Article
Chemistry, Multidisciplinary
Mayuri K. K. Porwal, Matthew M. M. Hausladen, Christopher J. J. Ellison, Theresa M. M. Reineke
Summary: A family of biobased networks was synthesized from triallyl levoglucosan and multifunctional thiols via UV-initiated thiol-ene click chemistry. The thermomechanical and hydrolytic degradation properties of the networks can be tailored based on the type and stoichiometric ratio of the thiol crosslinker. The levoglucosan-based resins showed excellent suitability for extrusion-based 3D printing and demonstrated potential for sustainable rapid prototyping and mass production applications.
Article
Polymer Science
Ming Zhang, Daai Li, Pengfei Shan, Xiaoyue Lian, Yuxi Qi, Kaicheng Du, Guoquan Ma, Liang Cai, Zhihui Li, Zhongyu Li
Summary: A dithiol reagent containing ketal and o-nitrobenzyl structures was used to synthesize the polymer PKNB and the amphiphilic triblock copolymer mPEG-PKNB-mPEG through thiol-ene click chemistry. The mPEG-PKNB-mPEG and its nanoparticles exhibited excellent light/acid degradation ability, suggesting promising applications in drug, gene, or pesticide delivery.
Article
Nanoscience & Nanotechnology
Maciej Podgorski, Sijia Huang, Christopher N. Bowman
Summary: A photoprintable dynamic thiol-ene resin was developed for 3D printing, with optimized curing properties and high conversion rates achieved within a short period of time. The dynamic chemistry allowed for rapid reversible exchange, enabling reconfiguration and depolymerization of printed objects at specific temperature ranges, showing potential for new applications in shape memory and 4D printable functional materials.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Polymer Science
Aneta Lewandowska, Piotr Gajewski, Katarzyna Szczesniak, Zbigniew Fojud, Mariola Robakowska, Andrzej Skrzypczak, Adam Voelkel, Agnieszka Marcinkowska
Summary: This work reports the synthesis of polymerizable ionic liquids (PILs) and the preparation of ionogels using thiol-ene photopolymerization. The ionogels prepared with the PILs showed excellent mechanical properties, high ionic conductivity, and thermal stability. The structure of the PILs affected the polymerization kinetics and properties of the ionogels.
Review
Chemistry, Multidisciplinary
Marzieh Ahangarpour, Iman Kavianinia, Paul W. R. Harris, Margaret A. Brimble
Summary: The global market for peptide/protein-based therapeutics is growing significantly, but the development of peptide drugs faces challenges that can be addressed through chemical modification. Recently, there has been a renewed interest in using photoinduced radical thiol-ene chemistry as a powerful tool for constructing therapeutic peptides.
CHEMICAL SOCIETY REVIEWS
(2021)
Article
Biochemistry & Molecular Biology
Laura Boetje, Xiaohong Lan, Jur van Dijken, Gerbrich Kaastra, Michael Polhuis, Katja Loos
Summary: In this study, biobased films were synthesized using different cross-linkers for starch, showing the potential for tuning the mechanical and thermal properties of the films. These films may have applications in packaging due to their increased flexibility.
Article
Polymer Science
Meiying Ge, Jia-Tao Miao, Kai Zhang, Yadong Wu, Longhui Zheng, Lixin Wu
Summary: The study focused on the synthesis of biobased flexible polymer networks with tunable properties through thiol-ene click photopolymerization, showing excellent mechanical performance, high transparency, and degradability in mild acetic acid solution.
Article
Materials Science, Multidisciplinary
Andreas Hoffmann, Klaus Kreuels, Arnold Gillner
Summary: This study investigates the rarely used thiol-ene click chemistry in stereolithography and develops new photo resins based on this chemistry. The resulting polymers are analyzed for their suitability as thiol-ene photo resins. The study also explores the influence of crosslinker functionality and the concept of prepolymerization of two bifunctional components for thiol-ene photo resins.
