CO2-Selective Absorbents in Air: Reverse Lipid Bilayer Structure Forming Neutral Carbamic Acid in Water without Hydration
CO2-Selective Absorbents in Air: Reverse Lipid Bilayer Structure Forming Neutral Carbamic Acid in Water without Hydration
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DOI：
10.1021/jacs.7b01049
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发表时间：
2017-04-05
影响因子：
15
通讯作者：
Mukai, Chisato
中科院分区：
文献类型：
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作者：
Inagaki, Fuyuhiko;Matsumoto, Chiaki;Mukai, Chisato
排放气体和空气不仅含有CO2，而且含有大量的水分，使得难以在不水合的情况下实现选择性CO2吸收。为了在加热下产生吸收的CO2（湿CO2），需要外部能量来释放吸收的水已经是二氧化碳捕获和储存（CCS）和直接空气捕获（DAC）领域中最严重的问题之一。研究发现，在CO2吸收剂的烷基胺中引入疏水性的苯基基团，提高了CO2和水的吸收选择性。此外，邻-，Meta-和对-苯二甲基二胺（OXDA，MXDA，PXDA，分别）吸收空气中的CO2没有任何水合作用。值得注意的是，即使在水中，MXDA中心点CO2也以无水氨基甲酸形式形成，可能是因为它被疏水苯基覆盖，这诱导了反向脂质双层结构。通过在103-120摄氏度下加热MXDA中心点CO2获得干燥CO2，这表明在化学上涉及格氏反应以高产率形成所得羧酸。
Emission gas and air contain not only CO2 but also, plentiful moisture, making it difficult to achieve selective CO2 absorption without hydration. To generate absorbed CO2 (wet CO2) under heating, the need for external energy to release the absorbed water has been among the most serious problems in the fields of carbon dioxide capture and storage (CCS) and direct air capture (DAC). We found that the introduction of the hydrophobic phenyl group into alkylamines of CO2 absorbents improved the absorption selectivity between CO2 and water. Furthermore, ortho-, meta-, and para-xylylenediamines (OXDA, MXDA, PXDA, respectively) absorbed only CO2 in air without any hydration. Notably, MXDA center dot CO2 was formed as an anhydrous carbamic acid even in water, presumably because it was covered with hydrophobic phenyl groups, which induces a reverse lipid bilayer structure. Dry CO2 was obtained from heating MXDA center dot CO2 at 103-120 degrees C, which was revealed to involve chemically the Grignard reaction to form the resulting carboxylic acids in high yields.