Metal鈥揙rganic Frameworks with Precisely Designed Interior for Carbon Dioxide Capture in the Presence of Water

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• 作者：Alejandro M. Fracaroli ; Hiroyasu Furukawa ; Mitsuharu Suzuki ; Matthew Dodd ; Satoshi Okajima ; Felipe G谩ndara ; Jeffrey A. Reimer ; Omar M. Yaghi
• 刊名：Journal of the American Chemical Society
• 出版年：2014
• 出版时间：June 25, 2014
• 年：2014
• 卷：136
• 期：25
• 页码：8863-8866
• 全文大小：287K
• ISSN：1520-5126

文摘

The selective capture of carbon dioxide in the presence of water is an outstanding challenge. Here, we show that the interior of IRMOF-74-III can be covalently functionalized with primary amine (IRMOF-74-III-CH₂NH₂) and used for the selective capture of CO₂ in 65% relative humidity. This study encompasses the synthesis, structural characterization, gas adsorption, and CO₂ capture properties of variously functionalized IRMOF-74-III compounds (IRMOF-74-III-CH₃, -NH₂, -CH₂NHBoc, -CH₂NMeBoc, -CH₂NH₂, and -CH₂NHMe). Cross-polarization magic angle spinning ¹³C NMR spectra showed that CO₂ binds chemically to IRMOF-74-III-CH₂NH₂ and -CH₂NHMe to make carbamic species. Carbon dioxide isotherms and breakthrough experiments show that IRMOF-74-III-CH₂NH₂ is especially efficient at taking up CO₂ (3.2 mmol of CO₂ per gram at 800 Torr) and, more significantly, removing CO₂ from wet nitrogen gas streams with breakthrough time of 610 卤 10 s g^鈥? and full preservation of the IRMOF structure.