Control over Aspect Ratio and Polymer Spatial Distribution of 2D Platelets via Living Crystallization-Driven Self-Assembly

IF 5.1 1区化学 Q1 POLYMER SCIENCE Macromolecules Pub Date : 2024-11-29 DOI:10.1021/acs.macromol.4c02496

Tianlai Xia, Laihui Xiao, Kaiwen Sun, Julia Y. Rho, Yujie Xie, Sam J. Parkinson, Leire Sangroniz, Jian Zhang, Jiaping Lin, Alejandro J. Müller, Liang Gao, Andrew P. Dove, Rachel K. O’Reilly

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Abstract

The aspect ratios of nano- and micrometer-sized features in nature have evolved to enable specific characteristics that are finely tuned for optimizing strength, surface area, optics, and heat dissipation. Despite the importance of aspect ratios, precise control over the aspect ratios of anisotropic polymeric nanoparticles is challenging to achieve and the formation mechanisms by which they occur are not fully understood. In this study, using the crystallization-driven self-assembly (CDSA) process, we achieved two-dimensional (2D) platelets with precisely controlled aspect ratios through the rational compositional adjustment of various polycaprolactone (PCL)-based homopolymers (HP) and block copolymers (BCP). These polymer compositions exhibit distinct polymer crystallization rates, which allow for highly controlled aspect ratios and polymer spatial distribution in 2D platelets. Brownian dynamics (BD) simulations provided an in-depth understanding of the formation of 2D platelets. The BD simulations help us further confirm the nature of living epitaxial growth, simulate the structural order of polymer chains during the CDSA process, and demonstrate the influence of PCL length on the aspect ratio. Our work opens up new possibilities for a nuanced understanding of the interplay between polymer composition, crystallization rate, and morphology, providing a method for the controlled synthesis of 2D nanostructures.

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来源期刊

Macromolecules 工程技术-高分子科学

CiteScore

9.30

自引率

16.40%

发文量

942

审稿时长

2 months

期刊介绍： Macromolecules publishes original, fundamental, and impactful research on all aspects of polymer science. Topics of interest include synthesis (e.g., controlled polymerizations, polymerization catalysis, post polymerization modification, new monomer structures and polymer architectures, and polymerization mechanisms/kinetics analysis); phase behavior, thermodynamics, dynamic, and ordering/disordering phenomena (e.g., self-assembly, gelation, crystallization, solution/melt/solid-state characteristics); structure and properties (e.g., mechanical and rheological properties, surface/interfacial characteristics, electronic and transport properties); new state of the art characterization (e.g., spectroscopy, scattering, microscopy, rheology), simulation (e.g., Monte Carlo, molecular dynamics, multi-scale/coarse-grained modeling), and theoretical methods. Renewable/sustainable polymers, polymer networks, responsive polymers, electro-, magneto- and opto-active macromolecules, inorganic polymers, charge-transporting polymers (ion-containing, semiconducting, and conducting), nanostructured polymers, and polymer composites are also of interest. Typical papers published in Macromolecules showcase important and innovative concepts, experimental methods/observations, and theoretical/computational approaches that demonstrate a fundamental advance in the understanding of polymers.