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dc.contributor.authorSavage, Mathew
dc.contributor.authorda Silva, Ivan
dc.contributor.authorJohnson, Mark
dc.contributor.authorCarter, Joseph H.
dc.contributor.authorNewby, Ruth
dc.contributor.authorSuetin, Mikhail
dc.contributor.authorBesley, Elena
dc.contributor.authorManuel, Pascal
dc.contributor.authorRudić, Svemir
dc.contributor.authorFitch, Andrew N.
dc.contributor.authorMurray, Claire
dc.contributor.authorDavid, William I. F.
dc.contributor.authorYang, Sihai
dc.contributor.authorSchröder, Martin
dc.date.accessioned2016-08-29T05:45:24Z
dc.date.available2016-08-29T05:45:24Z
dc.date.issued2016-07-27
dc.identifier.citationObservation of Binding and Rotation of Methane and Hydrogen within a Functional Metal–Organic Framework 2016, 138 (29):9119 Journal of the American Chemical Society
dc.identifier.issn0002-7863
dc.identifier.issn1520-5126
dc.identifier.doi10.1021/jacs.6b01323
dc.identifier.urihttp://hdl.handle.net/10754/618996
dc.description.abstractThe key requirement for a portable store of natural gas is to maximize the amount of gas within the smallest possible space. The packing of methane (CH4) in a given storage medium at the highest possible density is, therefore, a highly desirable but challenging target. We report a microporous hydroxyl-decorated material, MFM-300(In) (MFM = Manchester Framework Material, replacing the NOTT designation), which displays a high volumetric uptake of 202 v/v at 298 K and 35 bar for CH4 and 488 v/v at 77 K and 20 bar for H2. Direct observation and quantification of the location, binding, and rotational modes of adsorbed CH4 and H2 molecules within this host have been achieved, using neutron diffraction and inelastic neutron scattering experiments, coupled with density functional theory (DFT) modeling. These complementary techniques reveal a very efficient packing of H2 and CH4 molecules within MFM-300(In), reminiscent of the condensed gas in pure component crystalline solids. We also report here, for the first time, the experimental observation of a direct binding interaction between adsorbed CH4 molecules and the hydroxyl groups within the pore of a material. This is different from the arrangement found in CH4/water clathrates, the CH4 store of nature.
dc.description.sponsorshipWe thank the Universities of Manchester and Nottingham for funding. M.S. acknowledges receipt of an EPSRC Program Grant and ERC Advanced Grant. E.B. acknowledges receipt of an ERC Starter Grant. We are especially grateful to STFC and the ISIS Facility for access to TOSCA and WISH Beamlines, to Diamond Light Source for access to Beamline I11, and to the European Synchrotron Radiation Facility for access to Beamline ID31. INS simulations were carried out using the high performance computing resources at the ILL.
dc.language.isoen
dc.publisherAmerican Chemical Society (ACS)
dc.relation.urlhttp://pubs.acs.org/doi/abs/10.1021/jacs.6b01323
dc.rightsThis is an open access article published under a Creative Commons Attribution (CC-BY) License, which permits unrestricted use, distribution and reproduction in any medium, provided the author and source are cited. http://pubs.acs.org/page/policy/authorchoice_ccby_termsofuse.html
dc.titleObservation of Binding and Rotation of Methane and Hydrogen within a Functional Metal–Organic Framework
dc.typeArticle
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Division
dc.identifier.journalJournal of the American Chemical Society
dc.eprint.versionPublisher's Version/PDF
dc.contributor.institutionSchool of Chemistry, University of Manchester, Oxford Road, Manchester M13 9PL, United Kingdom
dc.contributor.institutionISIS Facility, STFC Rutherford Appleton Laboratory, Chilton, Oxfordshire OX11 0QX, United Kingdom
dc.contributor.institutionILL Neutron Facility, Grenoble 38043, France
dc.contributor.institutionSchool of Chemistry, University of Nottingham, University Park, Nottingham NG7 2RD, United Kingdom
dc.contributor.institutionEuropean Synchrotron Radiation Facility, Grenoble 38043, France
dc.contributor.institutionDiamond Light Source, Harwell Science Campus, Oxfordshire OX11 0DE, United Kingdom
dc.contributor.affiliationKing Abdullah University of Science and Technology (KAUST)
kaust.personSuetin, Mikhail
dc.relation.isSupplementedBySavage, M., Da Silva, I., Johnson, M., Carter, J. H., Newby, R., Suyetin, M., … Schröder, M. (2016). CCDC 1043464: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc140t43
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dc.relation.isSupplementedBySavage, M., Da Silva, I., Johnson, M., Carter, J. H., Newby, R., Suyetin, M., … Schröder, M. (2016). CCDC 1043465: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc140t54
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dc.relation.isSupplementedBySavage, M., Da Silva, I., Johnson, M., Carter, J. H., Newby, R., Suyetin, M., … Schröder, M. (2016). CCDC 1043466: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc140t65
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dc.relation.isSupplementedBySavage, M., Da Silva, I., Johnson, M., Carter, J. H., Newby, R., Suyetin, M., … Schröder, M. (2016). CCDC 1043467: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc140t76
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dc.relation.isSupplementedBySavage, M., Da Silva, I., Johnson, M., Carter, J. H., Newby, R., Suyetin, M., … Schröder, M. (2016). CCDC 1440038: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc1kbgv6
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dc.relation.isSupplementedBySavage, M., Da Silva, I., Johnson, M., Carter, J. H., Newby, R., Suyetin, M., … Schröder, M. (2016). CCDC 1440039: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc1kbgw7
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dc.relation.isSupplementedBySavage, M., Da Silva, I., Johnson, M., Carter, J. H., Newby, R., Suyetin, M., … Schröder, M. (2016). CCDC 1440040: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc1kbgx8
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dc.relation.isSupplementedBySavage, M., Da Silva, I., Johnson, M., Carter, J. H., Newby, R., Suyetin, M., … Schröder, M. (2016). CCDC 1440041: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc1kbgy9
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dc.relation.isSupplementedBySavage, M., Da Silva, I., Johnson, M., Carter, J. H., Newby, R., Suyetin, M., … Schröder, M. (2016). CCDC 1440042: Experimental Crystal Structure Determination [Data set]. Cambridge Crystallographic Data Centre. https://doi.org/10.5517/ccdc.csd.cc1kbgzb
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refterms.dateFOA2018-06-13T12:05:37Z


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