期刊
ACS APPLIED MATERIALS & INTERFACES
卷 11, 期 41, 页码 38232-38239出版社
AMER CHEMICAL SOC
DOI: 10.1021/acsami.9b10239
关键词
hyaluronic acid; hydrogel; aldol chemistry; tissue adhesive; biomaterial
资金
- Swedish Strategic Research StemTherapy [Dnr 2009-1035]
- European Union's Seventh Framework Programme [FP7/2007-2013/607868, 607868]
- Swedish Foundation for Strategic Research (SSF) [SBE13-0028]
- Swedish Foundation for Strategic Research (SSF) [SBE13-0028] Funding Source: Swedish Foundation for Strategic Research (SSF)
Currently, there are limited approaches to tailor 3D scaffolds cross-linked with a stable covalent C-C bond that does not require any catalysts or initiators. We present here the first hydrogels employing aldol condensation chemistry that exhibit exceptional physicochemical properties. We investigated the aldol-cross-linking chemistry using two types of aldehyde-modified hyaluronic acid (HA) derivatives, namely, an enolizable HA-aldehyde (HA-EaI) and a non-enolizable HA-aldehyde (HA-NaI). Hydrogels formed using HA-EaI demonstrate inferior cross linking efficiency (due to intramolecular loop formation), when compared with hydrogels formed by mixing HA-EaI and HA-NaI leading to a cross-aldol product. The change in mechanical properties as a result of cross-linking at different pH values is determined using rheological measurements and is interpreted in terms of molecular weight between cross-links (Me). The novel HA cross-aldol hydrogel demonstrate excellent hydrolytic stability and favorable mechanical properties but allow hyaluronidase-mediated enzymatic degradation. Interestingly, residual aldehyde functionality within the aldol product rendered the tissue adhesive properties by bonding two bone tissues. The aldehyde functionality also facilitated facile post-synthetic modifications with nucleophilic reagents. Finally, we demonstrate that the novel hydrogel is biocompatible with encapsulated stem cells that show a linear rate of expansion in our 3-6 days of study.
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