Predictably Engineering the Viscoelastic Behavior of Dynamic Hydrogels via Correlation with Molecular Parameters.
Predictably Engineering the Viscoelastic Behavior of Dynamic Hydrogels via Correlation with Molecular Parameters.
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DOI：
10.1002/adma.202104460
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发表时间：
2021-12
期刊：
影响因子：
--
通讯作者：
Xia Y
中科院分区：
文献类型：
--
作者：
Lou J;Friedowitz S;Will K;Qin J;Xia Y
合理设计具有理想粘弹性行为的动态水凝胶依赖于对分子参数和宏观性质相关原理的深入理解。为了定量地阐明这些原理，我们设计了一系列通过腙键交联的动态共价水凝胶。我们通过改变有机催化剂的浓度来调节腙键的交换速率，同时保持交联密度不变。这种策略的独立调整交换动力学的交联和交联密度允许明确的分析的粘弹性响应的动态水凝胶作为其网络参数的函数。我们发现，终端弛豫时间的动态水凝胶主要是由两个因素：交换率的交联和有效的交联每聚合物链的数量，是独立的网络结构。此外，一个普遍的相关性之间的终端松弛时间确定应力松弛和通过反应动力学确定的交换率，这可以推广到任何粘弹性水凝胶网络的原则。这种定量的相关性有利于动态水凝胶的发展与可变的所需的粘弹性响应的基础上分子设计。动态共价水凝胶的分子参数独立地变化，以研究它们对水凝胶的粘弹性行为的影响。通用的相关性被确定为定量预测动态水凝胶的粘弹性与不同的网络拓扑结构的基础上的交换速率的交联和每个聚合物链的有效交联的数量。
Rational design of dynamic hydrogels with desirable viscoelastic behaviors relies on an in-depth understanding of the principles correlating molecular parameters and macroscopic properties. To quantitatively elucidate such principles, we designed a series of dynamic covalent hydrogels crosslinked via hydrazone bonds. We tuned the exchange rate of hydrazone bond by varying the concentration of an organic catalyst, while maintaining the crosslinking density unchanged. This strategy of independently tuning exchange dynamics of crosslinks and crosslinking density allowed unambiguous analysis of the viscoelastic response of the dynamic hydrogels as a function of their network parameters. We found that the terminal relaxation time of the dynamic hydrogels is primarily determined by two factors: the exchange rate of crosslinks and the number of effective crosslinks per polymer chain, and is independent of the network architecture. Furthermore, a universal correlation is identified between the terminal relaxation time determined from stress relaxation and the exchange rate determined via reaction kinetics, which can be generalized to any viscoelastic hydrogel networks in principle. This quantitative correlation facilitates the development of dynamic hydrogels with variable desired viscoelastic response based on molecular design. Molecular parameters of dynamic covalent hydrogels are independently varied to investigate their effects on the viscoelastic behavior of hydrogels. Universal correlations are identified to quantitatively predict the viscoelastic properties of dynamic hydrogels with different network topologies based on the exchange rate of crosslinks and the number of effective crosslinks per polymer chain.
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影响因子：
29.4
作者：
Dooling, Lawrence J.;Buck, Maren E.;Tirrell, David A.
通讯作者：
Tirrell, David A.
DOI：
10.1002/adma.201303680
发表时间：
2014-02-12
期刊：
Advanced materials (Deerfield Beach, Fla.)
影响因子：
--
作者：
McKinnon DD;Domaille DW;Cha JN;Anseth KS
通讯作者：
Anseth KS
影响因子：
5.5
作者：
BAXANDALL, LG
通讯作者：
BAXANDALL, LG
影响因子：
5.5
作者：
Rubinstein, M;Semenov, AN
通讯作者：
Semenov, AN
影响因子：
41.2
作者：
Chaudhuri O;Gu L;Klumpers D;Darnell M;Bencherif SA;Weaver JC;Huebsch N;Lee HP;Lippens E;Duda GN;Mooney DJ
通讯作者：
Mooney DJ