A Flexible Interpenetrated Zirconium-Based Metal–Organic Framework with High Affinity toward Ammonia

Yuanyuan Zhang, Xuan Zhang, Zhijie Chen, Ken ichi Otake, Gregory W. Peterson, Yongwei Chen, Xingjie Wang, Louis R. Redfern, Subhadip Goswami, Peng Li, Timur Islamoglu, Bo Wang, Omar K. Farha*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

40 Scopus citations

Abstract

Flexible metal–organic frameworks (MOFs) are highly attractive porous crystalline materials presenting structural changes when exposed to external stimuli, the mechanism of which is often difficult to glean, owing to their complex and dynamic nature. Herein, a flexible interpenetrated Zr-MOF, NU-1401, composed of rare 4-connected Zr6 nodes and tetratopic naphthalenediimide (NDI)-based carboxylate linkers, was designed. The intra-framework pore opening deformation and inter-framework motions, when subjected to different solvent molecules, were investigated by single-crystal XRD. The distance and overlap angle between the stacked NDI pairs in the entangled structure could be finely tuned, and the interactions between NDI and solvent molecules led to solvochromism. Furthermore, the presence of electron-deficient NDI units in the linker and acid sites on the node of the interpenetrated porous structure offered high density of adsorption sites for ammonia molecules, resulting in high uptake at low pressures.

Original languageEnglish (US)
Pages (from-to)1710-1714
Number of pages5
JournalChemSusChem
Volume13
Issue number7
DOIs
StatePublished - Apr 7 2020

Funding

O.K.F. gratefully acknowledges support from the Defense Threat Reduction Agency (HDTRA1‐19‐1‐0007). Y.Z. acknowledges support from China Scholarship Council (CSC) during her visit to Northwestern University, and Fundamental Research Funds for the Central Universities and Beijing Institute of Technology Research Fund Program. This work made use of the IMSERC at Northwestern University, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS‐1542205), the State of Illinois, and the International Institute for Nanotechnology (IIN). This work made use of the EPIC facility of Northwestern University's NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS‐1542205); the MRSEC program (NSF DMR‐1720139) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois, through the IIN. The REACT Core facility acknowledges funding from the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Catalysis Science program (DE‐FG02‐03ER15457) used for the purchase of the Nicolet 6700 FT‐IR System. G.W.P. thanks the Defense Threat Reduction Agency (CB3934) for funding the ammonia work and Matthew Browe for running ammonia breakthrough experiments. O.K.F. gratefully acknowledges support from the Defense Threat Reduction Agency (HDTRA1-19-1-0007). Y.Z. acknowledges support from China Scholarship Council (CSC) during her visit to Northwestern University, and Fundamental Research Funds for the Central Universities and Beijing Institute of Technology Research Fund Program. This work made use of the IMSERC at Northwestern University, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205), the State of Illinois, and the International Institute for Nanotechnology (IIN). This work made use of the EPIC facility of Northwestern University's NUANCE Center, which has received support from the Soft and Hybrid Nanotechnology Experimental (SHyNE) Resource (NSF ECCS-1542205); the MRSEC program (NSF DMR-1720139) at the Materials Research Center; the International Institute for Nanotechnology (IIN); the Keck Foundation; and the State of Illinois, through the IIN. The REACT Core facility acknowledges funding from the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Catalysis Science program (DE-FG02-03ER15457) used for the purchase of the Nicolet 6700 FT-IR System. G.W.P. thanks the Defense Threat Reduction Agency (CB3934) for funding the ammonia work and Matthew Browe for running ammonia breakthrough experiments.

Keywords

  • ammonia capture
  • flexible MOF
  • interpenetrated structure
  • metal–organic frameworks
  • microporous materials

ASJC Scopus subject areas

  • Environmental Chemistry
  • General Chemical Engineering
  • General Materials Science
  • General Energy

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