Molecular origin of stress softening in elastomer-based nanocomposites via in situ elongational nuclear magnetic resonance spectroscopy
Abstract Understanding the molecular origin of stress softening in silica-reinforced polydimethylsiloxane remains a challenge. Here, we apply in situ elongational nuclear magnetic resonance (NMR) spectroscopy to selectively probe the polymer matrix under deformation. This allows us to address two ke...
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| Format: | Article |
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Nature Portfolio
2025-08-01
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| Series: | Communications Materials |
| Online Access: | https://doi.org/10.1038/s43246-025-00920-1 |
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| author | Yuqi Xiong Xiaojie Chen Lei Wu Chengyan Li Ai Lu Wei Chen |
| author_facet | Yuqi Xiong Xiaojie Chen Lei Wu Chengyan Li Ai Lu Wei Chen |
| author_sort | Yuqi Xiong |
| collection | DOAJ |
| description | Abstract Understanding the molecular origin of stress softening in silica-reinforced polydimethylsiloxane remains a challenge. Here, we apply in situ elongational nuclear magnetic resonance (NMR) spectroscopy to selectively probe the polymer matrix under deformation. This allows us to address two key questions: how silica nanoparticles influence microscopic polymer deformation and the critical contribution of the interfacial layer to stress softening. By exploiting differences in chain dynamics, we selectively detect protons in the polymer network strands between topological constraints and the interfacial layer. Combining in situ NMR with numerical modeling based on the nonaffine tube model helps us decouple contributions of network strand deformation and orientation to the magnetic resonance signal. We show that nanoparticles significantly influence network deformation via strand reorientation at small strains. However, the strain-independent interfacial fraction indicates a minor role for the interfacial layer in stress softening during quasistatic loading-reloading tests. |
| format | Article |
| id | doaj-art-084004e2cf3a48119cf74bc05e09eab9 |
| institution | Kabale University |
| issn | 2662-4443 |
| language | English |
| publishDate | 2025-08-01 |
| publisher | Nature Portfolio |
| record_format | Article |
| series | Communications Materials |
| spelling | doaj-art-084004e2cf3a48119cf74bc05e09eab92025-08-24T11:40:53ZengNature PortfolioCommunications Materials2662-44432025-08-016111210.1038/s43246-025-00920-1Molecular origin of stress softening in elastomer-based nanocomposites via in situ elongational nuclear magnetic resonance spectroscopyYuqi Xiong0Xiaojie Chen1Lei Wu2Chengyan Li3Ai Lu4Wei Chen5School of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, Anhui Provincial Engineering Laboratory of Advanced Functional Polymer Film, CAS Key Laboratory of Soft Matter Chemistry, University of Science and Technology of ChinaSchool of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, Anhui Provincial Engineering Laboratory of Advanced Functional Polymer Film, CAS Key Laboratory of Soft Matter Chemistry, University of Science and Technology of ChinaSchool of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, Anhui Provincial Engineering Laboratory of Advanced Functional Polymer Film, CAS Key Laboratory of Soft Matter Chemistry, University of Science and Technology of ChinaSchool of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, Anhui Provincial Engineering Laboratory of Advanced Functional Polymer Film, CAS Key Laboratory of Soft Matter Chemistry, University of Science and Technology of ChinaInstitute of Chemical Materials, China Academy of Engineering PhysicsSchool of Nuclear Science and Technology, National Synchrotron Radiation Laboratory, Anhui Provincial Engineering Laboratory of Advanced Functional Polymer Film, CAS Key Laboratory of Soft Matter Chemistry, University of Science and Technology of ChinaAbstract Understanding the molecular origin of stress softening in silica-reinforced polydimethylsiloxane remains a challenge. Here, we apply in situ elongational nuclear magnetic resonance (NMR) spectroscopy to selectively probe the polymer matrix under deformation. This allows us to address two key questions: how silica nanoparticles influence microscopic polymer deformation and the critical contribution of the interfacial layer to stress softening. By exploiting differences in chain dynamics, we selectively detect protons in the polymer network strands between topological constraints and the interfacial layer. Combining in situ NMR with numerical modeling based on the nonaffine tube model helps us decouple contributions of network strand deformation and orientation to the magnetic resonance signal. We show that nanoparticles significantly influence network deformation via strand reorientation at small strains. However, the strain-independent interfacial fraction indicates a minor role for the interfacial layer in stress softening during quasistatic loading-reloading tests.https://doi.org/10.1038/s43246-025-00920-1 |
| spellingShingle | Yuqi Xiong Xiaojie Chen Lei Wu Chengyan Li Ai Lu Wei Chen Molecular origin of stress softening in elastomer-based nanocomposites via in situ elongational nuclear magnetic resonance spectroscopy Communications Materials |
| title | Molecular origin of stress softening in elastomer-based nanocomposites via in situ elongational nuclear magnetic resonance spectroscopy |
| title_full | Molecular origin of stress softening in elastomer-based nanocomposites via in situ elongational nuclear magnetic resonance spectroscopy |
| title_fullStr | Molecular origin of stress softening in elastomer-based nanocomposites via in situ elongational nuclear magnetic resonance spectroscopy |
| title_full_unstemmed | Molecular origin of stress softening in elastomer-based nanocomposites via in situ elongational nuclear magnetic resonance spectroscopy |
| title_short | Molecular origin of stress softening in elastomer-based nanocomposites via in situ elongational nuclear magnetic resonance spectroscopy |
| title_sort | molecular origin of stress softening in elastomer based nanocomposites via in situ elongational nuclear magnetic resonance spectroscopy |
| url | https://doi.org/10.1038/s43246-025-00920-1 |
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