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Post-spin Stretch Improves Mechanical Properties, Reduces Necking, and Reverts Effects of Aging in Biomimetic Artificial Spider Silk Fibers

Gabriele Greco, Benjamin Schmuck, Fredrik G. Bäcklund, Günter Reiter and Anna Rising. ACS Applied Polymer Materials, published online

reiter-2024-05.jpgRecent biotechnological advancements in protein production and development of biomimetic spinning procedures make artificial spider silk a promising alternative to petroleum-based fibers. To enhance the competitiveness of artificial silk in terms of mechanical properties, refining the spinning techniques is imperative. One potential strategy involves the integration of post-spin stretching, known to improve fiber strength and stiffness while potentially offering additional advantages. Here, we demonstrate that post-spin stretching not only enhances the mechanical properties of artificial silk fibers but also restores a higher and more uniform alignment of the protein chains, leading to a higher fiber toughness. (more...)


Mechanistically Different Mechanochromophores Enable Calibration and Validation of Molecular Forces in Glassy Polymers and Elastomeric Networks

Raphael Hertel, Maximilian Raisch, Michael Walter, Günter Reiter, Michael Sommer. Angew. Chem. Int. Ed. 2024, e202409369

sommer.jpgSterically distorted donor-acceptor p‑systems, termed DA springs, can be progressively planarized under mechanical load causing a bathochromic shift of the photoluminescence (PL) spectrum. By combining theory and experiment, we here use a simple linear force calibration for two different conformational mechanochromophores to determine molecular forces in polymers from the mechanochromic shift in PL wavelength during multiple uniaxial tensile tests. Two systems are used, i) a highly entangled linear glassy polyphenylene and ii) a covalent elastomeric polydimethylsiloxane network. The mean forces estimated by this method are validated using known threshold forces for the mechanochemical ring-opening reactions of two different spiropyran force probes. The agreement between both approaches underlines that these DA springs provide the unique opportunity for the online monitoring of local molecular forces present in diverse polymer matrices.(more...)


"Printing" on Polymer Single Crystals through Microregional Heating

Tianyu Wu, Haimu Ye, Xinyi Pan, Yaning He, Jun Xu, Günter Reiter. ACS Appl. Polym. Mater. 2024, 6, 14, 7969–7977

tianyu.jpgPolymer single crystals are composed of well-ordered polymer chains and possess a characteristic symmetric shape. If one can precisely control the microregional morphology, polymer single crystals have the potential to be used as functional templates for applications like information storage or cell culture. However, with current experimental approaches, it is rather difficult to generate predictable structures of defined size within polymer single crystals. Here, we propose a research strategy based on a combination of fluorescence labeling and microregional heating by irradiation with focused red light. This approach enabled us to locally heat single crystals while simultaneously following the thereby induced changes via fluorescence imaging with a micrometer lateral resolution. We found that polymers diffused out of the heated region within a stacked single crystal and thereby produced a hole at the irradiated location. (more...)


Mechanism for the Formation of Millimeter-Long Solid Filaments by Spin Coating Dilute Solutions of a Crystallizable Polymer

Da Huang, Thorsten Hugel, and Günter Reiter. Macromolecules 2024, 57, 3696–3705

huang.jpgWe have investigated the formation of millimeter-long filaments induced by spin-coating ca. 130 °C dilute para-xylene solutions of rapidly crystallizable polyethylene chains with a contour length in the micrometer range onto ca. 80 °C mica substrates. These filaments were radially oriented and accumulated on the periphery of the substrate. Our observations can be explained by the stretching of polymers through the flow field induced by spinning the solution on a solid substrate. The corresponding loss in conformational entropy emphasized attractive interactions between polymers, which resulted in the formation of bundles and their assembly into long filaments. Caused by a Plateau–Rayleigh-type instability of a liquid coating on a solid filament and due to crystallization, these filaments were decorated with various small-scale structures. (more...)


