Laboratory of Wood and Paper Chemistry , Johan Gadolin Process Chemistry Centre , Åbo Akademi University , Porthansgatan 3 , 20500 Turku , Finland.
ARC Centre of Excellence for Electromaterials Science, Intelligent Polymer Research Institute , University of Wollongong , Wollongong , NSW 2522 , Australia.
ACS Appl Mater Interfaces. 2019 Mar 6;11(9):8838-8848. doi: 10.1021/acsami.8b21268. Epub 2019 Feb 20.
Cellulose nanofibrils (CNFs) in the form of hydrogels stand out as a platform biomaterial in bioink formulation for 3D printing because of their low cytotoxicity and structural similarity to extracellular matrices. In the present study, 3D scaffolds were successfully printed with low-concentration inks formulated by 1 w/v % 2,2,6,6-tetramethylpiperidine-1-oxyl radical (TEMPO)-oxidized CNF with less than 1 w/v % gelatin methacrylate (GelMA). Quartz crystal microbalance with dissipation monitoring (QCM-D) measurements showed strong interaction between the two biopolymers. The UV cross-linking ability of GelMA (≤1 w/v %) was enhanced in the presence of TEMPO-oxidized CNFs. Multiple factors including strong physical interaction between CNF and GelMA, in situ cross-linking of CNF by Ca, and UV cross-linking of GelMA enabled successful 3D printing of low-concentration inks of CNF/GelMA into scaffolds possessing good structural stability. The mechanical strength of the scaffolds was tuned in the range of 2.5 to 5 kPa. The cell culture with 3T3 fibroblasts revealed noncytotoxic and biocompatible features for the formulated inks and printed scaffolds. More importantly, the incorporated GelMA in the CNF hydrogel promoted the proliferation of fibroblasts. The developed low-concentration CNF/GelMA formulations with a facile yet effective approach to fabricate scaffolds showed great potential in 3D printing for wound healing application.
纤维素纳米纤维（CNFs）以水凝胶的形式作为生物墨水配方中的平台生物材料脱颖而出，因为其细胞毒性低，并且结构与细胞外基质相似。在本研究中，通过使用浓度低于 1 w/v%的明胶甲基丙烯酰胺（GelMA）配制的浓度为 1 w/v%的 2,2,6,6-四甲基哌啶-1-氧自由基（TEMPO）氧化的 CNF 低浓度油墨成功地打印了 3D 支架。石英晶体微天平耗散监测（QCM-D）测量显示两种生物聚合物之间存在强烈相互作用。在 TEMPO 氧化的 CNF 存在下，GelMA（≤1 w/v%）的 UV 交联能力增强。多种因素包括 CNF 和 GelMA 之间的强烈物理相互作用、CNF 通过 Ca 的原位交联以及 GelMA 的 UV 交联，使得 CNF/GelMA 低浓度油墨能够成功地打印成具有良好结构稳定性的支架。支架的机械强度可在 2.5 至 5 kPa 的范围内进行调节。用 3T3 成纤维细胞进行细胞培养表明，所配制的油墨和打印的支架具有非细胞毒性和生物相容性特征。更重要的是，掺入 CNF 水凝胶中的 GelMA 促进了成纤维细胞的增殖。开发的低浓度 CNF/GelMA 配方具有简便有效的制造支架的方法，在伤口愈合应用的 3D 打印中具有很大的潜力。
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