Gu Chad, Coalson Rob D, Jasnow David, Zilman Anton
Department of Physics, University of Toronto , Toronto, Ontario M5S 1A7, Canada.
Department of Chemistry, University of Pittsburgh , Pittsburgh, Pennsylvania 15260, United States.
J Phys Chem B. 2017 Jul 6;121(26):6425-6435. doi: 10.1021/acs.jpcb.7b00868. Epub 2017 Jun 20.
Characterization of the interactions between nanosize ligands and polymeric substrates is important for predictive design of nanomaterials and in biophysical applications. The multivalent nature of the polymer-nanoparticle interaction and the dynamics of multiple internal conformations of the polymer chains makes it difficult to infer microscopic interactions from macroscopic binding assays. Using coarse-grained simulations, we estimate the free energy of binding between a nanoparticle and a surface-grafted polymeric substrate as a function of pertinent parameters such as polymer chain length, nanoparticle size, and microscopic polymer-nanoparticle attraction. We also investigate how the presence of the nanoparticle affects the internal configurations of the polymeric substrate, and estimate the entropic cost of binding. The results have important implications for the understanding of complex macromolecular assemblies.
表征纳米尺寸配体与聚合物基质之间的相互作用对于纳米材料的预测设计和生物物理应用至关重要。聚合物-纳米颗粒相互作用的多价性质以及聚合物链多个内部构象的动力学使得难以从宏观结合测定中推断微观相互作用。通过粗粒度模拟，我们估计了纳米颗粒与表面接枝聚合物基质之间的结合自由能，它是聚合物链长度、纳米颗粒尺寸和微观聚合物-纳米颗粒吸引力等相关参数的函数。我们还研究了纳米颗粒的存在如何影响聚合物基质的内部构型，并估计了结合的熵成本。这些结果对于理解复杂的大分子组装具有重要意义。
