Water-Free Proton Conduction in Hexakis(p-Phosphonatophenyl)benzene Nanochannels
Water-Free Proton Conduction in Hexakis(p-Phosphonatophenyl)benzene Nanochannels
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DOI：
10.1021/jp4035024
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发表时间：
2013-06
影响因子：
3.7
通讯作者：
C. Wehmeyer;M. Schrader;D. Andrienko;D. Sebastiani
中科院分区：
文献类型：
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作者：
C. Wehmeyer;M. Schrader;D. Andrienko;D. Sebastiani
我们阐明了在不同温度（400-600 K）和零湿度条件下膦酸功能化分子（六（对磷酸苯基）苯）自组装堆叠中的质子传导机制。我们采用第一原理分子动力学模拟与大规模力场模拟相结合，形成柱状堆叠中分子的特定排列。这种排列为准一维氢键纳米线留下了空间，质子沿着该纳米线传输。我们观察到膦酸基团的自发自解离，导致质子沿着纳米线位移高达 10 A。我们的模拟表明，氢键网络的动力学存在快速（200 fs）和慢速（3-12 ps）分量，分别对应于氢键的方向波动和持久的长程质子输运。我们的结果支持这样的假设：该化合物在高温下可能发生显着的质子传导...
We elucidate the proton conduction mechanism in self-assembling stacks of phosphonic-acid-functionalized molecules (hexakis(p-phosphonatophenyl)benzene) at different temperatures (400–600 K) and at zero humidity conditions. We employ first-principles molecular dynamics simulations in combination with large-scale force-field simulations, forming a specific arrangement of the molecules in the columnar stacks. This arrangement leaves space for quasi-one-dimensional hydrogen bond nanowires along which protons are transported. We observe spontaneous autodissociation of the phosphonic acid groups, leading to proton displacements of up to 10 A along the nanowires. Our simulations show that there is a fast (200 fs) and a slow (3–12 ps) component in the dynamics of the hydrogen bond network, corresponding to orientation fluctuations of the hydrogen bonds and persistent long-range proton transport, respectively. Our results support the hypothesis that significant proton conduction is possible in this compound at fu...