This study focused on the cross-linking of poly(2-isopropenyl-2-oxazoline) (PiPOx) with gelatin to obtain strong, degradable hybrid hydrogels with good cell adhesion. The molecular weight and concentration of PiPOx and the PiPOx-to-gelatin ratio were varied to adjust the mechanical and swelling properties of the hybrid hydrogels. The swelling degree of PiPOx-gelatin hydrogels in water ranged between 1260 and 810%, with the corresponding Young's compressive moduli ranging from 77 to 215 kPa.
View Article and Find Full Text PDFPoly(2-isopropenyl-2-oxazoline) (PiPOx) is a functional polymer showing great potential for the development of smart biomaterials. The straightforward synthesis and post-polymerization functionalization of PiPOx offers many opportunities for tailoring the properties of the polymer towards biomaterials. In this study we report for the first time PiPOx-based cationic charged polymethacrylamides with amino acid side chains that can complex siRNA and promote transfection in vitro.
View Article and Find Full Text PDFThe synthesis of poly(-allyl acrylamide) (PNAllAm) as a platform for the preparation of functional hydrogels is described. The PNAllAm was synthesized via organocatalyzed amidation of poly(methyl acrylate) (PMA) with allylamine and characterized by H NMR spectroscopy, size exclusion chromatography (SEC), and turbidimetry, which allowed an estimation of the lower critical solution temperature of ∼26 °C in water. The PNAllAm was then used to make functional hydrogels via photoinitiated thiol-ene chemistry, where dithiothreitol (DTT) was used to cross-link the polymer chains.
View Article and Find Full Text PDFAzobenzenes are archetypal molecules that have a central role in fundamental and applied research. Over the course of almost two centuries, the area of azobenzenes has witnessed great achievements; azobenzenes have evolved from simple dyes to 'little engines' and have become ubiquitous in many aspects of our lives, ranging from textiles, cosmetics, food and medicine to energy and photonics. Despite their long history, azobenzenes continue to arouse academic interest, while being intensively produced for industrial purposes, owing to their rich chemistry, versatile and straightforward design, robust photoswitching process and biodegradability.
View Article and Find Full Text PDFThe design and synthesis of double network (DN) hydrogels that can mimic the properties and/or structure of natural tissue has flourished in recent years, overcoming the bottlenecks of mechanical performance of single network hydrogels and extending their potential applications in various fields. In recent years, such bioinspired DN hydrogels with extraordinary mechanical performance, excellent biocompatibility, and considerable strength have been demonstrated to be promising candidates for biomedical applications, such as tissue engineering and biomedicine. In this minireview, we provide an overview of the recent developments of bioinspired DN hydrogels defined as DN hydrogels that mimic the properties and/or structure of natural tissue, ranging from, e.
View Article and Find Full Text PDFBiomacromolecules
December 2021
Poly(2-isopropenyl-2-oxazoline) (PiPOx) is emerging as a promising, versatile polymer platform to design functional materials and particularly biomaterials that rely on the hydrophilic character of the 2-oxazoline side units. To be able to assess the applicability of PiPOx in a biomedical context, it is essential to understand its stability and degradation behavior in physiological conditions. In the present work, the hydrolytic stability of PiPOx was systematically investigated as a function of pH during incubation in various buffers.
View Article and Find Full Text PDFThe self-assembly of bis-tridentate ligands leads to the spontaneous formation of [2 × 2] grid-like metal complexes. However, the synthesis of such ligands is rather cumbersome. In the work, we demonstrate a straightforward synthesis route to prepare bis-tridentate 4,6-bis((1H-1,2,3-triazol-4-yl)-pyridin-2-yl)-2-phenylpyrimidine ligands through double CuAAC click chemistry with 4,6-bis(6-ethynylpyridin-2-yl)-2-phenylpyrimidine as well as their self-assembly into [2 × 2] grid-like metal complexes.
View Article and Find Full Text PDFTrigger-responsive materials are capable of controlled drug release in the presence of a specific trigger. Reduction induced drug release is especially interesting as the reductive stress is higher inside cells than in the bloodstream, providing a conceptual controlled release mechanism after cellular uptake. In this work, we report the synthesis of 5-fluorouracil (5-FU) molecularly imprinted polymers (MIPs) based on poly(2-isopropenyl-2-oxazoline) (PiPOx) using 3,3'-dithiodipropionic acid (DTDPA) as a reduction-responsive functional cross-linker.
View Article and Find Full Text PDFDespite the fact that pillar[n]arenes receive major interest as building blocks for supramolecular chemistry and advanced materials, their functionalization is generally limited to the modification of the hydroxy or alkoxy units present on the rims. This limited structural freedom restricts further developments and has very recently been overcome. In this article, we highlight three very recent studies demonstrating further structural diversification of pillar[n]arenes by partial removal of the alkoxy substituents on the rims, which can be considered as the next generation of pillar[n]arenes.
View Article and Find Full Text PDFIn this study, a supramolecular hydrogel formed by incorporating the 2,6-bis(1,2,3-triazol-4-yl)-pyridine (btp) ligand in the backbone of a polymer prepared by copper(I)-catalyzed alkyne-azide cycloaddition (CuAAC) "click" polyaddition reaction of 2,6-diethynylpyridine and diazido-poly(ethylene glycol) is reported. The hydrogelation is selectively triggered by the addition of Ni ions to aqueous copolymer solutions. The gelation and rheological properties could be tuned by the change of metal to ligand ratio and polymer concentration.
View Article and Find Full Text PDFThe design and synthesis of polymer-based metallomacrocycles relying on metal-ligand interactions remain a challenge in the polymer field. Instead of utilizing chemical reactions to synthesize macrocycles, a general approach is proposed to construct metallomacrocyclic structures through supramolecular self-assembly of a specific macroligand with suitable transition metal ions. Therefore, a new ditopic macroligand (L) consisting of PEG end-capped with 2,6-bis(1,2,3-triazol-4-yl)pyridine derivatives is prepared via CuAAC "click" reaction.
View Article and Find Full Text PDFPlasma polymerization is gaining popularity as a technique for coating surfaces due to the low cost, ease of operation, and substrate-independent nature. Recently, the plasma polymerization (or deposition) of 2-oxazoline monomers was reported resulting in coatings that have potential applications in regenerative medicine. Despite the structural versatility of 2-oxazolines, only a few monomers have been subjected to plasma polymerization.
View Article and Find Full Text PDFPhotoswitches: Exciting recent progress realized in the field of light-controlled polymeric materials is highlighted. It is discussed how the rational choice of azobenzene molecules and their incorporation into complex materials by making use of physical interactions can lead to genuine photocontrollable polymeric systems.
View Article and Find Full Text PDFWe report the observation of simultaneous two and three photon resonances, enhancing the third-order NLO susceptibility in a thin film of an azo-dye polymer. The possibility of 2-3 orders of magnitude increase in χ((3)) susceptibility is sustained by quantum mechanical calculations. This improves the applications of azo-polymers in all optical signal processing as well as in nonlinear optical imaging.
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