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Robust Biopolymeric Supramolecular “Host−Guest Macromer” Hydrogels Reinforced by in Situ Formed Multivalent Nanoclusters for Cartilage Regeneration
Macromolecules ( IF 5.1 ) Pub Date : 2016-01-28 00:00:00 , DOI: 10.1021/acs.macromol.5b02527
Kongchang Wei , Meiling Zhu , Yuxin Sun , Jianbin Xu , Qian Feng , Sien Lin , Tianyi Wu , Jia Xu 1 , Feng Tian 2 , Jiang Xia , Gang Li , Liming Bian 3
Affiliation  

Biopolymer-based supramolecular hydrogels cross-linked by host–guest interactions are usually mechanically weak as shown in “inverted vials” instead of freestanding 3D constructs. Herein, we describe a novel host–guest macromer (HGM) approach for preparation of biopolymer-based freestanding supramolecular hydrogels. Host–guest macromers are formed by molecular self-assembly between adamantane-functionalized hyaluronic acid (ADxHA) guest polymers and monoacrylated β-cyclodextrins (mono-Ac-βCD) host monomers. Supramolecular hydrogels are readily prepared by UV-induced polymerization of the preassembled host–guest macromers. Such hydrogels are soely cross-linked by in situ formed multivalent host–guest nanoclusters and show significantly reinforced mechanical properties yet still retain desirable supramolecular features. They can self-heal and be remolded into freestanding 3D constructs which afford effective protection on the encapsulated stem cells during the compression remolding, making them promising carriers for therapeutic cells that can quickly adapt to and integrate with surrounding tissues of the targeted defects. We demonstrate that such hydrogels not only sustain extended release of encapsulated proteinaceous growth factors (TGF-β1) but also support chondrogenesis of the human mesenchymal stem cells (hMSCs) and promote cartilage regeneration in a rat model.

中文翻译:

原位形成的多价纳米簇增强软骨的健壮生物聚合物超分子“宿主-客体大分子”水凝胶。

通过宿主-客体相互作用交联的基于生物聚合物的超分子水凝胶通常在机械上较弱,如“倒置的小瓶”所示,而不是独立的3D构建体。本文中,我们描述了一种新颖的宿主-客体大分子单体(HGM)方法,用于制备基于生物聚合物的独立式超分子水凝胶。主客体大分子单体是由金刚烷官能化的透明质酸(AD x HA)客体聚合物与单丙烯酸β-环糊精(mono-Ac-βCD)主体单体之间的分子自组装形成的。超分子水凝胶很容易通过紫外线诱导的预组装主体-客体大分子单体的聚合反应制备。这类水凝胶通过原位交联而被彻底交联。形成了多价主客体纳米簇,并显示出明显增强的机械性能,但仍保留了理想的超分子特征。它们可以自我修复并重塑成独立的3D构建体,在压缩重塑过程中对封装的干细胞提供有效的保护,使其成为治疗细胞的有希望的载体,可以快速适应靶缺陷的周围组织并与周围组织整合。我们证明这种水凝胶不仅维持胶囊蛋白生长因子(TGF-β1)的延长释放,而且还支持人间充质干细胞(hMSCs)的软骨形成并促进大鼠模型中的软骨再生。
更新日期:2016-01-28
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