将富马酸镓和富马酸MOF引入该家族：合成，综合表征，多孔疏水性观察和CO <sub>2</sub>动力学,ACS Applied Materials & Interfaces

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将富马酸镓和富马酸MOF引入该家族：合成，综合表征，多孔疏水性观察和CO ₂动力学
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2018-08-02 00:00:00 , DOI: 10.1021/acsami.8b08562
Yue Zhang ₁ , Bryan E. G. Lucier ₁ , Sarah M. McKenzie ₁ , Mihails Arhangelskis ₂ , Andrew J. Morris ₃ , Tomislav Friščić ₂ , Joel W. Reid ₄ , Victor V. Terskikh ₅ , Mansheng Chen ₁ , Yining Huang ₁

Affiliation

金属有机骨架（MOF）的性质和应用在很大程度上取决于金属和连接基的性质，以及合成过程中采用的特定条件。富马酸铝（商标名称为Basolite A520）是一种多孔MOF，它结合了铝中心和富马酸酯连接基，是一种用于涉及气体（如CO _2）吸附的有前途的材料。在这项工作中，描述了富马酸镓和富马酸铟MOF（富马酸酯，富马酸酯）的溶剂热合成和详细表征。结合使用粉末X射线衍射，Rietveld精制，固态NMR光谱，IR光谱和热重分析，发现富马酸和富马酸的拓扑与富马酸铝相似。超宽线⁶⁹ Ga，⁷¹ Ga和¹¹⁵ In在21.1 T的NMR实验中有力地支持了我们的精细结构。吸附等温线表明，Al-，Ga-和富马酸酯在MOF中均表现出对CO ₂的亲和力，富马酸酯在1 bar和273 K时是优良的吸附剂。静态直接激发和交叉极化¹³ C NMR实验允许调查CO ₂吸附位置，结合强度，运动速率和运动角度，这些对于增加这些材料的吸附能力和选择性至关重要。在甲醇中进行铟基骨架的合成表明，通过在MOF孔中掺入金属桥连的-OCH ₃基团，可将多孔疏水性引入MIL-53型骨架的简单方法。

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Welcoming Gallium- and Indium-Fumarate MOFs to the Family: Synthesis, Comprehensive Characterization, Observation of Porous Hydrophobicity, and CO2 Dynamics

The properties and applications of metal–organic frameworks (MOFs) are strongly dependent on the nature of the metals and linkers, along with the specific conditions employed during synthesis. Al-fumarate, trademarked as Basolite A520, is a porous MOF that incorporates aluminum centers along with fumarate linkers and is a promising material for applications involving adsorption of gases such as CO₂. In this work, the solvothermal synthesis and detailed characterization of the gallium- and indium-fumarate MOFs (Ga-fumarate, In-fumarate) are described. Using a combination of powder X-ray diffraction, Rietveld refinements, solid-state NMR spectroscopy, IR spectroscopy, and thermogravimetric analysis, the topologies of Ga-fumarate and In-fumarate are revealed to be analogous to Al-fumarate. Ultra-wideline ⁶⁹Ga, ⁷¹Ga, and ¹¹⁵In NMR experiments at 21.1 T strongly support our refined structure. Adsorption isotherms show that the Al-, Ga-, and In-fumarate MOFs all exhibit an affinity for CO₂, with Al-fumarate being the superior adsorbent at 1 bar and 273 K. Static direct excitation and cross-polarized ¹³C NMR experiments permit investigation of CO₂ adsorption locations, binding strengths, motional rates, and motional angles that are critical to increasing adsorption capacity and selectivity in these materials. Conducting the synthesis of the indium-based framework in methanol demonstrates a simple route to introduce porous hydrophobicity into a MIL-53-type framework by incorporation of metal-bridging −OCH₃ groups in the MOF pores.

更新日期：2018-08-02

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