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通过酰亚胺缩合和配位组装合成的金属有机框架的比较研究。

Comparative study of metal-organic frameworks synthesized imide condensation and coordination assembly.

作者信息

Liu Qiao, Hilliard Jordon S, Cai Zhongzheng, Wade Casey R

机构信息

Department of Chemistry and Biochemistry, The Ohio State University 100 West 18th Ave Columbus OH 43210 USA

出版信息

RSC Adv. 2024 Aug 30;14(38):27634-27643. doi: 10.1039/d4ra05563b. eCollection 2024 Aug 29.

DOI:10.1039/d4ra05563b
PMID:39221129
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC11363248/
Abstract

A series of metal-organic frameworks (1-XDI) have been synthesized by imide condensation reactions between an amine-functionalized pentanuclear zinc cluster, ZnCl(bt-NH), (bt-NH = 5-aminobenzotriazolate), and organic dianhydrides (pyromellitic dianhydride (PMDA), naphthalenetetracarboxylic dianhydride (NDA), 3,3',4,4'-biphenyltetracarboxylic dianhydride (BPDA) and 4,4'-(hexafluoroisopropylidene)diphthalic anhydride (HFIPA)). The properties of the 1-XDI MOFs have been compared with analogues (2-XDI) prepared using traditional coordination assembly. The resulting materials have been characterized by ATR-IR spectroscopy, acid-digested H NMR spectroscopy, elemental analysis, and gas adsorption measurements. N adsorption isotherm data reveal modest porosities and BET surface areas (30-552 m g). All of the new 1-XDI and 2-XDI MOFs show selective adsorption of CH over CO while 2-PMDI and 2-BPDI exhibit high selectivity toward CH/CH separation. This study establishes imide condensation of preformed metal-organic clusters with organic linkers as a viable route for MOF design.

摘要

通过胺官能化的五核锌簇ZnCl(bt-NH)（bt-NH = 5-氨基苯并三唑）与有机二酐（均苯四甲酸二酐（PMDA）、萘四甲酸二酐（NDA）、3,3',4,4'-联苯四甲酸二酐（BPDA）和4,4'-（六氟异亚丙基）二邻苯二甲酸酐（HFIPA））之间的酰亚胺缩合反应，合成了一系列金属有机框架（1-XDI）。将1-XDI金属有机框架的性质与使用传统配位组装制备的类似物（2-XDI）进行了比较。通过衰减全反射红外光谱（ATR-IR）、酸消解氢核磁共振光谱（H NMR）、元素分析和气体吸附测量对所得材料进行了表征。氮气吸附等温线数据显示出适度的孔隙率和比表面积（30 - 552 m²/g）。所有新的1-XDI和2-XDI金属有机框架都表现出对CH₄比对CO有选择性吸附，而2-PMDI和2-BPDI对CH₄/C₂H₄分离表现出高选择性。本研究确立了预制金属有机簇与有机连接体的酰亚胺缩合作为金属有机框架设计的可行途径。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/833b/11363248/20c8da069772/d4ra05563b-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/833b/11363248/dfd69120e4ab/d4ra05563b-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/833b/11363248/7e90314c97e1/d4ra05563b-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/833b/11363248/c74dbedd86d0/d4ra05563b-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/833b/11363248/376312e0dd1d/d4ra05563b-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/833b/11363248/20c8da069772/d4ra05563b-f4.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/833b/11363248/dfd69120e4ab/d4ra05563b-s1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/833b/11363248/7e90314c97e1/d4ra05563b-f1.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/833b/11363248/c74dbedd86d0/d4ra05563b-f2.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/833b/11363248/376312e0dd1d/d4ra05563b-f3.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/833b/11363248/20c8da069772/d4ra05563b-f4.jpg

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