Conformational Variations for Surface-Initiated Reversible Deactivation Radical Polymerization: From Flat to Curved Nanoparticle Surfaces

回转半径 聚合物 单体 化学 分子动力学 摩尔质量 聚合 自由基聚合 高分子化学 曲率 化学物理 材料科学 计算化学 几何学 有机化学 数学
作者
Francisco J. Arráez,Paul Van Steenberge,Julian Sobieski,Krzysztof Matyjaszewski,Dagmar D’hooge
出处
期刊:Macromolecules [American Chemical Society]
卷期号:54 (18): 8270-8288 被引量:20
标识
DOI:10.1021/acs.macromol.1c00855
摘要

Although progress in surface-initiated reversible deactivation radical polymerization (SI-RDRP) has already enabled the production of increasingly novel and advanced polymer structures on solid surfaces, fundamental kinetic questions remain regarding the impact of reaction conditions on the molecular properties of synthesized tethered chains. In the current work, we put forward a matrix-based kinetic Monte Carlo (kMC) model, which is based on an implicit SI-RDRP reaction scheme and continuous three-dimensional (3D) representations, capable of following the temporal evolution of the molecular properties of individual free and surface-tethered polymer chains. This is uniquely possible for variable surface curvature (nanoparticle radii from 4.5 to 32 nm; 353 K; monomer: methyl methacrylate), also including the comparison with the limiting case of a flat surface and addressing various (average) RDRP initiator surface coverages. For the tethered chains, we emphasize the prediction of the variation of the molecular height, monomer occupancy, and radius of gyration and also focus on the simulation of the chain length distribution (CLD) to enable a comparison with solution RDRP results. It is shown that confinement effects on the surface lead to the formation of heterogeneous polymer layers with a marked bimodality in the number CLD. This bimodality is, however, wiped out in experimental analysis based on log-molar mass distributions. It is also shown that an increase in the size of the spherical particles and, hence, a decrease in their curvature results in a deterioration of the control over molecular properties, leading to behavior more similar to that of flat surfaces. Average molecular heights and monomer occupancies can vary with a factor of 2. The impact of the targeted chain length is shown to be of lower importance.
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