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    Theoretical Investigations of CO 2 and H 2 Sorption in an Interpenetrated Square-Pillared Metal–Organic Material

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    Type
    Article
    Authors
    Pham, Tony
    Forrest, Katherine A.
    McLaughlin, Keith
    Tudor, Brant
    Nugent, Patrick
    Hogan, Adam
    Mullen, Ashley
    Cioce, Christian R.
    Zaworotko, Michael J.
    Space, Brian
    KAUST Grant Number
    FIC/2010/06
    Date
    2013-05-06
    Online Publication Date
    2013-05-06
    Print Publication Date
    2013-05-16
    Permanent link to this record
    http://hdl.handle.net/10754/599983
    
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    Abstract
    Simulations of CO2 and H2 sorption and separation were performed in [Cu(dpa)2SiF6-i], a metal-organic material (MOM) consisting of an interpenetrated square grid of Cu2+ ions coordinated to 4,4′-dipyridylacetylene (dpa) rings and pillars of SiF6 2- ions. This class of water stable MOMs shows great promise in practical gas sorption/separation with especially high selectivity for CO2 and variable selectivity for other energy related gases. Simulated CO2 sorption isotherms and isosteric heats of adsorption, Qst, at ambient temperatures were in excellent agreement with the experimental measurements at all pressures considered. Further, it was observed that the Qst for CO2 increases as a function of uptake in [Cu(dpa)2SiF6-i]. This suggests that nascently sorbed CO2 molecules within a channel contribute to a more energetically favorable site for additional CO2 molecules, i.e., in stark contrast to typical behavior, sorbate intermolecular interactions enhance sorption energetics with increased loading. The simulated structure at CO2 saturation shows a loading with tight packing of 8 CO2 molecules per unit cell. The CO2 molecules can be seen alternating between a vertical and horizontal alignment within a channel, with each CO2 molecule coordinating to an equatorial fluorine MOM atom. Calculated H 2 sorption isotherms and Qst values were also in good agreement with the experimental measurements in [Cu(dpa)2SiF 6-i]. H2 saturation corresponds to 10 H2 molecules per unit cell for the studied structure. Moreover, there were two observed binding sites for hydrogen sorption in [Cu(dpa)2SiF 6-i]. Simulations of a 30:70 CO2/H2 mixture, typical of syngas, in [Cu(dpa)2SiF6-i] showed that the MOM exhibited a high uptake and selectivity for CO2. In addition, it was observed that the presence of H2O had a negligible effect on the CO2 uptake and selectivity in [Cu(dpa)2SiF6-i], as simulations of a mixture containing CO2, H2, and small amounts of CO, N2, and H2O produced comparable results to the binary mixture simulations. © 2013 American Chemical Society.
    Citation
    Pham T, Forrest KA, McLaughlin K, Tudor B, Nugent P, et al. (2013) Theoretical Investigations of CO 2 and H 2 Sorption in an Interpenetrated Square-Pillared Metal–Organic Material . The Journal of Physical Chemistry C 117: 9970–9982. Available: http://dx.doi.org/10.1021/jp402764s.
    Sponsors
    This work was supported by the National Science Foundation (Award No. CHE-1152362). Computations were performed under a XSEDE Grant (No. TG-DMR090028) to B.S. This publication is also based on work supported by Award No. FIC/2010/06, made by King Abdullah University of Science and Technology (KAUST). The authors also thank the Space Foundation (Basic and Applied Research) for partial support. The authors would like to acknowledge the use of the services provided by Research Computing at the University of South Florida.
    Publisher
    American Chemical Society (ACS)
    Journal
    The Journal of Physical Chemistry C
    DOI
    10.1021/jp402764s
    ae974a485f413a2113503eed53cd6c53
    10.1021/jp402764s
    Scopus Count
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