Lee Hwangho, Song Inhak, Jeon Se Won, Kim Do Heui
School of Chemical and Biological Engineering, Institute of Chemical Processes, Seoul National University, Seoul 08826, Republic of Korea.
J Phys Chem Lett. 2021 Apr 1;12(12):3210-3216. doi: 10.1021/acs.jpclett.1c00181. Epub 2021 Mar 24.
Selective catalytic reduction of NO with NH (NH-SCR) in Cu-SSZ-13 has been proposed to have a unique homogeneous-like mechanism governed by the spatial proximity of mobile Cu ions. Among factors that determine the proximity, the effect of ion density on the SCR reaction is well established; however, it has not been verified how the different mobility of the Cu ion influences the SCR reaction. Herein, we try to reveal the mobility-dependent SCR reaction by controlling the Cu species with different ion mobilities in Cu-SSZ-13. Since the reaction kinetics is governed by the diffusion of Cu ions, the Cu ion mobility determines the reactivity of the Cu-SSZ-13. In terms of this correlation, enhanced ion mobility leads to improved NH-SCR activity. These findings help understand the behavior of Cu ions in Cu-SSZ-13 under a catalytic reaction and provide insights to design rational catalysts by tuning the ion mobility.
在Cu-SSZ-13中,用NH₃选择性催化还原NO(NH₃-SCR)被认为具有一种独特的类似均相的机制,该机制受移动Cu离子的空间 proximity 支配。在决定 proximity 的因素中,离子密度对SCR反应的影响已得到充分证实;然而,尚未证实Cu离子的不同迁移率如何影响SCR反应。在此,我们试图通过控制Cu-SSZ-13中具有不同离子迁移率的Cu物种来揭示迁移率依赖的SCR反应。由于反应动力学受Cu离子扩散支配,Cu离子迁移率决定了Cu-SSZ-13的反应活性。就这种相关性而言,增强的离子迁移率导致NH₃-SCR活性提高。这些发现有助于理解催化反应条件下Cu-SSZ-13中Cu离子的行为,并为通过调节离子迁移率设计合理的催化剂提供见解。