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Ligand Torsion Triggered Two Robust Fe-Tetratopic Carboxylate Frameworks with Enhanced Gas Uptake and Separation Performance

机译:配体扭转触发两种具有增强的气体吸收和分离性能的鲁棒Fe-Tetropic羧酸盒框架

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摘要

By regulating the tetratopic carboxylate ligands, two robust Fe-MOFs (MOF=Metal-organic framework) comprising trigonal prismatic building blocks under a DMA/DMSO/HBF_4 solvent system, namely, [(CH_3)_2NH_2][Fe~(II) 3(OH)(BPTC)_(1.5)(DMSO)_3] (SNNU-60) and [Fe~(II)IFe~(II) 2(OH)(ABTC)_(1.5)(DMSO)_3] (SNNU-61) (BPTC=3,3’,5,5’-biphenyltetracarboxylic acid, ABTC=3,3’,5,5’-azobenzenetetracarboxylic acid, SNNU=Shaanxi Normal University) have been successfully synthesized. The torsions between the benzene groups of the ligands result in two MOFs exhibiting completely different (4,6)-connected frameworks, which represent the only two MOF types constructed by [M_3(O/ OH)(COO)_6] trimeric building units and quadrilateral tetratopic carboxylate linkers until now. The robust Fe-MOFs SNNU- 60 and SNNU-61 both exhibit high thermal/chemical stability, permanent microporosity, and excellent gas uptake capability for H_2, CO_2, C_2H_2, and C_2H_4 under 1 bar. SNNU-60 in particular displays very high C_2H_2 capture under low pressure (85 cm~3cm~(-3) at 0.15 bar and 298 K), which is among the top C_2H_2 uptake MOF materials. Also, these two Fe-MOFs display high separation for CO_2 and C_2-hydrocarbons over CH_4. Significantly, thanks to the high stability, suitable pore size, open Fe sites, and ion skeleton, SNNU-60 has extremely high C_2H_2/CH_4 selectivity (83.6, 298 K), which surpasses most MOFs reported so far under the same conditions.
机译:通过调节右型羧酸盐配体,在DMA / DMSO / HBF_4溶剂系统下包括三角棱镜建筑物的两种鲁棒Fe-Mof(Mof =金属 - 有机框架),即[(CH_3)_2NH_2] [Fe〜(II)3 (OH)(BPTC)_(1.5)(DMSO)_3](SNNU-60)和[Fe〜(II)IFE〜(II)2(OH)(ABTC)_(1.5)(DMSO)_3](SNU -61)(BPTC = 3,3',5,5'-二苯基四羧酸,ABTC = 3,3',5,5'-偶氮苯甲酸四羧酸,SNNU =陕西师范大学)已经成功地合成。配体的苯之间的扭转导致两种MOFS表现出完全不同(4,6)连接的框架,其代表由[M_3(O / OH)(COO)_6]三聚体构建单元构成的仅两种MOF类型四边形四胸型羧酸盐接头直到现在。鲁棒Fe-MOFS SNNU-60和SNNU-61都表现出高热/化学稳定性,永久性微孔,以及用于H_2,CO_2,C_2H_2和1巴下的C_2H_4的优异的气体摄取能力。 SNNU-60尤其在低压(85cm〜3cm〜(-3)下显示非常高的C_2H_2捕获,在0.15巴和298 k)中,这是顶部C_2H_2摄取MOF材料。此外,这两个Fe-MOFS在CH_4上显示CO_2和C_2-烃的高分分离。显着地,由于高稳定性,合适的孔径,开放式Fe位点和离子骨架,SNNU-60具有极高的C_2H_2 / CH_4选择性(83.6,298 K),其超越了迄今为止在相同条件下报告的大多数MOF。

著录项

  • 来源
    《Chemistry: A European journal》 |2017年第27期|共8页
  • 作者单位

    Key Laboratory of Macromolecular Science of Shaanxi Province School of Chemistry &

    Chemical Engineering Shaanxi Normal University Xi’an Shaanxi 710062 (P. R. China);

    Key Laboratory of Macromolecular Science of Shaanxi Province School of Chemistry &

    Chemical Engineering Shaanxi Normal University Xi’an Shaanxi 710062 (P. R. China);

    Key Laboratory of Macromolecular Science of Shaanxi Province School of Chemistry &

    Chemical Engineering Shaanxi Normal University Xi’an Shaanxi 710062 (P. R. China);

    Key Laboratory of Macromolecular Science of Shaanxi Province School of Chemistry &

    Chemical Engineering Shaanxi Normal University Xi’an Shaanxi 710062 (P. R. China);

    Key Laboratory of Macromolecular Science of Shaanxi Province School of Chemistry &

    Chemical Engineering Shaanxi Normal University Xi’an Shaanxi 710062 (P. R. China);

  • 收录信息
  • 原文格式 PDF
  • 正文语种 eng
  • 中图分类 应用化学;
  • 关键词

    C_2-hydrocarbons/CH_4 selectivity; Fe_3-trimer; gas uptake; metal-organic frameworks; tetratopic carboxylate ligand;

    机译:C_2 - 碳氢化合物/ CH_4选择性;FE_3-三角形;气体吸收;金属 - 有机框架;左撇子羧酸盐配体;

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