Structural Analysis and Mechanical Characterization of Hyaluronic Acid-Based Doubly Cross-Linked Networks.

Structural Analysis and Mechanical Characterization of Hyaluronic Acid-Based Doubly Cross-Linked Networks.
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DOI:
10.1021/ma8019442
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发表时间:
2009
期刊:
影响因子:
5.5
通讯作者:
Jia, Xinqiao
Jia, Xinqiao
中科院分区:
化学1区
文献类型:
--
作者:
Jha, Amit K.;Hule, Rohan A.;Jiao, Tong;Teller, Sean S.;Clifton, Rodney J.;Duncan, Randall L.;Pochan, Darrin J.;Jia, Xinqiao

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我们已经创建了一类新的基于透明质酸(HA)的水凝胶材料,其中HA水凝胶颗粒(HGP)嵌入并共价交联到二级网络中。采用改进的反胶束聚合技术合成了平均粒径约为900 nm、粒径分布较窄的HA HGP。通过蛋白质摄取实验估计HGP的平均筛目尺寸为约5.5至7.0 nm。高碘酸钠氧化不仅引入了醛基,而且降低了平均粒径。所产生的醛基用作反应性柄,用于随后与含有酰肼基团的HA衍生物交联。由此产生的宏观凝胶包含两个不同的分层网络(双交联网络,DXN):一个在单个颗粒内,另一个在不同颗粒之间。包括通过直接混合具有相互反应基团的HA衍生物形成的块状凝胶(BG)用于比较。水凝胶的微观结构,其特征在于集体显微镜和中子散射技术。使用受控应力流变仪在低频(0.1 - 10 Hz)下和使用自制扭转波装置在高频(高达200 Hz)下对它们的粘弹性进行量化。BG和DXN都是稳定的弹性凝胶,在较高的频率下变得更硬。基于HA的DXN具有独特的结构层次和机械性能,适用于软组织再生。
We have created a new class of hyaluronic acid (HA)-based hydrogel materials with HA hydrogel particles (HGPs) embedded in and covalently cross-linked to a secondary network. HA HGPs with an average diameter of ∼900 nm and narrow particle size distribution were synthesized using a refined reverse micelle polymerization technique. The average mesh size of the HGPs was estimated to be approximately 5.5 to 7.0 nm by a protein uptake experiment. Sodium periodate oxidation not only introduced aldehyde groups to the particles but also reduced the average particle size. The aldehyde groups generated were used as reactive handles for subsequent cross-linking with an HA derivative containing hydrazide groups. The resulting macroscopic gels contain two distinct hierarchical networks (doubly cross-linked networks, DXNs): one within individual particles and another among different particles. Bulk gels (BGs) formed by direct mixing of HA derivatives with mutually reactive groups were included for comparison. The hydrogel microstructures were collectively characterized by microscopy and neutron scattering techniques. Their viscoelasticity was quantified at low frequencies (0.1−10 Hz) using a controlled stress rheometer and at high frequencies (up to 200 Hz) with a home-built torsional wave apparatus. Both BGs and DXNs are stable elastic gels that become stiffer at higher frequencies. The HA-based DXN offers unique structural hierarchy and mechanical properties that are suitable for soft tissue regeneration.
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