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首页> 外文期刊>ACS Macro Letters >Structural Evolution of Polylactide Molecular Bottlebrushes: Kinetics Study by Size Exclusion Chromatography, Small Angle Neutron Scattering, and Simulations
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Structural Evolution of Polylactide Molecular Bottlebrushes: Kinetics Study by Size Exclusion Chromatography, Small Angle Neutron Scattering, and Simulations

机译：聚丙交酯分子牙刷的结构演变：通过尺寸排阻色谱，小角度中子散射和模拟进行的动力学研究

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摘要

Structural evolution from poly(lactide) (PLA) macromonomer to resultant PLA molecular bottlebrush during ring opening metathesis polymerization (ROMP) was investigated for the first time by combining size exclusion chromatography (SEC), small-angle neutron scattering (SANS), and coarse-grained molecular dynamics (CG-MD) simulations. Multiple aliquots were collected at various reaction times during ROMP and subsequently analyzed by SEC and SANS. These complementary techniques enable the understanding of systematic changes in conversion, molecular weight and dispersity as well as structural details of PLA molecular bottlebrushes. CG-MD simulation not only predicts the experimental observations, but it also provides further insight into the analysis and interpretation of data obtained in SEC and SANS experiments. We find that PLA molecular bottlebrushes undergo three conformational transitions with increasing conversion (i.e., increasing the backbone length): (1) from an elongated to a globular shape due to longer side chain at low conversion, (2) from a globular to an elongated shape at intermediate conversion caused by excluded volume of PLA side chain, and (3) the saturation of contour length at high conversion due to chain transfer reactions.
机译：结合尺寸排阻色谱（SEC），小角度中子散射（SANS）和粗粒度分析，首次研究了在开环复分解聚合（ROMP）期间从聚丙交酯（PLA）大分子单体向所得PLA分子刷的结构演变。分子动力学（CG-MD）模拟。在ROMP期间的不同反应时间收集了多个等分试样，然后通过SEC和SANS分析。这些互补的技术使您能够了解PLA分子瓶的转化率，分子量和分散度以及结构细节的系统变化。 CG-MD模拟不仅可以预测实验观察结果，还可以进一步分析和解释SEC和SANS实验中获得的数据。我们发现，PLA分子瓶刷随着转化率的增加（即增加主链长度）经历了三个构象转变：（1）由于在低转化率下较长的侧链，从细长形变为球形，（2）从球形形变为细长PLA侧链的排他体积导致中间转化时的形状，以及（3）由于链转移反应，高转化时轮廓长度的饱和。

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