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在坚固的铝基金属有机框架中高效捕获和储存氨。

Efficient capture and storage of ammonia in robust aluminium-based metal-organic frameworks.

作者信息

Guo Lixia, Hurd Joseph, He Meng, Lu Wanpeng, Li Jiangnan, Crawshaw Danielle, Fan Mengtian, Sapchenko Sergei, Chen Yinlin, Zeng Xiangdi, Kippax-Jones Meredydd, Huang Wenyuan, Zhu Zhaodong, Manuel Pascal, Frogley Mark D, Lee Daniel, Schröder Martin, Yang Sihai

机构信息

Department of Chemistry, University of Manchester, Manchester, M13 9PL, UK.

Department of Chemical Engineering, University of Manchester, Manchester, M13 9PL, UK.

出版信息

Commun Chem. 2023 Mar 24;6(1):55. doi: 10.1038/s42004-023-00850-4.

Abstract

The development of stable sorbent materials to deliver reversible adsorption of ammonia (NH) is a challenging task. Here, we report the efficient capture and storage of NH in a series of robust microporous aluminium-based metal-organic framework materials, namely MIL-160, CAU-10-H, Al-fum, and MIL-53(Al). In particular, MIL-160 shows high uptakes of NH of 4.8 and 12.8 mmol g at both low and high pressure (0.001 and 1.0 bar, respectively) at 298 K. The combination of in situ neutron powder diffraction, synchrotron infrared micro-spectroscopy and solid-state nuclear magnetic resonance spectroscopy reveals the preferred adsorption domains of NH molecules in MIL-160, with H/D site-exchange between the host and guest and an unusual distortion of the local structure of [AlO] moieties being observed. Dynamic breakthrough experiments confirm the excellent ability of MIL-160 to capture of NH with a dynamic uptake of 4.2 mmol g at 1000 ppm. The combination of high porosity, pore aperture size and multiple binding sites promotes the significant binding affinity and capacity for NH, which makes it a promising candidate for practical applications.

摘要

开发能够实现氨(NH₃)可逆吸附的稳定吸附剂材料是一项具有挑战性的任务。在此,我们报道了在一系列坚固的微孔铝基金属有机骨架材料(即MIL - 160、CAU - 10 - H、Al - fum和MIL - 53(Al))中对NH₃的高效捕获和存储。特别地,在298 K时,MIL - 160在低压和高压(分别为0.001和1.0 bar)下对NH₃的吸附量分别高达4.8和12.8 mmol g⁻¹。原位中子粉末衍射、同步辐射红外显微光谱和固态核磁共振光谱相结合,揭示了MIL - 160中NH₃分子的优先吸附域,观察到主体与客体之间的H/D位点交换以及[AlO₄]部分局部结构的异常畸变。动态突破实验证实了MIL - 160在1000 ppm下对NH₃的捕获能力极佳,动态吸附量为4.2 mmol g⁻¹。高孔隙率、孔径大小和多个结合位点的结合促进了对NH₃的显著结合亲和力和容量,这使其成为实际应用中有前景的候选材料。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c4a1/10039057/5de2e8c7a851/42004_2023_850_Fig1_HTML.jpg

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