Katsukura Hirotaka, Miyata Tomohiro, Shirai Manabu, Matsumoto Hiroaki, Mizoguchi Teruyasu
Institute of Industrial Science, The University of Tokyo, 4-6-1 Komaba, Meguro, Tokyo, 153-8505, Japan.
Hitachi High-Technologies Corporation, 24-14, Nishi-shimbashi 1-chome, Minato-ku, Tokyo, 105-8717, Japan.
Sci Rep. 2017 Dec 12;7(1):16434. doi: 10.1038/s41598-017-16423-0.
Reactions in gaseous phases and at gas/solid interfaces are widely used in industry. Understanding of the reaction mechanism, namely where, when, and how these gaseous reactions proceed, is crucial for the development of further efficient reaction systems. To achieve such an understanding, it is indispensable to grasp the dynamic behavior of the gaseous molecules at the active site of the chemical reaction. However, estimation of the dynamic behavior of gaseous molecules in specific nanometer-scale regions is always accompanied by great difficulties. Here, we propose a method for the identification of the dynamic behavior of gaseous molecules using an electron spectroscopy observed with a transmission electron microscope in combination with theoretical calculations. We found that our method can successfully identify the dynamic behavior of some gaseous molecules, such as O and CH, and the sensitivity of the method is affected by the rigidity of the molecule. The method has potential to measure the local temperature of gaseous molecules as well. The knowledge obtained from this technique is fundamental for further high resolution studies of gaseous reactions using electron microscopy.
气相反应以及气/固界面反应在工业中有着广泛应用。理解反应机理，即这些气相反应在何处、何时以及如何进行，对于进一步开发高效反应系统至关重要。为了实现这种理解，掌握化学反应活性位点处气态分子的动态行为是必不可少的。然而，估计特定纳米尺度区域内气态分子的动态行为总是伴随着巨大困难。在此，我们提出一种利用透射电子显微镜观察的电子能谱结合理论计算来识别气态分子动态行为的方法。我们发现我们的方法能够成功识别一些气态分子的动态行为，如O和CH，并且该方法的灵敏度受分子刚性的影响。该方法还有测量气态分子局部温度的潜力。从这项技术中获得的知识对于利用电子显微镜对气相反应进行进一步的高分辨率研究至关重要。
