超稳定羧酸铜金属有机骨架。

IF 15.6 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Han Yang, Ming Xu, Min Mao, Lei Gao, Hao Zhang, Sha-Sha Meng, Wen-Qi Tang, Yu-Hao Gu, Shuai Yuan, Ling-Mei Liu and Zhi-Yuan Gu*, 
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引用次数: 0

摘要

直接合成酸碱稳定的羧酸铜金属有机骨架(MOFs)具有重要的意义,但也面临着严峻的挑战。本文提出了一种纳米包膜策略,通过AB堆叠保护Cu(II)与4,4',4″,4′-(1,3,6,8-芘四烷基)四苯甲酸(h4tbay)之间组装中的铜桨轮簇。这种结构出人意料地限制了水进入Cu-O键,创造了在水中(240天,RT)以及酸和碱溶液(pH从0到13)中最稳定的mof之一。水蒸气吸附实验、密度泛函理论(DFT)计算和径向分布函数(RDF)分析进一步证实了cu2tbby的高阻水性。此外,还实现了对二甲苯异构体的极好分离,其分辨率为18.2(间二甲苯/对二甲苯),耐久性为31个月,超过了所有以前的材料。对二甲苯异构体杂质的分离检出限低至1.33 pg。cu2tbby优异的稳定性为高水稳定性羧酸铜mof的设计和合成提供了有价值的指导。
本文章由计算机程序翻译,如有差异,请以英文原文为准。

Ultrastable Copper Carboxylate Metal–Organic Frameworks

Ultrastable Copper Carboxylate Metal–Organic Frameworks

Direct synthesis of acid–base-stable copper carboxylate metal–organic frameworks (MOFs) is of great significance but faces substantial challenges. Herein, a nanoenvelope strategy was proposed to protect the copper paddle-wheel cluster in the assembly between Cu(II) and 4,4′,4″,4‴-(1,3,6,8-pyrenetetrayl)tetrakis-benzoic acid (H4TBAPy) through AB stacking. This structure unexpectedly restricted the access of water to the Cu–O bonds, creating one of the most stable MOFs in water (240 days, RT) as well as in acid and base solutions (pH from 0 to 13). Water vapor adsorption experiments, density functional theory (DFT) calculations, and radial distribution function (RDF) analyses further confirmed the high water resistance of Cu2TBAPy. Moreover, excellent separation for xylene isomers was achieved, with a resolution of 18.2 (meta-xylene/para-xylene) and a durability of 31 months, which surpassed all previous materials. Xylene isomer impurities were separated with a detection limit as low as 1.33 pg. The remarkable stability of Cu2TBAPy offers valuable guidance for the design and synthesis of highly water-stable copper carboxylate MOFs.

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来源期刊
CiteScore
24.40
自引率
6.00%
发文量
2398
审稿时长
1.6 months
期刊介绍: The flagship journal of the American Chemical Society, known as the Journal of the American Chemical Society (JACS), has been a prestigious publication since its establishment in 1879. It holds a preeminent position in the field of chemistry and related interdisciplinary sciences. JACS is committed to disseminating cutting-edge research papers, covering a wide range of topics, and encompasses approximately 19,000 pages of Articles, Communications, and Perspectives annually. With a weekly publication frequency, JACS plays a vital role in advancing the field of chemistry by providing essential research.
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