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Selective Dissolution as a Tool for Detecting Spatial Variations in the Degree of Metastability within Lamellar Polymer Crystals

Binghua Wang, Hailong Zou, Xuchen Wang, Changyu Shen, Jingbo Chen, Günter Reiter, Bin Zhang. Nature Communications 16 (2025) 3275

The dissolution of polymer crystals often proceeds at rates varying in time and space. Here, using low molecular weight poly(ethylene oxide) as a model polymer, we exploit step-wise selective dissolution for unveiling how spatial variations in metastability are generated during the growth of lamellar polymer single crystals. The dissolution velocity along defined crystal faces is constant, but ca. 5 times faster for rough than for smooth faces. From the temperature dependence of dissolution, we derive detachment energies of 420 ± 40 kJ/mol and 650 ± 50 kJ/mol for rough and smooth faces, respectively, suggesting that on a rough face polymer chains have ca. 1/3 less neighboring molecules to interact with. The observed high values of the activation energy indicate that, for dissolving a polymer crystal, the progressive detachment of whole chains is indispensable. Our study reveals a strong relation between growth kinetics and the resulting metastability of polymer crystals. (more...)


London dispersion forces and steric effects within nanocomposites tune interaction energies and chain conformation

Baode Zhang, Snežana D. Zarić, Sonja S. Zrilić, Iosif Gofman, Barbara Heck, Günter Reiter. Communications Chemistry 8 (2025) 21

baode.jpgThe interplay between attractive London dispersion forces and steric effects due to repulsive forces resulting from the Pauli principle often determines the geometry and stability of nanostructures. Aromatic polyimides (PI) and carbon nanotubes (CNT) were chosen as building blocks as two components in the hetero delocalized electron nanostructures. Two PIs, having the same diamine part and different linkage substituents between two phenyl rings of dianhydride part, one linked with ether bond (C-O-C) (OPI), the other with C-(CF3)2 (FPI), were investigated. Surprisingly, two CNT/PI nanocomposites show distinct failure mode from CNT yielding to CNT pull-out failure. Calculation of the interaction energy and chain conformations of each PI upon CNT was performed by accurate density functional theory (DFT) calculations and molecular dynamic simulation (MDS). (more...)


Effect of chemical structure on the crystallization kinetics of triple polymorphic high-sulfur-content polythioethers

Valentina Pirela, Leire Unanue, Justine Elgoyhen, Javier Ramos, Juan Francisco Vega, Agurtzane Mugica, Manuela Zubitur, Cuong Minh Quoc Le, Abraham Chemtob, Radmila Tomovska, Günter Reiter, Jaime Martín, Alejandro J. Müller. European Polymer Journal (2025) 113721

This work studies how the chemical structure of relatively similar high-sulfur alternating polythioether homopolymers (DMDS-alt-DVE, DMDS-alt-TEGDVE, and DMDS-alt-BDDVE) affects their structural properties, morphology, polymorphism, and crystallization kinetics. Differential scanning calorimetry (DSC) and polarized light optical microscopy (PLOM) experiments revealed a complex crystallization for the samples in which up to three different polymorphic phases were identified: a very low melting crystal form (VL-Tm form), a low melting crystal form (L-Tm form) and a high melting crystal form (H-Tm form), characterized by their corresponding melting temperature ranges and confirmed via Wide-Angle X-ray Scattering (WAXS). A coexistence of negative and positive spherulites was found, and their origin was revealed by atomic force microscopy (AFM), which showed how the lamellar arrangement varied in the samples from predominantly radial to a cross-hatched morphology. (more...) 


 

