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2. Molecular Modelling Combined with Advanced Chemistry for the Rational Design of Efficient Graphene Dispersing Agents

Author

Papadimitriou, Konstantinia D., Skountzos, Emmanuel N., Gkermpoura, Sandra S., Polyzos, Ioannis, Mavrantzas, Vlasis G., Galiotisa, Costas, and Tsitsilianis, Constantinos

Subjects
Condensed Matter - Soft Condensed Matter, Physics - Applied Physics
Abstract

Pyrene-functional PMMAs were prepared via ATRP-controlled polymerization and click reaction, as efficient dispersing agents for the exfoliation of few-layered graphene sheets (GS) in easily processable low boiling point chloroform. In parallel, detailed atomistic simulations showed fine dispersion of the GS/polymer hybrids in good agreement with the experiment. Moreover, the molecular dynamics simulations revealed interesting conformations (bridges, loops, dangling ends, free chains) of GS/polymer hybrids and allowed us to monitor their time evolution both in solution and in the polymer nanocomposite where the solvent molecules were replaced with PMMA chains. Microscopic information about these structures is very important for optimizing mechanical performance. It seems that the combination of atomistic simulation with advanced chemistry constitutes a powerful tool for the design of effective graphene dispersing agents that could be used for the production of graphene-based nanocomposites with tailor-made mechanical properties.

Published
2018
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3. Colloidal stabilization of graphene sheets by ionizable amphiphilic block copolymers in various media

Author

Popescu, Maria-Teodora, Tasis, Dimitrios, Papadimitriou, Konstantinia D., Gkermpoura, Sandra, Galiotisac, Costas, and Tsitsilianis, Constantinos

Subjects
Condensed Matter - Materials Science
Abstract

In this work, linear polystyrene-poly(2-vinylpyridine) (PS-b-P2VP) and heteroarm star PS_22P2VP_22 ionizable block copolymers were used as dispersing agents for the liquid-phase exfoliation of pristine graphene. Various strategies such as direct exfoliation, film hydration and phase transfer have been employed and compared. The best strategy involved a two-step process, namely, pre-exfoliation of graphite in polymer/CHCl3 solutions followed by phase transfer to acidified water. High concentrations of stable aqueous suspensions of graphene flakes, highly enriched in monolayer structures, were then obtained by using the star-shaped copolymers as stabilizers. The as-prepared graphene/copolymer hybrids were used as a filler material in order to prepare functional polymer composites for mechanical reinforcement. Such copolymer-modified graphene sheets have proven to be efficient reinforcing agents of PVA, as a significant increase of storage modulus (145% higher than that of neat PVA) was achieved even at a low graphene weight fraction of 0.1 wt%.

Published
2018
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6. Soft matter roadmap

