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通过原子力显微镜确定的金属有机框架的纳米级弯曲机制

Nanoscale Flexing Mechanism of a Metal-Organic Framework Determined by Atomic Force Microscopy.

作者信息

Trueman Mollie, Pooley Rachel J S, Lutton-Gething A R Bonity J, Hasija Avantika, Whitehead George F S, O'Shea Sean J, Anderson Michael W, Attfield Martin P

机构信息

Department of Chemistry, School of Natural Sciences, The University of Manchester, Oxford Road, Manchester M13 9PL, U.K.

Agency for Science Technology and Research, Institute of Materials Research and Engineering, Singapore 138634, Singapore.

出版信息

J Am Chem Soc. 2025 May 21;147(20):17201-17208. doi: 10.1021/jacs.5c02868. Epub 2025 May 9.

DOI:10.1021/jacs.5c02868
PMID:40346449
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC12100706/
Abstract

Flexible metal-organic frameworks (MOFs) are a unique set of compounds with applications in diverse areas. The nanoscale mechanism through which they flex is unproven. Herein, we use atomic force microscopy to observe the crystal surface of Ga-MIL-53 MOF, [Ga(OH)(BDC)] () (BDC - 1, 4-benzenedicarboxylate) as it undergoes flexing transformations during the guest exchange between N,N-dimethylformamide (DMF) and ethanol (EtOH)-containing . ·0.96DMF undergoes a flexing expansion transformation on guest exchange to form ·EtOH through the passage of wavefronts of cooperatively transforming, consecutive rows of unit cells parallel to the (011) plane, resulting in whole (011) layers of unit cells transforming by a layer-by-layer shear mechanism. The reverse process involves ·EtOH undergoing a flexing contraction transformation on guest exchange to form ·0.96DMF through a layer-by-layer shear mechanism involving layers of unit cells parallel to the (011̅) plane transforming in a cooperative manner. This proves a nanoscale mechanism through which a MOF can flex and the coexistence of phases with different degrees of expansion within a crystal, thus providing a missing link in the multilength scale understanding of MOF flexing transformations, which will support future design and application of flexible MOFs and other extended crystalline solids.

摘要

柔性金属有机框架材料（MOFs）是一类独特的化合物，在多个领域都有应用。其发生柔性变化的纳米尺度机制尚未得到证实。在此，我们使用原子力显微镜观察了Ga-MIL-53 MOF [Ga(OH)(BDC)] （BDC为1,4-苯二甲酸）在N,N-二甲基甲酰胺（DMF）与含乙醇（EtOH）的物质进行客体交换过程中发生柔性转变时的晶体表面。·0.96DMF在客体交换时通过协同转变的波前进行柔性膨胀转变，平行于（011）平面的连续晶胞行形成·EtOH，导致整个（011）层的晶胞通过逐层剪切机制发生转变。相反的过程是·EtOH在客体交换时通过逐层剪切机制发生柔性收缩转变，平行于（011̅）平面的晶胞层协同转变形成·0.96DMF。这证明了MOF能够发生柔性变化的纳米尺度机制以及晶体中不同膨胀程度相的共存，从而为在多长度尺度上理解MOF柔性转变提供了缺失的环节，这将为未来柔性MOF及其他扩展晶体固体的设计和应用提供支持。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5403/12100706/4cf1a931a1fb/ja5c02868_0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5403/12100706/b2640302991e/ja5c02868_0001.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5403/12100706/90f6b0996368/ja5c02868_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5403/12100706/03fdb16af315/ja5c02868_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5403/12100706/4cf1a931a1fb/ja5c02868_0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5403/12100706/b2640302991e/ja5c02868_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5403/12100706/5d30be461bb5/ja5c02868_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5403/12100706/053f34af43ca/ja5c02868_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5403/12100706/1f64830e755c/ja5c02868_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5403/12100706/08f5d9d84b7b/ja5c02868_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5403/12100706/90f6b0996368/ja5c02868_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5403/12100706/03fdb16af315/ja5c02868_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/5403/12100706/4cf1a931a1fb/ja5c02868_0008.jpg

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