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Title: Entropy-driven thermo-gelling vitrimer
Authors: Xia, Xiuyang
Rao, Peilin
Yang, Juan
Ciamarra, Massimo Pica
Ni, Ran
Keywords: Science::Chemistry
Issue Date: 2022
Source: Xia, X., Rao, P., Yang, J., Ciamarra, M. P. & Ni, R. (2022). Entropy-driven thermo-gelling vitrimer. JACS Au, 2(10), 2359-2366.
Project: RG59/21 
Journal: JACS Au 
Abstract: Thermo-gelling polymers have been envisioned as promising smart biomaterials but limited by their weak mechanical and thermodynamic stabilities. Here, we propose a new thermo-gelling vitrimer, which remains at a liquid state because of the addition of protector molecules preventing the crosslinking, and with increasing temperature, an entropy-driven crosslinking occurs to induce the sol-gel transition. Moreover, we find that the activation barrier in the metathesis reaction of vitrimers plays an important role, and experimentally, one can use catalysts to tune the activation barrier to drive the vitrimer to form an equilibrium gel at high temperature, which is not subject to any thermodynamic instability. We formulate a mean-field theory to describe the entropy-driven crosslinking of the vitrimer, which agrees quantitatively with computer simulations and paves the way for the design and fabrication of novel vitrimers for biomedical applications.
ISSN: 2691-3704
DOI: 10.1021/jacsau.2c00425
Schools: School of Chemical and Biomedical Engineering 
School of Physical and Mathematical Sciences 
Rights: © 2022 The Authors. Published by American Chemical Society. This is an open-access article distributed under the terms of the Creative Commons Attribution License.
Fulltext Permission: open
Fulltext Availability: With Fulltext
Appears in Collections:CCEB Journal Articles
SPMS Journal Articles

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