Author

Sub Soft Condensed Matter, Soft Condensed Matter and Biophysics, Barrat, Jean Louis, Del Gado, Emanuela, Egelhaaf, Stefan U., Mao, Xiaoming, Dijkstra, Marjolein, Pine, David J., Kumar, Sanat K., Bishop, Kyle, Gang, Oleg, Obermeyer, Allie, Papadakis, Christine M., Tsitsilianis, Constantinos, Smalyukh, Ivan I., Hourlier-Fargette, Aurelie, Andrieux, Sebastien, Drenckhan, Wiebke, Wagner, Norman, Murphy, Ryan P., Weeks, Eric R., Cerbino, Roberto, Han, Yilong, Cipelletti, Luca, Ramos, Laurence, Poon, Wilson C.K., Richards, James A., Cohen, Itai, Furst, Eric M., Nelson, Alshakim, Craig, Stephen L., Ganapathy, Rajesh, Sood, Ajay Kumar, Sciortino, Francesco, Mungan, Muhittin, Sastry, Srikanth, Scheibner, Colin, Fruchart, Michel, Vitelli, Vincenzo, Ridout, S. A., Stern, M., Tah, I., Zhang, G., Liu, Andrea J., Osuji, Chinedum O., Xu, Yuan, Shewan, Heather M., Stokes, Jason R., Merkel, Matthias, Ronceray, Pierre, Rupprecht, Jean François, Matsarskaia, Olga, Schreiber, Frank, Roosen-Runge, Felix, Aubin-Tam, Marie Eve, Koenderink, Gijsje H., Espinosa-Marzal, Rosa M., Yus, Joaquin, Kwon, Jiheon, Sub Soft Condensed Matter, Soft Condensed Matter and Biophysics, Barrat, Jean Louis, Del Gado, Emanuela, Egelhaaf, Stefan U., Mao, Xiaoming, Dijkstra, Marjolein, Pine, David J., Kumar, Sanat K., Bishop, Kyle, Gang, Oleg, Obermeyer, Allie, Papadakis, Christine M., Tsitsilianis, Constantinos, Smalyukh, Ivan I., Hourlier-Fargette, Aurelie, Andrieux, Sebastien, Drenckhan, Wiebke, Wagner, Norman, Murphy, Ryan P., Weeks, Eric R., Cerbino, Roberto, Han, Yilong, Cipelletti, Luca, Ramos, Laurence, Poon, Wilson C.K., Richards, James A., Cohen, Itai, Furst, Eric M., Nelson, Alshakim, Craig, Stephen L., Ganapathy, Rajesh, Sood, Ajay Kumar, Sciortino, Francesco, Mungan, Muhittin, Sastry, Srikanth, Scheibner, Colin, Fruchart, Michel, Vitelli, Vincenzo, Ridout, S. A., Stern, M., Tah, I., Zhang, G., Liu, Andrea J., Osuji, Chinedum O., Xu, Yuan, Shewan, Heather M., Stokes, Jason R., Merkel, Matthias, Ronceray, Pierre, Rupprecht, Jean François, Matsarskaia, Olga, Schreiber, Frank, Roosen-Runge, Felix, Aubin-Tam, Marie Eve, Koenderink, Gijsje H., Espinosa-Marzal, Rosa M., Yus, Joaquin, and Kwon, Jiheon

Published
2024

7. Soft matter roadmap

Author

Barrat, Jean-Louis, Del Gado, Emanuela, Egelhaaf, Stefan U., Mao, Xiaoming, Dijkstra, Marjolein, Pine, David J., Kumar, Sanat K., Bishop, Kyle, Gang, Oleg, Obermeyer, Allie, Papadakis, Christine M., Tsitsilianis, Constantinos, Smalyukh, Ivan I., Hourlier-Fargette, Aurelie, Andrieux, Sebastien, Drenckhan, Wiebke, Wagner, Norman, Murphy, Ryan P., Weeks, Eric R., Cerbino, Roberto, Han, Yilong, Cipelletti, Luca, Ramos, Laurence, Poon, Wilson C. K., Richards, James A., Cohen, Itai, Furst, Eric M., Nelson, Alshakim, Craig, Stephen L., Ganapathy, Rajesh, Sood, Ajay Kumar, Sciortino, Francesco, Mungan, Muhittin, Sastry, Srikanth, Scheibner, Colin, Fruchart, Michel, Vitelli, Vincenzo, Ridout, S. A., Stern, M., Tah, I, Zhang, G., Liu, Andrea J., Osuji, Chinedum O., Xu, Yuan, Shewan, Heather M., Stokes, Jason R., Merkel, Matthias, Ronceray, Pierre, Rupprecht, Jean-Francois, Matsarskaia, Olga, Schreiber, Frank, Roosen-Runge, Felix, Aubin-Tam, Marie-Eve, Koenderink, Gijsje H., Espinosa-Marzal, Rosa M., Yus, Joaquin, Kwon, Jiheon, Barrat, Jean-Louis, Del Gado, Emanuela, Egelhaaf, Stefan U., Mao, Xiaoming, Dijkstra, Marjolein, Pine, David J., Kumar, Sanat K., Bishop, Kyle, Gang, Oleg, Obermeyer, Allie, Papadakis, Christine M., Tsitsilianis, Constantinos, Smalyukh, Ivan I., Hourlier-Fargette, Aurelie, Andrieux, Sebastien, Drenckhan, Wiebke, Wagner, Norman, Murphy, Ryan P., Weeks, Eric R., Cerbino, Roberto, Han, Yilong, Cipelletti, Luca, Ramos, Laurence, Poon, Wilson C. K., Richards, James A., Cohen, Itai, Furst, Eric M., Nelson, Alshakim, Craig, Stephen L., Ganapathy, Rajesh, Sood, Ajay Kumar, Sciortino, Francesco, Mungan, Muhittin, Sastry, Srikanth, Scheibner, Colin, Fruchart, Michel, Vitelli, Vincenzo, Ridout, S. A., Stern, M., Tah, I, Zhang, G., Liu, Andrea J., Osuji, Chinedum O., Xu, Yuan, Shewan, Heather M., Stokes, Jason R., Merkel, Matthias, Ronceray, Pierre, Rupprecht, Jean-Francois, Matsarskaia, Olga, Schreiber, Frank, Roosen-Runge, Felix, Aubin-Tam, Marie-Eve, Koenderink, Gijsje H., Espinosa-Marzal, Rosa M., Yus, Joaquin, and Kwon, Jiheon

