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通过抗衡离子的策略性选择改善草酸铜（II）金属有机框架的质子传导

Improvement of the Proton Conduction of Copper(II)-Mesoxalate Metal-Organic Frameworks by Strategic Selection of the Counterions.

作者信息

Gil-Hernández Beatriz, Millan Simon, Gruber Irina, Quirós Miguel, Marrero-López David, Janiak Christoph, Sanchiz Joaquín

机构信息

Departamento de Química, Facultad de Ciencias, Sección Química, Universidad de La Laguna, La Laguna 38206, Tenerife, Spain.

Institute of Materials and Nanotechnology, Universidad de La Laguna, P.O. Box 456, La Laguna E-38200, Tenerife, Spain.

出版信息

Inorg Chem. 2022 Aug 1;61(30):11651-11666. doi: 10.1021/acs.inorgchem.2c01241. Epub 2022 Jul 15.

DOI:10.1021/acs.inorgchem.2c01241
PMID:35838657
原文链接:https://pmc.ncbi.nlm.nih.gov/articles/PMC9377511/
Abstract

Three copper(II)/mesoxalate-based MOFs with formulas (HO)[Cu(Hmesox)(HO)Cl]·8HO (), (NHMe)(HO)[Cu(Hmesox)(HO)Cl]·8HO (), and (enH)(enH)[Cu(Hmesox)(mesox)(HO)Cl]Cl·5.25HO () were synthesized (Hmesox = mesoxalic acid = 2,2-dihydroxypropanedioic acid, en = ethylenediamine). Essentially, all of the compounds display the same anionic network with a different arrangement of the cations, which have a remarkable effect on the proton conduction of the materials, ranging from 1.16 × 10 S cm for to 1.87 × 10 S cm for (at 80 °C and 95% RH). These compounds also display antiferromagnetic coupling among the copper(II) ions through both the carboxylate and alkoxido bridges. The values of the principal magnetic coupling constants were calculated by density functional theory (DFT), leading to congruent values that confirm the predominant antiferromagnetic nature of the interactions.

摘要

合成了三种基于草酸铜（II）的金属有机框架材料，其化学式分别为(HO)[Cu(Hmesox)(HO)Cl]·8HO （）、(NHMe)(HO)[Cu(Hmesox)(HO)Cl]·8HO （）和(enH)(enH)[Cu(Hmesox)(mesox)(HO)Cl]Cl·5.25HO （）（Hmesox = 草酸 = 2,2 - 二羟基丙二酸，en = 乙二胺）。本质上，所有这些化合物都具有相同的阴离子网络，只是阳离子的排列方式不同，这对材料的质子传导有显著影响，传导率范围从 的1.16 × 10 S cm到 的1.87 × 10 S cm（在80°C和95%相对湿度下）。这些化合物还通过羧酸盐和烷氧基桥在铜（II）离子之间表现出反铁磁耦合。主要磁耦合常数的值通过密度泛函理论（DFT）计算得出，得到的一致值证实了相互作用主要为反铁磁性质。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/5484a77368d2/ic2c01241_0012.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/79dca6ab0668/ic2c01241_0013.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/8c5d2524c0ba/ic2c01241_0002.jpg
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https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/aba4ad10c9b7/ic2c01241_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/f15672fcdf04/ic2c01241_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/e91dd0ded0b7/ic2c01241_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/6d91994ba1e9/ic2c01241_0014.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/b504fb9f3d79/ic2c01241_0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/bfbc0dd5600b/ic2c01241_0009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/ba2db63abfc8/ic2c01241_0010.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/a351b5e02986/ic2c01241_0011.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/5484a77368d2/ic2c01241_0012.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/79dca6ab0668/ic2c01241_0013.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/8c5d2524c0ba/ic2c01241_0002.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/348f865d709b/ic2c01241_0003.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/8e33ccb5eef3/ic2c01241_0004.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/aba4ad10c9b7/ic2c01241_0005.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/f15672fcdf04/ic2c01241_0006.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/e91dd0ded0b7/ic2c01241_0007.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/6d91994ba1e9/ic2c01241_0014.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/b504fb9f3d79/ic2c01241_0008.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/bfbc0dd5600b/ic2c01241_0009.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/ba2db63abfc8/ic2c01241_0010.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/a351b5e02986/ic2c01241_0011.jpg
https://cdn.ncbi.nlm.nih.gov/pmc/blobs/72fd/9377511/5484a77368d2/ic2c01241_0012.jpg

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