Marsh Christopher, Han Xue, Li Jiangnan, Lu Zhenzhong, Argent Stephen P, da Silva Ivan, Cheng Yongqiang, Daemen Luke L, Ramirez-Cuesta Anibal J, Thompson Stephen P, Blake Alexander J, Yang Sihai, Schröder Martin
Department of Chemistry, University of Manchester, Manchester, M13 9PL, U.K.
School of Chemistry, University of Nottingham, Nottingham, NG7 2RD, U.K.
J Am Chem Soc. 2021 May 5;143(17):6586-6592. doi: 10.1021/jacs.1c01749. Epub 2021 Apr 22.
We report the reversible adsorption of ammonia (NH) up to 9.9 mmol g in a robust Al-based metal-organic framework, MFM-303(Al), which is functionalized with free carboxylic acid and hydroxyl groups. The unique pore environment decorated with these acidic sites results in an exceptional packing density of NH at 293 K (0.801 g cm) comparable to that of solid NH at 193 K (0.817 g cm). synchrotron X-ray diffraction and inelastic neutron scattering reveal the critical role of free -COOH and -OH groups in immobilizing NH molecules. Breakthrough experiments confirm the excellent performance of MFM-303(Al) for the capture of NH at low concentrations under both dry and wet conditions.
我们报道了在一种坚固的铝基金属有机框架MFM-303(Al)中，氨（NH₃）的可逆吸附量可达9.9 mmol g⁻¹，该框架用游离羧酸和羟基进行了功能化修饰。这些酸性位点修饰的独特孔环境导致在293 K时NH₃具有异常高的堆积密度（0.801 g cm⁻³），与193 K时固态NH₃的堆积密度（0.817 g cm⁻³）相当。同步加速器X射线衍射和非弹性中子散射揭示了游离 -COOH和 -OH基团在固定NH₃分子中的关键作用。突破实验证实了MFM-303(Al)在干燥和潮湿条件下对低浓度NH₃捕获的优异性能。