Abstract

Soft materials are usually defined as materials made of mesoscopic entities, often self-organised, sensitive to thermal fluctuations and to weak perturbations. Archetypal examples are colloids, polymers, amphiphiles, liquid crystals, foams. The importance of soft materials in everyday commodity products, as well as in technological applications, is enormous, and controlling or improving their properties is the focus of many efforts. From a fundamental perspective, the possibility of manipulating soft material properties, by tuning interactions between constituents and by applying external perturbations, gives rise to an almost unlimited variety in physical properties. Together with the relative ease to observe and characterise them, this renders soft matter systems powerful model systems to investigate statistical physics phenomena, many of them relevant as well to hard condensed matter systems. Understanding the emerging properties from mesoscale constituents still poses enormous challenges, which have stimulated a wealth of new experimental approaches, including the synthesis of new systems with, e.g. tailored self-assembling properties, or novel experimental techniques in imaging, scattering or rheology. Theoretical and numerical methods, and coarse-grained models, have become central to predict physical properties of soft materials, while computational approaches that also use machine learning tools are playing a progressively major role in many investigations. This Roadmap intends to give a broad overview of recent and possible future activities in the field of soft materials, with experts covering various developments and challenges in material synthesis and characterisation, instrumental, simulation and theoretical methods as well as general concepts.

Published
2024
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18. Structural Properties of Micelles Formed by Telechelic Pentablock Quaterpolymers with pH-Responsive Midblocks and Thermoresponsive End Blocks in Aqueous Solution

Author

Jung, Florian A., Panteli, Panayiota A., Ko, Chia-Hsin, Kang, Jia-Jhen, Barnsley, Lester C., Tsitsilianis, Constantinos, Patrickios, Costas S., Papadakis, Christine M., Patrickios, Costas S. [0000-0001-8855-0370], Tsitsilianis, Constantinos [0000-0002-7265-9037], and Panteli, Panayiota A. [0000-0001-7920-0934]

Subjects
chemistry.chemical_classification, Aqueous solution, Hydrodynamic radius, Polymers and Plastics, Organic Chemistry, 02 engineering and technology, Polymer, 010402 general chemistry, 021001 nanoscience & nanotechnology, Methacrylate, 01 natural sciences, Micelle, Polyelectrolyte, 0104 chemical sciences, Inorganic Chemistry, chemistry.chemical_compound, chemistry, Dynamic light scattering, Chemical engineering, ddc:540, Materials Chemistry, 0210 nano-technology, Ethylene glycol
Abstract

We investigated the structural properties of dynamic micelles arising from the self-assembly of the multiresponsive pentablock quaterpolymer P(nBuMA8-co-TEGMA8)-b-PDMAEMA50-b-PEG46-b-PDMAEMA50-b-P(nBuMA8-co-TEGMA8) (nBuMA, TEGMA, DMAEMA, and EG are n-butyl methacrylate, tri(ethylene glycol) methyl ether methacrylate, 2-(dimethylamino)ethyl methacrylate, and ethylene glycol, respectively) in aqueous solution using a combination of scattering methods. In this multisegmented polymer, a pH-responsive BAB triblock copolymer from the weak cationic polyelectrolyte PDMAEMA and the hydrophilic PEG is end-capped by two blocks comprising random sequences of thermoresponsive TEGMA units and hydrophobic nBuMA units. Dynamic light scattering revealed the existence of single micelles and small clusters in dilute aqueous solution. The hydrodynamic radius of the micelles depends strongly on pH and temperature. The inner structure of the micelles was investigated by small-angle X-ray scattering, small-angle neutron scattering, and static light scattering, and micelles with a hydrophobic core containing a rather high fraction of water and a strongly swollen corona were found. The ratio of loops and dangling ends depends on temperature and pH. 52 24 9746 9758

