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自适应纳米石墨烯金属有机框架的一步合成:吸附气体依赖的几何多样性

One-Step Synthesis of an Adaptive Nanographene MOF: Adsorbed Gas-Dependent Geometrical Diversity.

作者信息

Suginome Shun, Sato Hiroshi, Hori Akihiro, Mishima Akio, Harada Yuki, Kusaka Shinpei, Matsuda Ryotaro, Pirillo Jenny, Hijikata Yuh, Aida Takuzo

机构信息

Department of Chemistry and Biotechnology, School of Engineering , The University of Tokyo , 7-3-1 Hongo , Bunkyo-ku, Tokyo 113-8656 , Japan.

Department of Chemistry and Biotechnology, School of Engineering , Nagoya University , Chikusa-ku, Nagoya , Aichi 464-8603 , Japan.

出版信息

J Am Chem Soc. 2019 Oct 2;141(39):15649-15655. doi: 10.1021/jacs.9b07732. Epub 2019 Sep 18.

DOI:10.1021/jacs.9b07732
PMID:31491075
Abstract

A layered metal-organic framework (MOF) comprising extra-large nanographene sheets, , was successfully synthesized using a dicarboxylic acid derivative of hexa--hexabenzocoronene (LH), and its structure was characterized by single-crystal X-ray diffraction analysis. The crystal structure shows that 2D layers composed of a dinuclear Zn complex unit and L are located on top of each other through multiple weak interlayer bonds, affording , having three dimensionally connected nanopores with large nanographene surfaces. The HBC-based nanographene sheets are anchored to the MOF framework via two zinc carboxylate linkages and therefore have an axial rotational freedom. The sorption isotherms of gaseous molecules such as carbon dioxide and hydrocarbons (acetylene, propane, propylene, benzene, and cyclohexane) on all displayed a hysteretic profile with reversible structural changes, as observed by in situ powder X-ray diffraction studies.

摘要

使用六苯并蔻的二羧酸衍生物(LH)成功合成了一种包含超大纳米石墨烯片的层状金属有机框架(MOF),并通过单晶X射线衍射分析对其结构进行了表征。晶体结构表明,由双核锌络合物单元和L组成的二维层通过多个弱层间键相互堆叠,形成了具有三维连通纳米孔且表面为大纳米石墨烯的结构。基于六苯并蔻的纳米石墨烯片通过两个羧酸锌键连接到MOF框架上,因此具有轴向旋转自由度。原位粉末X射线衍射研究表明,二氧化碳和碳氢化合物(乙炔、丙烷、丙烯、苯和环己烷)等气体分子在该MOF上的吸附等温线均呈现出具有可逆结构变化的滞后曲线。

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