Carbohydrate Polymers ( IF 10.7 ) Pub Date : 2023-07-01 , DOI: 10.1016/j.carbpol.2023.121173 Tessali X Morrison 1 , William M Gramlich 2
Carboxymethyl cellulose modified with norbornene groups (NorCMC) and cellulose nanofibrils (CNFs) produced through mechanical refining without chemical pretreatment formed interpenetrating network hydrogels through a UV-light initiated thiol-ene reaction. The molar ratio of thiols in crosslinkers to norbornene groups off the NorCMC (T:N), total polymer weight percent in the hydrogel, and weight percent of CNFs of the total polymer content of the hydrogels were varied to control hydrogel properties. This method enabled orders of magnitude changes to behavior. Swelling in aqueous environments could be significant (>150 %) without CNFs to minimal (<15 %) with the use of 50 % CNFs. NorCMC and CNF networks interacted synergistically to create hydrogels with compression modulus values spanning 1 to 150 kPa - the values of most biological tissues. T:N and total polymer weight percent could be varied to create hydrogels with different CNF content, but the same compression modulus, targeting 10 and 100 kPa hydrogels and providing a system that can independently vary fibrillar content and bulk modulus. Analysis of the effective crosslinks, thiol-ene network mesh size, and burst release of the polymer indicated synergistic interactions of the NorCMC thiol-ene and CNFs networks. These interactions enhanced modulus and degradation control of the network under physiological conditions.
中文翻译:
降冰片烯改性羧甲基纤维素和纤维素纳米原纤维的可调节硫醇烯互穿网络水凝胶
降冰片烯基团改性的羧甲基纤维素(NorCMC)和通过机械精炼生产的纤维素纳米原纤维(CNF)无需化学预处理,通过紫外光引发的硫醇-烯反应形成互穿网络水凝胶。改变交联剂中的硫醇与 NorCMC 上的降冰片烯基团的摩尔比 (T:N)、水凝胶中的总聚合物重量百分比以及水凝胶的总聚合物含量中 CNF 的重量百分比,以控制水凝胶性能。这种方法使行为发生了数量级的变化。在没有 CNF 的情况下,水性环境中的膨胀可能会很显着 (>150 %),而在使用 50 % CNF 的情况下,膨胀可能会很小 (< 15 %)。NorCMC 和 CNF 网络协同相互作用,产生压缩模量值范围为 1 至 150 kPa(大多数生物组织的值)的水凝胶。T:N 和总聚合物重量百分比可以变化,以产生具有不同 CNF 含量但相同压缩模量的水凝胶,目标是 10 和 100 kPa 水凝胶,并提供一个可以独立改变原纤维含量和体积模量的系统。对聚合物的有效交联、硫醇-烯网络网格尺寸和突发释放的分析表明 NorCMC 硫醇-烯和 CNF 网络之间存在协同相互作用。这些相互作用增强了生理条件下网络的模量和降解控制。