High-throughput computational screening of Cu-MOFs with open metal sites for efficient C_2H_2/C_2H_4 separation

• 作者: Chongli Zhong Dahuan Liu Lei Liu Lei Wang Qingyuan Yang
• 来源期刊: 绿色能源与环境:英文版
• 学科: 化学
• 关键词: Acetylene and ethylene Metal-organic frameworks Open metal sites Large-scale computation Materials design
• 年，卷（期）: 2020,（3）
• 页码范围: 333-340
• 页数: 8页
• 分类号: O64

摘要

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.