School of Chemical & Biomolecular Engineering, Georgia Institute of Technology, Atlanta, Georgia 30332-0100, United States.
Langmuir. 2012 Oct 9;28(40):14114-28. doi: 10.1021/la301915s. Epub 2012 Jul 26.
The selection of metal-organic frameworks (MOFs) for gas adsorption and separation has become a significant challenge over the past decade because of the large number of new structures reported every year. We applied a multiscale computational approach to screen existing MOFs for CO(2)/N(2) separation. Pore characteristics of 1163 MOFs were analyzed by the method developed by Haldoupis, Nair, and Sholl (Haldoupis, E.; Nair, S.; Sholl, D. S. J. Am. Chem. Soc.2010, 132, 7528) using a simple steric model. On the basis of the pore size analysis, 359 MOFs were examined by classical molecular simulations. Adsorption and diffusion properties were computed using grand canonical Monte Carlo (GCMC) and molecular dynamics (MD) simulations, respectively. These molecular simulations were used to assess which materials hold the greatest promise as membrane materials for CO(2)/N(2) separations. Finally, density functional theory (DFT) calculations were performed to provide preliminary information on the dynamic framework motion of selected MOFs.
在过去的十年中，由于每年都有大量新结构被报道，因此选择用于气体吸附和分离的金属有机骨架（MOFs）已成为一项重大挑战。我们应用了一种多尺度计算方法来筛选现有的 MOFs 以进行 CO(2)/N(2)分离。通过 Haldoupis、Nair 和 Sholl（Haldoupis，E.；Nair，S.；Sholl，D. S. J. Am. Chem. Soc.2010，132，7528）开发的方法分析了 1163 个 MOFs 的孔特性，该方法使用简单的空间模型。在此基础上，对 359 个 MOFs 进行了经典分子模拟研究。使用巨正则蒙特卡罗（GCMC）和分子动力学（MD）模拟分别计算了吸附和扩散特性。这些分子模拟用于评估哪些材料最有希望成为 CO(2)/N(2)分离的膜材料。最后，进行密度泛函理论（DFT）计算，以提供选定 MOFs 的动态框架运动的初步信息。
