Exceptional Packing Density of Ammonia in a Dual-Functionalized Metal-Organic Framework

Christopher Marsh; Xue Han; Jiangnan Li; Zhenzhong Lu; Stephen P. Argent; Ivan Da Silva; Yongqiang Cheng; Luke L. Daemen; Anibal J. Ramirez-Cuesta; Stephen P. Thompson; Alexander J. Blake; Sihai Yang; Martin Schröder

doi:10.1021/jacs.1c01749

Exceptional Packing Density of Ammonia in a Dual-Functionalized Metal-Organic Framework

Christopher Marsh, Xue Han, Jiangnan Li, Zhenzhong Lu, Stephen P. Argent, Ivan Da Silva, Yongqiang Cheng, Luke L. Daemen, Anibal J. Ramirez-Cuesta, Stephen P. Thompson, Alexander J. Blake, Sihai Yang, Martin Schröder

Research output: Contribution to journal › Article › peer-review

47 Scopus citations

Abstract

We report the reversible adsorption of ammonia (NH3) up to 9.9 mmol g-1 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 NH3 at 293 K (0.801 g cm-3) comparable to that of solid NH3 at 193 K (0.817 g cm-3). In situ synchrotron X-ray diffraction and inelastic neutron scattering reveal the critical role of free-COOH and-OH groups in immobilizing NH3 molecules. Breakthrough experiments confirm the excellent performance of MFM-303(Al) for the capture of NH3 at low concentrations under both dry and wet conditions.

Original language	English
Pages (from-to)	6586-6592
Number of pages	7
Journal	Journal of the American Chemical Society
Volume	143
Issue number	17
DOIs	https://doi.org/10.1021/jacs.1c01749
State	Published - May 5 2021

Funding

We thank the EPSRC (EP/I011870), the Royal Society and the University of Manchester for funding. This project has received funding from the European Research Council (ERC) under the European Union’s Horizon 2020 research and innovation programme (grant agreement No 742401, NANOCHEM). We are grateful to Diamond Light Source for access to the beamlines I11 and I19. A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory. The computing resources were made available through the VirtuES and the ICE-MAN projects, funded by Laboratory Directed Research and Development program and Compute and Data Environment for Science (CADES) at ORNL. J.L. thanks China Scholarship Council (20160625002) for funding.

Funders	Funder number
Compute and Data Environment for Science
Laboratory Directed Research and Development
Horizon 2020 Framework Programme	742401
Engineering and Physical Sciences Research Council	EP/I011870
Royal Society
University of Manchester
European Research Council
China Scholarship Council	20160625002

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title = "Exceptional Packing Density of Ammonia in a Dual-Functionalized Metal-Organic Framework",

abstract = "We report the reversible adsorption of ammonia (NH3) up to 9.9 mmol g-1 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 NH3 at 293 K (0.801 g cm-3) comparable to that of solid NH3 at 193 K (0.817 g cm-3). In situ synchrotron X-ray diffraction and inelastic neutron scattering reveal the critical role of free-COOH and-OH groups in immobilizing NH3 molecules. Breakthrough experiments confirm the excellent performance of MFM-303(Al) for the capture of NH3 at low concentrations under both dry and wet conditions.",

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AU - Han, Xue

AU - Li, Jiangnan

AU - Lu, Zhenzhong

AU - Argent, Stephen P.

AU - Da Silva, Ivan

AU - Cheng, Yongqiang

AU - Daemen, Luke L.

AU - Ramirez-Cuesta, Anibal J.

AU - Thompson, Stephen P.

AU - Blake, Alexander J.

AU - Yang, Sihai

AU - Schröder, Martin

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AB - We report the reversible adsorption of ammonia (NH3) up to 9.9 mmol g-1 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 NH3 at 293 K (0.801 g cm-3) comparable to that of solid NH3 at 193 K (0.817 g cm-3). In situ synchrotron X-ray diffraction and inelastic neutron scattering reveal the critical role of free-COOH and-OH groups in immobilizing NH3 molecules. Breakthrough experiments confirm the excellent performance of MFM-303(Al) for the capture of NH3 at low concentrations under both dry and wet conditions.

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Exceptional Packing Density of Ammonia in a Dual-Functionalized Metal-Organic Framework

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