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通过水解法合成的含2,5-二羟基-1,4-苯醌和4,4'-联吡啶的配位聚合物的合成、结构与性质

Syntheses, Structures, and Properties of Coordination Polymers with 2,5-Dihydroxy-1,4-Benzoquinone and 4,4'-Bipyridyl Synthesized by Hydrolysis Method.

作者信息

Yamazui Daiki, Uchida Kaiji, Koyama Shohei, Wu Bin, Iguchi Hiroaki, Kosaka Wataru, Miyasaka Hitoshi, Takaishi Shinya

机构信息

Department of Chemistry, Graduate School of Science, Tohoku University, 6-3 Aramaki-Aza-Aoba, Aoba-ku, Sendai, Miyagi 980-8578, Japan.

Institute for Materials Research, Tohoku University, 2-1-1 Katahira, Aoba-ku, Sendai 980-8577, Japan.

出版信息

ACS Omega. 2022 May 24;7(22):18259-18266. doi: 10.1021/acsomega.1c07077. eCollection 2022 Jun 7.

DOI:10.1021/acsomega.1c07077
PMID:35694494
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9178755/
Abstract

The coordination polymers (CPs) with binary ligands, including 2,5-dihydroxy-1,4-benzoquinone (H2DHBQ) and 4,4'-bipyridyl (bpy), were synthesized using hydrolysis of 2,5-dimethoxy-1,4-benzoquinone (DMBQ). Three kinds of CPs were obtained depending on the metal ions. For M = Mn and Zn, a 1D zigzag chain structure with cis conformation ( ) was obtained, whereas Co, Ni, and Cu compounds afforded a 2D net structure with trans conformation ( ) with a 1D pore. A linear chain structure was also obtained for M = Cu. Magnetic susceptibility (χ ) at 300 K in and was evaluated to be 4.421 and 2.950 cm K mol, respectively, indicating that both compounds are in the high-spin state. According to the N adsorption isotherms at 77 K, showed microporosity with the BET surface area of 177 m g, whereas the isomorphic rarely adsorbed N at 77 K. This phenomenon was explained by the difference of diffusion kinetics of the adsorbent molecules, which was supported by the CO adsorption isotherms at 195 K. The optical band gaps of , , , and were estimated to be 1.6, 1.8, 1.0, and 1.1 eV, respectively, by using UV-vis-NIR spectroscopy.

摘要

通过2,5 - 二甲氧基 - 1,4 - 苯醌（DMBQ）的水解反应，合成了包含2,5 - 二羟基 - 1,4 - 苯醌（H2DHBQ）和4,4'-联吡啶（bpy）的二元配体配位聚合物（CPs）。根据金属离子的不同，得到了三种CPs。当M = Mn和Zn时，得到了具有顺式构象（ ）的一维之字形链结构，而Co、Ni和Cu化合物则提供了具有反式构象（ ）和一维孔道的二维网络结构。对于M = Cu，还得到了线性链结构。在300 K下， 和 中的磁化率（χ ）分别评估为4.421和2.950 cm³ K⁻¹ mol⁻¹，表明这两种化合物均处于高自旋状态。根据77 K下的N₂吸附等温线， 表现出微孔性，BET表面积为177 m² g⁻¹，而同构的 在77 K时几乎不吸附N₂。这种现象通过吸附剂分子扩散动力学的差异来解释，这得到了195 K下CO吸附等温线的支持。通过紫外 - 可见 - 近红外光谱法估计， 、 、 和 的光学带隙分别为1.6、1.8、1.0和1.1 eV。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7b82/9178755/aad6d7fa2cef/ao1c07077_0008.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7b82/9178755/69c2e6bbd809/ao1c07077_0005.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/7b82/9178755/aad6d7fa2cef/ao1c07077_0008.jpg

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