Molecular Design of Zirconium Tetrazolate Metal–Organic Frameworks for CO2 Capture

详细信息    查看全文

• 作者：Kang Zhang ; Zhiwei Qiao ; Jianwen Jiang
• 刊名：Crystal Growth & Design
• 出版年：2017
• 出版时间：February 1, 2017
• 年：2017
• 卷：17
• 期：2
• 页码：543-549
• 全文大小：544K
• ISSN：1528-7505

文摘

Zirconium (Zr) metal–organic frameworks (MOFs) have received considerable interest due to their superior hydrolytic, thermal, and chemical stability. On the basis of 40 topological nets, 120 Zr-MOFs with 8-, 10-, and 12-coordination are designed in this study with nitrogen-rich CO₂-philic tetrazolate toward CO₂ capture. The Zr-tetrazolate MOFs are revealed to exhibit substantially stronger CO₂ adsorption than their carboxylate counterparts of identical topologies. By synergizing multiscale modeling from molecular simulation to breakthrough prediction, MOF-eft-P is identified among the 120 Zr-MOFs to possess the largest isosteric heat at infinite dilution and uptake at 1 bar for CO₂, as well as the highest CO₂/N₂ selectivity; it outperforms many typical MOFs and other adsorbents reported in the literature. The breakthrough time of CO₂ in MOF-eft-P is predicted to be 25 min and significantly longer than that of N₂, indicating excellent CO₂/N₂ separation. This study demonstrates the bottom-up strategy to design Zr-MOFs and suggests MOF-eft-P to be an interesting candidate for CO₂ capture.