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Bio-based glyco-bolaamphiphile forms a temperature-responsive hydrogel with tunable elastic properties

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Abstract

A bio-based glycolipid bolaamphiphile (glyco-bolaamphiphile) has recently been produced (Van Renterghem et al., Biotechnol. Bioeng., 2018, 115, 1195–1206) on a gram scale by using the genetically-engineered S. bombicola strain Δat Δsble Δfao1. The glyco-bolaamphiphile bears two symmetrical sophorose headgroups at the extremities of a C16:0 (ω-1 hydroxylated palmitic alcohol) spacer. Its atypical structure has been obtained by redesigning the S. bombicola strain Δat Δsble, producing non-symmetrical glyco-bolaamphiphile, with an additional knock out (Δfao1) and feeding this new strain with fatty alcohols. The molecular structure of the glyco-bolaamphiphile is obtained by feeding the new strain a saturated C16 substrate (palmitic alcohol), which enables the biosynthesis of bolaform glycolipids. In this work, we show that the bio-based glyco-bolaamphiphile readily forms a hydrogel in water at room temperature, and that the hydrogel formation depends on the formation of self-assembled fibers. Above 28 °C, the molecules undergo a gel-to-sol transition, which is due to a fiber-to-micelle phase change. We provide a quantitative description of the Self-Assembled Fibrillar Network (SAFiN) hydrogel formed by the glyco-bolaampiphile. We identify the sol–gel transition temperature, the gelling time, and the minimal gel concentration; additionally, we explore the fibrillation mechanism as a function of time and temperature and determine the activation energy of the micelle-to-fiber phase transition. These parameters allow control of the elastic properties of the glyco-bolaamphiphile hydrogel: at 3 wt% and 25 °C, the elastic modulus G′ is above the kPa range, while at 5 °C, G′ can be tuned between 100 Pa and 20 kPa, by controlling the undercooling protocol.

Graphical abstract: Bio-based glyco-bolaamphiphile forms a temperature-responsive hydrogel with tunable elastic properties

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Publication details

The article was received on 07 Jun 2018, accepted on 22 Jul 2018 and first published on 13 Sep 2018


Article type: Paper
DOI: 10.1039/C8SM01167B
Citation: Soft Matter, 2018, Advance Article
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    Bio-based glyco-bolaamphiphile forms a temperature-responsive hydrogel with tunable elastic properties

    N. Baccile, L. Van Renterghem, P. Le Griel, G. Ducouret, M. Brennich, V. Cristiglio, S. L. K. W. Roelants and W. Soetaert, Soft Matter, 2018, Advance Article , DOI: 10.1039/C8SM01167B

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