Liste der Veröffentlichungen

London dispersion forces and steric effects within nanocomposites tune interaction energies and chain conformation
Baode Zhang, Snežana D. Zarić, Sonja S. Zrilić, Iosif Gofman, Barbara Heck, Günter Reiter. Communications Chemistry 8 (2025) 21
Effect of chemical structure on the crystallization kinetics of triple polymorphic high-sulfur-content polythioethers
Valentina Pirela, Leire Unanue, Justine Elgoyhen, Javier Ramos, Juan Francisco Vega, Agurtzane Mugica, Manuela Zubitur, Cuong Minh Quoc Le, Abraham Chemtob, Radmila Tomovska, Günter Reiter, Jaime Martín, Alejandro J. Müller. European Polymer Journal (2025) 113721
Hydro-elastic interactions for shaping hydrodynamic properties in microfluidic flows
Claas-Hendrik Stamp, Inauguraldissertation der Fakultät für Mathematik und Physik, 2024
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 Appl. Polym. Mater. 6 (2024) 14342–14350
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
Mechanism for the formation of millimeter-long solid filaments by spin coating dilute solutions of a crystallizable polymer
Da Huang, Thorsten Hugel, Günter Reiter. Macromolecules 57 (2024) 3696–3705
Competing influences of cooling rate and diluent concentration on crystallization of poly(3-hexylthiophene)
Mina Alizadehaghdam, Farhang Abbasi, Günter Reiter. J. Phys. Chem. C 128 (2024) 4757–4765
Selective Dissolution as a Tool for Detecting Spatial Variations in the Degree of Metastability within Lamellar Polymer Crystals
Binghua Wang, Hailong Zou, Xuchen Wang, Changyu Shen, Jingbo Chen, Günter Reiter, Bin Zhang. Nature Communications 16 (2025) 3275
“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
Identifying a Mesomorphic Boundary Zone within Polybutene-1 Single Crystals Emerging during a Crystal-Crystal Transformation
Jinlong Chen, Binghua Wang, Changyu Shen, Jingbo Chen, Günter Reiter, Bin Zhang. Macromolecules 56 (2023) 5050–5057
Determining the maximum melting temperature of polymer crystals from a change in morphology of dewetting rims
Gang Wang, Guotao Shi, Anchenyi Yang, Binghua Wang, Changyu Shen, Jingbo Chen, Günter Reiter, Bin Zhang. Polymer 274 (2023) 125874
Unraveling the complex polymorphic crystallization behavior of the alternating copolymer DMDS-alt-DVE
Valentina Pirela, Justine Elgoyhen, Radmila Tomovska, Jaime Martin Perez, Cuong Minh Quoc Le, Abraham Chemtob, Brahim Bessif, Barbara Heck, Günter Reiter, and Alejandro Müller. ACS Appl. Polym. Mater. 5 (2023) 5260–5269
Nucleation Assisted through the Memory of a Polymer Melt: A Different Polymorph Emerging from the Melt of another One
Brahim Bessif, Barbara Heck, Thomas Pfohl, Cuong Minh Quoc Le, Abraham Chemtob, Valentina Pirela, Justine Elgoyhen, Radmila Tomovska, Alejandro Müller, Günter Reiter. Macromolecules 56 (2023) 1461–1470
Tuning the hydraulic resistance by swelling-induced buckling of membranes in high-aspect-ratio microfluidic devices
Claas-Hendrik Stamp, Binyam Solomon, Friederike Lang, Efstathios Mitropoulos and Thomas Pfohl. Lab Chip 23 (2023) 3662-3670
Reversible Dehydration-Hydration of Poly(ethylene glycol) in Langmuir Monolayers of a Diblock Copolymer Inferred from Changes in Filament Curvature
Emna Khechine, Sebastian Noack, Helmut Schlaad, Jun Xu, Günter Reiter, Renate Reiter. Langmuir 39 (2023) 2710–2718
Improving the order of crystalline regions of poly(3-hexylthiophene) by crystallization from the self-nucleation domains
Mina Alizadehaghdam, Farhang Abbasia, and Günter Reiter. Thermochimica Acta 717 (2022) 179352
Determining Entanglement Molar Mass of Glassy Polyphenylenes Using Mechanochromic Molecular Springs
Maximilian Raisch, Günter Reiter, Michael Sommer. ACS Macro Lett. 11, 760–765, 2022
Editorial on the Special Topic “Polymer Crystallization”
Jun Xu, Günter Reiter, and Rufina G. Alamo. Crystals 12, 618 (2022)
In situ dissolution and swelling of confined lamellar polymer crystals through exposure to humid air
Brahim Bessif, Thomas Pfohl, Barbara Heck, Yaser Alshetwi, Emna Khechine, Jun Xu, and Günter Reiter. Macromolecules 55, 6015–6022, 2022
The memory of thin polymer films generated by spin coating
Günter Reiter, Farzad Ramezani, Jörg Baschnagel. EPJE 45 (2022) 51
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