title: Destruction of chemical warfare agents using metal-organic frameworks.
abstract: Chemical warfare agents containing phosphonate ester bonds are among the most toxic chemicals known to mankind. Recent global military events, such as the conflict and disarmament in Syria, have brought into focus the need to find effective strategies for the rapid destruction of these banned chemicals. Solutions are needed for immediate personal protection (for example, the filtration and catalytic destruction of airborne versions of agents), bulk destruction of chemical weapon stockpiles, protection (via coating) of clothing, equipment and buildings, and containment of agent spills. Solid heterogeneous materials such as modified activated carbon or metal oxides exhibit many desirable characteristics for the destruction of chemical warfare agents. However, low sorptive capacities, low effective active site loadings, deactivation of the active site, slow degradation kinetics, and/or a lack of tailorability offer significant room for improvement in these materials. Here, we report a carefully chosen metal-organic framework (MOF) material featuring high porosity and exceptional chemical stability that is extraordinarily effective for the degradation of nerve agents and their simulants. Experimental and computational evidence points to Lewis-acidic Zr(IV) ions as the active sites and to their superb accessibility as a defining element of their efficacy.
authors.affiliation: Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, USA.
authors.forename: Joseph E
authors.initials: JE
authors.lastname: Mondloch
authors.affiliation: Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, USA.
authors.forename: Michael J
authors.initials: MJ
authors.lastname: Katz
authors.affiliation: Department of Chemistry, Supercomputing Institute, and Chemical Theory Center, University of Minnesota, Minneapolis, Minnesota 55455, USA.
authors.forename: William C
authors.initials: WC
authors.lastname: Isley
authors.affiliation: Department of Chemical &Biological Engineering, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, USA.
authors.forename: Pritha
authors.initials: P
authors.lastname: Ghosh
authors.affiliation: Department of Chemical &Biological Engineering, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, USA.
authors.forename: Peilin
authors.initials: P
authors.lastname: Liao
authors.affiliation: Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, USA.
authors.forename: Wojciech
authors.initials: W
authors.lastname: Bury
authors.affiliation: Edgewood Chemical Biological Center, US Army Research, Development, and Engineering Command, 5183 Blackhawk Road, Aberdeen Proving Ground, Maryland 21010, USA.
authors.forename: George W
authors.initials: GW
authors.lastname: Wagner
authors.affiliation: Edgewood Chemical Biological Center, US Army Research, Development, and Engineering Command, 5183 Blackhawk Road, Aberdeen Proving Ground, Maryland 21010, USA.
authors.forename: Morgan G
authors.initials: MG
authors.lastname: Hall
authors.affiliation: Leidos Inc., PO Box 68 Gunpowder, Maryland 21010, USA.
authors.forename: Jared B
authors.initials: JB
authors.lastname: DeCoste
authors.affiliation: Edgewood Chemical Biological Center, US Army Research, Development, and Engineering Command, 5183 Blackhawk Road, Aberdeen Proving Ground, Maryland 21010, USA.
authors.forename: Gregory W
authors.initials: GW
authors.lastname: Peterson
authors.affiliation: Department of Chemical &Biological Engineering, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, USA.
authors.forename: Randall Q
authors.initials: RQ
authors.lastname: Snurr
authors.affiliation: Department of Chemistry, Supercomputing Institute, and Chemical Theory Center, University of Minnesota, Minneapolis, Minnesota 55455, USA.
authors.forename: Christopher J
authors.initials: CJ
authors.lastname: Cramer
authors.affiliation: Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, USA.
authors.forename: Joseph T
authors.initials: JT
authors.lastname: Hupp
authors.affiliation: 1] Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, Illinois 60208, USA [2] Department of Chemistry, Faculty of Science, King Abdulaziz University, Jeddah 21589, Saudi Arabia.
authors.forename: Omar K
authors.initials: OK
authors.lastname: Farha