MACROMOLECULAR MATERIALS AND ENGINEERING
(2022)
Article
Polymer Science
Sergio Cespedes, Rachel A. Hand, Nikola Chmel, Graeme Moad, Daniel J. Keddie, Tara L. Schiller
Summary: The STMRT strategy was used to produce poly(ethylene glycol)-based model networks, allowing for the establishment of a structure-property relationship. The properties of the model networks can be finely tuned by manipulation of crosslink density and average polymer chain length.
EUROPEAN POLYMER JOURNAL
(2021)
Article
Polymer Science
Miao Huo, Jerry G. Hu, David R. Clarke
Summary: PhotoCAN silicone elastomers show rapid and reversible changes in dynamic modulus at room temperature under UV illumination, thanks to the thiol-ene reaction. Through a combination of solid-state NMR, EPR, and rheometry measurements, it is found that the mechanical response is a result of dissociative, associative, and oxidation reactions. The reversible dissociative reaction, involving the cleavage of C-S bonds under UV in the presence of excess thiyl radicals, leads to abrupt drops in storage modulus. A slower termination process involving the formation of disulfide bonds by thiyl radicals is also observed. A kinetic model is developed to relate the rates of these reactions to the changes in storage modulus. These findings lay the foundation for the design of new photoresponsive covalently adaptive network materials at ambient temperature.
Article
Materials Science, Multidisciplinary
Farhad Shohraty, Julian Hniopek, Josefine Meurer, Stefan Zechel, Michael Schmitt, Juergen Popp, Martin D. Hager
Summary: In addition to thermal transitions and supramolecular interactions, shape-memory polymers can also be based on covalent bonds. This study demonstrates the use of the reversible thiol-ene reaction as a reversible cross-linker for the design of shape-memory polymers. The resulting polymers feature excellent shape-memory behavior with fixity and recovery rates above 90%.
MACROMOLECULAR MATERIALS AND ENGINEERING
(2023)
Article
Polymer Science
Nicholas J. Bongiardina, Shafer M. Soars, Maciej Podgorski, Christopher N. Bowman
Summary: This study evaluated radical-disulfide exchange reactions in thiol-ene-disulfide networks using different thiol and disulfide containing monomers. The results show that the stress relaxation rate in these networks can be controlled by changing the thiol-disulfide stoichiometry or the disulfide type. The combination of different thiol and disulfide monomers also influences the polymerization rate of the thiol-ene reaction.
Article
Polymer Science
Logan D. Dugas, William D. Walker, Rahul Shankar, Keely S. Hoppmeyer, Travis L. Thornell, Sarah E. Morgan, Robson F. Storey, Derek L. Patton, Yoan C. Simon
Summary: This work describes a photopolymerized thiol-ene-based vitrimer that combines stability, healability, and reprocessability. The introduction of excess primary amines enables the degradation and regeneration of the vitrimer. Photopolymerization provides unique control over the network topology, facilitating further investigation of vitrimer properties.
MACROMOLECULAR RAPID COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Xin-Da Huang, Ge-Hua Wen, Song-Song Bao, Jia-Ge Jia, Li-Min Zheng
Summary: The research reported the design and synthesis of a new lanthanide mononuclear complex, demonstrating reversible thermo-responsive phase transition and photo-induced dimerization, leading to synergistic switching of multiple properties.
Article
Chemistry, Physical
Rossella Laurano, Monica Boffito, Claudio Cassino, Ludovica Midei, Roberta Pappalardo, Valeria Chiono, Gianluca Ciardelli
Summary: In this study, new amphiphilic poly(ether urethane)s bearing photo-sensitive moieties were designed and synthesized. Thiol-ene photo-click hydrogels with thermo- and Vis-light responsiveness were prepared using these polymers. The addition of green light-induced photo-curing and co-initiator resulted in improved gel state and mechanical performance. The optimized composition of thiol-norbornene formulations showed prevalent elastic behavior at lower frequency due to the formation of purely bio-orthogonal gel networks.
