Adsorptive separation of C2/C3/C4-hydrocarbons on a flexible Cu-MOF: The influence of temperature, chain length and bonding character
Adsorptive separation of C2/C3/C4-hydrocarbons on a flexible Cu-MOF: The influence of temperature, chain length and bonding character
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DOI：
10.1016/j.micromeso.2015.12.056
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发表时间：
2016-04-01
影响因子：
5.2
通讯作者：
Krautscheid, Harald
中科院分区：
文献类型：
--
作者：
Haehnel, Thomas;Kalies, Grit;Krautscheid, Harald
在这项工作中，提出并讨论了在柔性铜MOF材料Cu-4（mu（4）-O）（mu（2）-OH）（2）（Me（2）trzpba）（4）（1）上的压力测量和重量测量的吸附等温线。这包括在77.3 K下的氮（N-2）吸附、在298.15 K下的二氧化碳（CO2）吸附（补充材料）以及在273.15 K、298.15 K和323.15 K下的五种烃乙烷、乙烯、丙烷、正丁烷和1-丁烯的吸附。直到饱和压力，所有等温线显示出明显的拐点特征，这与柔性固体的结构转变有关。拐点的数量和拐点出现的相对压力取决于相关吸附剂的特性和温度。对于烃类吸附等温线，我们研究了i）测量温度，ii）成键特性，iii）烷烃和烯烃的链长的影响。此外，讨论了柔性MOF材料1上的氮吸附等温线中的平衡压力随着吸附体积的增加而降低的起因。使用理想吸附溶液理论（LAST）的计算，基于一元等温线拟合，沿着瞬态穿透模拟，用于证明Cu-MOF 1具有分离5组分乙烷/乙烯/丙烷/正丁烷/1-丁烯混合物以产生具有增加的碳数的三个不同馏分的潜力。(C)2016 Elsevier Inc. All rights reserved.
In this work, manometrically and gravimetrically measured adsorption isotherms on the flexible copper MOF material Cu-4(mu(4)-O)(mu(2)-OH)(2)(Me(2)trzpba)(4) (1) are presented and discussed. This includes nitrogen (N-2) adsorption at 77.3 K, carbon dioxide (CO2) adsorption at 298.15 K (Supplementary Material) and the adsorption of the five hydrocarbons ethane, ethene, propane, n-butane and 1-butene at 273.15 K, 298.15 K and 323.15 K. Up to the saturation pressure, all isotherms show distinct inflection characteristics, that are relatable to structural transitions of the flexible solid. The number of inflections and the relative pressure at which the inflections manifest depend on the characteristics of the relevant adsorptive and on temperature. For the hydrocarbon adsorption isotherms, we studied the influence of i) measurement temperature, ii) bonding character, and iii) the chain length of the alkanes and alkenes. In addition, the origin of decreasing equilibrium pressure with increasing adsorbed volume in the nitrogen adsorption isotherms on the flexible MOF material 1 is discussed. Calculations using the Ideal Adsorbed Solution Theory (LAST), based on the unary isotherm fits, along with transient breakthrough simulations, are used to demonstrate that Cu-MOF 1 has the potential to separate 5-component ethane/ethene/propane/n-butane/1-butene mixtures to yield three different fractions with increasing carbon numbers. (C) 2016 Elsevier Inc. All rights reserved.