Observation of Binding and Rotation of Methane and Hydrogen within a Functional Metal–Organic Framework

Handle URI:
http://hdl.handle.net/10754/618996
Title:
Observation of Binding and Rotation of Methane and Hydrogen within a Functional Metal–Organic Framework
Authors:
Savage, Mathew; da Silva, Ivan; Johnson, Mark; Carter, Joseph H.; Newby, Ruth; Suetin, Mikhail ( 0000-0002-4570-8905 ) ; Besley, Elena; Manuel, Pascal; Rudić, Svemir; Fitch, Andrew N.; Murray, Claire; David, William I. F.; Yang, Sihai; Schröder, Martin
Abstract:
The 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.
KAUST Department:
Physical Sciences and Engineering (PSE) Division
Citation:
Observation of Binding and Rotation of Methane and Hydrogen within a Functional Metal–Organic Framework 2016, 138 (29):9119 Journal of the American Chemical Society
Publisher:
American Chemical Society (ACS)
Journal:
Journal of the American Chemical Society
Issue Date:
27-Jul-2016
DOI:
10.1021/jacs.6b01323
Type:
Article
ISSN:
0002-7863; 1520-5126
Sponsors:
We 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.
Is Supplemented By:
Savage, 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; DOI:10.5517/ccdc.csd.cc140t43; HANDLE:http://hdl.handle.net/10754/624497; Savage, 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; DOI:10.5517/ccdc.csd.cc140t54; HANDLE:http://hdl.handle.net/10754/624498; Savage, 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; DOI:10.5517/ccdc.csd.cc140t65; HANDLE:http://hdl.handle.net/10754/624499; Savage, 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; DOI:10.5517/ccdc.csd.cc140t76; HANDLE:http://hdl.handle.net/10754/624500; Savage, 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; DOI:10.5517/ccdc.csd.cc1kbgv6; HANDLE:http://hdl.handle.net/10754/624540; Savage, 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; DOI:10.5517/ccdc.csd.cc1kbgw7; HANDLE:http://hdl.handle.net/10754/624541; Savage, 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; DOI:10.5517/ccdc.csd.cc1kbgx8; HANDLE:http://hdl.handle.net/10754/624542; Savage, 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; DOI:10.5517/ccdc.csd.cc1kbgy9; HANDLE:http://hdl.handle.net/10754/624543; Savage, 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; DOI:10.5517/ccdc.csd.cc1kbgzb; HANDLE:http://hdl.handle.net/10754/624544
Additional Links:
http://pubs.acs.org/doi/abs/10.1021/jacs.6b01323
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Articles

Full metadata record

DC FieldValue Language
dc.contributor.authorSavage, Mathewen
dc.contributor.authorda Silva, Ivanen
dc.contributor.authorJohnson, Marken
dc.contributor.authorCarter, Joseph H.en
dc.contributor.authorNewby, Ruthen
dc.contributor.authorSuetin, Mikhailen
dc.contributor.authorBesley, Elenaen
dc.contributor.authorManuel, Pascalen
dc.contributor.authorRudić, Svemiren
dc.contributor.authorFitch, Andrew N.en
dc.contributor.authorMurray, Claireen
dc.contributor.authorDavid, William I. F.en
dc.contributor.authorYang, Sihaien
dc.contributor.authorSchröder, Martinen
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 Societyen
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.en
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.en
dc.language.isoenen
dc.publisherAmerican Chemical Society (ACS)en
dc.relation.urlhttp://pubs.acs.org/doi/abs/10.1021/jacs.6b01323en
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.htmlen
dc.titleObservation of Binding and Rotation of Methane and Hydrogen within a Functional Metal–Organic Frameworken
dc.typeArticleen
dc.contributor.departmentPhysical Sciences and Engineering (PSE) Divisionen
dc.identifier.journalJournal of the American Chemical Societyen
dc.eprint.versionPublisher's Version/PDFen
dc.contributor.institutionSchool of Chemistry, University of Manchester, Oxford Road, Manchester M13 9PL, United Kingdomen
dc.contributor.institutionISIS Facility, STFC Rutherford Appleton Laboratory, Chilton, Oxfordshire OX11 0QX, United Kingdomen
dc.contributor.institutionILL Neutron Facility, Grenoble 38043, Franceen
dc.contributor.institutionSchool of Chemistry, University of Nottingham, University Park, Nottingham NG7 2RD, United Kingdomen
dc.contributor.institutionEuropean Synchrotron Radiation Facility, Grenoble 38043, Franceen
dc.contributor.institutionDiamond Light Source, Harwell Science Campus, Oxfordshire OX11 0DE, United Kingdomen
dc.contributor.affiliationKing Abdullah University of Science and Technology (KAUST)en
kaust.authorSuetin, Mikhailen
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