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- Item4D Biofabrication of fibrous artificial nerve graft for neuron regeneration(Bristol : IOP Publ., 2020) Apsite, Indra; Constante, Gissela; Dulle, Martin; Vogt, Lena; Caspari, Anja; Boccaccini, Aldo R.; Synytska, Alla; Salehi, Sahar; Ionov, LeonidIn this paper, we describe the application of the 4D biofabrication approach for the fabrication of artificial nerve graft. Bilayer scaffolds consisting of uniaxially aligned polycaprolactone-poly(glycerol sebacate) (PCL-PGS) and randomly aligned methacrylated hyaluronic acid (HA-MA) fibers were fabricated using electrospinning and further used for the culture of PC-12 neuron cells. Tubular structures form instantly after immersion of fibrous bilayer in an aqueous buffer and the diameter of obtained tubes can be controlled by changing bilayer parameters such as the thickness of each layer, overall bilayer thickness, and medium counterion concentration. Designed scaffolds showed a self-folded scroll-like structure with high stability after four weeks of real-time degradation. The significance of this research is in the fabrication of tuneable tubular nerve guide conduits that can simplify the current existing clinical treatment of neural injuries. © 2020 The Author(s). Published by IOP Publishing Ltd.
- ItemFunktionalisierte Kern-Schale-Partikel als Träger zur Enzymimmobilisierung und deren Anwendung(Weinheim : Wiley-VCH Verl., 2020) Matura, Anke; Köpke, Dorina; Marschelke, Claudia; Kramer, Julius; Synytska, Alla; Sallat, MarcoMono- und bifunktionale hybride Kern-Schale-Partikel wurden für die Enzymimmobilisierung eingesetzt. An monofunktionalen Poly(2-dimethylamino)ethylmethacrylat-modifizierten Partikeln wurden die idealen Bedingungen für die Immobilisierung untersucht. Anschließend erfolgte die Übertragung auf bifunktionale Janus-Partikel-Systeme, mit denen gleichzeitig die schaltbare Abtrennung und der erneute Einsatz der Enzyme möglich waren. Abschließend wurde der mehrfache Einsatz der enzymbeladenen Partikel modellhaft am Beispiel der Prozesswasserentfärbung aus der Textilindustrie mit Laccase gezeigt und eine Kostenrechnung durchgeführt.
- ItemUniversal emulsion stabilization from the arrested adsorption of rough particles at liquid-liquid interfaces([London] : Nature Publishing Group UK, 2017) Zanini, Michele; Marschelke, Claudia; Anachkov, Svetoslav E.; Marini, Emanuele; Synytska, Alla; Isa, LucioSurface heterogeneities, including roughness, significantly affect the adsorption, motion and interactions of particles at fluid interfaces. However, a systematic experimental study, linking surface roughness to particle wettability at a microscopic level, is currently missing. Here we synthesize a library of all-silica microparticles with uniform surface chemistry, but tuneable surface roughness and study their spontaneous adsorption at oil-water interfaces. We demonstrate that surface roughness strongly pins the particles' contact lines and arrests their adsorption in long-lived metastable positions, and we directly measure the roughness-induced interface deformations around isolated particles. Pinning imparts tremendous contact angle hysteresis, which can practically invert the particle wettability for sufficient roughness, irrespective of their chemical nature. As a unique consequence, the same rough particles stabilize both water-in-oil and oil-in-water emulsions depending on the phase they are initially dispersed in. These results both shed light on fundamental phenomena concerning particle adsorption at fluid interfaces and indicate future design rules for particle-based emulsifiers.
