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How the Aggregates Determine Bound Rubber Models in Silicone Rubber? A Contrast Matching Neutron Scattering Study

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Abstract

The correlation between aggregates and bound rubber structures in silicone rubbers (S(phr)) with various silica fractions (ΦSi) has been investigated by contrast matching small-angle neutron scattering (SANS), swelling kinetics, and low-field nuclear magnetic resonance (NMR). Mixed solvents with deuterated cyclohexane fractions of 4.9% and 53.7% were chosen to match the scattering length densities of the matrix (SMP(phr)) and the filler (SMS(phr)), respectively. All the data consistently suggest that: (i) There is a critical threshold ΦSic between 10 and 30 phr; below Φsic, the isolated aggregates are dominant, while beyond Φsic, some rubber fraction is trapped among the agglomerate; (ii) Φsr-independent thicknesses around 7.5 nm (NMR) and 8.6 nm (SANS) suggest that the bound rubber formation is determined by inherent properties of the components, and the power-law around 4.2 suggests an exponential changed gradient density of the bound rubber; (iii) SMS(80) presents a bicontinuous bound rubber with three characteristic lengths of 41, 100, and 234 nm. The expanded correlation length, a 20 nm smaller aggregate sizes suggest that such existent bicontinuous network in dry samples with less ΦSi is kind of impacted by swelling. With the obtained bound rubber models, the reinforcing mechanism of filled silicone rubber is elucidated.

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Acknowledgments

This work was financially supported by the National Key R&D Program of China (No. 2018YFB0704200), the National Natural Science Foundation of China (Nos. 11605171 and 11705173), and the Foundation of President of CAEP (No. YZJJLX2018004).

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Authors and Affiliations

  1. Key Laboratory of Neutron Physics and Institute of Nuclear Physics and Chemistry (INPC), China Academy of Engineering Physics (CAEP), Mianyang, 621999, China

    Li-Zhao Huang, Yue Shui, Hong-Tao Song, Guang-Ai Sun & Dong Liu

  2. National Synchrotron Radiation Lab, CAS Key Laboratory of Soft Matter Chemistry, Anhui Provincial Engineering Laboratory of Advanced Functional Polymer Film, University of Science and Technology of China, Hefei, 230026, China

    Li-Zhao Huang & Wei Chen

  3. College of Polymer Science and Engineering, State Key Laboratory of Polymer Materials Engineering, Sichuan University, Chengdu, 610065, China

    Zhong-Ming Li, Jia-Zhuang Xu & Gan-Ji Zhong

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  1. Li-Zhao Huang
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Huang, LZ., Shui, Y., Chen, W. et al. How the Aggregates Determine Bound Rubber Models in Silicone Rubber? A Contrast Matching Neutron Scattering Study. Chin J Polym Sci 39, 365–376 (2021). https://doi.org/10.1007/s10118-020-2485-8

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