Article
Materials Science, Multidisciplinary
Negin Madelat, Benny Wouters, Ehsan Jalilian, Guy Van Assche, Annick Hubin, Herman Terryn, Tom Hauffman
Summary: This study characterized the separate diffusion of water and ions in a polyethylene glycol diacrylate (PEGDA) coating using an integrated spectro-electrochemical technique. The ingress front position profile of ions in the coating was determined by fitting odd random phase electrochemical impedance spectroscopy (ORP-EIS) data with a physically relevant electrochemical equivalent circuit (EEC). The arrival time of ions at the coating/metal oxide interface was obtained from the EEC and verified through in situ attenuated total reflection Fourier transform infrared spectroscopy (ATR-FTIR) measurements in the Kretschmann geometry integrated in the ORP-EIS set-up.
Article
Polymer Science
Tapas Debsharma, Stephanie Engelen, Ives De Baere, Wim Van Paepegem, Filip Du Prez
Summary: Natural fiber-reinforced composites can be made thermally reshapable using a resorcinol-based epoxy resin and fast exchanging siloxane bonds. The stress relaxation time at 220 degrees C is only about 6 seconds. This research demonstrates the potential for sustainable and reshapable composite materials in the form of flax fiber-reinforced composites.
MACROMOLECULAR RAPID COMMUNICATIONS
(2023)
Article
Polymer Science
Jasper Delaey, Laurens Parmentier, Lincy Pyl, Joost Brancart, Peter Adriaensens, Agnes Dobos, Peter Dubruel, Sandra Van Vlierberghe
Summary: Acrylate-endcapped urethane-based precursors were synthesized to form a poly(D,L-lactide)/poly(epsilon-caprolactone) (PDLLA/PCL) random copolymer backbone with different architectures and molar masses. By adjusting the monomer content, the glass transition temperature and actuation temperature of the polymers could be controlled. The resulting polymers showed excellent shape-memory properties and compatibility with additive manufacturing techniques. Moreover, they exhibited biocompatibility in in vitro cell assays.
MACROMOLECULAR RAPID COMMUNICATIONS
(2023)
Article
Polymer Science
Ali Safaei, Seppe Terryn, Bram Vanderborght, Guy Van Assche, Joost Brancart
Summary: The thermophysical properties, mechanical behavior, and healing performance of Diels-Alder-based polymer networks can be widely tuned through changes in the molar mass, functionality, and stoichiometric ratio of the multifunctional diene and dienophile monomers. Blending furan-functionalized monomers with different molar masses allows for tuning the properties of the resulting reversible polymer network blends, providing a balance of elastomeric and thermoset phases with various crosslink densities and glass transitions. Increasing the thermoset content enhances the mechanical properties of the elastomers, while the addition of the elastomer phase improves the toughness of the thermosets by dissipating stress. The phase-separated morphologies of the blends can be observed through DSC and DMA.
Article
Polymer Science
Stephan Maes, Filip Van Lijsebetten, Johan M. Winne, Filip E. Du Prez
Summary: In this study, it was shown that the introduction of N-sulfonyl urethane bonds leads to dynamic covalent exchange reactions under milder conditions. These exchangeable N-sulfonyl urethane motifs were then incorporated into a cross-linked PU matrix to facilitate plastic flow at lower temperatures. The resulting materials demonstrated good (re)processability and retained their thermal properties.
Article
Engineering, Electrical & Electronic
Huaijin Chen, Kevin Langlois, Joost Brancart, Ellen Roels, Tom Verstraten, Bram Vanderborght
Summary: A sensorized physical human-robot interface was proposed based on electrical impedance tomography (EIT), allowing continuous pressure measurement over a large area for wearable robots. The reconstruction method using convolutional neural network-enhanced Tikhonov regularization achieved accurate localization and size estimation of compressed areas, as well as distinguishing multiple compressed areas. The experimental results validated the suitability of the EIT pressure sensor for physical interfaces.
