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http://www.complexfluids.ethz.ch/snf19 This project is supported by the Swiss National Supercomputing Centre
Complex interfaces stabilized by proteins, polymers or nanoparticles, have a much richer dynamics than those stabilized by simple surfactants. By subjecting fluid-fluid interfaces to step extension-compression deformations, we show that in general these complex interfaces have dynamic heterogeneity in their relaxation response that is well described by a Kohlrausch-Williams-Watts function, with stretch exponent beta between 0.4-0.6 for extension, and 0.6-1.0 for compression. The difference in beta between expansion and compression points to an asymmetry in the dynamics. Using atomic force microscopy and simulations we prove that the dynamic heterogeneity is intimately related to interfacial structural heterogeneity and show that the dominant mode for stretched exponential relaxation is momentum transfer between bulk and interface, a mechanism which has so far largely been ignored in experimental surface rheology. We describe how its rate constant can be determined using molecular dynamics simulations. These interfaces clearly behave like disordered viscoelastic solids and need to be described substantially different from the 2d homogeneous viscoelastic fluids typically formed by simple surfactants. [Sagis, Leonard M. C.; Essers, Jeffrey; Yang, Jack] Wageningen Univ, Phys & Phys Chem Foods, Bornse Weilanden 9, NL-6708 WG Wageningen, Netherlands. [Sagis, Leonard M. C.; Moghimikheirabadi, Ahmad] Swiss Fed Inst Technol, Dept Mat, Polymer Phys, Leopold Ruzicka Weg 4, CH-8093 Zurich, Switzerland. [Liu, Bingxue; Li, Yuan] China Agr Univ, Coll Food Sci & Nutr Engn, Key Lab Funct Dairy, Beijing Adv Innovat Ctr Food Nutr & Human Hlth, Beijing 100083, Peoples R China. [Essers, Jeffrey; Hinderink, Emma; Berton-Carabin, Claire; Schroen, Karin] Wageningen Univ, Food Proc Engn Grp, NL-6700 AA Wageningen, Netherlands. Sagis, LMC (corresponding author), Wageningen Univ, Phys & Phys Chem Foods, Bornse Weilanden 9, NL-6708 WG Wageningen, Netherlands.; Sagis, LMC (corresponding author), Swiss Fed Inst Technol, Dept Mat, Polymer Phys, Leopold Ruzicka Weg 4, CH-8093 Zurich, Switzerland.; Li, Y (corresponding author), China Agr Univ, Coll Food Sci & Nutr Engn, Key Lab Funct Dairy, Beijing Adv Innovat Ctr Food Nutr & Human Hlth, Beijing 100083, Peoples R China. leonard.sagis@wur.nl; yuanli@cau.edu.cn Yang, Jack/0000-0001-8217-1759; Moghimikheirabadi, Ahmad/0000-0001-6836-1521; Berton-Carabin, Claire/0000-0002-5585-640X National Natural Science Foundation of ChinaNational Natural Science Foundation of China (NSFC) [NSFC31471577]; NWO Earth and Life Sciences [ALWTF. 2016.001]; Swiss National Science FoundationSwiss National Science Foundation (SNSF)European Commission [200021 156106] L.M.C.S would like to acknowledge insightful discussions of this manuscript with Patrick Ilg (University of Reading) and Hans Christian Ottinger (ETH Zurich). This work was financially supported by National Natural Science Foundation of China (NSFC31471577), by NWO Earth and Life Sciences (project ALWTF. 2016.001), and by the Swiss National Science Foundation (Grant No. 200021 156106). 44 [hide]
Principal Investigators
Argyrios Karatrantos (PI)
Institute of Science and Technology, Luxembourg ►
Martin Kröger (PI)
Polymer Physics, ETH Zurich, Switzerland ►
Project Partners
Clement Mugemana
Institute of Science and Technology, Luxembourg ►
Jeremy Odent
Laboratory of polymeric and composite materials, Mons University, Belgium ►
Scientific Staff
Ahmad Moghimikheirabadi
Polymer Physics, ETH Zurich, Switzerland ►
Secretary
Patricia Horn
Polymer Physics, ETH Zurich, Switzerland ►
Enjoy your reading
M Kroger,
Developments in Polymer Theory and Simulation
POLYMERS English 12 (2020) 30 ►Selected conferences (co-)organized by project members
3rd Global Summit Nanotechnology & Nanomedicine
Sep 2019, 3rd Global Summit Nanotechnology & Nanomedicine, Barcelona, Spain ►
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About this project
Fundamentally important to the processability and the material properties of polymer nanocomposites is the underlying interaction between polymer and nanoparticles, the resulting structure and dynamics. A high degree of nanoparticle dispersion is necessary for an effective reinforcement in a polymer matrix. A recent experimental approach to distributing nanoparticles into a polymer matrix is to let the interaction between nanoparticles and polymer chains to be of ionic nature.Ionic nanoparticles can impart charged polymers with unique mechanical and functional properties such as self-healing and shape memory. Upon studying a single model nanocomposite via molecular simulation, we found that nanoparticle dispersion can indeed be achieved due to the insertion of electrostatic charge, that nanoparticle diffusion slows down due to this electrostatic charge, and that the ionic nanoparticles move according to a hopping mechanism.
