Direct Structural Evidence for Interfacial Gradients in Asymmetric Polymer Nanocomposite Blends
العنوان: | Direct Structural Evidence for Interfacial Gradients in Asymmetric Polymer Nanocomposite Blends |
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المؤلفون: | Anne-Caroline Genix, Philippe Dieudonné-George, Ralf Schweins, Michael Sztucki, Alexei P. Sokolov, Bobby Carroll, Julian Oberdisse, Vera Bocharova |
المساهمون: | Laboratoire Charles Coulomb (L2C), Université de Montpellier (UM)-Centre National de la Recherche Scientifique (CNRS), Oak Ridge National Laboratory [Oak Ridge] (ORNL), UT-Battelle, LLC, European Synchrotron Radiation Facility (ESRF), Institut Laue-Langevin (ILL), ILL, The University of Tennessee [Knoxville] |
المصدر: | ACS Applied Materials & Interfaces ACS Applied Materials & Interfaces, Washington, D.C. : American Chemical Society, 2021, 13 (30), pp.36262-36274. ⟨10.1021/acsami.1c06971⟩ |
بيانات النشر: | American Chemical Society (ACS), 2021. |
سنة النشر: | 2021 |
مصطلحات موضوعية: | Materials science, Polymer nanocomposite, low-q upturn, Nanoparticle, Neutron scattering, 010402 general chemistry, 01 natural sciences, small-angle scattering, polymer nanocomposites, 0103 physical sciences, General Materials Science, interfacial segregation, concentration fluctuations, 010306 general physics, chemistry.chemical_classification, Nanocomposite, Scattering, Polymer, 0104 chemical sciences, chemistry, Chemical physics, chain-mass asymmetry, Polymer blend, Small-angle scattering, [PHYS.COND.CM-SCM]Physics [physics]/Condensed Matter [cond-mat]/Soft Condensed Matter [cond-mat.soft], isotopic polymer blends |
الوصف: | International audience; Understanding the complex structure of polymer blends filled with nanoparticles (NPs) is the key to designing their macroscopic properties. Here, the spatial distribution of hydrogenated (H) and deuterated (D) polymer chains asymmetric in mass is studied by small-angle neutron scattering. Depending on the chain mass, a qualitatively new large-scale organization of poly(vinyl acetate) chains beyond the random-phase approximation is evidenced in nanocomposites with attractive polymersilica interactions. The silica is found to systematically induce bulk segregation. Only with long H-chains, a strong scattering signature is observed in the q-range of the NP size: it is the sign of interfacial isotopic enrichment, i.e., of contrasted polymer shells close to the NP surface. A quantitative model describing both the bulk segregation and the interfacial gradient (over ca. 10-20 nm depending on the NP size) is developed, showing that both are of comparable strength. In all cases, NP surfaces trap the polymer blend in a non-equilibrium state, with preferential adsorption around NPs only if chain length and isotopic preference towards the surface combine their entropic and enthalpic driving forces. This structural evidence for interfacial polymer gradients will open the road to quantitative understanding of the dynamics of many-chain nanocomposite systems. |
تدمد: | 1944-8252 1944-8244 |
URL الوصول: | https://explore.openaire.eu/search/publication?articleId=doi_dedup___::3ae8f030a4c45b598dc62a44706beb2a https://doi.org/10.1021/acsami.1c06971 |
حقوق: | CLOSED |
رقم الأكسشن: | edsair.doi.dedup.....3ae8f030a4c45b598dc62a44706beb2a |
قاعدة البيانات: | OpenAIRE |
تدمد: | 19448252 19448244 |
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