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Issue 10, 2017
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Multi-component hybrid hydrogels – understanding the extent of orthogonal assembly and its impact on controlled release

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Abstract

This paper reports self-assembled multi-component hybrid hydrogels including a range of nanoscale systems and characterizes the extent to which each component maintains its own unique functionality, demonstrating that multi-functionality can be achieved by simply mixing carefully-chosen constituents. Specifically, the individual components are: (i) pH-activated low-molecular-weight gelator (LMWG) 1,3;2,4-dibenzylidenesorbitol-4′,4′′-dicarboxylic acid (DBS–COOH), (ii) thermally-activated polymer gelator (PG) agarose, (iii) anionic biopolymer heparin, and (iv) cationic self-assembled multivalent (SAMul) micelles capable of binding heparin. The LMWG still self-assembles in the presence of PG agarose, is slightly modified on the nanoscale by heparin, but is totally disrupted by the micelles. However, if the SAMul micelles are bound to heparin, DBS–COOH self-assembly is largely unaffected. The LMWG endows hybrid materials with pH-responsive behavior, while the PG provides mechanical robustness. The rate of heparin release can be controlled through network density and composition, with the LMWG and PG behaving differently in this regard, while the presence of the heparin binder completely inhibits heparin release through complexation. This study demonstrates that a multi-component approach can yield exquisite control over self-assembled materials. We reason that controlling orthogonality in such systems will underpin further development of controlled release systems with biomedical applications.

Graphical abstract: Multi-component hybrid hydrogels – understanding the extent of orthogonal assembly and its impact on controlled release

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Publication details

The article was received on 28 Jul 2017, accepted on 18 Aug 2017 and first published on 24 Aug 2017


Article type: Edge Article
DOI: 10.1039/C7SC03301J
Citation: Chem. Sci., 2017,8, 6981-6990
  • Open access: Creative Commons BY-NC license
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    Multi-component hybrid hydrogels – understanding the extent of orthogonal assembly and its impact on controlled release

    V. M. P. Vieira, L. L. Hay and D. K. Smith, Chem. Sci., 2017, 8, 6981
    DOI: 10.1039/C7SC03301J

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