Theory and computer modelling of self-organization of linear-dendritic macromolecules into colloidal nano-structures: impacts of topological and molecular mass polydispersity

线性树枝状大分子自组织成胶体纳米结构的理论和计算机建模：拓扑和分子质量多分散性的影响

• 批准号: 446008821
• 负责人: Professorin Dr. Friederike Schmid
• 金额: --
• 依托单位: Institut für Physik
• 依托单位国家: 德国
• 项目类别: Research Grants
• 资助国家: 德国
• 项目状态: 未结题
• 来源: https://gepris.dfg.de/gepris/projekt/446008821?language=en
• 关键词: Theory; computer; modelling; self; organization

We propose to explore the influence of intrinsic molecular-level disorder on the structure andproperties of self-assembled colloidal nanostructures made of block copolymers . Such structures are considered to have a huge potential in (bio)nanotechnology and medicine, e.g., as nano-scale carriers for drugs and genetic materials because their size, loading capacity and cargo release profiles can be fine-tuned by proper design of constituent copolymers. Dendritically branched copolymers are of particular interest, because of the large number of terminal groups that can be functionalized with targetable ligands. This allows one to efficiently connect different functional groups on one molecule and exploit bio-recognition mechanisms for controlled targetted delivery of the drugs to specific tissues or cells.Up-to-date experiments on the copolymer self-assembly were mostly rationalized on the basis of theories developed for perfectly monodisperse linear block copolymers.However, industrial manufacturing of novel pharmaceuticals requires the application of robust synthetic protocols that unavoidably result in molecular mass polydispersity and structural (topological) disorder of the products, i.e., the block copolymers. Preliminary studies of the PIs indicate that this is not necessarily a drawback: A certain amount of molecular disorder can even stabilize self-assembled nanostructures and improve their properties.The aim of the project is to extend our theoretical knowledge beyond traditional“idealized” systems and investigate the combined effects of molecular mass distribution and irregular branched structure (topological diversity) of self-assembling block-copolymers. In particular, we will investigate to which extent such molecular disorder can be exploited to optimize and tune the structure and properties of the nano-aggregates. To this end, we will combine analytical thermodynamic approaches that lead to exact results and numerical simulations.

我们打算探索内在的分子水平无序对嵌段共聚物自组装胶体纳米结构的结构和性能的影响。这种结构被认为在（生物）纳米技术和医学中具有巨大的潜力，例如，作为药物和遗传物质的纳米级载体，因为它们的尺寸、负载能力和货物释放曲线可以通过组成共聚物的适当设计来微调。树枝状支化共聚物是特别感兴趣的，因为大量的端基可以用可靶向配体官能化。这使得人们可以有效地将不同的官能团连接在一个分子上，并利用生物识别机制将药物控制靶向递送到特定的组织或细胞。迄今为止，关于共聚物自组装的实验大多是基于完美的单分散线性嵌段共聚物的理论。新药物的工业生产需要应用稳健的合成方案，该方案必然导致产物的分子量多分散性和结构（拓扑）无序，即，嵌段共聚物。初步研究表明，这并不一定是一个缺点：一定量的分子无序甚至可以稳定自组装纳米结构并改善其性能。该项目的目的是将我们的理论知识扩展到传统的“理想化”系统之外，并研究自组装嵌段共聚物的分子质量分布和不规则支化结构（拓扑多样性）的综合效应。特别是，我们将研究在何种程度上可以利用这种分子无序来优化和调整纳米聚集体的结构和性质。为此，我们将结合联合收割机分析热力学方法，导致精确的结果和数值模拟。