Isotope effect of proton and deuteron adsorption site on zeolite-templated carbon using path integral molecular dynamics
Isotope effect of proton and deuteron adsorption site on zeolite-templated carbon using path integral molecular dynamics
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DOI：
10.1007/s00214-011-1031-8
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发表时间：
2011-09
影响因子：
1.7
通讯作者：
Kimichi Suzuki;M. Tachikawa;H. Ogawa;S. Ittisanronnachai;H. Nishihara;T. Kyotani;U. Nagashima
中科院分区：
文献类型：
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作者：
Kimichi Suzuki;M. Tachikawa;H. Ogawa;S. Ittisanronnachai;H. Nishihara;T. Kyotani;U. Nagashima
为了分析质子/氘核（H/D）同位素对沸石模板碳（ZTC）稳定吸附位点的影响，我们在300 K的半经验PM3电位下进行了路径积分分子动力学模拟，包括热效应和核量子效应。在这里，对于额外的质子（H*）和氘核（D*）的吸附位置，我们选择了不同的5个碳原子，从边缘到底部分别标记为α-、β1-、β2-、γ-和δ-碳原子作为buckybowl内部（c36h12和C36D12）。D*在所有碳原子上都有稳定的吸附位点，而H*在δ-碳原子上没有稳定的吸附位点，只在α-、β1-、β2-和γ-碳原子上有稳定的吸附位点。由于H*的零点能大于D*的零点能，因此在300 K时H*可以很容易地越过氢从δ-碳向β -碳转移的势垒高度。
To analyze the proton/deuteron (H/D) isotope effect on the stable adsorption sites on zeolite-templated carbon (ZTC), we have performed path integral molecular dynamics simulations including thermal and nuclear quantum effects with the semi-empirical PM3 potential at 300 K. Here, for the adsorption sites of additional proton (H*) and deuteron (D*), we chose different five carbon atoms labeled as α-, β1-, β2-, γ-, and δ-carbons from edge to bottom for inside of buckybowl (C36H12and C36D12). The stable adsorption sites of D* are observed on all carbon atoms, while those of H* are not observed on δ-carbon atom, but only on α-, β1-, β2-, and γ-carbon atoms. This result is explained by the fact that H* can easily go over the barrier height for hydrogen transferring from δ- to β2-carbons at 300 K, since the zero-point energy of H* is greater than that of D*.