Kishimoto Fuminao, Yoshioka Tatsushi, Ishibashi Ryo, Yamada Hiroki, Muraoka Koki, Taniguchi Hiroki, Wakihara Toru, Takanabe Kazuhiro
Department of Chemical System Engineering, School of Engineering, The University of Tokyo, 7-3-1 Hongo, Bunkyo-ku, Tokyo 113-8656, Japan.
Japan Synchrotron Radiation Research Institute, SPring-8, 1-1-1 Kouto, Sayo-cho, Sayo-gun, Hyogo 679-5198, Japan.
Sci Adv. 2023 Aug 18;9(33):eadi1744. doi: 10.1126/sciadv.adi1744.
Microwave (MW)-driven catalytic systems are attracting attention not only as an aggressive electrification strategy of the chemical industry but also as creating a unique catalytic reaction field that conventional equilibrium heating cannot achieve. This study unlocked direct and selective heating of single alkali metal cations in the pores of aluminosilicate zeolites under MW. Selectively heated Cs cations in FAU zeolite exhibited selective CH combustion performance, that is, CO generation at the heated Cs cations selectively occurred while side reactions in the low-temperature gas phase were suppressed. The Cs-O pair distribution function revealed by synchrotron-based in situ x-ray total scattering gave us direct evidence of peculiar displacement induced by MW, which was consistent with the results of molecular dynamics simulation mimicking MW heating. The concept of selective monoatomic heating by MW is expected to open a next stage in "microwave catalysis" science by providing physicochemical insights into "microwave effects."
微波（MW）驱动的催化系统不仅作为化学工业激进的电气化策略而备受关注，而且还因其创造了传统平衡加热无法实现的独特催化反应场而受到关注。本研究实现了在微波作用下对铝硅酸盐沸石孔道中单一碱金属阳离子的直接和选择性加热。在FAU沸石中被选择性加热的铯阳离子表现出选择性CH燃烧性能，即在加热的铯阳离子处选择性地产生CO，同时抑制了低温气相中的副反应。基于同步加速器的原位X射线全散射揭示的Cs-O对分布函数为微波引起的特殊位移提供了直接证据，这与模拟微波加热的分子动力学模拟结果一致。微波选择性单原子加热的概念有望通过提供对“微波效应”的物理化学见解，开启“微波催化”科学的下一个阶段。
