Unraveling bilayer interfacial features and their effects in polar polymer nanocomposites

Xinhui Li, Shan He, Yanda Jiang, Jian Wang, Yi Yu, Xiaofei Liu, Feng Zhu, Yimei Xie, Youyong Li, Cheng Ma, Zhonghui Shen, Baowen Li, Yang Shen, Xin Zhang (), Shujun Zhang () and Ce-Wen Nan ()
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Xinhui Li: Wuhan University of Technology
Shan He: Tsinghua University
Yanda Jiang: Wuhan University of Technology
Jian Wang: Wuhan University of Technology
Yi Yu: Soochow University
Xiaofei Liu: Wuhan University of Technology
Feng Zhu: University of Science and Technology of China
Yimei Xie: Wuhan University of Technology
Youyong Li: Soochow University
Cheng Ma: University of Science and Technology of China
Zhonghui Shen: Wuhan University of Technology
Baowen Li: Wuhan University of Technology
Yang Shen: Tsinghua University
Xin Zhang: Wuhan University of Technology
Shujun Zhang: University of Wollongong
Ce-Wen Nan: Tsinghua University

Nature Communications, 2023, vol. 14, issue 1, 1-10

Abstract: Abstract Polymer nanocomposites with nanoparticles dispersed in polymer matrices have attracted extensive attention due to their significantly improved overall performance, in which the nanoparticle-polymer interface plays a key role. Understanding the structures and properties of the interfacial region, however, remains a major challenge for polymer nanocomposites. Here, we directly observe the presence of two interfacial polymer layers around a nanoparticle in polar polymers, i.e., an inner bound polar layer (~10 nm thick) with aligned dipoles and an outer polar layer (over 100 nm thick) with randomly orientated dipoles. Our results reveal that the impacts of the local nanoparticle surface potential and interparticle distance on molecular dipoles induce interfacial polymer layers with different polar molecular conformations from the bulk polymer. The bilayer interfacial features lead to an exceptional enhancement in polarity-related properties of polymer nanocomposites at ultralow nanoparticle loadings. By maximizing the contribution of inner bound polar layer via a nanolamination design, we achieve an ultrahigh dielectric energy storage density of 86 J/cm3, far superior to state-of-the-art polymers and nanocomposites.

Date: 2023
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DOI: 10.1038/s41467-023-41479-0

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