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Hydrocarbon Separations in a Metal-Organic Framework with Open Iron(II) Coordination Sites

Eric D. BlochDepartment of Chemistry, University of California, Berkeley, CA 94720, USAWendy L. QueenCenter for Neutron Research, National Institute of Standards and Technology, Gaithersburg, MD 20899, USARajamani KrishnaVan’t Hoff Institute for Molecular Sciences, University of Amsterdam, Science Park 904, 1098 XH Amsterdam, NetherlandsJoseph M. ZadroznyDepartment of Chemistry, University of California, Berkeley, CA 94720, USACraig M. BrownCenter for Neutron Research, National Institute of Standards and Technology, Gaithersburg, MD 20899, USAJeffrey R. LongDepartment of Chemistry, University of California, Berkeley, CA 94720, USA

2012en

ABI

Annotatsiya

The energy costs associated with large-scale industrial separation of light hydrocarbons by cryogenic distillation could potentially be lowered through development of selective solid adsorbents that operate at higher temperatures. Here, the metal-organic framework Fe(2)(dobdc) (dobdc(4-) : 2,5-dioxido-1,4-benzenedicarboxylate) is demonstrated to exhibit excellent performance characteristics for separation of ethylene/ethane and propylene/propane mixtures at 318 kelvin. Breakthrough data obtained for these mixtures provide experimental validation of simulations, which in turn predict high selectivities and capacities of this material for the fractionation of methane/ethane/ethylene/acetylene mixtures, removal of acetylene impurities from ethylene, and membrane-based olefin/paraffin separations. Neutron powder diffraction data confirm a side-on coordination of acetylene, ethylene, and propylene at the iron(II) centers, while also providing solid-state structural characterization of the much weaker interactions of ethane and propane with the metal.

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Identifikatorlar

DOI: 10.1126/science.1217544

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