Leveraging the Polymer Glass Transition to Access Thermally Switchable Shear Jamming Suspensions.
Leveraging the Polymer Glass Transition to Access Thermally Switchable Shear Jamming Suspensions.
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DOI：
10.1021/acscentsci.2c01338
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发表时间：
2023-04-26
影响因子：
18.2
通讯作者：
de Pablo, Juan J.
中科院分区：
文献类型：
--
作者：
Chen, Chuqiao;van der Naald, Michael;Singh, Abhinendra;Dolinski, Neil D.;Jackson, Grayson L.;Jaeger, Heinrich M.;Rowan, Stuart J.;de Pablo, Juan J.
聚合物纳米和微粒悬浮液是一种令人着迷的应力响应材料系统，根据它们的组成，它们可以在剪切作用下表现出多种流动特性，例如急剧变薄、变厚，甚至堵塞（由剪切驱动的可逆凝固）。然而，迄今为止的研究几乎全部集中在无响应颗粒上，这使得无法对流动特性进行原位调整。聚合物材料具有丰富的相变，可以通过其化学结构直接调节，这使得研究人员能够设计出能够对目标外部刺激做出反应的多功能自适应材料。本文报道了（容易制备的）微米大小的聚合物颗粒的悬浮液，其玻璃化转变温度（Tg）可用于热控制其非牛顿流变性。在Tg附近，潜在的机械刚度和颗粒间摩擦发生了显著变化。利用这些特性，研究表明，与传统体系相比，当悬浮液通过颗粒的Tg转变时，剪切增厚发生了戏剧性的非单调变化。这种简单的策略可以通过改变相对于Tg的温度来开启（或关闭）系统剪切堵塞的能力，并通过聚合物化学为其他类型的刺激响应干扰系统奠定基础。由聚合物颗粒组成的悬浮液可以经历玻璃化转变，可以通过改变温度来开启（或关闭）系统剪切堵塞的能力。
Suspensions of polymeric nano- and microparticles are fascinating stress-responsive material systems that, depending on their composition, can display a diverse range of flow properties under shear, such as drastic thinning, thickening, and even jamming (reversible solidification driven by shear). However, investigations to date have almost exclusively focused on nonresponsive particles, which do not allow in situ tuning of the flow properties. Polymeric materials possess rich phase transitions that can be directly tuned by their chemical structures, which has enabled researchers to engineer versatile adaptive materials that can respond to targeted external stimuli. Reported herein are suspensions of (readily prepared) micrometer-sized polymeric particles with accessible glass transition temperatures (Tg) designed to thermally control their non-Newtonian rheology. The underlying mechanical stiffness and interparticle friction between particles change dramatically near Tg. Capitalizing on these properties, it is shown that, in contrast to conventional systems, a dramatic and nonmonotonic change in shear thickening occurs as the suspensions transition through the particles’ Tg. This straightforward strategy enables the in situ turning on (or off) of the system’s ability to shear jam by varying the temperature relative to Tg and lays the groundwork for other types of stimuli-responsive jamming systems through polymer chemistry. Suspensions consisting of polymer particles that can undergo glass transition are designed to enable the in situ turning on (or off) of the system’s ability to shear jam by varying the temperature.
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