These recent findings have the potential to spur new studies in modelling ionic polymer nanocomposites containing ionic functionalized silica nanoparticles.
We hereby propose to focus in a more detailed and conclusive fashion on four combined experimental/theoretical research objectives:
Investigate the role of ionic interactions and calculate viscoelastic properties (viscosity, storage modulus, loss modulus) with nanoparticle loading, for differently charged and sequenced polymers.
Quantify the lifetime of dynamic crosslinks between nanoparticles and polymers, formed in ionic nanocomposites, during deformation processes.
Calculate the dynamics and structure of polymers and their entanglements for differently charged and filled polymer ionic nanocomposite models,
Resolve the role of nanosilica surface confinement on polymer entanglements and dynamics. The novelty of the proposed work stems from the combination of experiments, simulation and theoretical models to capture the interactions and polymer structural/dynamical, as well as rheological phenomena present in these ionic nanocomposites, who seem to offer qualitatively new properties worth being quantified and supplemented with an informed microscopic picture.
Lay-Summary (German only, as required by SNF)Hintergrund: Polymer-Nanokomposite (PNCs) stellen eine zunehmend wichtige Hybrid-Materialklasse dar. Das fehlende Verständnis der chemischen und physikalischen Mechanismen stellt seit Jahrzehnten ein Hindernis bei der weiteren Entwicklung dar. Für die Verarbeitung und die Eigenschaften von PNCs ist die Wechselwirkung zwischen Polymer und Nanoteilchen, sowie die resultierende Struktur und Dynamik von fundamentalem Interesse. Eine gute Dispersion der Nanoteilchen wird für die effiziente Verst&aauml;rkung von Polymer-Muttergewebe benötigt. Einer der neueren Ansätze, die diese Eigenschaft bewerkstelligen soll, ist die Verwendung von ionischen PNCs. Ionische Nanoteilchen können den ionischen Polymeren zudem neuartige mechanische und funktionelle Eigenschaften verleihen. Inhalt und Ziel des Forschungsprojekts ist ein besseres Verstädnis der ionischen PNCs. Dazu untersuchen wir die (i) Rolle von ionischen Wechselwirkungen und berechnen viskoelastische/mechanische Eigenschaften und ihre Abhäigkeit von System-Parametern (Konzentration, Ladungen, Ladungs-Sequenzen); (ii) Lebensdauer von Vernetzungspunkten in PNCs, isbesondere während Deformationsprozessen; (iii) Dynamik und Struktur der Polymere und deren Verschlaufungs-Netzwerke in Abhängigkeit der Ladungs-Sequenz; (iv) Rolle der Oberflächen-Beschaffenheit von Nano-Silikaten. Wissenschaftlicher und gesellschaftlicher Kontext des Forschungsprojekts. Wir möchten neuen Technologien für PNCs den Weg bereiten, die benötigt werden, um leichte, hoch-qualitative, und multifunktionelle Materialien weiter zu entwickeln. Ionische PNCs verprechen nicht nur die genannten mechanischen Eigenschaften, sondern auch ein Potential für Selstheilung, ionische Leitfähigkeit, und selektive Permeabilitä Simulationsmodelle erlauben uns, die genannten Abhäigkeiten im Detail zu untersuchen, und öffnen eue Horizonte für das Design ionischer PNCs für Anwendungen etwa in der Biomedizin, Biotechnologie, Energiespeicherung, Gastrennung.
04 May 2025
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