纤维素纳米晶体和 Pluronic F127 的热响应和可注射复合水凝胶,ACS Applied Bio Materials

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纤维素纳米晶体和 Pluronic F127 的热响应和可注射复合水凝胶
ACS Applied Bio Materials ( IF 4.6 ) Pub Date : 2021-03-10 , DOI: 10.1021/acsabm.1c00046
Eren Kushan ₁ , Erkan Senses ₁

Affiliation

由于其临界凝胶温度与人体温度接近，热响应性两亲 Pluronic F127 三嵌段共聚物溶液已在智能生物材料应用中得到广泛研究。同时，纤维素纳米晶体（CNCs）由于其生物相容性、丰富性、与药物分子结合的能力以及优异的流变特性，迅速成为许多药物递送和组织工程应用的焦点。在此，我们研究了含有纤维素纳米晶体（按重量计高达 5%）和温度响应性 Pluronic F127 的复合水凝胶的相行为和热流变特性。我们的结果揭示了 CNC 网络形成对三嵌段共聚物的胶束化和胶凝行为的前所未有的作用。线性和非线性流变分析表明，与纯 Pluronic F127 凝胶相比，在低和中等纳米晶体负载量（1-3% 重量）下，复合凝胶显着变得更柔软和可变形。软化效果是由棒状 CNC 破坏紧密堆积的胶束引起的。然而，在高浓度下，纳米晶体形成自己的网络，胶束被困在 CNC 网格内。结果，原始（纯 F127）硬凝胶模量在 4% 至 5% 的纳米晶体负载下恢复，但复合凝胶在 CNC 网络存在下更易变形（且更坚韧）。我们的温度扫描实验表明，添加高达 3% 的 CNC 不会改变 F127 溶液的快速热凝胶化；因此，这些复合材料适用于智能给药系统。另一方面，在较高的 CNC 浓度下，没有观察到突然的粘度转变，而是复合凝胶随着温度的升高而平滑地增稠，而水性纯 CNC 的热变薄则相反。因此，它们可以用作智能适应性生物润滑剂和生物粘性材料。

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Thermoresponsive and Injectable Composite Hydrogels of Cellulose Nanocrystals and Pluronic F127

Thermoresponsive amphiphilic Pluronic F127 triblock copolymer solutions have been widely investigated in smart biomaterial applications due to the proximity of its critical gel temperature to human body temperature. Meanwhile, cellulose nanocrystals (CNCs) have quickly become the focus of many drug delivery and tissue engineering applications due to their biocompatibility, abundance, ability to conjugate with drug molecules, and superior rheological properties. Herein, we investigate the phase behavior and thermo-rheological properties of the composite hydrogels containing cellulose nanocrystals (up to 5% by weight) and the temperature responsive Pluronic F127. Our results revealed an unprecedented role of CNC network formation on micellization and gelation behavior of the triblock copolymer. Linear and nonlinear rheological analysis suggest that at low and moderate nanocrystal loadings (1–3% by weight), the composite gel remarkably becomes softer and deformable compared to the neat Pluronic F127 gels. The softening effect results from the disruption of the close packed micelles by the rodlike CNCs. At high concentrations, however, the nanocrystals form their own network and the micelles are trapped within the CNC meshes. As a result, the original (neat F127) hard-gel modulus is recovered at 4 to 5% nanocrystal loading, yet the composite gel is much more deformable (and tougher) in the presence of the CNC network. Our temperature sweep experiments show that the CNC addition up to 3% does not change the rapid thermal gelation of the F127 solutions; therefore, these composites are suitable for smart drug delivery systems. On the other hand, at higher CNC concentrations, abrupt viscosity transition is not observed, rather the composite gels smoothly thicken with temperature in contrast to thermal thinning of the aqueous neat CNC. Thus, they can be used as smartly adaptive biolubricants and bioviscostatic materials.

更新日期：2021-04-19

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