脱水金属配位聚合物网络中结合水与机械应力松弛的定量相关性,Chemistry of Materials

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脱水金属配位聚合物网络中结合水与机械应力松弛的定量相关性
Chemistry of Materials ( IF 7.2 ) Pub Date : 2022-11-30 , DOI: 10.1021/acs.chemmater.2c01795
Sungjin Kim ₁ , Myungwoon Lee ₂ , Mei Hong ₂ , Niels Holten-Andersen ₁

Affiliation

动态金属配位交联在许多生物和人造金属聚合物网络中通过脱水凝固的不同阶段中的部署赋予智能和卓越的物理化学性质。尽管如此，缺少描述金属配位键从水合状态转变为脱水状态的动态行为在多大程度上的定量模型。在之前的工作中，我们已经表明局部水结合有助于金属配位键在整体网络脱水过程中保持其动态特性，从而为深入脱水固态的网络提供机械阻尼特性。使用受贻贝启发的水凝胶和化学调节的金属配位交联部分，在这里，我们揭示了脱水网络的宏观弛豫时间与金属配位交联键结合的微观水量之间的直接比例关系。脱水金属坐标网络力学和金属坐标交联动力学之间的这种定量关系可以帮助我们更好地理解和模拟通过时空控制的承重材料脱水在自然界中广泛展示的可持续凝固过程。

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Quantitative Correlation between Bound Water and Mechanical Stress Relaxation in Dehydrated Metal-Coordinate Polymer Networks

Dynamic metal-coordinate cross-links impart smart and superior physicochemical properties in their deployments in many biological and artificial metallopolymer networks in various stages of solidification via dehydration. Nonetheless, a quantitative model that describes to what extent the dynamic behaviors of metal-coordinate bond transition from the hydrated to the dehydrated state is missing. In previous work, we have shown that local water binding helps metal-coordinate bonds to maintain their dynamic properties during bulk network dehydration, thereby offering mechanical damping properties to the network deep into the dehydrated solid state. Using mussel-inspired hydrogels with chemically tuned fractions of metal-coordinate cross-links, here, we reveal the direct scaling relationship between the macroscopic relaxation time of the dehydrated network and the amount of microscopic water bound by metal-coordinate cross-links. This quantitative relationship between dehydrated metal-coordinate network mechanics and metal-coordinate cross-link dynamics may help us better understand and emulate the sustainable process of solidification via spatiotemporally controlled dehydration of load-bearing materials on wide display in nature.

更新日期：2022-11-30

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