The first example of commensurate adsorption of atomic gas in a MOF and effective separation of xenon from other noble gases

In industry, cryogenic rectification for separating xenon from other noble gases such as krypton and argon is an energy and capital intensive process. Here we show that a microporous metal–organic framework, namely Co3(HCOO)6 is capable of effective capture and separation of xenon from other noble gases. Henry's constant, isosteric heat of adsorption (Qst), and IAST selectivity are calculated based on single component sorption isotherms. Having the highest Qst reported to date, Co3(HCOO)6 demonstrates high adsorption capacity for xenon and its IAST selectivity for Xe–Kr is the largest among all MOFs investigated to date. To mimic real world conditions, breakthrough experiments are conducted on Xe–Kr binary mixtures at room temperature and 1 atmosphere. The results are consistent with the calculated data. These findings show that Co3(HCOO)6 is a promising candidate for xenon capture and purification. Our gas adsorption measurements and molecular simulation study also reveal that the adsorption of xenon represents the first example of commensurate adsorption of atomic gases near ambient conditions.

[1]  Chad L. Staiger,et al.  Screening metal-organic frameworks for selective noble gas adsorption in air: effect of pore size and framework topology. , 2013, Physical chemistry chemical physics : PCCP.

[2]  J. Long,et al.  Selective adsorption of ethylene over ethane and propylene over propane in the metal–organic frameworks M2(dobdc) (M = Mg, Mn, Fe, Co, Ni, Zn) , 2013 .

[3]  Yamil J. Colón,et al.  High xenon/krypton selectivity in a metal-organic framework with small pores and strong adsorption sites , 2013 .

[4]  Stephen D. Burd,et al.  Porous materials with optimal adsorption thermodynamics and kinetics for CO2 separation , 2013, Nature.

[5]  Jing Li,et al.  MOFs for CO2 capture and separation from flue gas mixtures: the effect of multifunctional sites on their adsorption capacity and selectivity. , 2013, Chemical communications.

[6]  M. Hirscher,et al.  Noble gases and microporous frameworks; from interaction to application , 2012 .

[7]  P. Thallapally,et al.  Metal-organic frameworks for removal of Xe and Kr from nuclear fuel reprocessing plants. , 2012, Langmuir : the ACS journal of surfaces and colloids.

[8]  P. Thallapally,et al.  Switching Kr/Xe selectivity with temperature in a metal-organic framework. , 2012, Journal of the American Chemical Society.

[9]  Zhijuan Zhang,et al.  Experimental and theoretical investigations on the MMOF selectivity for CO2 vs. N2 in flue gas mixtures. , 2012, Dalton transactions.

[10]  Hong-Cai Zhou,et al.  Metal-organic frameworks for separations. , 2012, Chemical reviews.

[11]  Kenji Sumida,et al.  Carbon dioxide capture in metal-organic frameworks. , 2012, Chemical reviews.

[12]  J. Long,et al.  Introduction to metal-organic frameworks. , 2012, Chemical reviews.

[13]  D. Olson,et al.  Commensurate adsorption of hydrocarbons and alcohols in microporous metal organic frameworks. , 2012, Chemical reviews.

[14]  J. Grate,et al.  Facile xenon capture and release at room temperature using a metal-organic framework: a comparison with activated charcoal. , 2012, Chemical communications.

[15]  Kenji Sumida,et al.  Evaluating metal–organic frameworks for post-combustion carbon dioxide capture via temperature swing adsorption , 2011 .

[16]  Jiahui Chen,et al.  An Ideal Absorbed Solution Theory (IAST) Study of Adsorption Equilibria of Binary Mixtures of Methane and Ethane on a Templated Carbon , 2011 .

[17]  D. Ruthven,et al.  The nature of surface barriers on nanoporous solids explored by microimaging of transient guest distributions. , 2011, Journal of the American Chemical Society.

[18]  P. Wright,et al.  Xenon adsorption in synthetic chabazite zeolites , 2010 .

[19]  François-Xavier Coudert,et al.  Breathing transitions in MIL-53(Al) metal-organic framework upon xenon adsorption. , 2009, Angewandte Chemie.

[20]  Hong-Cai Zhou,et al.  Selective gas adsorption and separation in metal-organic frameworks. , 2009, Chemical Society reviews.

[21]  Alexander M. Spokoyny,et al.  Carborane-based metal-organic frameworks as highly selective sorbents for CO(2) over methane. , 2008, Chemical communications.

[22]  D. Olson,et al.  Multifunctional Microporous MOFs Exhibiting Gas/Hydrocarbon Adsorption Selectivity, Separation Capability and Three‐Dimensional Magnetic Ordering , 2008 .

[23]  Patrick Ryan,et al.  Separation of CO2 from CH4 using mixed-ligand metal-organic frameworks. , 2008, Langmuir : the ACS journal of surfaces and colloids.

[24]  D. Sholl,et al.  Examining the accuracy of ideal adsorbed solution theory without curve-fitting using transition matrix Monte Carlo simulations. , 2007, Langmuir : the ACS journal of surfaces and colloids.

[25]  Frank G. Kerry,et al.  Industrial Gas Handbook: Gas Separation and Purification , 2007 .

[26]  Jürg Hulliger,et al.  Reversible sorption of nitrogen and xenon gas by the guest-free zeolite tris(o-phenylenedioxy)cyclotriphosphazene (TPP) , 2006 .

[27]  J. Johnson,et al.  Microporous metal organic materials: promising candidates as sorbents for hydrogen storage. , 2004, Journal of the American Chemical Society.

[28]  M. Heuchel,et al.  Adsorption of CH4−CF4 Mixtures in Silicalite: Simulation, Experiment, and Theory , 1997 .

[29]  Alan R. Tait,et al.  Anesthetics as teratogens: nitrous oxide is fetotoxic, xenon is not , 1980 .

[30]  J. Marshall,et al.  A comparative histopathological study of argon and krypton laser irradiations of the human retina. , 1979, The British journal of ophthalmology.

[31]  W. Marsden.  I and J , 2012 .

[32]  T. Taffary,et al.  Atmospheric xenon radioactive isotope monitoring. , 2004, Journal of environmental radioactivity.

[33]  Alan L. Myers,et al.  Thermodynamics of mixed‐gas adsorption , 1965 .