 

Liste der Veröffentlichungen

Viscous-force-dominated tensile deformation behavior of oriented polyethylene
B. Na, Q. Zhang, Q. Fu, Y.F. Men, K. Hong, G. Strobl. Macromolecules 39, 2584-2591 (2006)
Low-field NMR studies of polymer crystallization kinetics: changes in the melt dynamics
C. Hertlein, K.Saalwächter, G. Strobl. Polymer 47, 7216 (2006)
Crystallization and Melting of Bulk Polymers: New Observations, Conclusions and a Thermodynamic Scheme
Gert Strobl. Prog. Polym. Sci. 31, 398 (2006)
Time dependent light attenuation measurements used in studies of the kinetics of polymer crystallization
Barbara Heck, Takahiko Kawai, Gert Strobl. Polymer 47, 5538-5543 (2006)
凝縮系物理学: 結晶からソフトマターへ
G. ストローブル (著), 田口 健 (翻訳), 深尾 浩次 (翻訳). 出版社: シュプリンガー・ジャパン(株) 2006, ISBN 978-4431712206
Variation of the Network Anisotropy of Cholesteric Side Chain Elastomers
Christian Bourgerette, Bin Chen, Heino Finkelmann, Michel Mitov, Jürgen Schmidtke, Werner Stille. Macromolecules 39, 8163 (2006)
Effects of comonomers on lamellar and noncrystalline microstructure of ethylene copolymers
T.Y. Cho, E.J. Shin, W. Jeong, B. Heck, R. Graf, G. Strobl, H.W. Spiess, D.Y. Yoon. Macromolecular Rapid Communications 27, 322-327 (2006)
Deriving Molecular Parameters of Interfaces Between Chemically Identical Polymers from Macroscopically Observed Phenomena
Günter Reiter. Macromol. Symp. 229, 81–92 (2005)
Structure Formation of Polystyrene-block-poly(gamma-benzyl L-glutamate) in Thin Films
S. Ludwigs, G. Krausch, G. Reiter, M. Losik, M. Antonietti, H. Schlaad. Macromolecules 38, 7532 (2005)
Residual stresses in thin polymer films cause rupture and dominate early stages of dewetting
Günter Reiter, Moustafa Hamieh, Pascal Damman, Séverine Sclavons, Sylvain Gabriele, Thomas Vilmin, Elie Raphaël. Nature Materials 4, 754 (2005)
Reply: Discussion of problems of non-equilibrium thermodynamics of polymers
J.-U. Sommer and G. Reiter. Thermochimica Acta, 432, 153 (2005)
Crystallization in Ultra-Thin Polymer Films/ Morphogenesis and Thermodynamical Aspects
J.-U. Sommer and G. Reiter. Thermochimica Acta, 432, 135 (2005)
Evolution of rim instabilities in the dewetting of slipping thin polymer films
Günter Reiter. J. Adhesion 81, 381 (2005)
Instability and droplet formation in evaporating thin films of a binary solution
Leonid V. Govor, Jürgen Parisi, Gottfried H. Bauer and Günter Reiter. Phys. Rev. E 71, 051603 (2005)
Morphology of an asymmetric ethyleneoxide-butadiene di-block copolymer in bulk and thin films
D.M. Lambreva, R. Opitz, G. Reiter, P.M. Frederik and W.H. de Jeu. Polymer 46, 4868 (2005)
Evolution of multilevel order in supramolecular assemblies
F. Vonau, D. Suhr, D. Aubel, L. Bouteiller, G. Reiter and L. Simon. Phys. Rev. Lett. 94, 066103 (2005)
Block formation during polymer crystallization
T. Hippler, S. Jiang, G. Strobl. Macromolecules 38, 9396 (2005)
Crystallization of a poly(ethylene-co-octene): I - A precursor structure and two competing mechanisms
Andreas Häfele, Barbara Heck, Takahiko Kawai, Peter Kohn, Gert Strobl. Eur. Phys. J. E 16, 207-216 (2005)
A thermodynamic multiphase scheme treating polymer crystallization and melting
G. Strobl. Eur. Phys. J. E 18, 295-309 (2005)
Crystallization of poly(ethylene-co-octene): II - Melt memory effects on first order kinetics
Andreas Häfele, Barbara Heck, Thomas Hippler, Takahiko Kawai, Peter Kohn, Gert Strobl. Eur. Phys. J. E 16, 217-224 (2005)
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