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Visualizing the Toughening Mechanism of Nanofiller with 3D X-ray Nano-CT: Stress-Induced Phase Separation of Silica Nanofiller and Silicone Polymer Double Networks
Macromolecules ( IF 5.1 ) Pub Date : 2017-09-08 00:00:00 , DOI: 10.1021/acs.macromol.7b00539
Lixian Song 1, 2 , Zhen Wang 1 , Xiaoliang Tang 1 , Liang Chen 1 , Pinzhang Chen 1 , Qingxi Yuan 3 , Liangbin Li 1
Affiliation  

Adding silica nanofiller in silicone rubber can toughen the matrix 3 orders in terms of fracture energy, which is far larger than most other nanofiller–rubber systems. To unveil the astonishing toughening mechanism, we employ in situ synchrotron radiation X-ray nanocomputed tomography (Nano-CT) technique with high spatial resolution (64 nm) to study the structural evolution of silica nanofiller in silicone rubber matrix at different strains. The imaging results show that silica nanofiller forms three-dimensional connected network, which couples with silicone chain network to construct a double-network structure. Stress-induced phase separation between silica nanofiller and silicone polymer chain networks is observed during tensile deformation. Unexpectedly, though the spatial position and morphology of nanofiller network changes greatly at large strains, the connectivity of nanofiller network shows negligible reduction. This indicates that nanofiller network undergoes destruction and reconstruction simultaneously, during which silica nanofiller serves as reversible high functionality cross-linker. The reversible bonding between silica nanofiller and silicone rubber or between nanofiller particles can dissipate mechanical energy effectively, which may account for the 3 orders enhancement of toughness.

中文翻译:

用3D X射线纳米CT可视化纳米填料的增韧机理:二氧化硅纳米填料和有机硅聚合物双网络的应力诱导相分离

在硅橡胶中添加二氧化硅纳米填料可以使基体的断裂能提高3个数量级,远大于大多数其他纳米填料-橡胶系统。为了揭示惊人的增韧机理,我们采用了具有高空间分辨率(64 nm)的原位同步辐射X射线纳米计算机断层扫描(Nano-CT)技术来研究不同应变下硅橡胶基质中二氧化硅纳米填料的结构演变。成像结果表明,二氧化硅纳米填料形成三维连接网络,与硅酮链网络耦合构成双网状结构。在拉伸变形过程中观察到了二氧化硅纳米填料与有机硅聚合物链网络之间的应力诱导相分离。不料,尽管纳米填料网络的空间位置和形态在大应变下会发生很大变化,但纳米填料网络的连通性却可以忽略不计。这表明纳米填料网络同时遭到破坏和重建,其间二氧化硅纳米填料充当可逆的高功能交联剂。二氧化硅纳米填料与硅橡胶之间或纳米填料颗粒之间的可逆键合可以有效地耗散机械能,这可能是韧性提高了三个数量级的原因。
更新日期:2017-09-08
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