- ItemReconfigurable assembly of charged polymer-modified Janus and non-Janus particles: From half-raspberries to colloidal clusters and chains(Cambridge : Royal Society of Chemistry, 2019) Marschelke, Claudia; Diring, Olga; Synytska, AllaUnderstanding the dynamic and reversible assembly of colloids and particles into complex constructs, inspired by natural phenomena, is of fundamental significance for the fabrication of multi-scale responsive and reconfigurable materials. In this work, we investigate the pH-triggered and reconfigurable assembly of structures composed of binary mixtures of oppositely charged polyacrylic acid (PAA)-modified non-Janus and poly(2-dimethylamino)ethyl methacrylate (PDMAEMA)/poly(N-isopropylacrylamide) (PNIPAM)-modified Janus particles driven by electrostatic interactions. Three different target structures are visible both in dispersions and in dry state: half-raspberry structures, colloidal clusters and colloidal chains depending on the mass, numerical and particle size ratio. All formed structures are well-defined and stable in a certain pH range. Half-raspberry-like structures are obtained at pH 6 and numerical ratios NJP/PAA-HP of 1 : 500 (for 200-PAA-HP), 1 : 44 (for 450-PAA-HP) and 1 : 15 (for 650-PAA-HP), respectively, due to electrostatic interactions between the central JP and the excessive PAA-HP. Colloidal chains and cluster-like structures are generated at numerical ratios NJP/PAA-HP of 4 : 5 (for 200-PAA-HP), 4 : 3 (for 450-PAA-HP), and 4 : 1 (for 650-PAA-HP). Moreover, the smaller the size of a "connecting" PAA colloid, the larger is the average length of a colloidal chain. Depending on the particle size ratio SJP/PAA-HP, some of the observed structures can be disassembled on demand by changing the pH value either close to the IEP of the PDMAEMA (for half-raspberries) or PAA (for colloidal clusters and chains) and then reassembled into new stable structures many times. The obtained results open a pathway to pH-controlled reconfigurable assembly of a binary mixture composed of polymeric-modified non-Janus and Janus particles, which allow the reuse of particle building blocks. © 2019 The Royal Society of Chemistry.
- ItemThermo-responsive polymer brushes with side graft chains: Relationship between molecular architecture and underwater adherence(Basel : Molecular Diversity Preservation International, 2019) Sidoli, Ugo; Tee, Hisaschi T.; Raguzin, Ivan; Mühldorfer, Jakob; Wurm, Frederik R.; Synytska, AllaDuring the last few decades, wet adhesives have been developed for applications in various fields. Nonetheless, key questions such as the most suitable polymer architecture as well as the most suitable chemical composition remain open. In this article, we investigate the underwater adhesion properties of novel responsive polymer brushes with side graft chain architecture prepared using “grafting through” approach on flat surfaces. The incorporation in the backbone of thermo-responsive poly(N-isopropylacrylamide) (PNIPAm) allowed us to obtain LCST behavior in the final layers. PNIPAm is co-polymerized with poly(methyl ethylene phosphate) (PMEP), a poloyphosphoester. The final materials are characterized studying the surface-grafted polymer as well as the polymer from the bulk solution, and pure PNIPAm brush is used as reference. PNIPAm-g-PMEP copolymers retain the responsive behavior of PNIPAm: when T > LCST, a clear switching of properties is observed. More specifically, all layers above the critical temperature show collapse of the chains, increased hydrophobicity and variation of the surface charge even if no ionizable groups are present. Secondly, effect of adhesion parameters such as debonding rate and contact time is studied. Thirdly, the reversibility of the adhesive properties is confirmed by performing adhesion cycles. Finally, the adhesive properties of the layers are studied below and above the LCST against hydrophilic and hydrophobic substrates. © 2019 by the authors. Licensee MDPI, Basel, Switzerland.
