Mussel-inspired histidine-based transient network metal coordination hydrogels.
Mussel-inspired histidine-based transient network metal coordination hydrogels.
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DOI：
10.1021/ma301791n
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发表时间：
2013-02-12
期刊：
影响因子：
5.5
通讯作者：
Messersmith PB
中科院分区：
文献类型：
--
作者：
Fullenkamp DE;He L;Barrett DG;Burghardt WR;Messersmith PB
以组氨酸修饰的星星型聚乙二醇（PEG）聚合物为材料，采用常规流变学方法研究了通过组氨酸-二价阳离子配位键交联的瞬态网络水凝胶。这些材料的灵感来自于贻贝，人们认为贻贝使用组氨酸-金属配位键来赋予贻贝深渊线自我修复的特性。水凝胶的粘弹性机械性能进行了研究，作为金属，pH值，浓度和离子强度的函数。通过稀溶液电位滴定法测定的单官能组氨酸改性的甲氧基-PEG的平衡金属结合常数，并被发现是与以前研究的小分子类似物的结合常数一致。pH依赖的形态曲线，然后使用电位滴定法确定的平衡常数计算，提供洞察到pH依赖的组氨酸-金属离子配位和指导金属配位水凝胶的设计。凝胶弛豫动力学被认为是不相关的平衡常数测量，但预期的配位键解离速率常数。
Transient network hydrogels cross-linked through histidine-divalent cation coordination bonds were studied by conventional rheologic methods using histidine-modified star poly(ethylene glycol) (PEG) polymers. These materials were inspired by the mussel, which is thought to use histidine-metal coordination bonds to impart self-healing properties in the mussel byssal thread. Hydrogel viscoelastic mechanical properties were studied as a function of metal, pH, concentration, and ionic strength. The equilibrium metal-binding constants were determined by dilute solution potentiometric titration of monofunctional histidine-modified methoxy-PEG and were found to be consistent with binding constants of small molecule analogs previously studied. pH-dependent speciation curves were then calculated using the equilibrium constants determined by potentiometric titration, providing insight into the pH dependence of histidine-metal ion coordination and guiding the design of metal coordination hydrogels. Gel relaxation dynamics were found to be uncorrelated with the equilibrium constants measured, but were correlated to the expected coordination bond dissociation rate constants.
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