论文标题

使用热敏宿主“中凝胶”控制玻璃形成胶体悬浮液的体积分数

Controlling the volume fraction of glass-forming colloidal suspensions using thermosensitive host `mesogels'

论文作者

Behra, J. S., Thiriez, A., Truzzolillo, D., Ramos, L., Cipelletti, L.

论文摘要

控制胶体悬浮液的玻璃转变的关键参数为$φ$,是颗粒所占据的样品体积的比例。不幸的是,不可能通过改变外部参数,\ textit {eftextit {eftextiT {ef。}温度$ t $与分子玻璃板一样,除非一个人使用热敏感的胶体颗粒,例如流行的poly(N-异丙基酰基酰胺)(PNIPAM)(PNIPAM)微凝胶。然而,这些缺点,包括高变形性,渗透性解渗透和互穿,这使它们用作研究胶体玻璃转变的模型系统的使用复杂化。在这里,我们提出了一个新系统,该系统由不可构造的球形二氧化硅纳米颗粒的胶体悬浮液组成,其中PNIPAM水凝胶球体约为$100-200μm$ $。这些非胶体“中凝结盘”允许控制二氧化硅纳米颗粒可用的样品体积,因此由于$ t $诱导的中凝胶体积的变化,因此可以控制其$φ$。使用光学显微镜,我们首先表明中凝胶在悬挂在Ludox悬浮液中时保留了$ T $改变尺寸的能力,与水中类似。然后,我们证明它们的大小独立于样品热历史记录,因此可以建立$ t $和$φ$之间的明确,可逆的关系。最后,我们使用空间分辨的动态光散射来证明,在不同的$ t $中,我们的系统在整个玻璃过渡及其他方面表现出广泛的动力学行为,与一系列不同$φ$的一系列独特的硅纳米粒子悬浮液所展示的动态行为。

The key parameter controlling the glass transition of colloidal suspensions is $φ$, the fraction of the sample volume occupied by the particles. Unfortunately, changing $φ$ by varying an external parameter, \textit{e.g.} temperature $T$ as in molecular glass formers, is not possible, unless one uses thermosensitive colloidal particles, like the popular poly(N-isopropylacrylamide) (PNiPAM) microgels. These however have several drawbacks, including high deformability, osmotic deswelling and interpenetration, which complicate their use as a model system to study the colloidal glass transition. Here, we propose a new system consisting of a colloidal suspension of non-deformable spherical silica nanoparticles, in which PNiPAM hydrogel spheres of ~$100-200 μm$ size are suspended. These non-colloidal `mesogels' allow for controlling the sample volume effectively available to the silica nanoparticles and hence their $φ$, thanks to the $T$-induced change in mesogels volume. Using optical microscopy, we first show that the mesogels retain their ability to change size with $T$ when suspended in Ludox suspensions, similarly as in water. We then show that their size is independent of the sample thermal history, such that a well-defined, reversible relationship between $T$ and $φ$ may be established. Finally, we use space-resolved dynamic light scattering to demonstrate that, upon varying $T$, our system exhibits a broad range of dynamical behaviors across the glass transition and beyond, comparable with those exhibited by a series of distinct silica nanoparticle suspensions of various $φ$.

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