- ItemTuning the Interactions in Multiresponsive Complex Coacervate-Based Underwater Adhesives(Basel : Molecular Diversity Preservation International, 2020) Dompé, Marco; Cedano-Serrano, Francisco J.; Vahdati, Mehdi; Sidoli, Ugo; Heckert, Olaf; Synytska, Alla; Hourdet, Dominique; Creton, Costantino; van der Gucht, Jasper; Kodger, Thomas; Kamperman, MarleenIn this work, we report the systematic investigation of a multiresponsive complex coacervate-based underwater adhesive, obtained by combining polyelectrolyte domains and thermoresponsive poly(N-isopropylacrylamide) (PNIPAM) units. This material exhibits a transition from liquid to solid but, differently from most reactive glues, is completely held together by non-covalent interactions, i.e., electrostatic and hydrophobic. Because the solidification results in a kinetically trapped morphology, the final mechanical properties strongly depend on the preparation conditions and on the surrounding environment. A systematic study is performed to assess the effect of ionic strength and of PNIPAM content on the thermal, rheological and adhesive properties. This study enables the optimization of polymer composition and environmental conditions for this underwater adhesive system. The best performance with a work of adhesion of 6.5 J/m2 was found for the complex coacervates prepared at high ionic strength (0.75 M NaCl) and at an optimal PNIPAM content around 30% mol/mol. The high ionic strength enables injectability, while the hydrated PNIPAM domains provide additional dissipation, without softening the material so much that it becomes too weak to resist detaching stress. © 2019 by the authors. Licensee MDPI, Basel, Switzerland.
- ItemJanus particles: from concepts to environmentally friendly materials and sustainable applications(Berlin ; Heidelberg : Springer, 2020) Marschelke, Claudia; Fery, Andreas; Synytska, AllaJanus particles represent a unique group of patchy particles combining two or more different physical or chemical functionalities at their opposite sides. Especially, individual Janus particles (JPs) with both chemical and geometrical anisotropy as well as their assembled layers provide considerable advantages over the conventional monofunctional particles or surfactant molecules offering (a) a high surface-to-volume ratio; (b) high interfacial activity; (c) target controlling and manipulation of their interfacial activity by external signals such as temperature, light, pH, or ionic strength and achieving switching between stable emulsions and macro-phase separation; (d) recovery and recycling; (e) controlling the mass transport across the interface between the two phases; and finally (f) tunable several functionalities in one particle allowing their use either as carrier materials for immobilized catalytically active substances or, alternatively, their site-selective attachment to substrates keeping another functionality active for further reactions. All these advantages of JPs make them exclusive materials for application in (bio-)catalysis and (bio-)sensing. Considering “green chemistry” aspects covering biogenic materials based on either natural or fully synthetic biocompatible and biodegradable polymers for the design of JPs may solve the problem of toxicity of some existing materials and open new paths for the development of more environmentally friendly and sustainable materials in the very near future. Considering the number of contributions published each year on the topic of Janus particles in general, the number of contributions regarding their environmentally friendly and sustainable applications is by far smaller. This certainly pinpoints an important challenge and is addressed in this review article. The first part of the review focuses on the synthesis of sustainable biogenic or biocompatible Janus particles, as well as strategies for their recovery, recycling, and reusability. The second part addresses recent advances in applications of biogenic/biocompatible and non-biocompatible JPs in environmental and biotechnological fields such as sensing of hazardous pollutants, water decontamination, and hydrogen production. Finally, we provide implications for the rational design of environmentally friendly and sustainable materials based on Janus particles. [Figure not available: see fulltext.]. © 2020, The Author(s).
- ItemImpact of surface charge on the motion of light-activated Janus micromotors(Berlin ; Heidelberg : Springer, 2021) Huang, Tao; Ibarlucea, Bergoi; Caspari, Anja; Synytska, Alla; Cuniberti, Gianaurelio; de Graaf, Joost; Baraban, LarysaControl over micromotors' motion is of high relevance for lab-on-a-chip and biomedical engineering, wherein such particles encounter complex microenvironments. Here, we introduce an efficient way to influence Janus micromotors' direction of motion and speed by modifying their surface properties and those of their immediate surroundings. We fabricated light-responsive Janus micromotors with positive and negative surface charge, both driven by ionic self-diffusiophoresis. These were used to observe direction-of-motion reversal in proximity to glass substrates for which we varied the surface charge. Quantitative analysis allowed us to extract the dependence of the particle velocity on the surface charge density of the substrate. This constitutes the first quantitative demonstration of the substrate's surface charge on the motility of the light-activated diffusiophoretic motors in water. We provide qualitative understanding of these observations in terms of osmotic flow along the substrate generated through the ions released by the propulsion mechanism. Our results constitute a crucial step in moving toward practical application of self-phoretic artificial micromotors.