Issue 17, 2021

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

Abstract

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.

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

Supplementary files

Article information

Article type
Research Article
Submitted
09 מאי 2021
Accepted
17 יונ 2021
First published
07 יול 2021

Org. Chem. Front., 2021,8, 4715-4722

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

G. Wu, C. Liang, H. Li, X. Zhang, G. Yao, F. Zhu, Y. Hu, G. Yin, W. Zheng and Z. Lu, Org. Chem. Front., 2021, 8, 4715 DOI: 10.1039/D1QO00692D

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