Ryan Joshua L, Sosso Gabriele C, Bon Stefan A F
Department of Chemistry, The University of Warwick Coventry CV4 7AL UK https://bonlab.info
Chem Sci. 2024 Aug 12;15(35):14458-70. doi: 10.1039/d4sc02574a.
Legislative change and shifting consumer sentiment drive a need to replace polymers in certain products. Herein, we highlight that eutectic molecular glasses and liquids are promising but underutilized candidate materials. We formulate a series of hydrophobic eutectic molecular liquids and glasses by mixing their crystalline components. The eutectic composition of each mixture was determined by both differential scanning calorimetry (DSC) and UV-vis spectroscopic measurements, which were processed and analyzed using a trained partial least squares regression model. With product shelf-life in mind, the long-term stability (up to 14 months) of the amorphous materials towards crystallization was proven using powder X-ray diffraction (PXRD). Molecular dynamics (MD) simulations put forward potential design rules in terms of the physical stability of these glasses. Rheological properties were investigated from the perspective of processability. Low fragility indices were found for all liquids, aiding processability through glassblowing, fiber pulling, film formation and molding. We show that properties can be tailored by blending two different eutectic systems or simply adding a plasticizer. To demonstrate a potential application area, the 4-hydroxychalcone and bifonazole eutectic system was used as a matrix for controlled release studies of a model active ingredient.
立法变革和消费者观念的转变促使某些产品需要更换聚合物。在此,我们强调低共熔分子玻璃和液体是有前景但未得到充分利用的候选材料。我们通过混合其晶体成分配制了一系列疏水性低共熔分子液体和玻璃。每种混合物的低共熔组成通过差示扫描量热法(DSC)和紫外可见光谱测量来确定,这些测量数据使用经过训练的偏最小二乘回归模型进行处理和分析。考虑到产品保质期,使用粉末X射线衍射(PXRD)证明了无定形材料对结晶的长期稳定性(长达14个月)。分子动力学(MD)模拟从这些玻璃的物理稳定性方面提出了潜在的设计规则。从加工性能的角度研究了流变性能。发现所有液体的脆性指数都很低,有助于通过吹玻璃、拉纤维、成膜和成型等加工过程。我们表明,可以通过混合两种不同的低共熔体系或简单地添加增塑剂来调整性能。为了展示一个潜在的应用领域,4-羟基查耳酮和联苯苄唑低共熔体系被用作模型活性成分控释研究的基质。