Surface-Vinylated Cellulose Nanocrystals as Cross-Linkers for Hydrogel Composites

IF 5.4 2区化学 Q1 BIOCHEMISTRY & MOLECULAR BIOLOGY Biomacromolecules Pub Date : 2025-04-14 Epub Date: 2025-03-11 DOI:10.1021/acs.biomac.4c01619

Marcel Kröger , Timo Pääkkönen , Lukas Fliri , Anna F. Lehrhofer , Irina Sulaeva , Antje Potthast , Eero Kontturi

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Abstract

Cellulose nanocrystal (CNC) fillers have been shown to significantly improve the performance of polymer composites and hydrogels, elevating both strength and toughness. Polymer grafting from the surface of the nanocrystals has been employed to enhance matrix–filler interactions and keep the fillers dispersed within the matrix. However, such approaches often rely on multistep syntheses and diligent process control. Here, we propose modifying the nanocrystal surface to carry vinyl moieties, turning the particles into cross-linking comonomers. Using allyl glycidyl ether in an aqueous modification route, we were able to decorate the CNCs with varying amounts of vinyl moieties. Subsequent dispersion in 2-hydroxy methacrylate and thermally initiated free radical polymerization yielded composite materials that showed superior mechanical performance compared to those obtained from monomeric cross-linkers and unmodified CNCs. The large discrepancies in the observed glass transition temperatures of the obtained materials suggest, however, that the impact of the fillers on the polymerization kinetics is significant and less easily explained.

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表面乙烯化纤维素纳米晶作为水凝胶复合材料的交联剂。

纤维素纳米晶（CNC）填料已被证明可以显著改善聚合物复合材料和水凝胶的性能，提高强度和韧性。从纳米晶体表面接枝聚合物被用来增强基质-填料的相互作用，并保持填料在基质内的分散。然而，这种方法往往依赖于多步合成和勤奋的过程控制。在这里，我们建议修改纳米晶体表面以携带乙烯基基团，将颗粒转变为交联共聚物。使用烯丙基缩水甘油酯在水改性路线，我们能够用不同数量的乙烯基部分装饰CNCs。随后在2-羟基甲基丙烯酸酯中分散和热引发自由基聚合得到的复合材料与单体交联剂和未改性的cnc得到的复合材料相比，具有优越的机械性能。然而，所获得的材料在观察到的玻璃化转变温度上的巨大差异表明，填料对聚合动力学的影响是显著的，而且不容易解释。

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来源期刊

Biomacromolecules 化学-高分子科学

CiteScore

10.60

自引率

4.80%

发文量

417

审稿时长

1.6 months

期刊介绍： Biomacromolecules is a leading forum for the dissemination of cutting-edge research at the interface of polymer science and biology. Submissions to Biomacromolecules should contain strong elements of innovation in terms of macromolecular design, synthesis and characterization, or in the application of polymer materials to biology and medicine. Topics covered by Biomacromolecules include, but are not exclusively limited to: sustainable polymers, polymers based on natural and renewable resources, degradable polymers, polymer conjugates, polymeric drugs, polymers in biocatalysis, biomacromolecular assembly, biomimetic polymers, polymer-biomineral hybrids, biomimetic-polymer processing, polymer recycling, bioactive polymer surfaces, original polymer design for biomedical applications such as immunotherapy, drug delivery, gene delivery, antimicrobial applications, diagnostic imaging and biosensing, polymers in tissue engineering and regenerative medicine, polymeric scaffolds and hydrogels for cell culture and delivery.