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A multi-responsive supramolecular heparin-based biohybrid metallogel constructed by controlled self-assembly based on metal–ligand, host–guest and electrostatic interactions

Heparin-based gels constructed by non-covalent interactions can self-assemble into various nanostructures in solution, and can find applications in many fields such as nanodevices, drug delivery, and stimulus responsive materials synthesis. Herein, we describe the construction of a new class of supr...

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Published in:Organic chemistry frontiers an international journal of organic chemistry 2021-08, Vol.8 (17), p.4715-4722
Main Authors: Gui-Yuan, Wu, Liang, Chao, Li, Hao, Zhang, Xianyi, Yao, Guanxin, Fan-Fan, Zhu, Yi-Xiong, Hu, Guang-Qiang Yin, Zheng, Wei, Zhou, Lu
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Language:English
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Summary:Heparin-based gels constructed by non-covalent interactions can self-assemble into various nanostructures in solution, and can find applications in many fields such as nanodevices, drug delivery, and stimulus responsive materials synthesis. Herein, we describe the construction of a new class of supramolecular heparin-based biohybrid metallogels (HBMGs) with multiple stimuli-responsive behaviours through controlled self-assembly based on three orthogonal interactions, namely metal–ligand, host–guest and electrostatic interactions, within a single system. Specifically, a tris-[2]pseudorotaxane hexagonal metallacycle was synthesized by the orthogonal coordination-driven self-assembly and host–guest interactions. It was found that the obtained positively charged tris-[2]pseudorotaxane metallacycle can further form supramolecular HBMGs with heparin, one of the highest negatively charged biomolecule, via acid–base controlled multiple electrostatic interactions at lower concentrations. Notably, thermo-, acid–base and cation-induced gel–sol transitions were found to be completely reversible, reflecting the dynamic and controllable nature of such supramolecular materials. Hence, this research not only provides a simple yet highly efficient strategy for the fabrication of functional biohybrid materials involving metal–organic complexes and biomacromolecules, but also offers broad prospects for supramolecular engineering using precisely controlled self-assembly strategies.
ISSN:2052-4110
2052-4110
DOI:10.1039/d1qo00692d