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单链纳米颗粒熔体弛豫过程中涉及的动态过程和机制

Dynamic Processes and Mechanisms Involved in Relaxations of Single-Chain Nano-Particle Melts.

作者信息

Maiz Jon, Verde-Sesto Ester, Asenjo-Sanz Isabel, Malo de Molina Paula, Frick Bernhard, Pomposo José A, Arbe Arantxa, Colmenero Juan

机构信息

Centro de Física de Materiales (CFM) (CSIC-UPV/EHU)-Materials Physics Center (MPC), Paseo Manuel de Lardizábal 5, 20018 Donostia-San Sebastián, Spain.

IKERBASQUE-Basque Foundation for Science, Plaza Euskadi 5, 48009 Bilbao, Spain.

出版信息

Polymers (Basel). 2021 Jul 14;13(14):2316. doi: 10.3390/polym13142316.

DOI:10.3390/polym13142316
PMID:34301072
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC8309259/
Abstract

We present a combined study by quasielastic neutron scattering (QENS), dielectric and mechanical spectroscopy, calorimetry and wide-angle X-ray diffraction on single-chain nano-particles (SCNPs), using the corresponding linear precursor chains as reference, to elucidate the impact of internal bonds involving bulky cross-links on the properties of polymer melts. Internal cross-links do not appreciably alter local properties and fast dynamics. This is the case of the average inter-molecular distances, the β-relaxation and the extent of the atomic displacements at timescales faster than some picoseconds. Contrarily, the α-relaxation is slowed down with respect to the linear precursor, as detected by DSC, dielectric spectroscopy and QENS. QENS has also resolved broader response functions and stronger deviations from Gaussian behavior in the SCNPs melt, hinting at additional heterogeneities. The rheological properties are also clearly affected by internal cross-links. We discuss these results together with those previously reported on the deuterated counterpart samples and on SCNPs obtained through a different synthesis route to discern the effect of the nature of the cross-links on the modification of the diverse properties of the melts.

摘要

我们通过准弹性中子散射（QENS）、介电和机械光谱、量热法以及广角X射线衍射对单链纳米颗粒（SCNP）进行了一项联合研究，以相应的线性前体链作为参考，来阐明涉及庞大交联键的内部键对聚合物熔体性质的影响。内部交联不会明显改变局部性质和快速动力学。平均分子间距离、β弛豫以及在快于某些皮秒的时间尺度下的原子位移程度就是这种情况。相反，如通过差示扫描量热法（DSC）、介电光谱和QENS所检测到的，相对于线性前体，α弛豫减慢。QENS还解析出SCNP熔体中更宽的响应函数以及与高斯行为更强的偏差，这暗示了额外的不均匀性。流变性质也明显受到内部交联的影响。我们将这些结果与之前关于氘代对应样品以及通过不同合成路线获得的SCNP的报道结果一起进行讨论，以辨别交联键的性质对熔体各种性质改性的影响。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/bf972e88e292/polymers-13-02316-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/9d003de42cac/polymers-13-02316-sch001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/77c4206ab58e/polymers-13-02316-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/5270aa8a662d/polymers-13-02316-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/8e3288913cbb/polymers-13-02316-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/cf660df4165f/polymers-13-02316-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/573d278b7331/polymers-13-02316-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/a424ae343016/polymers-13-02316-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/4705206ab5ab/polymers-13-02316-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/bf972e88e292/polymers-13-02316-g008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/9d003de42cac/polymers-13-02316-sch001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/77c4206ab58e/polymers-13-02316-g001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/5270aa8a662d/polymers-13-02316-g002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/8e3288913cbb/polymers-13-02316-g003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/cf660df4165f/polymers-13-02316-g004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/573d278b7331/polymers-13-02316-g005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/a424ae343016/polymers-13-02316-g006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/4705206ab5ab/polymers-13-02316-g007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/182c/8309259/bf972e88e292/polymers-13-02316-g008.jpg

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Facile Access to Completely Deuterated Single-Chain Nanoparticles Enabled by Intramolecular Azide Photodecomposition.通过分子内叠氮化物光解实现完全氘代单链纳米颗粒的简易获取。
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