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通过烃类物理吸附探究介孔金属有机骨架材料DUT-76(铜)的机械稳定性极限

Probing the Limits of Mechanical Stability of the Mesoporous Metal-Organic Framework DUT-76(Cu) by Hydrocarbon Physisorption.

作者信息

Konowski Kai, Bon Volodymyr, Karlsen Martin A, Etter Martin, Bönisch Nadine, De Ankita, Kaskel Stefan

机构信息

Chair of Inorganic Chemistry I, Technische Universität Dresden, Bergstraße 66, Dresden 01069, Germany.

P02.1 Beamline, PETRA III Synchrotron, DESY, Notkestraße 85, Hamburg 22607, Germany.

出版信息

ACS Appl Mater Interfaces. 2025 Apr 23;17(16):24096-24105. doi: 10.1021/acsami.5c00164. Epub 2025 Apr 8.

DOI:10.1021/acsami.5c00164
PMID:40196993
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12022944/
Abstract

The mechanical robustness of MOFs is crucial in most adsorption-related applications. Herein, we investigated the interaction of the mesoporous metal-organic framework DUT-76(Cu) with various C1-C4 hydrocarbons at their boiling points. During adsorption, the pore structure partially collapsed into an amorphous phase while retaining a residual porosity. We employed a combination of multicycle physisorption experiments using different hydrocarbons (methane, ethane, ethylene, propane, propylene, -butane, and 1,3-butadiene) along with X-ray diffraction, scanning electron microscopy, and total scattering to examine this transition. This methodology allowed us to gain a comprehensive understanding of the effects on the crystal structure, local structure, and macroscopic behavior of the material. Furthermore, we identified specific correlations among the chain length, number of double bonds, and adsorption/desorption cycle stability, which are influenced by adsorption-induced stress. These multicycle adsorption experiments served as semiquantitative tools for assessing the mechanical stability of mesoporous frameworks.

摘要

在大多数与吸附相关的应用中,金属有机框架材料(MOFs)的机械稳定性至关重要。在此,我们研究了介孔金属有机框架材料DUT-76(铜)在沸点下与各种C1-C4碳氢化合物的相互作用。在吸附过程中,孔隙结构部分坍塌成非晶相,同时保留了残余孔隙率。我们结合使用不同碳氢化合物(甲烷、乙烷、乙烯、丙烷、丙烯、丁烷和1,3-丁二烯)进行多循环物理吸附实验,并结合X射线衍射、扫描电子显微镜和全散射来研究这种转变。这种方法使我们能够全面了解对材料晶体结构、局部结构和宏观行为的影响。此外,我们确定了链长、双键数量与吸附/脱附循环稳定性之间的特定相关性,这些相关性受到吸附诱导应力的影响。这些多循环吸附实验作为评估介孔框架材料机械稳定性的半定量工具。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bef6/12022944/8a5279466c55/am5c00164_0007.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bef6/12022944/44b9a0bd4df2/am5c00164_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bef6/12022944/8a5279466c55/am5c00164_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bef6/12022944/84a0f294e02f/am5c00164_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bef6/12022944/06001f08eb52/am5c00164_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bef6/12022944/665e34861ef4/am5c00164_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bef6/12022944/9bbd4f1c0f5f/am5c00164_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bef6/12022944/89ca86c37ea8/am5c00164_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bef6/12022944/44b9a0bd4df2/am5c00164_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/bef6/12022944/8a5279466c55/am5c00164_0007.jpg

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本文引用的文献

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