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Author: Gaitzsch, Jens × Has files: Yes ×

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    Novel monomers in radical ring-opening polymerisation for biodegradable and pH responsive nanoparticles
    (Brookfield, Conn. : Society of Plastic Engineers, 2019) Folini, Jenny; Huang, Chao-Hung; Anderson, James C.; Meier, Wolfgang P.; Gaitzsch, Jens
    Responsive and biodegradable nanoparticles are essential for functional drug delivery systems. We herein report the first pH sensitive polyester from radical ring-opening polymerisation of novel amine-bearing cyclic ketene acetals (CKAs). The CKAs were synthesised via an intermediate carbonate and the resulting polyesters showed a pKa around pH 6. Together with an initial application in biodegradable nanoparticles, they open the pathway for a new generation of functional polyesters.
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    Synthesis and complex self-assembly of amphiphilic block copolymers with a branched hydrophobic poly(2-oxazoline) into multicompartment micelles, pseudo-vesicles and yolk/shell nanoparticles
    (Cambridge : RSC Publ., 2020) Daubian, Davy; Gaitzsch, Jens; Meier, Wolfgang
    We report on the synthesis and self-assembly of poly(ethylene oxide)-block-poly(2-(3-ethylheptyl)-2-oxazoline) (PEO-b-PEHOx), a new amphiphilic diblock copolymer obtained via microwave-assisted polymerization of EHOx using a new nosylated PEO macroinitiator. The kinetics of the polymerization in different solvents was crucial to optimize the synthesis and revealed a controlled, yet fast polymerization of the AB diblock copolymer. Differential scanning calorimetry proved that PEO-b-PEHOx shows glass transition temperatures below room temperature, making it suitable for a wide range of self-assembly methods, especially under mild and solvent-free conditions. Self-assembly of PEO-b-PEHOx was then performed using film rehydration and solvent switch. In both cases, we were able to show the formation of various complex structures (multi-compartment micelles (MCMs), pseudo-vesicles and yolk/shell nanoparticles) by light scattering, TEM and Cryo-TEM. Our results show that PEO-b-PEHOx is a potent new AB diblock copolymer due to its fast synthesis and unique self-assembly behavior.
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    The chemistry of cross-linked polymeric vesicles and their functionalization towards biocatalytic nanoreactors
    (Berlin ; Heidelberg : Springer, 2020) Moreno, Silvia; Voit, Brigitte; Gaitzsch, Jens
    Self-assembly of amphiphilic block copolymers into polymersomes continues to be a hot topic in modern research on biomimetics. Their well-known and valued mechanical strength can be increased even further if they are cross-linked. These additional bonds prevent a collapse or disassembly of the polymersomes and open the way towards smart nanoreactors. A variety of chemistries have been applied to obtain the desired cross-linked polymersomes, and therefore, the chemical approaches performed over time will be highlighted in this mini-review. Due to the large number of studies, a selected set of photo-cross-linked and pH-sensitive polymersomes will be specifically highlighted. This system has proven to be a very potent candidate for the formation of nanoreactors and drug delivery systems, and even for the formation of functional multicompartment cell mimics. [Figure not available: see fulltext.]. © 2020, The Author(s).
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    Updating radical ring-opening polymerisation of cyclic ketene acetals from synthesis to degradation
    (Oxford : Elsevier, 2020) Folini, Jenny; Murad, Wigdan; Mehner, Fabian; Meier, Wolfgang; Gaitzsch, Jens
    Radical ring-opening polymerisation (RROP) of cyclic ketene acetals (CKAs) has gained momentum as it yields polyesters as biodegradable polymers from a radical polymerisation. In order to advance the polymerisation, some of its major limitations were addressed in the research presented, focussing on the four mainly used CKAs in modern research on RROP. Monomer synthesis has been updated towards a cobalt/TMSCl-based system that was performed reliably on several monomers at room temperature. Calculations using the density functional theory (DFT) revealed that the ring-opening step is energetically hampered in comparison to a ring-retaining reaction, which explained the challenges faced to promote the ring-opening reaction. Higher molecular weights up to four times the values reached by thermally initiated polymerisation were obtained by exploiting UV light and ultrasound as alternative methods to facilitate the polymerisation. The reaction procedure also influenced thermal properties of the polymers, which in turn affected the enzymatic degradation of nanoparticles based on those polymers. Altogether, the present study offers a holistic update to enhance the RROP of CKAs.
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    Deepening the insight into poly(butylene oxide)-block-poly(glycidol) synthesis and self-assemblies: micelles, worms and vesicles
    (Cambridge : RSC, 2020) Wehr, Riccardo; Gaitzsch, Jens; Daubian, Davy; Fodor, Csaba; Meier, Wolfgang
    Aqueous self-assembly of amphiphilic block copolymers is studied extensively for biomedical applications like drug delivery and nanoreactors. The commonly used hydrophilic block poly(ethylene oxide) (PEO), however, suffers from several drawbacks. As a potent alternative, poly(glycidol) (PG) has gained increasing interest, benefiting from its easy synthesis, high biocompatibility and flexibility as well as enhanced functionality compared to PEO. In this study, we present a quick and well-controlled synthesis of poly(butylene oxide)-block-poly(glycidol) (PBO-b-PG) amphiphilic diblock copolymers together with a straight-forward self-assembly protocol. Depending on the hydrophilic mass fraction of the copolymer, nanoscopic micelles, worms and polymersomes were formed as well as microscopic giant unilamellar vesicles. The particles were analysed regarding their size and shape, using dynamic and static light scattering, TEM and Cryo-TEM imaging as well as confocal laser scanning microscopy. We have discovered a strong dependence of the formed morphology on the self-assembly method and show that only solvent exchange leads to the formation of homogenous phases. Thus, a variety of different structures can be obtained from a highly flexible copolymer, justifying a potential use in biomedical applications. This journal is © The Royal Society of Chemistry.