- Advanced Polymer Synthesis and Characterization
- biodegradable polymer synthesis and properties
- Synthesis and properties of polymers
- X-ray Diffraction in Crystallography
- Crystallization and Solubility Studies
- Chemical Synthesis and Analysis
- Synthetic Organic Chemistry Methods
- Marine Sponges and Natural Products
- Polymer Surface Interaction Studies
- Oxidative Organic Chemistry Reactions
- Carbon dioxide utilization in catalysis
- Microbial Natural Products and Biosynthesis
- Click Chemistry and Applications
- Supramolecular Chemistry and Complexes
- Surfactants and Colloidal Systems
- Phytochemistry and Bioactive Compounds
- Chemical Synthesis and Reactions
- Surgical Sutures and Adhesives
- Traditional and Medicinal Uses of Annonaceae
- Bioactive Compounds and Antitumor Agents
- Catalytic Alkyne Reactions
- Machine Learning in Materials Science
- Fuel Cells and Related Materials
- Electrospun Nanofibers in Biomedical Applications
- Phosphorus compounds and reactions
Ghent University
1984-2022
Ghent University Hospital
2015-2020
Abstract The era of poly(ethylene glycol) (PEG) brushes as a universal panacea for preventing non‐specific protein adsorption and providing lubrication to surfaces is coming an end. In the functionalization medical devices implants, in addition cell adhesion, polymer‐brush formulations are often required generate highly lubricious films. Poly(2‐alkyl‐2‐oxazoline) (PAOXA) meet these requirements, depending on their side‐group composition, they can form films that match, some cases surpass,...
Poly(2-alkyl-2-oxazoline)s (PAOx) are regaining interest for biomedical applications. However, their full potential is hampered by the inability to synthesise uniform high-molar mass PAOx. In this work, we proposed alternative intrinsic chain transfer mechanisms based on 2-oxazoline and oxazolinium chain-end tautomerisation derived improved polymerization conditions suppress transfer, allowing synthesis of highly defined poly(2-ethyl-2-oxazoline)s up ca. 50 kDa (dispersity (Ð) <1.05)...
Abstract Even though functional copolymers with a low percentage of comonomer units (up to 20 mol%) are widely used, for instance the development polymer therapeutics and hydrogels, insights in group distribution over actual chains lacking average composition is conventionally used describe functionalization degree. Here we report visualization monomer different by synergetic combination experimental theoretical analysis aiming at construction functionality-chain length distributions...
Crosslinked hydrophilic poly(2-oxazoline)-based nanofibers amenable to facile multifunctionalization are fabricated using alkene-containing poly(2-alkyl-2-oxazoline)s (PAOx) via in situ photoinitiated radical thiol-ene crosslinking during electrospinning. The resulting crosslinked demonstrated be multifunctionalizable different chemistries as they contain two functional handles, being the alkene moieties from parent copolymer and residual thiol groups tetra-thiol-based crosslinker. While...
Herein, we describe a new method for the synthesis of superhydrophilic poly(2-alkyl-2-oxazoline)s (PAOx) from poly(2-ethyl-2-oxazoline) (PEtOx). A well-defined linear polyethylenimine was prepared PEtOx by controlled acidic hydrolysis its side-chains followed reacylation with different carboxylic acids. Using this protocol, obtained series hydrophilic PAOx containing side-chain ether groups potential in biomaterials science. The relative hydrophilicity polymers assessed, revealing that...
Poly(2-oxazoline)s and, more recently, also poly(2-oxazine)s represent an emerging class of polymers with a broad range applications. Surprisingly, to date, the statistical copolymerization these two cyclic imino ether monomers has not yet been reported. Herein, we demonstrate that 2-oxazines 2-oxazolines can lead formation amphiphilic gradient copolymers in single step. These combine high structural modularity poly(2-oxazoline)s excellent biological properties poly(2-oxazine)s, especially...
Herein, we provide a direct proof for differences in the micellar structure of amphiphilic diblock and gradient copolymers, thereby unambiguously demonstrating influence monomer distribution along polymer chains on micellization behavior. The internal block co poly(2-oxazolines) based hydrophilic poly(2-methyl-2-oxazoline) (PMeOx) hydrophobic poly(2-phenyl-2-oxazoline) (PPhOx) was studied water water-ethanol mixtures by small-angle X-ray scattering (SAXS), neutron (SANS), static dynamic...
Continuous flow synthesis in coupled microreactors is used to synthesize poly(2-oxazoline) triblock copolymers with very high precision times, which are from classical batch almost not accessible. Also, reactions speed up significantly leading full minutes rather than hours or days.
Cyclic versus linear: The superiority of cyclic polymers over their linear counterparts is highlighted. poly(2-oxazoline)s have been shown to provide excellent shielding properties when grafted TiO2 surfaces and Fe3 O4 nanoparticles owing ultrahigh grafting densities leading low friction surfaces, superior antifouling properties, extreme nanoparticle stabilization.
