Thermodynamic Analysis of the Selectivity Enhancement Obtained by Using Smart Hydrogels That Are Zwitterionic When Detecting Glucose With Boronic Acid Moieties.
Thermodynamic Analysis of the Selectivity Enhancement Obtained by Using Smart Hydrogels That Are Zwitterionic When Detecting Glucose With Boronic Acid Moieties.
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DOI：
10.1016/j.snb.2011.09.079
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发表时间：
2011-12-15
影响因子：
8.4
通讯作者：
Magda, J.
中科院分区：
文献类型：
--
作者：
Horkay, F.;Cho, S. H.;Tathireddy, P.;Rieth, L.;Solzbacher, F.;Magda, J.
由于硼酸部分可逆地结合到糖分子上并且具有低细胞毒性，因此含硼酸的水凝胶被用于开发中的各种可植入葡萄糖传感器，包括基于光学、荧光和溶胀压力测量的传感器。然而，一些葡萄糖选择性增强的方法通常是必要的，因为分离的硼酸分子与葡萄糖的结合常数比它们与果糖（人体中第二丰富的糖）的结合常数小大约40倍。在许多情况下，葡萄糖选择性增强是通过将悬垂叔胺纳入到水凝胶网络中，从而产生在生理pH下为两性离子的水凝胶来获得的。然而，叔胺的掺入赋予选择性增强的机制知之甚少。为了阐明这一机制，我们使用的渗透去溶胀技术比较葡萄糖和果糖与含有硼酸部分的两性离子智能水凝胶的热力学相互作用。我们还研究了当它与葡萄糖或果糖结合时，使用小角中子散射技术发生的水凝胶结构的变化。
Because the boronic acid moiety reversibly binds to sugar molecules and has low cytotoxicity, boronic acid-containing hydrogels are being used in a variety of implantable glucose sensors under development, including sensors based on optical, fluorescence, and swelling pressure measurements. However, some method of glucose selectivity enhancement is often necessary, because isolated boronic acid molecules have a binding constant with glucose that is some forty times smaller than their binding constant with fructose, the second most abundant sugar in the human body. In many cases, glucose selectivity enhancement is obtained by incorporating pendant tertiary amines into the hydrogel network, thereby giving rise to a hydrogel that is zwitterionic at physiological pH. However, the mechanism by which incorporation of tertiary amines confers selectivity enhancement is poorly understood. In order to clarify this mechanism, we use the osmotic deswelling technique to compare the thermodynamic interactions of glucose and fructose with a zwitterionic smart hydrogel containing boronic acid moieties. We also investigate the change in the structure of the hydrogel that occurs when it binds to glucose or to fructose using the technique of small angle neutron scattering.
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