Delayed Mechanical Response to Chemical Kinetics in Self-Oscillating Hydrogels Driven by the Belousov-Zhabotinsky Reaction.
Delayed Mechanical Response to Chemical Kinetics in Self-Oscillating Hydrogels Driven by the Belousov-Zhabotinsky Reaction.
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DOI：
10.1021/acs.macromol.1c00402
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发表时间：
2021-07-13
期刊：
影响因子：
5.5
通讯作者：
Hayashi Y
中科院分区：
文献类型：
--
作者：
Geher-Herczegh T;Wang Z;Masuda T;Yoshida R;Vasudevan N;Hayashi Y
我们的实验表明，化学和机械的自振荡在Belousov-Zhabotinsky水凝胶本质上是异步的，也就是说，有一个可检测到的延迟在化学氧化还原状态的变化后的溶胀-去溶胀响应。这种现象在许多以前的实验研究中都可以观察到，并且可能对材料在未来应用中的功能和响应时间产生深远的影响;然而，到目前为止，它还没有被系统地量化或报告。在这里，我们提供了一个全面的定性和定量描述的化学机械延迟，我们建议解释它作为一个结果的聚合物材料的缓慢的非平衡溶胀-去溶胀动力学。具体地，标准水凝胶块足够大，使得运输过程（例如，对流迁移和水扩散）不能在整个凝胶块中瞬时发生，这与先前的理论考虑相反。因此，聚合物对化学变化的体积响应可以由特征响应时间控制，这导致机械振荡延迟的出现。这是由我们的理论计算支持的。
We show experimentally that chemical and mechanical self-oscillations in Belousov–Zhabotinsky hydrogels are inherently asynchronous, that is, there is a detectable delay in swelling–deswelling response after a change in the chemical redox state. This phenomenon is observable in many previous experimental studies and potentially has far-reaching implications for the functionality and response time of the material in future applications; however, so far, it has not been quantified or reported systematically. Here, we provide a comprehensive qualitative and quantitative description of the chemical-to-mechanical delay, and we propose to explain it as a consequence of the slow nonequilibrium swelling–deswelling dynamics of the polymer material. Specifically, standard hydrogel pieces are large enough that transport processes, for example, counterion migration and water diffusion, cannot occur instantaneously throughout the entire gel piece, as opposed to previous theoretical considerations. As a result, the volume response of the polymer to a chemical change may be governed by a characteristic response time, which leads to the emergence of delay in mechanical oscillation. This is supported by our theoretical calculations.
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