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Modulating supramolecular binding of carbon dioxide in a redox-active porous metal-organic framework

Author

Listed:
  • Zhenzhong Lu

    (School of Chemistry, University of Manchester)

  • Harry G. W. Godfrey

    (School of Chemistry, University of Manchester)

  • Ivan da Silva

    (ISIS Facility, STFC Rutherford Appleton Laboratory)

  • Yongqiang Cheng

    (Neutron Sciences Directorate, Oak Ridge National Laboratory)

  • Mathew Savage

    (School of Chemistry, University of Manchester)

  • Floriana Tuna

    (School of Chemistry, University of Manchester)

  • Eric J. L. McInnes

    (School of Chemistry, University of Manchester)

  • Simon J. Teat

    (Advanced Light Source, Lawrence Berkeley National Laboratory)

  • Kevin J. Gagnon

    (Advanced Light Source, Lawrence Berkeley National Laboratory)

  • Mark D. Frogley

    (Diamond Light Source, Harwell Science Campus)

  • Pascal Manuel

    (ISIS Facility, STFC Rutherford Appleton Laboratory)

  • Svemir Rudić

    (ISIS Facility, STFC Rutherford Appleton Laboratory)

  • Anibal J. Ramirez-Cuesta

    (Neutron Sciences Directorate, Oak Ridge National Laboratory)

  • Timothy L. Easun

    (School of Chemistry, Cardiff University)

  • Sihai Yang

    (School of Chemistry, University of Manchester)

  • Martin Schröder

    (School of Chemistry, University of Manchester)

Abstract

Hydrogen bonds dominate many chemical and biological processes, and chemical modification enables control and modulation of host–guest systems. Here we report a targeted modification of hydrogen bonding and its effect on guest binding in redox-active materials. MFM-300(VIII) {[VIII2(OH)2(L)], LH4=biphenyl-3,3′,5,5′-tetracarboxylic acid} can be oxidized to isostructural MFM-300(VIV), [VIV2O2(L)], in which deprotonation of the bridging hydroxyl groups occurs. MFM-300(VIII) shows the second highest CO2 uptake capacity in metal-organic framework materials at 298 K and 1 bar (6.0 mmol g−1) and involves hydrogen bonding between the OH group of the host and the O-donor of CO2, which binds in an end-on manner, =1.863(1) Å. In contrast, CO2-loaded MFM-300(VIV) shows CO2 bound side-on to the oxy group and sandwiched between two phenyl groups involving a unique ···c.g.phenyl interaction [3.069(2), 3.146(3) Å]. The macroscopic packing of CO2 in the pores is directly influenced by these primary binding sites.

Suggested Citation

  • Zhenzhong Lu & Harry G. W. Godfrey & Ivan da Silva & Yongqiang Cheng & Mathew Savage & Floriana Tuna & Eric J. L. McInnes & Simon J. Teat & Kevin J. Gagnon & Mark D. Frogley & Pascal Manuel & Svemir R, 2017. "Modulating supramolecular binding of carbon dioxide in a redox-active porous metal-organic framework," Nature Communications, Nature, vol. 8(1), pages 1-10, April.
    • Handle: RePEc:nat:natcom:v:8:y:2017:i:1:d:10.1038_ncomms14212
    DOI: 10.1038/ncomms14212
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