Atomic resolution tracking of nerve-agent simulant decomposition and host metal-organic framework response in real space

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dc.contributor.authorTerban, Maxwell W.en
dc.contributor.authorGhose, Sanjit K.en
dc.contributor.authorPlonka, Anna M.en
dc.contributor.authorTroya, Diegoen
dc.contributor.authorJuhas, Pavolen
dc.contributor.authorDinnebier, Robert E.en
dc.contributor.authorMahle, John J.en
dc.contributor.authorGordon, Wesley O.en
dc.contributor.authorFrenkel, Anatoly I.en
dc.contributor.departmentChemistryen
dc.date.accessioned2021-06-07T18:37:05Zen
dc.date.available2021-06-07T18:37:05Zen
dc.date.issued2021-01-04en
dc.description.abstractGas capture and sequestration are valuable properties of metal-organic frameworks (MOFs) driving tremendous interest in their use as filtration materials for chemical warfare agents. Recently, the Zr-based MOF UiO-67 was shown to effectively adsorb and decompose the nerve-agent simulant, dimethyl methylphosphonate (DMMP). Understanding mechanisms of MOF-agent interaction is challenging due to the need to distinguish between the roles of the MOF framework and its particular sites for the activation and sequestration process. Here, we demonstrate the quantitative tracking of both framework and binding component structures using in situ X-ray total scattering measurements of UiO-67 under DMMP exposure, pair distribution function analysis, and theoretical calculations. The sorption and desorption of DMMP within the pores, association with linker-deficient Zr6 cores, and decomposition to irreversibly bound methyl methylphosphonate were directly observed and analyzed with atomic resolution. Metal-organic frameworks have been shown to adsorb and decompose chemical warfare agents, but their mechanism of action is not completely understood. Here the authors quantitatively track the binding and decomposition product structures of nerve-agent simulant dimethyl methylphosphonate in host UiO-67 through in situ X-ray total scattering measurements, pair distribution function analysis, and density functional theory calculations.en
dc.description.notesM.W.T. gratefully acknowledges support from BASF. A.M.P., D.T., and A.I.F. acknowledge support by the U.S. Army Research Office under grant number W911NF15-2-0107. J.J.M. and W.O.G. thank the Defense Threat Reduction Agency for support under program CB3587. This research used beamline 28-ID-2 of the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Brookhaven National Laboratory under Contract No. DE-SC0012704. Advanced Research Computing at Virginia Tech is gratefully acknowledged for computational resources.en
dc.description.sponsorshipBASF; U.S. Army Research Office [W911NF15-2-0107]; Defense Threat Reduction AgencyUnited States Department of DefenseDefense Threat Reduction Agency [CB3587]; DOE Office of ScienceUnited States Department of Energy (DOE) [DE-SC0012704]en
dc.description.versionPublished versionen
dc.format.mimetypeapplication/pdfen
dc.identifier.doihttps://doi.org/10.1038/s42004-020-00439-1en
dc.identifier.issn2399-3669en
dc.identifier.issue1en
dc.identifier.other2en
dc.identifier.urihttp://hdl.handle.net/10919/103659en
dc.identifier.volume4en
dc.language.isoenen
dc.rightsCreative Commons Attribution 4.0 Internationalen
dc.rights.urihttp://creativecommons.org/licenses/by/4.0/en
dc.titleAtomic resolution tracking of nerve-agent simulant decomposition and host metal-organic framework response in real spaceen
dc.title.serialCommunications Chemistryen
dc.typeArticle - Refereeden
dc.type.dcmitypeTexten
dc.type.dcmitypeStillImageen

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