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Nonlinear stress relaxation and failure of time‒strain separability of aqueous poly(ethylene oxide)/silica nanoparticle mixtures

Polymer Journal volume 57, pages 163–170 (2025)Cite this article

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Abstract

The stress relaxation test is an effective and facile method for clarifying the nonlinear rheological behavior of soft materials. A thorough analysis of the stress relaxation behavior offers valuable insights into the molecular dynamics. However, the stress relaxation behavior and underlying molecular dynamics of polymer/particle mixtures remain poorly understood, despite their widespread industrial application. In this study, we systematically investigated the nonlinear stress relaxation behavior of a simple-structured poly(ethylene oxide) (PEO)/silica nanoparticle aqueous mixture. Time‒strain separability was observed at high polymer concentrations, with the stress relaxation attributable to the relaxation of the polymer matrix. At lower polymer concentrations, the time‒strain separability was no longer valid, and changes in absorbance over time suggested that stress relaxation originated from the relaxation of the aggregated structures. A transition from time‒strain separability to inseparability was observed when the estimated number of PEO molecules forming interparticle bridges was less than 1; this suggests that structural changes during shear loading occur only when new interparticle polymer bridges are formed, leading to the development of clustered structures. These results provide a basic understanding of the relationship between deformation and relaxation, which is crucial for systematically understanding the nonlinear rheology of polymeric materials.

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Acknowledgements

This work was supported by the Japan Society for the Promotion of Science (JSPS) through Grants-in-Aid for JSPS Fellows (No. 22J21871 to SK) and the Mitsubishi Foundation to YA.

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Authors and Affiliations

  1. Department of Bioengineering, Graduate School of Engineering, The University of Tokyo, Bunkyo-ku, Tokyo, Japan

    Saki Kusakabe, Takuya Katashima & Ichiro Sakuma

  2. Department of Applied Physics, Tokyo University of Agriculture and Technology, Koganei-shi, Tokyo, Japan

    Yuki Akagi

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  1. Saki Kusakabe
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  2. Takuya Katashima
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  3. Ichiro Sakuma
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  4. Yuki Akagi
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Correspondence to Yuki Akagi.

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Kusakabe, S., Katashima, T., Sakuma, I. et al. Nonlinear stress relaxation and failure of time‒strain separability of aqueous poly(ethylene oxide)/silica nanoparticle mixtures. Polym J 57, 163–170 (2025). https://doi.org/10.1038/s41428-024-00974-x

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