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PreprintCC BYChemRxiv

Interfacial Chain Mobility in Polymer–Silica Elastomers Governs the Balance between Biocompatibility and Tissue-Like Mechanics

  • Daiki Miyake1,2
  • Karin Ito1,2
  • Moeka Higuchi1,2
  • Moe Sakamoto1,2
  • Fumio Asai1,2
  • Xiaobin Liang3,4
  • Ken Nakajima3,4
  • Taiki Hoshino5,6,7
  • Daichi Nozaki8,9
  • Kenji Urayama8,9
  • Masaru Tanaka10,11
  • Jea-Marie Raquez12
2 more authors
  • Jeremy Odent12
  • Yukikazu Takeoka1,2
12 affiliations
  1. 1Department of Molecular & Macromolecular Chemistry
  2. 2Nagoya University
  3. 3School of Materials and Chemical Technology
  4. 4Institute of Science Tokyo
  5. 5International Center for Synchrotron Radiation Innovation Smart, Tohoku University, Aoba-ku, Sendai, Japan, 980-8572
  6. 6RIKEN SPring-8 Center, 1-1-1 Kouto, Sayo-cho, Sayo-gun, Hyogo, Japan, 679-5148
  7. 7Institute of Multidisciplinary Research for Advanced Materials, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai, Japan, 980-8577
  8. 8Department of Material Chemistry
  9. 9Kyoto University
  10. 10Department of Applied Chemistry
  11. 11Kyushu University
  12. 12Laboratory of Polymeric and Composite Materials (LPCM, University of Mons (UMONS, Place du Parc 20, Mons, Belgium, 7000
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Abstract

Soft biological tissues combine biocompatibility, viscoelastic energy dissipation and J-shaped nonlinear elasticity, yet the molecular principles for reproducing these properties in artificial soft materials remain unclear. Here we identify interfacial chain mobility, rather than interaction strength, as a key parameter governing tissue-like mechanics in composite elastomers. Using non-aggregated silica particles dispersed in biocompatible PMEA and PMEO2MA networks, we decouple polymer–particle interactions from filler aggregation. Strong multipoint interactions in PMEO2MA create a constrained interphase that suppresses chain mobility and promotes premature stiffening. By contrast, moderate PMEA–silica interactions preserve interfacial mobility while enabling efficient stress transfer. This balance produces J-shaped elasticity through finite chain extensibility and pronounced hysteresis through reversible interfacial stress transfer. Our results reveal complementary molecular origins of nonlinear elasticity and energy dissipation, establishing interfacial chain mobility as a design principle for biointegrated soft materials combining flexibility, damping, biocompatibility and tissue-like mechanical performance.

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Cite

BibTeXRIS
BibTeX
@misc{miyake2026interfacial,
  title = {{Interfacial Chain Mobility in Polymer–Silica Elastomers Governs the Balance between Biocompatibility and Tissue-Like Mechanics}},
  author = {Daiki Miyake and Karin Ito and Moeka Higuchi and Moe Sakamoto and Fumio Asai and Xiaobin Liang and Ken Nakajima and Taiki Hoshino and Daichi Nozaki and Kenji Urayama and Masaru Tanaka and Jea-Marie Raquez and Jeremy Odent and Yukikazu Takeoka},
  howpublished = {ChemRxiv},
  year = {2026},
  month = sep,
  doi = {10.26434/chemrxiv.15008986/v1},
  url = {https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008986/v1},
  note = {CC BY},
}
RIS
TY  - UNPB
TI  - Interfacial Chain Mobility in Polymer–Silica Elastomers Governs the Balance between Biocompatibility and Tissue-Like Mechanics
AU  - Daiki Miyake
AU  - Karin Ito
AU  - Moeka Higuchi
AU  - Moe Sakamoto
AU  - Fumio Asai
AU  - Xiaobin Liang
AU  - Ken Nakajima
AU  - Taiki Hoshino
AU  - Daichi Nozaki
AU  - Kenji Urayama
AU  - Masaru Tanaka
AU  - Jea-Marie Raquez
AU  - Jeremy Odent
AU  - Yukikazu Takeoka
PY  - 2026
DA  - 2026/09/17
PB  - ChemRxiv
DO  - 10.26434/chemrxiv.15008986/v1
UR  - https://chemrxiv.org/doi/full/10.26434/chemrxiv.15008986/v1
AB  - Soft biological tissues combine biocompatibility, viscoelastic energy dissipation and J-shaped nonlinear elasticity, yet the molecular principles for reproducing these properties in artificial soft materials remain unclear. Here we identify interfacial chain mobility, rather than interaction strength, as a key parameter governing tissue-like mechanics in composite elastomers. Using non-aggregated silica particles dispersed in biocompatible PMEA and PMEO2MA networks, we decouple polymer–particle interactions from filler aggregation. Strong multipoint interactions in PMEO2MA create a constrained interphase that suppresses chain mobility and promotes premature stiffening. By contrast, moderate PMEA–silica interactions preserve interfacial mobility while enabling efficient stress transfer. This balance produces J-shaped elasticity through finite chain extensibility and pronounced hysteresis through reversible interfacial stress transfer. Our results reveal complementary molecular origins of nonlinear elasticity and energy dissipation, establishing interfacial chain mobility as a design principle for biointegrated soft materials combining flexibility, damping, biocompatibility and tissue-like mechanical performance.
ER  -