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

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
Journal	Journal of the American Chemical Society
Volume	143
Issue number	17
DOIs	https://doi.org/10.1021/jacs.1c01749
Publication status	Published - 22 Apr 2021

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https://pubs.acs.org/doi/10.1021/jacs.1c01749

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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.",

author = "Christopher Marsh and Xue Han and Jiangnan Li and Zhenzhong Lu and Argent, \{Stephen P.\} and \{Da Silva\}, Ivan and Yongqiang Cheng and Daemen, \{Luke L.\} and Ramirez-cuesta, \{Anibal J.\} and Thompson, \{Stephen P.\} and Blake, \{Alexander J.\} and Sihai Yang and Martin Schr{\"o}der",

year = "2021",

month = apr,

day = "22",

doi = "10.1021/jacs.1c01749",

language = "English",

volume = "143",

pages = "6586--6592",

journal = "Journal of the American Chemical Society",

issn = "0002-7863",

publisher = "American Chemical Society",

number = "17",

}

TY - JOUR

T1 - Exceptional Packing Density of Ammonia in a Dual-Functionalized Metal–Organic Framework

AU - Marsh, Christopher

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

PY - 2021/4/22

Y1 - 2021/4/22

N2 - 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.

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.

U2 - 10.1021/jacs.1c01749

DO - 10.1021/jacs.1c01749

M3 - Article

SN - 0002-7863

VL - 143

SP - 6586

EP - 6592

JO - Journal of the American Chemical Society

JF - Journal of the American Chemical Society

IS - 17

ER -

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

Abstract

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