Ercakir Goktug, Aksu Gokhan Onder, Keskin Seda
Department of Chemical and Biological Engineering, Koc University, Rumelifeneri Yolu, Sariyer, 34450 Istanbul, Turkey.
J Chem Phys. 2024 Feb 28;160(8). doi: 10.1063/5.0189493.
In this study, we used a high-throughput computational screening approach to examine the potential of metal-organic frameworks (MOFs) for capturing propane (C3H8) from different gas mixtures. We focused on Quantum MOF (QMOF) database composed of both synthesized and hypothetical MOFs and performed Grand Canonical Monte Carlo (GCMC) simulations to compute C3H8/N2/O2/Ar and C3H8/C2H6/CH4 mixture adsorption properties of MOFs. The separation of C3H8 from air mixture and the simultaneous separation of C3H8 and C2H6 from CH4 were studied for six different adsorption-based processes at various temperatures and pressures, including vacuum-swing adsorption (VSA), pressure-swing adsorption (PSA), vacuum-temperature swing adsorption (VTSA), and pressure-temperature swing adsorption (PTSA). The results of molecular simulations were used to evaluate the MOF adsorbents and the type of separation processes based on selectivity, working capacity, adsorbent performance score, and regenerability. Our results showed that VTSA is the most effective process since many MOFs offer high regenerability (>90%) combined with high C3H8 selectivity (>7 × 103) and high C2H6 + C3H8 selectivity (>100) for C3H8 capture from air and natural gas mixtures, respectively. Analysis of the top MOFs revealed that materials with narrow pores (<10 Å) and low porosities (<0.7), having aromatic ring linkers, alumina or zinc metal nodes, typically exhibit a superior C3H8 separation performance. The top MOFs were shown to outperform commercial zeolite, MFI for C3H8 capture from air, and several well-known MOFs for C3H8 capture from natural gas stream. These results will direct the experimental efforts to the most efficient C3H8 capture processes by providing key molecular insights into selecting the most useful adsorbents.
在本研究中，我们采用高通量计算筛选方法，研究金属有机框架材料（MOF）从不同气体混合物中捕获丙烷（C3H8）的潜力。我们聚焦于由合成的和假设的MOF组成的量子MOF（QMOF）数据库，并进行巨正则蒙特卡罗（GCMC）模拟，以计算MOF对C3H8/N2/O2/Ar和C3H8/C2H6/CH4混合气体的吸附特性。研究了在不同温度和压力下，包括变压吸附（VSA）、变温吸附（VTSA）、变压变温吸附（PTSA）等六种不同的基于吸附的过程，从空气混合物中分离C3H8以及从CH4中同时分离C3H8和C2H6。分子模拟结果用于基于选择性、工作容量、吸附剂性能评分和可再生性来评估MOF吸附剂和分离过程类型。我们的结果表明，VTSA是最有效的过程，因为许多MOF具有高可再生性（>90%），同时分别对从空气和天然气混合物中捕获C3H8具有高C3H8选择性（>7×103）和高C2H6 + C3H8选择性（>100）。对顶级MOF的分析表明，具有窄孔（<10 Å）和低孔隙率（<0.7）、带有芳香环连接体、氧化铝或锌金属节点的材料通常表现出优异的C3H8分离性能。顶级MOF在从空气中捕获C3H8方面优于商用沸石MFI，在从天然气流中捕获C3H8方面优于几种知名的MOF。这些结果将通过提供有关选择最有用吸附剂的关键分子见解，指导实验工作朝着最有效的C3H8捕获过程发展。
