Diversiform and Transformable Glyco-Nanostructures Constructed from Amphiphilic Supramolecular Metallocarbohydrates through Hierarchical Self-Assembly: The Balance between Metallacycles and Saccharides

  • During the past decade, self-assembly of saccharide-containing amphiphilic molecules toward bioinspired functional glycomaterials has attracted continuous attention due to their various applications in fundamental and practical areas. However, it still remains a great challenge to prepare hierarchical glycoassemblies with controllable and diversiform structures because of the complexity of saccharide structures and carbohydrate-carbohydrate interactions. Herein, through hierarchical self-assembly of modulated amphiphilic supramolecular metallocarbohydrates, we successfully prepared various well-defined glyco-nanostructures in aqueous solution, including vesicles, solid spheres, and opened vesicles depending on the molecular structures of metallocarbohydrates. More attractively, these glyco-nanostructures can further transform into other morphological structures in aqueous solutions such as worm-like micelles, tubules, and even tupanvirus-like vesicles (TVVs). It is worth mentioning that distinctive anisotropic structures including theDuring the past decade, self-assembly of saccharide-containing amphiphilic molecules toward bioinspired functional glycomaterials has attracted continuous attention due to their various applications in fundamental and practical areas. However, it still remains a great challenge to prepare hierarchical glycoassemblies with controllable and diversiform structures because of the complexity of saccharide structures and carbohydrate-carbohydrate interactions. Herein, through hierarchical self-assembly of modulated amphiphilic supramolecular metallocarbohydrates, we successfully prepared various well-defined glyco-nanostructures in aqueous solution, including vesicles, solid spheres, and opened vesicles depending on the molecular structures of metallocarbohydrates. More attractively, these glyco-nanostructures can further transform into other morphological structures in aqueous solutions such as worm-like micelles, tubules, and even tupanvirus-like vesicles (TVVs). It is worth mentioning that distinctive anisotropic structures including the opened vesicles (OVs) and TVVs were rarely reported in glycobased nano-objects. This intriguing diversity was mainly controlled by the subtle structural trade-off of the two major components of the amphiphiles, i.e., the saccharides and metallacycles. To further understand this precise structural control, molecular simulations provided deep physical insights on the morphology evolution and balancing of the contributions from saccharides and metallacycles. Moreover, the multivalency of glyco-nanostructures with different shapes and sizes was demonstrated by agglutination with a diversity of sugarbinding protein receptors such as the plant lectins Concanavalin A (ConA). This modular synthesis strategy provides access to systematic tuning of molecular structure and self-assembled architecture, which undoubtedly will broaden our horizons on the controllable fabrication of biomimetic glycomaterials such as biological membranes and supramolecular lectin inhibitors.show moreshow less

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Author:Guang Yang, Wei Zheng, Guoqing Tao, Libin Wu, Qi-Feng Zhou, Zdravko KochovskiORCiD, Tan Ji, Huaijun Chen, Xiaopeng LiORCiD, Yan Lu, Hong-ming DingORCiD, Hai-Bo YangORCiDGND, Guosong ChenORCiD, Ming Jiang
DOI:https://doi.org/10.1021/acsnano.9b07134
ISSN:1936-0851
ISSN:1936-086X
Pubmed Id:http://www.ncbi.nlm.nih.gov/pubmed?term=31651143
Parent Title (English):ACS nano
Publisher:American Chemical Society
Place of publication:Washington
Document Type:Article
Language:English
Date of first Publication:2019/09/26
Year of Completion:2019
Release Date:2020/10/11
Tag:anisotropic structures; diversiform structures; glycomaterials; hierarchical self-assembly; metallocarbohydrates
Volume:13
Issue:11
Pagenumber:12
First Page:13474
Last Page:13485
Funder:NSFC/ChinaNational Natural Science Foundation of China [21625202, 51721002, 21861132012, 21975047, 91527305]; STCSMScience & Technology Commission of Shanghai Municipality (STCSM) [16XD1401000]; Program for Changjiang Scholars and Innovative Research Team in UniversityProgram for Changjiang Scholars & Innovative Research Team in University (PCSIRT); CPSFChina Postdoctoral Science Foundation [2017M621354, 2018T110335]; Open Research Fund Program of Shandong Provincial Key Laboratory of Glycoscience & Glycotechnology (Ocean University of China)
Organizational units:Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie
Dewey Decimal Classification:5 Naturwissenschaften und Mathematik / 54 Chemie / 540 Chemie und zugeordnete Wissenschaften
Peer Review:Referiert