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

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 Rudić, Anibal J. Ramirez-Cuesta, Timothy L. Easun, Sihai Yang () and Martin Schröder ()
Additional contact information
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

Nature Communications, 2017, vol. 8, issue 1, 1-10

Abstract: 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.

Date: 2017
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DOI: 10.1038/ncomms14212

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