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 journalArticlepeer-review

37 Citations (SciVal)

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 languageEnglish
Pages (from-to)6586-6592
Number of pages7
JournalJournal of the American Chemical Society
Volume143
Issue number17
Early online date22 Apr 2021
DOIs
Publication statusPublished - 5 May 2021

Bibliographical note

Funding Information:
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.

Publisher Copyright:
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ASJC Scopus subject areas

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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