IEEE SENSORS JOURNAL
(2023)
Article
Chemistry, Applied
M. Meeusen, J. P. B. van Dam, N. Madelat, E. Jalilian, B. Wouters, T. Hauffman, G. Van Assche, J. M. C. Mol, A. Hubin, H. Terryn
Summary: In this study, a new finite element modelling (FEM) approach is used to simulate the spatiotemporally resolved water uptake in organic coatings. A physical model is developed considering both Fickian diffusion and the adsorption/desorption reaction of water on the polymer matrix. The model is validated and improved by comparing the calculated water concentration and virtual capacitance values with experimental measurements.
PROGRESS IN ORGANIC COATINGS
(2023)
Article
Chemistry, Multidisciplinary
Resat Aksakal, Corentin Tonneaux, Annemiek Uvyn, Mathieu Fossepre, Hatice Turgut, Nezha Badi, Mathieu Surin, Bruno G. De Geest, Filip. E. Du Prez
Summary: Antibody-recruiting molecules are a new type of therapeutic agents that can recruit endogenous antibodies to target cells for elimination. Macromolecular scaffolds with multiple copies of an antibody-binding ligand offer advantages in terms of increased avidity. In this study, we synthesized sequence-defined macromolecules with dinitrophenol (DNP) as a model antibody-recruiting motif and observed enhanced avidity for anti-DNP antibodies with adjacent DNP motifs. These findings provide insights for designing novel antibody-recruiting therapeutic agents.
Article
Automation & Control Systems
Zhanwei Wang, Seppe Terryn, Huijiang Wang, Julie Legrand, Ali Safaei, Joost Brancart, Guy Van Assche, Bram Vanderborght
Summary: In this article, a comprehensive approach to address the environmental impact of energy waste in vacuum grippers is presented. The approach involves the development of a self-closing, multi-material, and self-healing system based on reversible elastomers. The system effectively prevents energy waste, achieves versatility and stability, and enables self-repair within a short period of time.
ADVANCED INTELLIGENT SYSTEMS
(2023)
Article
Automation & Control Systems
Pasquale Ferrentino, Ellen Roels, Joost Brancart, Seppe Terryn, Guy Van Assche, Bram Vanderborght
Summary: This article presents a tutorial on how to build a soft-robot model using an open source finite element analysis (FEA) simulator called SOFA. The tutorial explains the basic working principles of SOFA and demonstrates its capability to generate a simulation scene from Python or XML code. It also highlights the importance of knowledge of constitutive material properties for good modeling of the mechanical system and the ability of SOFA to handle multidisciplinary subjects and teach simulation and programming language principles to engineering students.
IEEE ROBOTICS & AUTOMATION MAGAZINE
(2023)
Article
Polymer Science
Alyssa J. J. Ghielmetti, Christopher Barner-Kowollik, Filip E. E. Du Prez, Hannes A. A. Houck
Summary: The molecular network connectivity in dynamic polymer networks significantly affects material properties and reprocessing conditions. The influence of regioisomerism in light-stabilized dynamic materials has been highlighted. Interchanging regioisomer fractions of substituted naphthalenes with triazolinediones (TADs) in a photo-driven cycloaddition reaction has been demonstrated to affect the cycloreversion kinetics and is important for the design of dynamic covalent materials. The development of completely regioselective TAD/naphthalene systems and the control of cycloreversion kinetics through naphthalene substitution offer new opportunities for the advancement and applications of light-stabilized dynamic materials.
Article
Chemistry, Multidisciplinary
S. Utrera-Barrios, N. Steenackers, S. Terryn, P. Ferrentino, R. Verdejo, G. Van Asche, M. A. Lopez-Manchado, J. Brancart, M. Hernandez Santana
Summary: This study introduces mechanically strong, self-healing, and recyclable ionic elastomers for soft robotics, which possess excellent mechanical properties, high self-healing capabilities, and recyclability. These materials can be molded and scaled easily, making them promising for various soft robotics applications.
MATERIALS HORIZONS
(2023)
