Reference : Selective Binding of O2 over N2 in a Redox-Active Metal-Organic Framework with Open Iron...
Scientific journals : Article
Physical, chemical, mathematical & earth Sciences : Chemistry
http://hdl.handle.net/2268/128434
Selective Binding of O2 over N2 in a Redox-Active Metal-Organic Framework with Open Iron(II) Coordination Sites
English
[en] Liaison préférentielle de O2 sur N2 dans un réseau métal-organique actif en redox avec des sites ouverts de coordination de fer(II).
Bloch, Eric [Berkeley University of California - UC Berkeley > Chemistry > > >]
Murray, Leslie [Berkeley University of California - UC Berkeley > Chemistry > > >]
Queen, Wendy [NIST > > > >]
Chavan, S []
Maximoff, Sergei [Berkeley University of California - UC Berkeley > Chemistry > > >]
Bigi, J [Berkeley University of California - UC Berkeley > Chemistry > > >]
Krishna, R []
Peterson, V []
Grandjean, Fernande mailto [Université de Liège - ULg > Département de physique > Département de physique >]
Long, Gary J mailto [Missouri University of Science and Technology > Chemistry > > >]
Smit, B []
Bordiga, S []
Brown, C []
Long, Jeffrey R. [Berkeley University of California - UC Berkeley > Chemistry > > >]
2011
Journal of the American Chemical Society
American Chemical Society
133
14814-14822
Yes (verified by ORBi)
International
0002-7863
1520-5126
Washington
DC
[en] neutron diffraction ; Mossbauer spectroscopy ; x-ray diffraction
[en] The air-free reaction of FeCl2 and H4dobdc (dobdc4- = 2,5-dioxido-1,4- benzenedicarboxylate) in a mixture of DMF and methanol affords Fe2(dobdc), a metal-organic framework isostructural to M2(dobdc) (M = Mg2+, Mn2+, Co2+, Ni2+, Zn2+). The desolvated form of this material has a BET surface area of 1360 m2/g and features 1-D hexagonal pores lined with coordinatively unsaturated Fe2+ cations. O2 adsorption isotherms indicate Fe2(dobdc) irreversibly binds oxygen at 298 K at a capacity over 0.10 mass fraction, corresponding to the adsorption of one O2 molecule per two framework Fe2+ cations. Remarkably, O2 uptake is reversible and the capacity increases two-fold to 0.19 mass fraction at 211 K. Powder neutron diffraction and IR spectroscopy indicate that in both scenarios O2 is coordinated side-on to the iron centers as superoxide at low temperatures and peroxide at room temperature, an observation that is confirmed by Mössbauer spectroscopy. Ideal adsorbed solution theory calculations reveal that Fe2(dobdc) is a promising material for the separation of O2 from air at temperatures well above those currently used in industrial settings.
Researchers
http://hdl.handle.net/2268/128434

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