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] polyoxonio...

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Autores principales:	Qi Wang, Robert C. Chapleski, Anna M. Plonka, Wesley O. Gordon, Weiwei Guo, Thuy-Duong Nguyen-Phan, Conor H. Sharp, Nebojsa S. Marinkovic, Sanjaya D. Senanayake, John R. Morris, Craig L. Hill, Diego Troya, Anatoly I. Frenkel
Formato:	article
Lenguaje:	EN
Publicado:	Nature Portfolio 2017
Materias:	Medicine R Science Q
Acceso en línea:	https://doaj.org/article/16b8a132825d464d9a8b54a360957962
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spelling	oai:doaj.org-article:16b8a132825d464d9a8b54a3609579622021-12-02T16:07:44ZAtomic-Level Structural Dynamics of Polyoxoniobates during DMMP Decomposition10.1038/s41598-017-00772-x2045-2322https://doaj.org/article/16b8a132825d464d9a8b54a3609579622017-04-01T00:00:00Zhttps://doi.org/10.1038/s41598-017-00772-xhttps://doaj.org/toc/2045-2322Abstract 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.Qi WangRobert C. ChapleskiAnna M. PlonkaWesley O. GordonWeiwei GuoThuy-Duong Nguyen-PhanConor H. SharpNebojsa S. MarinkovicSanjaya D. SenanayakeJohn R. MorrisCraig L. HillDiego TroyaAnatoly I. FrenkelNature PortfolioarticleMedicineRScienceQENScientific Reports, Vol 7, Iss 1, Pp 1-8 (2017)
institution	DOAJ
collection	DOAJ
language	EN
topic	Medicine R Science Q
spellingShingle	Medicine R Science Q Qi Wang Robert C. Chapleski Anna M. Plonka Wesley O. Gordon Weiwei Guo Thuy-Duong Nguyen-Phan Conor H. Sharp Nebojsa S. Marinkovic Sanjaya D. Senanayake John R. Morris Craig L. Hill Diego Troya Anatoly I. Frenkel Atomic-Level Structural Dynamics of Polyoxoniobates during DMMP Decomposition
description	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.
format	article
author	Qi Wang Robert C. Chapleski Anna M. Plonka Wesley O. Gordon Weiwei Guo Thuy-Duong Nguyen-Phan Conor H. Sharp Nebojsa S. Marinkovic Sanjaya D. Senanayake John R. Morris Craig L. Hill Diego Troya Anatoly I. Frenkel
author_facet	Qi Wang Robert C. Chapleski Anna M. Plonka Wesley O. Gordon Weiwei Guo Thuy-Duong Nguyen-Phan Conor H. Sharp Nebojsa S. Marinkovic Sanjaya D. Senanayake John R. Morris Craig L. Hill Diego Troya Anatoly I. Frenkel
author_sort	Qi Wang
title	Atomic-Level Structural Dynamics of Polyoxoniobates during DMMP Decomposition
title_short	Atomic-Level Structural Dynamics of Polyoxoniobates during DMMP Decomposition
title_full	Atomic-Level Structural Dynamics of Polyoxoniobates during DMMP Decomposition
title_fullStr	Atomic-Level Structural Dynamics of Polyoxoniobates during DMMP Decomposition
title_full_unstemmed	Atomic-Level Structural Dynamics of Polyoxoniobates during DMMP Decomposition
title_sort	atomic-level structural dynamics of polyoxoniobates during dmmp decomposition
publisher	Nature Portfolio
publishDate	2017
url	https://doaj.org/article/16b8a132825d464d9a8b54a360957962
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Atomic-Level Structural Dynamics of Polyoxoniobates during DMMP Decomposition

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