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Adaptable covalently cross-linked fibers.

ABSTRACT: Fibers, with over 100 million tons produced each year, have been widely used in various areas. Recent efforts have focused on improving mechanical properties and chemical resistance of fibers via covalent cross-linking. However, the covalently cross-linked polymers are usually insoluble and infusible, and thus fiber fabrication is difficult. Those reported require complex multiple-step preparation processes. Herein, we present a facile and effective strategy to prepare adaptable covalently cross-linked fibers by direct melt spinning of covalent adaptable networks (CANs). At processing temperature, dynamic covalent bonds are reversibly dissociated/associated and the CANs are temporarily disconnected to enable melt spinning; at the service temperature, the dynamic covalent bonds are frozen, and the CANs exhibit favorable structural stability. We demonstrate the efficiency of this strategy via dynamic oxime-urethane based CANs, and successfully prepare adaptable covalently cross-linked fibers with robust mechanical properties (maximum elongation of 2639%, tensile strength of 87.68 MPa, almost complete recovery from an elongation of 800%) and solvent resistance. Application of this technology is demonstrated by an organic solvent resistant and stretchable conductive fiber.

SUBMITTER: Tan H

PROVIDER: S-EPMC10113382 | biostudies-literature | 2023 Apr

REPOSITORIES: biostudies-literature

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Adaptable covalently cross-linked fibers.

Tan Hui H Zhang Luzhi L Ma Xiaopeng X Sun Lijie L Yu Dingle D You Zhengwei Z

Nature communications 20230418 1

Fibers, with over 100 million tons produced each year, have been widely used in various areas. Recent efforts have focused on improving mechanical properties and chemical resistance of fibers via covalent cross-linking. However, the covalently cross-linked polymers are usually insoluble and infusible, and thus fiber fabrication is difficult. Those reported require complex multiple-step preparation processes. Herein, we present a facile and effective strategy to prepare adaptable covalently cross ...[more]

PMID: 37072415

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Project description:A versatile method is presented to form dendrimer superstructures by exploiting coacervate-core micelles as a template to confine and organize the hyperbranched macromolecules. First, complex coacervate-core micelles are formed from negative-neutral block copolymers and positively charged polyamidoamine dendrimers. The dendrimers inside the micellar core are then covalently cross-linked with each other upon addition of glutaraldehyde. After removal of the block copolymer from the assembly by increasing the salt concentration, consecutively, the formed Schiff bases cross-linking the dendrimers are reduced to amines, followed by a final dialysis step. This leads to well-defined covalently cross-linked nanostructures, coined dendroids, with a size of around 30 nm in diameter and a molecular weight of approximately 2.5 MDa. By incorporating dendrimer-encapsulated gold nanoparticles (AuDENs) into the micelle template strategy, the aggregation number of dendrimers inside the dendroids is determined by counting the nanoparticles in TEM micrographs. Furthermore, TEM performed at different tilt angles and AFM analysis corroborate formation of stable, covalently linked three-dimensional structures. Reconstruction of the TEM tilt series results in a tomogram further illustrating the 3D distribution of the gold nanoparticles, and hence the individual dendrimers, in the nanostructure. These dendroids appear to have a hard, poorly compressible core and a relatively soft outside. The versatility of the hierarchical building up of the supermolecules is illustrated by the controlled and synchronous incorporation of empty dendrimers and AuDENs into a single hybrid dendroid structure. The presented strategy allows for the preparation of a variety of classes of supermolecules, depending on the type of micellar-core macromolecule, e.g., dendrimer, cross-linker, and nanoparticles, used. Considering the broad interest in dendrimers as well as micelles in a plethora of research areas, e.g., (targeted) drug delivery, biomedical imaging, theragnostics, and catalysis, there is a great potential for dendroids and related classes of covalently linked macromolecules, viz., supermolecules.

Project description:The 3D printability of poly(l-lysine-ran-l-alanine) and four-arm poly(ethylene glycol) (P(KA)/4-PEG) hydrogels as 3D biomaterial inks was investigated using two approaches to develop P(KA)/4-PEG into 3D biomaterial inks. Only the "composite microgel" inks were 3D printable. In this approach, P(KA)/4-PEG hydrogels were processed into microparticles and incorporated into a polymer solution to produce a composite microgel paste. Polymer solutions composed of either 4-arm PEG-acrylate (4-PEG-Ac), chitosan (CS), or poly(vinyl alcohol) (PVA) were used as the matrix material for the composite paste. The three respective composite microgel inks displayed good 3D printability in terms of extrudability, layer-stacking ability, solidification mechanism, and 3D print fidelity. The biocompatibility of P(KA)/4-PEG hydrogels was retained in the 3D printed scaffolds, and the biofunctionality of bioinert 4-PEG and PVA hydrogels was enhanced. CS-P(KA)/4-PEG inks demonstrated excellent 3D printability and proved highly successful in printing scaffolds with a narrow strand diameter (∼200 μm) and narrow strand spacing (∼500 μm) while the integrity of the vertical and horizontal pores was maintained. Using different needle IDs and strand spacing, certain physical properties of the hydrogels could be tuned, while the 3D printed porosity was kept constant. This included the surface area to volume ratio, the macropore sizes, and the mechanical properties. The scaffolds demonstrated adequate adhesion and spreading of NIH 3T3 fibroblasts seeded on the scaffold surfaces for 4 days. Consequently, the scaffolds were considered suitable for potential applications in wound healing, as well as other soft tissue engineering applications. Apart from the contribution to new 3D biomaterial inks, this work also presented a new and facile method of processing covalently cross-linked hydrogels into 3D printed scaffolds. This could potentially "unlock" the 3D printability of biofunctional hydrogels, which are generally excluded from 3D printing applications.

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Adaptable covalently cross-linked fibers.

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Adaptable covalently cross-linked fibers.

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