Carbon Monoxide Hydrogenation on Ice Surfaces
Carbon Monoxide Hydrogenation on Ice Surfaces
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冰表面一氧化碳氢化
DOI：
10.1002/cphc.201701346
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发表时间：
2018
期刊：
影响因子：
2.9
通讯作者：
Kazuaki Kuwahata Kaoru Ohno
中科院分区：
文献类型：
--
作者：
Miki Takako;Eguchi Masafumi;Akter Shamima;Kochi Takeshi;Kuwahara Keisuke;Kashino Ikuko;Hu Huanhuan;Kabe Isamu;Kawakami Norito;Nanri Akiko;Mizoue Tetsuya;Kazuaki Kuwahata Kaoru Ohno
我们已经进行了密度泛函计算来研究一氧化碳氢化反应（H+CO→HCO），这是重要的星际云。我们发现，在无定形冰上的反应活化能低于在结晶冰上的。在这项研究的过程中，我们证明，它大致可以使用的反应物分子（CO）的激发能的地方的活化能。这种关系也适用于CCSD计算水平和两层水平ONIOM（CCSD：X3LYP）计算的小水团簇。一般来说，由于在许多水分子的情况下估计化学反应的活化能在计算上要求很高，因此这种关系使得人们能够仅根据CO的激发能的知识来确定冰表面上的该反应的活化能。除了量子隧穿效应，我们还讨论了冰表面上的反应速率。我们的估计，在无定形冰的反应速率几乎是在结晶冰的两倍大，定性与日高等人报道的实验证据一致。 [Chem.Phys.Lett.， 2008，456，36.]
We have performed density functional calculations to investigate the carbon monoxide hydrogenation reaction (H+CO→HCO), which is important in interstellar clouds. We found that the activation energy of the reaction on amorphous ice is lower than that on crystalline ice. In the course of this study, we demonstrated that it is roughly possible to use the excitation energy of the reactant molecule (CO) in place of the activation energy. This relationship holds also for small water clusters at the CCSD level of calculation and the two‐layer‐level ONIOM (CCSD : X3LYP) calculation. Generally, since it is computationally demanding to estimate activation energies of chemical reactions in a circumstance of many water molecules, this relationship enables one to determine the activation energy of this reaction on ice surfaces from the knowledge of the excitation energy of CO only. Incorporating quantum‐tunneling effects, we discuss the reaction rate on ice surfaces. Our estimate that the reaction rate on amorphous ice is almost twice as large as that on crystalline ice is qualitatively consistent with the experimental evidence reported by Hidaka et al. [Chem. Phys. Lett., 2008,456, 36.]