Molecular insight into the hydrogen bonding and micro-segregation of a cryoprotectant molecule.

Molecular insight into the hydrogen bonding and micro-segregation of a cryoprotectant molecule.
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对冷冻保护剂分子的氢键和微观偏析的分子洞察。

DOI:
10.1021/jp3093034
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发表时间:
2012
期刊:
The journal of physical chemistry. B
影响因子:
--
通讯作者:
Towey JJ
Towey JJ
中科院分区:
--
文献类型:
--
作者:
Towey JJ

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甘油-水液体混合物是有趣的氢键系统,在许多化学领域都是必不可少的,从基础分子研究到广泛用于工业和生物医学应用的低温保护溶液。尽管对这些混合物进行了大量研究,但其微观结构的细节仍然不清楚。一个常见的观点是,甘油的作用是减少水的氢键结合能力,这是一个反复出现的假设,尚未通过直接的实验方法进行验证。目前的工作特点的甘油-水混合物的结构,在整个浓度范围内,使用中子衍射实验和计算建模相结合。与以前的预期相反,我们表明,水的氢键结合能力在甘油的存在下并没有减少。我们表明,甘油-水氢键有效地取代水-水氢键,使水保持其完整的氢键结合能力,无论环境中的甘油的量。我们提供了一个定量测量的系统中的所有氢键,并揭示了一个浓度范围内的一个microsegregated的,biphericating液体混合物共存的一个相当大的界面区域。这项工作突出了氢键连接的作用,而不是水的结构化/解构在这些重要的低温保护系统的影响。
Glycerol–water liquid mixtures are intriguing hydrogen-bonded systems and essential in many fields of chemistry, ranging from basic molecular research to widespread use in industrial and biomedical applications as cryoprotective solutions. Despite much research on these mixtures, the details of their microscopic structure are still not understood. One common notion is that glycerol acts to diminish the hydrogen bonding ability of water, a recurring hypothesis that remains untested by direct experimental approaches. The present work characterizes the structure of glycerol–water mixtures, across the concentration range, using a combination of neutron diffraction experiments and computational modeling. Contrary to previous expectations, we show that the hydrogen bonding ability of water is not diminished in the presence of glycerol. We show that glycerol–water hydrogen bonds effectively take the place of water–water hydrogen bonds, allowing water to maintain its full hydrogen bonding capacity regardless of the quantity of glycerol in the environment. We provide a quantitative measurement of all hydrogen bonding in the system and reveal a concentration range where a microsegregated, bipercolating liquid mixture exists in coexistence with a considerable interface region. This work highlights the role of hydrogen bonding connectivity rather than water structuring/destructuring effects in these important cryoprotective systems.
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