A computational study was firstly performed in this work to examine the applicability of an acid-functionalized metal-organic framework(MOF), Ui O-66(Zr)-(COOH)2, in membrane-based H2S/CH4 separation. The results show that this MOF could be potentially interesting when being used as the pure membrane material for the separation of the mixture with low H2 S concentration. Further, the performance of 10 different mixed matrix membranes(MMMs) on the basis of the MOF was predicted by combing the molecular simulation data and the Maxwell permeation model. The results indicate that using this MOF as filler particles in MMMs can signi ficantly enhance the permeation performance of pure polymers. The findings obtained in this work may be helpful in facilitating the application of this promising MOF for practical desulfurization process of fuel gas.
The globally increasing concentrations of greenhouse gases in atmosphere after combustion of coal-or petroleum-based fuels give rise to tremendous interest in searching for porous materials to efficiently capture carbon dioxide(CO_2) and store methane(CH4), where the latter is a kind of clean energy source with abundant reserves and lower CO_2 emission. Hundreds of thousands of porous materials can be enrolled on the candidate list, but how to quickly identify the really promising ones, or even evolve materials(namely, rational design high-performing candidates) based on the large database of present porous materials? In this context, high-throughput computational techniques, which have emerged in the past few years as powerful tools, make the targets of fast evaluation of adsorbents and evolving materials for CO_2 capture and CH_4 storage feasible. This review provides an overview of the recent computational efforts on such related topics and discusses the further development in this field.
Cost effective separation of acetylene(C_2H_2)and ethylene(C_2H_4)is of key importance to obtain essential chemical raw materials for polymer industry.Due to the low compression limit of C_2H_2,there is an urgent demand to develop suitable materials for efficiently separating the two gases under ambient conditions.In this paper,we provided a high-throughput screening strategy to study porous metal-organic frameworks(MOFs)containing open metal sites(OMS)for C_2H_2/C_2H_4 separation,followed by a rational design of novel MOFs in-silico.A set of accurate force fields was established from ab initio calculations to describe the critical role of OMS towards guest molecules.From a large-scale computational screening of 916 experimental Cu-paddlewheel-based MOFs,three materials were identified with excellent separation performance.The structure-performance relationships revealed that the optimal materials should have the largest cavity diameter around 5-10?and pore volume in-between 0.3-1.0 cm^3 g^(-1).Based on the systematic screening study result,three novel MOFs were further designed with the incorporation of fluorine functional group.The results showed that Cu-OMS and the-F group on the aromatic rings close to Cu sites could generate a synergistic effect on the preferential adsorption of C_2H_2 over C_2H_4,leading to a remarkable improvement of C_2H_2 separation performance of the materials.The findings could provide insight for future experimental design and synthesis of high-performance nanostructured materials for C_2H_2/C_2H_4 separation.
Lei LiuLei WangDahuan LiuQingyuan YangChongli Zhong
