Metal–organic frameworks with a sulfur-rich heterocycle: synthesis, gas adsorption properties, and metal exchange†

IF 3.3 3区化学 Q2 CHEMISTRY, INORGANIC & NUCLEAR Dalton Transactions Pub Date : 2024-09-20 DOI:10.1039/D4DT02209B

Vadim A. Dubskikh, Anna A. Lysova, Konstantin A. Kovalenko, Denis G. Samsonenko, Danil N. Dybtsev and Vladimir P. Fedin

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Abstract

Three new three-dimensional (3D) metal–organic frameworks [M₂(ttdc)₂(dabco)] (M = Zn(II), 1-Zn; Cu(II), 1-Cu; and Zn/Cu, 1-ZnCu) based on thieno[3,2-b]thiophene-2,5-dicarboxylate (ttdc²⁻) were synthesized and characterized by a combination of physicochemical methods (single crystal X-ray diffraction, powder X-ray diffraction, chemical and thermogravimetric analyses and IR spectroscopy). 1-Cu demonstrated permanent porosity (V_pore = 0.790 cm³ g⁻¹ and S_BET = 1725 m² g⁻¹) and significant CO₂, CH₄, C₂H₂, C₂H₄ and C₂H₆ gas uptakes under ambient conditions. The adsorption selectivities for gas mixtures, calculated by IAST, were 10.8 (10.7), 14.6 (9.4), 1.7 (1.6) and 1.5 (1.6) for the equimolar gas mixture compositions CO₂/N₂, C₂H₆/CH₄, C₂H₆/C₂H₄ and C₂H₆/C₂H₂ at 1 bar and 273 K (298 K), respectively. The mixed-metal compound 1-ZnCu was prepared by a crystal-to-crystal ion exchange metathesis reaction from 1-Zn with a 52% degree of ion substitution, confirmed by energy-dispersive X-ray spectroscopy, optical microscopy and single crystal X-ray diffraction analysis.

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具有富硫杂环的金属有机框架：合成、气体吸附特性和金属交换

基于噻吩并[3,2-b]噻吩-2,5-二羧酸盐（tdc2-）合成了三种三维金属有机框架[M2(tdc)2(dabco)]（М = Zn(II)，1-Zn；Cu(II)，1-Cu；合成了基于噻吩并[3,2-b]噻吩-2,5-二羧酸盐（tdc2-）的 M2(tdc)2(dabco)]（М = Zn(II)，1-Zn；Cu(II)，1-Cu；Zn/Cu，1-ZnCu），并通过多种物理化学方法（单晶 X 射线衍射、粉末 X 射线衍射、化学、热重分析和红外光谱）对其进行了表征。在环境条件下，1-Cu 表现出永久多孔性（Vpore = 0.790 cm3-g-1，SBET = 1725 m2-g-1）和显著的 CO2、CH4、C2H2、C2H4 和 C2H6 气体吸附性。在 1 巴和 273 K (298 K) 条件下，通过 IAST 计算得出的等摩尔混合气体成分 CO2/N2、C2H6/CH4、C2H6/C2H4 和 C2H6/C2H2 的吸附选择性分别为 10.8 (10.7)、14.6 (9.4)、1.7 (1.6) 和 1.5 (1.6)。能量色散 X 射线光谱、光学显微镜和单晶 X 射线衍射分析证实，混合金属化合物 1-ZnCu 是由离子取代度为 52% 的 1-Zn 通过晶体间离子交换偏析反应制备的。

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来源期刊

Dalton Transactions 化学-无机化学与核化学

CiteScore

6.60

自引率

7.50%

发文量

1832

审稿时长

1.5 months

期刊介绍： Dalton Transactions is a journal for all areas of inorganic chemistry, which encompasses the organometallic, bioinorganic and materials chemistry of the elements, with applications including synthesis, catalysis, energy conversion/storage, electrical devices and medicine. Dalton Transactions welcomes high-quality, original submissions in all of these areas and more, where the advancement of knowledge in inorganic chemistry is significant.