Covalent Organic Frameworks for Carbon Dioxide Capture from Air
Covalent Organic Frameworks for Carbon Dioxide Capture from Air
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DOI：
10.1021/jacs.2c05382
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发表时间：
2022-07-05
影响因子：
15
通讯作者：
Yaghi, Omar M.
中科院分区：
文献类型：
--
作者：
Lyu, Hao;Li, Haozhe;Yaghi, Omar M.
摘要：我们报告了第一个将活性脂肪胺共价结合到共价有机框架（COF）中的方法。这是通过结晶亚胺连接的COF（称为COF-609-Im），然后通过氮杂-Diels-桤木环加成将其亚胺连接转化为碱稳定的四氢喹啉连接，最后将三（3-氨基丙基）胺共价结合到骨架中来实现的。与原始框架相比，所获得的COF-609表现出1360倍的CO2吸收能力增加，并且在湿度存在下进一步增强29%。我们证实了化学框架转换和证实了增强CO2吸收现象，并通过同位素标记的傅里叶变换红外光谱和固态核磁共振光谱。通过这项研究，我们建立了一种新的合成策略，以获得一类化学吸附剂，其特征在于对稀释源（如空气）中的CO2具有高亲和力。
ABSTRACT: We report the first covalent incorporation of reactive aliphatic amine species into covalent organic frameworks (COFs). This was achieved through the crystallization of an iminelinked COF, termed COF-609-Im, followed by conversion of its imine linkage to base-stable tetrahydroquinoline linkage through aza-Diels-Alder cycloaddition, and finally, the covalent incorporation of tris(3-aminopropyl)amine into the framework. The obtained COF-609 exhibits a 1360-fold increase in CO2 uptake capacity compared to the pristine framework and a further 29% enhancement in the presence of humidity. We confirmed the chemistry of framework conversion and corroborated the enhanced CO2 uptake phenomenon with and without humidity through isotope-labeled Fourier transform infrared spectroscopy and solidstate nuclear magnetic resonance spectroscopy. With this study, we established a new synthetic strategy to access a class of chemisorbents characterized by high affinity to CO2 in dilute sources, such as the air.