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共价键合的金属有机框架/共价有机框架气凝胶作为用于快速分解神经毒剂的坚固催化过滤器。

Covalently Bound MOF/COF Aerogels as Robust Catalytic Filters for Rapid Nerve Agent Decomposition.

作者信息

Sahul' Martin, Benseghir Youven, Eder Tanja, Schöfbeck Flora, Ge Lingcong, Hetey Dániel, Reithofer Michael R, Chin Jia Min

机构信息

Institute of Functional Materials and Catalysis, Faculty of Chemistry, University of Vienna, Währinger Str. 42, 1090 Vienna, Austria.

Vienna Doctoral School in Chemistry (DoSChem), University of Vienna, Währinger Str. 42, 1090 Vienna, Austria.

出版信息

ACS Appl Mater Interfaces. 2025 Mar 12;17(10):15938-15947. doi: 10.1021/acsami.4c19759. Epub 2025 Mar 3.

DOI:10.1021/acsami.4c19759
PMID:40028880
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11912193/
Abstract

Metal-organic frameworks (MOFs) show promising results in various fields, such as gas separation and catalysis, but they face limitations due to problems associated with their low processability. This study addresses these challenges by utilizing postsynthetic modification (PSM) of NH-UiO-66 and NH-MOF-808 with 1,3,5-benzene tricarbaldehyde (BTCA) to form hybrid aerogels consisting of MOF-loaded covalent organic framework (COF). BTCA-modified MOF nanoparticles via imine bond formation were confirmed by H NMR, FTIR, and solid-state C NMR spectroscopies. MOF/COF composites were analyzed via TGA, PXRD, BET, and solid-state C NMR, showing retained crystallinity and increased porosity in comparison to the sum of the individual components. Moreover, improved aerogel mechanical properties and increased MOF loading of up to 75 wt % were achieved for covalently bound aerogels. Hybrid aerogel composites were successfully utilized as catalytic filters for the decomposition of nerve agent simulant and pesticide dimethyl-4-nitrophenylphosphate (DMNP), avoiding secondary pollution associated with MOF powder catalysis.

摘要

金属有机框架材料(MOFs)在气体分离和催化等各个领域展现出了良好的效果,但由于其加工性能低的相关问题,它们面临着局限性。本研究通过用1,3,5-苯三甲酸(BTCA)对NH-UiO-66和NH-MOF-808进行后合成修饰(PSM)来解决这些挑战,以形成由负载MOF的共价有机框架(COF)组成的混合气凝胶。通过¹H NMR、FTIR和固态¹³C NMR光谱证实了通过亚胺键形成的BTCA修饰的MOF纳米颗粒。通过TGA、PXRD、BET和固态¹³C NMR对MOF/COF复合材料进行了分析,结果表明与各单个组分的总和相比,其保留了结晶度且孔隙率增加。此外,对于共价键合的气凝胶,实现了气凝胶机械性能的改善以及高达75 wt%的MOF负载量增加。混合气凝胶复合材料成功用作催化过滤器,用于分解神经毒剂模拟物和农药4-硝基苯基磷酸二甲酯(DMNP),避免了与MOF粉末催化相关的二次污染。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/567a/11912193/79c02c2bcfe2/am4c19759_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/567a/11912193/60756d7f4c1c/am4c19759_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/567a/11912193/39b7d5fe9dd4/am4c19759_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/567a/11912193/3e6cb946659e/am4c19759_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/567a/11912193/7523dd28c489/am4c19759_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/567a/11912193/ba864bdd044b/am4c19759_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/567a/11912193/79c02c2bcfe2/am4c19759_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/567a/11912193/60756d7f4c1c/am4c19759_0001.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/567a/11912193/39b7d5fe9dd4/am4c19759_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/567a/11912193/3e6cb946659e/am4c19759_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/567a/11912193/7523dd28c489/am4c19759_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/567a/11912193/ba864bdd044b/am4c19759_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/567a/11912193/79c02c2bcfe2/am4c19759_0006.jpg

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本文引用的文献

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Macromorphological Control of Zr-Based Metal-Organic Frameworks for Hydrolysis of a Nerve Agent Simulant.用于神经毒剂模拟物水解的锆基金属有机框架的宏观形态控制
ACS Appl Mater Interfaces. 2024 Oct 2;16(39):52703-52711. doi: 10.1021/acsami.4c11928. Epub 2024 Sep 18.
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Nitrogen-rich and core-sheath polyamide/polyethyleneimine@Zr-MOF for iodine adsorption and nerve agent simulant degradation.
用于碘吸附和神经毒剂模拟物降解的富氮核壳结构聚酰胺/聚乙烯亚胺@锆基金属有机框架材料
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