Interpenetrated Zirconium–Organic Frameworks: Small Cavities versus Functionalization for CO2 Capture

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• 作者：Ravichandar Babarao ; Marta Rubio-Martinez ; Matthew R. Hill ; Aaron W. Thornton
• 刊名：Journal of Physical Chemistry C
• 出版年：2016
• 出版时间：June 23, 2016
• 年：2016
• 卷：120
• 期：24
• 页码：13013-13023
• 全文大小：641K
• 年卷期：0
• ISSN：1932-7455

文摘

Porous interpenetrated zirconium–organic frameworks (PIZOFs) with various functional groups are explored for CO₂ capture using molecular simulation and experiment. Functionalization enhances the CO₂ uptake and selectivity over other gases, but small cavities play an even more important role. Particularly at low pressures, small cavities enhance the CO₂ adsorption density nearly 5 times greater than the functionalization. PIZOF-2 outperforms the other PIZOF structures for CO₂ separation from methane and nitrogen (related to raw natural gas and postcombustion of coal mixtures) due to the combination of small cavities around 5 Å in diameter and functionalized linkers with methoxy groups attached to the central ligand. The small cavities within the interpenetrated structures are crucial for achieving high selectivities, especially for cavities surrounded by a combination of 6 benzene rings, 2 metal clusters, and 4 methoxy groups that offer a tight overlapping potential energy field, ideal for “catching” CO₂.