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铜离子在Cu-SSZ-13中的迁移率决定了用氨选择性催化还原NO的反应活性。

Mobility of Cu Ions in Cu-SSZ-13 Determines the Reactivity of Selective Catalytic Reduction of NO with NH.

作者信息

Lee Hwangho, Song Inhak, Jeon Se Won, Kim Do Heui

机构信息

School of Chemical and Biological Engineering, Institute of Chemical Processes, Seoul National University, Seoul 08826, Republic of Korea.

出版信息

J Phys Chem Lett. 2021 Apr 1;12(12):3210-3216. doi: 10.1021/acs.jpclett.1c00181. Epub 2021 Mar 24.

Abstract

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.

摘要

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。

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