Atomic-Level Structural Dynamics of Polyoxoniobates during DMMP Decomposition
Abstract
Ambient pressure in situ synchrotron-based spectroscopic techniques have been correlated to illuminate atomic-level details of bond breaking and formation during the hydrolysis of a chemical warfare nerve agent simulant over a polyoxometalate catalyst. Specifically, a Cs8[Nb6O19] polyoxoniobate catalyst has been shown to react readily with dimethyl methylphosphonate (DMMP). The atomic-level transformations of all reactant moieties, the [Nb6O19]8- polyanion, its Cs+ counterions, and the DMMP substrate, were tracked under ambient conditions by a combination of X-ray absorption fine structure spectroscopy, Raman spectroscopy, and X-ray diffraction. Results reveal that the reaction mechanism follows general base (in contrast to specific base) hydrolysis. Together with computational results, the work demonstrates that the ultimate fate of DMMP hydrolysis at the Cs8[Nb6O19] catalyst is strong binding of the (methyl) methylphosphonic acid ((M)MPA) product to the polyanions, which ultimately inhibits catalytic turnover.
- Authors:
-
[2];
- Stony Brook Univ., NY (United States)
- Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
- U.S. Army Edgewood Chemical Biological Center, APG, MD (United States)
- Emory Univ., Atlanta, GA (United States)
- Brookhaven National Lab. (BNL), Upton, NY (United States)
- Columbia Univ., New York, NY (United States)
- Publication Date:
- Research Org.:
- Brookhaven National Laboratory (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States); Emory Univ., Atlanta, GA (United States); Virginia Polytechnic Inst. and State Univ. (Virginia Tech), Blacksburg, VA (United States)
- Sponsoring Org.:
- USDOE; Army Research Laboratory (ARL) (United States); US Army Research Office (ARO); Defense Threat Reduction Agency (DTRA) (United States)
- OSTI Identifier:
- 1395944
- Report Number(s):
- BNL-114371-2017-JA
Journal ID: ISSN 2045-2322; R&D Project: CO040; KC0302010
- Grant/Contract Number:
- SC0012704; AC02-06CH11357; AC02-76SF00515; W911NF-15-2-0107; BB11PHM156
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Scientific Reports
- Additional Journal Information:
- Journal Volume: 7; Journal ID: ISSN 2045-2322
- Publisher:
- Nature Publishing Group
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; catalysis; physical chemistry
Citation Formats
Wang, Qi, Chapleski, Robert C., Plonka, Anna M., Gordon, Wesley O., Guo, Weiwei, Nguyen-Phan, Thuy-Duong, Sharp, Conor H., Marinkovic, Nebojsa S., Senanayake, Sanjaya D., Morris, John R., Hill, Craig L., Troya, Diego, and Frenkel, Anatoly I. Atomic-Level Structural Dynamics of Polyoxoniobates during DMMP Decomposition. United States: N. p., 2017.
Web. doi:10.1038/s41598-017-00772-x.
Wang, Qi, Chapleski, Robert C., Plonka, Anna M., Gordon, Wesley O., Guo, Weiwei, Nguyen-Phan, Thuy-Duong, Sharp, Conor H., Marinkovic, Nebojsa S., Senanayake, Sanjaya D., Morris, John R., Hill, Craig L., Troya, Diego, & Frenkel, Anatoly I. Atomic-Level Structural Dynamics of Polyoxoniobates during DMMP Decomposition. United States. https://doi.org/10.1038/s41598-017-00772-x
Wang, Qi, Chapleski, Robert C., Plonka, Anna M., Gordon, Wesley O., Guo, Weiwei, Nguyen-Phan, Thuy-Duong, Sharp, Conor H., Marinkovic, Nebojsa S., Senanayake, Sanjaya D., Morris, John R., Hill, Craig L., Troya, Diego, and Frenkel, Anatoly I. Mon .
"Atomic-Level Structural Dynamics of Polyoxoniobates during DMMP Decomposition". United States. https://doi.org/10.1038/s41598-017-00772-x. https://www.osti.gov/servlets/purl/1395944.
@article{osti_1395944,
title = {Atomic-Level Structural Dynamics of Polyoxoniobates during DMMP Decomposition},
author = {Wang, Qi and Chapleski, Robert C. and Plonka, Anna M. and Gordon, Wesley O. and Guo, Weiwei and Nguyen-Phan, Thuy-Duong and Sharp, Conor H. and Marinkovic, Nebojsa S. and Senanayake, Sanjaya D. and Morris, John R. and Hill, Craig L. and Troya, Diego and Frenkel, Anatoly I.},
abstractNote = {Ambient pressure in situ synchrotron-based spectroscopic techniques have been correlated to illuminate atomic-level details of bond breaking and formation during the hydrolysis of a chemical warfare nerve agent simulant over a polyoxometalate catalyst. Specifically, a Cs8[Nb6O19] polyoxoniobate catalyst has been shown to react readily with dimethyl methylphosphonate (DMMP). The atomic-level transformations of all reactant moieties, the [Nb6O19]8- polyanion, its Cs+ counterions, and the DMMP substrate, were tracked under ambient conditions by a combination of X-ray absorption fine structure spectroscopy, Raman spectroscopy, and X-ray diffraction. Results reveal that the reaction mechanism follows general base (in contrast to specific base) hydrolysis. Together with computational results, the work demonstrates that the ultimate fate of DMMP hydrolysis at the Cs8[Nb6O19] catalyst is strong binding of the (methyl) methylphosphonic acid ((M)MPA) product to the polyanions, which ultimately inhibits catalytic turnover.},
doi = {10.1038/s41598-017-00772-x},
journal = {Scientific Reports},
number = ,
volume = 7,
place = {United States},
year = {Mon Apr 10 00:00:00 EDT 2017},
month = {Mon Apr 10 00:00:00 EDT 2017}
}
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