI ID:: 1875532

Alternate ID(s):: OSTI ID: 1798905

Journal Information:: Journal of Colloid and Interface Science, Journal Name: Journal of Colloid and Interface Science Vol. 601; ISSN 0021-9797

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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