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通过对时间分辨客体分布进行超分辨率显微成像,探索沸石中表面屏障的晶间和晶内多样性对质量传输的影响。

Exploring the Influence of Inter- and Intra-crystal Diversity of Surface Barriers in Zeolites on Mass Transport by Using Super-Resolution Microimaging of Time-Resolved Guest Profiles.

作者信息

Peng Shichao, Xie Yiwei, Wang Linying, Liu Wenjuan, Li Hua, Xu Zhaochao, Ye Mao, Liu Zhongmin

机构信息

National Engineering Research Center of Lower-Carbon Catalysis Technology, Dalian National Laboratory for Clean Energy, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian, 116023, P. R. China.

University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.

出版信息

Angew Chem Int Ed Engl. 2022 Jul 25;61(30):e202203903. doi: 10.1002/anie.202203903. Epub 2022 Jun 8.

Abstract

The applications of nanoporous crystalline materials are closely related to the mass transfer of guest molecules. However, the fundamental knowledge of mass transfer, and in particular the surface barriers controlled by the permeation of guest molecules through the external surfaces of materials, is still incomplete. The diversity of surface permeability at the single-crystal level, caused by the varying origins of surface transport resistance, hinders the rational materials design and needs better understanding. Herein, we probe the molecular transport in single zeolite crystals with fluorescent 4-(4-diethylaminostyryl-1-methylpyridinium iodide) (DAMPI) using super-resolution structured illumination microscopy (SIM). It showed that both the inter- and intra-crystal diversity of surface barriers could be monitored by detecting the diffusion behaviors on the center and surface planes in single crystals. This adds a new perspective for studying the origins of the surface barriers as well as the molecular transport mechanisms in nanoporous materials.

摘要

纳米多孔晶体材料的应用与客体分子的传质密切相关。然而,传质的基础知识,尤其是由客体分子透过材料外表面的渗透所控制的表面屏障,仍然不完整。由表面传输阻力的不同来源导致的单晶水平表面渗透率的多样性,阻碍了合理的材料设计,需要更好的理解。在此,我们使用超分辨率结构光照显微镜(SIM),用荧光4-(4-二乙氨基苯乙烯基-1-甲基碘化吡啶鎓)(DAMPI)探测单个沸石晶体中的分子传输。结果表明,通过检测单晶中心和表面平面上的扩散行为,可以监测表面屏障的晶间和晶内多样性。这为研究表面屏障的起源以及纳米多孔材料中的分子传输机制提供了一个新的视角。

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