Abstract
Tyre rubber has been continuously developed to improve its performance, but the microscopic mechanisms behind these improvements, e.g. by adding nanoparticles to the rubber, are still not fully understood. We study the microscopic polymer dynamics of a rubber nanocomposite system consisting of polymer polybutadiene with 20 volume% of silica nanoparticles with diameters of 100 nm via quasi-elastic scattering experiments using gamma-ray time-domain interferometry. The result shows that the presence of silica nanoparticles caused the inter-chain α-relaxation dynamics to slow down in a shallowly supercooled state suggesting that the presence of the nanoparticles that came in contact with the polymer controlled the timescale of the polymer’s α-relaxation dynamics. Conversely, the presence of nanoparticles less affects the dynamics in a lower temperature region near T g. It is consistent with the result of the differential scanning calorimetry study showing negligible T g difference among the pure polymer and the nanocomposite system. It also shows that the quasi-elastic scattering experiment can be used to reveal the polymer dynamics in nanocomposites and is appropriate for characterising their microscopic dynamics for the purpose of improving tyre performance.
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References
Mai, Y.-W., Yu, Z.-Z.: Polymer Nanocomposites. Woodhead Publishing Ltd, Cambridge (2006)
Jancar, J., Douglas, J.F., Starr, F.W., Kumar, S.K., Cassagnau, P., Lesser, A.J., Sternstein, S.S.: Current issues in research on structure property relationships in polymer nanocomposites. Polymer 51, 3321 (2010)
Arrighi, V., Higgins, J.S., Burgess, A.N., Floudas, G.: Local dynamics of poly(dimethyl siloxane) in the presence of reinforcing filler particles. Polymer 39, 6369 (1998)
Gagliardi, S., Arrighi, V., Ferguson, R., Telling, M.T.F.: Restricted dynamics in polymer-filler systems. Physica B 301, 110 (2001)
Nusser, K., Schneidera, G.J., Richter, D.: Microscopic origin of the terminal relaxation time in polymer nanocomposites: an experimental precedent. Soft Matter 7, 7988 (2011)
Schneider, G.J., Nusser, K., Willner, L., Falus, P., Richter, D.: Dynamics of entangled chains in polymer nanocomposites. Macromolecules 44, 5857 (2011)
Roh, J.H., Tyagi, M., Hogan, T.E., Roland, C.M.: Space-dependent dynamics in 1,4-polybutadiene nanocomposite. Macromolecules 46, 6667 (2013)
Roh, J.H., Tyagi, M., Hogan, T.E., Roland, C.M.: Effect of binding to carbon black on the dynamics of 1, 4-polybutadiene. J. Chem. Phys. 139, 134905 (2013)
Glomann, T., Hamm, A., Allgaier, J., Hubner, E.G., Radulescu, A., Farago, B., Schneider, G.J.: A microscopic view on the large scale chain dynamics in nanocomposites with attractive interactions. Soft Matter 9, 10559 (2013)
Glomann, T., Schneider, G.J., Allgaier, J., Radulescu, A., Lohstroh, W., Farago, B., Richter, D.: Microscopic dynamics of polyethylene glycol chains interacting with silica nanoparticles. Phys. Rev. Lett. 110, 178001 (2013)
Schneider, G.J., Nusser, K., Neueder, S., Brodeck, M., Willner, L., Farago, B., Holderer, O., Brielsd, W.J., Richter, D.: Anomalous chain diffusion in unentangled model polymer nanocomposite. Soft Matter 9, 4336 (2013)
Guo, H., Bourret, G., Lennox, R.B., Sutton, M., Harden, J.L., Leheny, R.L.: Entanglement-controlled subdiffusion of nanoparticles within concentrated polymer solutions. Phys. Rev. Lett. 109, 055901 (2012)
Baron, A.Q.R., Franz, H., Meyer, A., Rüffer, R., Chumakov, A.I., Burkel, E., Petry, W.: Quasielastic scattering of synchrotron radiation by time domain interferometry. Phys. Rev. Lett. 79, 2823 (1997)
Saito, M., Seto, M., Kitao, S., Kobayashi, Y., Kurokuzu, M., Yoda, Y.: Time-domain interferometry experiments using multi-line nuclear absorbers. Hyperfine Interact. 206, 87 (2012)
Saito, M., Masuda, R., Yoda, Y., Seto, M.: Synchrotron radiation-based quasi-elastic scattering using time domain interferometry with multiline gamma rays. Sci. Rep. 7, 12558 (2017)
Kanaya, T., Inoue, R., Saito, M., Seto, M., Yoda, Y.: Relaxation transition in glass-forming polybutadiene as revealed by nuclear resonance X-ray scattering. J. Chem. Phys. 140, 144906 (2014)
Feigin, L.A., Svergun, D.I., Edited by Taylor, G.W.: Structure Analysis by Small-Angle X-ray and Neutron Scattering. Plenum Press, New York (1987)
Richter, D., Frick, B., Farago, B.: Neutron-spin-echo investigation on the dynamics of polybutadiene near the glass transition. Phys. Rev. Lett. 61, 2465 (1988)
Deegan, R.D., Nagel, S.R.: Dielectric susceptibility measurements of the primary and secondary relaxation in polybutadiene. Phys. Rev. B 52, 5653 (1995)
Acknowledgements
We wish to thank Prof. S. Kishimoto (High-Energy Accelerator Research Organization) for developing the detectors. We are also grateful to Prof. T. Kanaya (Material and Life Science Division, J-PARC Center, KEK) and Dr. R. Inoue (Research Reactor Institute of Kyoto University) for their constructive comments. The experiment was performed with the approval of the Japan Synchrotron Radiation Research Institute (proposal nos. 2014B3366, 2015A1397, 2015B1185, 2015A3366, 2015B3366 and 2016A3366). This work was supported by JSPS KAKENHI (Grant-in-Aid for Scientific Research (S)) Grant Number 24221005 and JSPS KAKENHI (Grant-in-Aid for Young Scientists (B)) Grant Number 15K17736.
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This article is part of the Topical Collection on Proceedings of the International Conference on the Applications of the Mössbauer Effect (ICAME 2017), Saint-Petersburg, Russia, 3-8 September 2017
Edited by Valentin Semenov
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Saito, M., Mashita, R., Kishimoto, H. et al. Effect of silica nanoparticle filler on microscopic polymer α-relaxation dynamics. Hyperfine Interact 238, 99 (2017). https://doi.org/10.1007/s10751-017-1466-y
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DOI: https://doi.org/10.1007/s10751-017-1466-y