Published
2019

26. Highly Tunable Nanostructures in a Doubly pH‐Responsive Pentablock Terpolymer in Solution and in Thin Films

Author

Jung, Florian A., primary, Schart, Maximilian, additional, Bührend, Lukas, additional, Meidinger, Elisabeth, additional, Kang, Jia‐Jhen, additional, Niebuur, Bart‐Jan, additional, Ariaee, Sina, additional, Molodenskiy, Dmitry S., additional, Posselt, Dorthe, additional, Amenitsch, Heinz, additional, Tsitsilianis, Constantinos, additional, and Papadakis, Christine M., additional

Published
2021
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38. Thermoresponsive Hydrogels Based on Telechelic Polyelectrolytes: From Dynamic to 'Frozen' Networks

Author

Tsitsilianis, Constantinos, Serras, George, Ko, Chia-Hsin, Jung, Florian, Papadakis, Christine M., Rikkou-Kalourkoti, Maria, Patrickios, Costas S., Schweins, Ralf, Chassenieux, Christophe, Patrickios, Costas S. [0000-0001-8855-0370], Tsitsilianis, Constantinos [0000-0002-7265-9037], and Rikkou-Kalourkoti, Maria [0000-0002-4012-1486]

Subjects
Materials science, Polymers and Plastics, Organic Chemistry, 02 engineering and technology, 010402 general chemistry, 021001 nanoscience & nanotechnology, Methacrylate, 01 natural sciences, Polyelectrolyte, Viscoelasticity, 0104 chemical sciences, Inorganic Chemistry, chemistry.chemical_compound, Viscosity, Chemical engineering, chemistry, Self-healing hydrogels, Materials Chemistry, Copolymer, 0210 nano-technology, Triethylene glycol, Complex fluid
Abstract

A novel thermoresponsive gelator of (B-co-C)-b-A-b-(B-co-C) topology, comprising a poly(2-(dimethylamino)ethyl methacrylate) (PDMAEMA) weak polyelectrolyte as central block, end-capped by thermosensitive poly(triethylene glycol methyl ether methacrylate/n-butyl methacrylate) [P(TEGMA-co-nBuMA)] random copolymers, was designed and explored in aqueous media. The main target of this design was to control the dynamics of the stickers by temperature as to create an injectable hydrogel that behaves as a weak gel at low temperature and as a strong gel at physiological temperature. Indeed, at low temperatures, the system behaves like a viscoelastic complex fluid (dynamic network), while at higher temperatures, an elastic hydrogel is formed (“frozen” network). The viscosity increases exponentially upon heating, about 5 orders of magnitude from 5 to 45 °C, which is attributed to the exponential increase of the lifetime of the self-assembled stickers. The integration of thermo- and shear responsive properties in the gelator endows the gel with injectability. Moreover, the gel can be rapidly recovered upon cessation of the applied stress at 37 °C, simulating conditions similar to those of injection through a 28-gauge syringe needle. All these hydrogel properties render it a good candidate for potential applications in cell transplantation through injection strategies. 51 6 2169 2179

Published
2018

44. 3-Arm star pyrene-functional PMMAs for efficient exfoliation of graphite in chloroform: fabrication of graphene-reinforced fibrous veils

Author

Gkermpoura, Sandra S., primary, Papadimitriou, Konstantinia D., additional, Skountzos, Emmanuel N., additional, Polyzos, Ioannis, additional, Pastore Carbone, Maria Giovanna, additional, Kotrotsos, Athanasios, additional, Mavrantzas, Vlasis G., additional, Galiotis, Costas, additional, and Tsitsilianis, Constantinos, additional

Published
2019
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