Molecular Sieving of Ethane from Ethylene through the Molecular Cross-Section Size Differentiation in Gallate-based Metal-Organic Frameworks.
Molecular Sieving of Ethane from Ethylene through the Molecular Cross-Section Size Differentiation in Gallate-based Metal-Organic Frameworks.
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DOI：
10.1002/anie.201808716
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发表时间：
2018-12-03
期刊：
影响因子：
--
通讯作者：
Ren Q
中科院分区：
文献类型：
--
作者：
Bao Z;Wang J;Zhang Z;Xing H;Yang Q;Yang Y;Wu H;Krishna R;Zhou W;Chen B;Ren Q
从C2 H4/C2 H6混合物中纯化C2 H4是最重要但具有挑战性的工业分离方法之一，主要是通过能量密集型低温蒸馏。现在，提出了一类基于没食子酸盐的金属有机框架（MOF）材料，M-没食子酸盐（M=Ni、Mg、Co），其特征在于3D互连的锯齿形通道，其孔径尺寸（3.47-3.69 μ m）非常适合乙烯的分子筛（3.28 × 4.18 × 4.84 × 3）和乙烷（3.81 × 4.08 × 4.82 × 3）。在298 K和1 bar下，Co-没食子酸盐显示出前所未有的C2 H4对C2 H6的IAST选择性为52，C2 H4吸收量为3.37 mmolg−1，优于最先进的MOF材料NOTT-300。用等摩尔C2 H4/C2 H6混合物的直接穿透实验证实，M-没食子酸酯对乙烯具有高度选择性。通过中子衍射实验进一步研究了没食子酸间酯对乙烯的吸附结构和机理。
Purification of C2H4 from an C2H4/C2H6 mixture, one of the most important while challenging industrial separation processes, is mainly through energy-intensive cryogenic distillation. Now a family of gallate-based metal–organic framework (MOF) materials is presented, M-gallate (M=Ni, Mg, Co), featuring 3D interconnected zigzag channels, the aperture sizes of which (3.47–3.69 Å) are ideally suitable for molecular sieving of ethylene (3.28 × 4.18 × 4.84 Å3) and ethane (3.81 × 4.08 × 4.82 Å3) through molecular cross-section size differentiation. Co-gallate shows an unprecedented IAST selectivity of 52 for C2H4 over C2H6 with a C2H4 uptake of 3.37 mmolg−1 at 298 K and 1 bar, outperforming the state-of-the-art MOF material NOTT-300. Direct breakthrough experiments with equimolar C2H4/C2H6 mixtures confirmed that M-gallate is highly selective for ethylene. The adsorption structure and mechanism of ethylene in the M-gallate was further studied through neutron diffraction experiments.
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