论文标题
熵驱动的热胶合二聚体
Entropy driven thermo-gelling vitrimer
论文作者
论文摘要
热凝胶聚合物被认为是有希望的智能生物材料，但仅限于它们的机械和热力学稳定性弱。在这里，我们提出了一种新的热纤维玻璃二聚体，该玻璃二聚体保持在液态状态，因为添加了防止交联的保护剂分子，并且随着温度的升高，会发生熵驱动的交联以诱导Sol-gel transition。此外，我们发现，玻璃二聚体的分解反应中的激活屏障起着重要作用，并且在实验上可以使用催化剂来调整激活屏障以驱动玻璃体在高温下形成平衡凝胶，这不受任何热力学不稳定性的影响。我们制定了一种平均场理论来描述玻璃二聚体的熵驱动的交联，该玻璃二聚体与计算机模拟定量一致，并为生物医学应用设计和制造新型玻璃体的设计和制造铺平了道路。
Thermo-gelling polymers have been envisioned as promising smart biomaterials but limited to 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 design and fabrication of novel vitrimers for biomedical applications.
