热凝胶半秃胶束和相应的渗透凝胶网络【复旦大学】

2019-04-22

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Semi-bald Micelles and Corresponding Percolated Micelle Networks of Thermogels

Author:Shuquan Cui, Lin Yu , and Jiandong Ding* 

State Key Laboratory of Molecular Engineering of Polymers, Department of Macromolecular Science, Fudan University, Shanghai 200438, China

Source:Macromolecules, 2018, 51 (16), pp 6405–6420

DOI:10.1021/acs.macromol.8b01014

Publication Date (Web):August 14, 2018

Subject:

Monte Carlo method, aqueous solutions, biodegradability, composite polymers, computer simulation, energy transfer, fluorescence, hydrogels, hydrophobicity, light scattering, micelles, nuclear magnetic resonance spectroscopy, polyesters, polymerization

Abstract:

As an injectable and biodegradable hydrogel, thermogels of amphiphilic block copolymers of polyester and polyether in water show great potential in biomedical fields. It is challenging to reveal the mechanism behind the reversed thermogelling with sol–gel transition upon heating. Herein, a computer simulation and corresponding experiments are combined to examine aqueous systems of amphiphilic diblock copolymer of methoxypoly(ethylene glycol) and poly(d,l-lactide-co-glycolide). We synthesized the copolymer via ring-opening polymerization and characterized the thermogelling behavior of its aqueous solution by 3D dynamic light scattering and diffusing wave spectroscopy. Fluorescence resonance energy transfer and 13C NMR spectroscopy etc. were also adopted to explore the structure change during thermogelation. A dynamic Monte Carlo simulation was performed for a corresponding multichain system. A new type of micelle, the semi-bald micelle, was first proposed as the precursor for thermogelling and was confirmed from both simulations and experiments. We demonstrate that the thermogel structure is a percolated micelle network with hydrophobic channels that evolved from the semi-bald micelles. The thermogelling mechanism is discussed at the chain level. On the basis of the mechanism study, we put forward the molecular design principle of the thermogels.

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