Dataset Information

Spatially Resolved Crosslinking of Hydroxypropyl Cellulose Esters for the Generation of Functional Surface-Attached Organogels.

ABSTRACT: Chemistry, geometric shape and swelling behavior are the key parameters that determine any successful use of man-made polymeric networks (gels). While understanding of the swelling behavior of both water-swellable hydrogels and organogels that swell in organic solvents can be considered well-advanced with respect to fossil fuel-based polymer networks, the understanding, in particular, of wood-derived polymers in such a network architecture is still lacking. In this work, we focus on organogels derived from hydroxypropyl cellulose (HPC) ester. The latter polymer was functionalized with saturated and unsaturated fatty acids, respectively. Due to their tailored chemical constitution, we demonstrated that such polysaccharide can be crosslinked and simultaneously surface-bound by using a photo-induced radical reaction using a photo-initiator. Based on the choice of fatty acid used in the design of the HPC ester, and by controlling the degree of substitution (DS) obtained during the esterification of the polysaccharide, modular manipulation of the physical properties (e.g., polarity) of the resulting gel is possible. Depending on the initiator employed, different wavelengths of light, from UV to visible, can be utilized for the crosslinking reaction, which facilitates the deployment of a range of light sources and different lithographic methods. Additionally, we showed that altering of the illumination time allows to tailor the netpoint density, and thus, the degree of linear deformation in equilibrium and the swelling kinetics. Finally, we performed a proof-of-principle experiment to demonstrate the application of our material for the generation of spatially resolved polymer patches to enrich organic molecules from a solution within a microfluidic channel.

SUBMITTER: Nau M

PROVIDER: S-EPMC6543898 | biostudies-literature | 2019

REPOSITORIES: biostudies-literature

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Spatially Resolved Crosslinking of Hydroxypropyl Cellulose Esters for the Generation of Functional Surface-Attached Organogels.

Nau Maximilian M Trosien Simon S Seelinger David D Boehm Anna K AK Biesalski Markus M

Frontiers in chemistry 20190524

Chemistry, geometric shape and swelling behavior are the key parameters that determine any successful use of man-made polymeric networks (gels). While understanding of the swelling behavior of both water-swellable hydrogels and organogels that swell in organic solvents can be considered well-advanced with respect to fossil fuel-based polymer networks, the understanding, in particular, of wood-derived polymers in such a network architecture is still lacking. In this work, we focus on organogels d ...[more]

PMID: 31179272

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Project description:The lateral dimensions of micro- and nanostructures obtained by microcontact printing (μCP) can be easily varied by selecting stamps with the desired spacing and pattern. However, the height of these structures cannot be tuned as easily, and in most cases only 2D structures are obtained. Here, we show how the chemical cross-linking properties of polymer inks designed for μCP can be used to obtain 3D structures with heights ranging from 3 to 750 nm using the same μCP stamps. This is technologically relevant because the ink concentration affects the quality and resolution of the printed image, and therefore can only be varied in a certain range. By exploiting the cross-linking efficiency to tune the height, an additional parameter is available to reach the desired structure height without compromising the image quality. The inks were made from copolymers containing a low percentage of different UV cross-linkable repeat units: nitrobenzoxadiazole (NBD), coumarin (COU), and/or benzophenone (BP). The base polymer of the here presented model system was an antimicrobially active poly(oxanorbornene) (SMAMP), however the concept should be transferable to many other polymer backbones. We describe the fabrication and characterization of the printed micro- and nanostructures made from pure SMAMP, NBD-SMAMP, coumarin-SMAMP, BP-SMAMP, BP-NBD-SMAMP and BP-coumarin-SMAMP polymer inks. The photo-dimerization of COU during UV irradiation at λ = 254 nm was confirmed by UV-Vis spectroscopy. Since NBD and COU are fluorescent, the polymer could be visualized by fluorescence microscopy. Additionally, their height profiles were measured by atomic force microscopy (AFM). The heights of the 3D surface-attached polymer networks obtained from the here presented polymer inks correlated with the gel-content of the corresponding unstructured polymer layers, and thus with the cross-linking efficiency of the NBD, COU and BP cross-linkers. Due to being covalently cross-linked, these 3D-surface attached polymer structures were solvent-stable and stable in aqueous surroundings.

Dataset Information

Spatially Resolved Crosslinking of Hydroxypropyl Cellulose Esters for the Generation of Functional Surface-Attached Organogels.

Publications

Spatially Resolved Crosslinking of Hydroxypropyl Cellulose Esters for the Generation of Functional Surface-Attached Organogels.

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