Poly(2-oxazoline)s are receiving large current interest based on their potential use in biomedical applications. Here we report a novel, straightforward route towards functional poly(2-oxazoline)s by Passerini and Ugi reactions.
The search for alternative solvents the cationic ring-opening polymerization (CROP) of 2-methyl-2-oxazoline (MeOx) is driven by poor solubility P(MeOx) in such as acetonitrile (CH3CN) and chlorobenzene well MeOx itself. In this study, solvent screening has revealed that especially sulfolane a good PMeOx. Unexpectedly, an increased propagation rate constant (kp) was found CROP sulfolane. Further extended kinetic studies at different temperatures (60–180 °C), acceleration due to increase...
Abstract A recently developed (4+3) cycloaddition between dienes and furfuryl alcohols, as precursors of oxyallyl‐type cations, has been used a key step in the racemic syntheses two natural products: frondosin B liphagal. This work demonstrates synthetic potential this reaction, offers short route to an interesting family products. full account these studies is presented, further illustrating mechanism, scope, limitations straightforward method for seven‐membered rings.
For the first time, formation of monomer sequences individual macromolecules during cationic ring-opening copolymerization (CROcoP) 2-methyl-2-oxazoline (MeOx) and 2-phenyl-2-oxazoline (PhOx) in acetonitrile (3 mol L–1; 100–140 °C; target degree polymerization (DP): 50–400) is visualized via kinetic Monte Carlo simulations with model parameters optimized based on experimental data. It shown that chain transfer β-elimination branching reactions are required to describe At complete conversion...
The photohydrogelation reaction of functional poly(2-oxazoline)s can be significantly accelerated by the presence weak hydrophobic interactions. Here we describe synthesis and cross-linking water-soluble poly(2-oxazoline) copolymers containing vinyl groups in side chains copolymerizing 2-methyl-2-oxazoline 2-undecenyl-2-oxazoline or 2-(3-butenyl)-2-oxazoline. An improved synthetic pathway to 2-(3-butenyl)-2-oxazoline monomer based on α-deprotonation is also included. When exposed radical...
Three new amidation approaches are evaluated to incorporate tyramine on methyl ester functional poly(2-oxazolines).
Addressing the polymerization of 2-ethyl-2-oxazoline (EtOx) in ethyl acetate to replace current state-of-the-art solvents. The switch is important towards pharmaceutical compliance/compatibility PEtOx, besides low environmental burden.
Cyclic imino ether heterocycles are used as ligands in transition metal catalysis, various drugs and reactive monomers living cationic ring-opening polymerization (CROP). While five- six-membered cyclic ethers, i.e. 2-oxazolines 4,5-dihydro-1,3-oxazines, have extensively been studied these areas, their seven-membered ring counterparts remained unexplored. Herein, we report the synthesis of 2-phenyl-4,5,6,7-tetrahydro-1,3-oxazepine allowing reassignment earlier, incorrectly reported...
Poly(2-alkyl-2-oxazoline)s (PAOx) exhibit different crystallization behavior depending on the length of alkyl side chain. PAOx having methyl, ethyl, or propyl chains do not show any bulk crystallization. Crystallization in heating cycle, that is, cold crystallization, is observed for with butyl and pentyl chains. For longer occurs cooling cycle. The attributed to polymer chain mobility line glass transition temperature (Tg) dependency length. decrease decreasing hinders relaxation backbone...
This work focuses on the synthesis and self-assembly of triphilic poly(2-oxazoline) triblock copolymers with high fluorine content toward our future aim developing magnetic resonance imaging (MRI) contrast agents. A highly fluorinated 2-substituted-2-oxazoline monomer, namely 2-(1H,1H,2H,2H-perfluorooctyl)-2-oxazoline, was synthesized using Grignard reaction. The polymerization kinetics monomer studied, it used for preparation hydrophilic 2-methyl-2-oxazoline, hydrophobic...
Naturally occurring oligoamines, such as spermine, spermidine, and putrescine, are well-known regulators of gene expression. These oligoamines frequently have short alkyl spacers with varying lengths between the amines. Linear polyethylenimine (PEI) is a polyamine that has been widely applied vector, various formulations currently in clinical trials. In order to emulate natural oligoamine regulators, linear random copolymers containing both PEI polypropylenimine (PPI) repeat units were...
The synthesis of new 2-cycloalkyl-2-oxazoline monomers, namely 2-cyclobutyl (cBuOx), 2-cyclopentyl (cPentOx) and 2-cyclohexyl-2-oxazoline (cHexOx) is described. Polymers thereof are semi-crystalline reveal unexpectedly high melting transitions.