Tao Ze-Rong, Wu Jian-Xiang, Zhao Ying-Jie, Xu Ming, Tang Wen-Qi, Zhang Qing-Hua, Gu Lin, Liu Da-Huan, Gu Zhi-Yuan
Jiangsu Key Laboratory of Biofunctional Materials, Jiangsu Collaborative Innovation Center of Biomedical Functional Materials, College of Chemistry and Materials Science, Nanjing Normal University, 210023, Nanjing, China.
State Key Laboratory of Organic-Inorganic Composites, Beijing Advanced Innovation Center for Soft Matter Science and Engineering, Beijing University of Chemical Technology, 100029, Beijing, China.
Nat Commun. 2019 Jul 2;10(1):2911. doi: 10.1038/s41467-019-10971-x.
The stacking between nanosheets is an intriguing and inevitable phenomenon in the chemistry of nano-interfaces. Two-dimensional metal-organic framework nanosheets are an emerging type of nanosheets with ultrathin and porous features, which have high potential in separation applications. Here, the stacking between single-layer metal-organic framework nanosheets is revealed to show three representative conformations with tilted angles of 8°, 14°, and 30° for Zr-1, 3, 5-(4-carboxylphenyl)-benzene framework as an example. Efficient untwisted stacking strategy by simple heating is proposed. A detailed structural analysis of stacking modes reveals the creation of highly ordered sub-nanometer micropores in the interspacing of untwisted nano-layers, yielding a high-resolution separator for the pair of para-/meta-isomers over the twisted counterparts and commercial HP-5MS and VF-WAXMS columns. This general method is proven by additional nanosheet examples and supported by Grand Canonical Monte Carlo simulation. This finding will provide a synthetic route in the rational design of functionalities in two-dimensional metal-organic framework nanosheet.
在纳米界面化学中，纳米片之间的堆叠是一种有趣且不可避免的现象。二维金属有机框架纳米片是一种新兴的具有超薄和多孔特征的纳米片类型，在分离应用中具有很高的潜力。在此，以Zr-1,3,5-(4-羧基苯基)-苯框架为例，揭示了单层金属有机框架纳米片之间的堆叠呈现出三种代表性构象，倾斜角度分别为8°、14°和30°。提出了通过简单加热实现高效解缠堆叠的策略。对堆叠模式的详细结构分析表明，在解缠纳米层的间距中形成了高度有序的亚纳米微孔，从而为对映/间位异构体对提供了比扭曲对应物以及商用HP-5MS和VF-WAXMS柱更高分辨率的分离器。通过其他纳米片实例证明了这种通用方法，并得到了巨正则蒙特卡罗模拟的支持。这一发现将为二维金属有机框架纳米片功能的合理设计提供一条合成途径。
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