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Water-Enhanced Direct Air Capture of Carbon Dioxide in Metal–Organic Frameworks
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2024-01-18 , DOI: 10.1021/jacs.3c14125
Oscar Iu-Fan Chen 1, 2 , Cheng-Hsin Liu 1, 2 , Kaiyu Wang 1, 2 , Emilio Borrego-Marin 3 , Haozhe Li 1, 2 , Ali H Alawadhi 1, 2 , Jorge A R Navarro 3 , Omar M Yaghi 1, 2, 4
Affiliation  

We have developed two series of amine-functionalized zirconium (Zr) metal–organic framework-808 (MOF-808), which were produced by postsynthetic modifications to have either amino acids coordinated to Zr ions (MOF-808-AAs) or polyamines covalently bound to the chloro-functionalized structure (MOF-808-PAs). These MOF variants were comprehensively characterized by liquid-state 1H nuclear magnetic resonance (NMR) measurements and potentiometric acid–base titration to determine the amounts of amines, energy-dispersive X-ray spectroscopy to assess the extent of covalent substitution by polyamines, powder X-ray diffraction analysis to verify the maintenance of the MOF crystallinity and structure after postsynthetic modifications, nitrogen sorption isotherm measurements to confirm retention of the porosity, and water sorption isotherm measurements to find the water uptake in the pores of each member of the series. Evaluation and testing of these compounds in direct air capture (DAC) of CO2 showed improved CO2 capture performance for the functionalized forms, especially under humid conditions: In dry conditions, the l-lysine- and tris(3-aminopropyl)amine-functionalized variants, termed as MOF-808-Lys and MOF-808-TAPA, exhibited the highest CO2 uptakes at 400 ppm, measuring 0.612 and 0.498 mmol g–1, and further capacity enhancement was achieved by introducing 50% relative humidity, resulting in remarkable uptakes of 1.205 and 0.872 mmol g–1 corresponding to 97 and 75% increase compared to the dry uptakes, respectively. The mechanism underlying the enhanced uptake efficiency was revealed by 13C solid-state NMR and temperature-programmed desorption measurements, indicating the formation of bicarbonate species, and therefore a stoichiometry of 1:1 CO2 to each amine site.

中文翻译:


水增强金属有机框架中二氧化碳的直接空气捕获



我们开发了两个系列的胺官能化锆(Zr)金属有机骨架-808(MOF-808),它们是通过合成后修饰产生的,使氨基酸与Zr离子配位(MOF-808-AAs)或多胺共价与氯官能化结构 (MOF-808-PA) 结合。通过液态1 H 核磁共振 (NMR) 测量和电位酸碱滴定法对这些 MOF 变体进行了全面表征,以确定胺的含量,通过能量色散 X 射线光谱法评估多胺的共价取代程度,粉末X 射线衍射分析用于验证 MOF 结晶度和结构在后合成修饰后的保持情况,氮吸附等温线测量用于确认孔隙率的保留,水吸附等温线测量用于确定该系列每个成员的孔中的吸水量。对这些化合物在 CO 2的直接空气捕获 (DAC) 中的评估和测试表明,功能化形式的 CO 2捕获性能得到改善,特别是在潮湿条件下:在干燥条件下, l -赖氨酸-和三(3-氨基丙基)胺-称为 MOF-808-Lys 和 MOF-808-TAPA 的功能化变体在 400 ppm 时表现出最高的 CO 2吸收量,测量值分别为 0.612 和 0.498 mmol g –1 ,并且通过引入 50% 相对湿度实现了进一步的容量增强,从而产生显着的吸收量为 1.205 和 0.872 mmol g –1 ,与干吸收相比分别增加了 97% 和 75%。 13 C固态NMR和程序升温解吸测量揭示了吸收效率增强的机制,表明形成了碳酸氢盐物质,因此每个胺位点的化学计量为1:1 CO 2
更新日期:2024-01-18
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