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Title: Influence of Background H{sub 2}O on the Collision-Induced Dissociation Products Generated from [UO{sub 2}NO{sub 3}]{sup +}

Abstract

Developing a comprehensive understanding of the reactivity of uranium-containing species remains an important goal in areas ranging from the development of nuclear fuel processing methods to studies of the migration and fate of the element in the environment. Electrospray ionization (ESI) is an effective way to generate gas-phase complexes containing uranium for subsequent studies of intrinsic structure and reactivity. Recent experiments by our group have demonstrated that the relatively low levels of residual H{sub 2}O in a 2-D, linear ion trap (LIT) make it possible to examine fragmentation pathways and reactions not observed in earlier studies conducted with 3-D ion traps (Van Stipdonk et al. J. Am. Soc. Mass Spectrom. 14, 1205–1214, 2003). In the present study, we revisited the dissociation of complexes composed of uranyl nitrate cation [U{sup VI}O{sub 2}(NO{sub 3})]{sup +} coordinated by alcohol ligands (methanol and ethanol) using the 2-D LIT. With relatively low levels of background H{sub 2}O, collision-induced dissociation (CID) of [U{sup VI}O{sub 2}(NO{sub 3})]{sup +} primarily creates [UO{sub 2}(O{sub 2})]{sup +} by the ejection of NO. However, CID (using He as collision gas) of [U{sup VI}O{sub 2}(NO{sub 3})]{sup +} creates [UO{sub 2}(H{sub 2}O)]{sup +} and UO{sub 2}{sup +} when the 2-D LIT is usedmore » with higher levels of background H{sub 2}O. Based on the results presented here, we propose that product ion spectrum in the previous experiments was the result of a two-step process: initial formation of [U{sup VI}O{sub 2}(O{sub 2})]{sup +} followed by rapid exchange of O{sub 2} for H{sub 2}O by ion-molecule reaction. Our experiments illustrate the impact of residual H{sub 2}O in ion trap instruments on the product ions generated by CID and provide a more accurate description of the intrinsic dissociation pathway for [U{sup VI}O{sub 2}(NO{sub 3})]{sup +}. .« less

Authors:
; ;  [1]
  1. Duquesne University, Department of Chemistry (United States)
Publication Date:
OSTI Identifier:
22776891
Resource Type:
Journal Article
Journal Name:
Journal of the American Society for Mass Spectrometry
Additional Journal Information:
Journal Volume: 29; Journal Issue: 7; Other Information: Copyright (c) 2018 American Society for Mass Spectrometry; http://www.springer-ny.com; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 1044-0305
Country of Publication:
United States
Language:
English
Subject:
74 ATOMIC AND MOLECULAR PHYSICS; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; DISSOCIATION; FRAGMENTATION; IONIZATION; ION-MOLECULE COLLISIONS; MASS; MASS SPECTROSCOPY; NUCLEAR FUELS; PROCESSING; REACTIVITY; SPECTRA; TRAPS; URANIUM DIOXIDE; URANYL NITRATES; WATER

Citation Formats

Stipdonk, Michael J. Van,, Iacovino, Anna, and Tatosian, Irena. Influence of Background H{sub 2}O on the Collision-Induced Dissociation Products Generated from [UO{sub 2}NO{sub 3}]{sup +}. United States: N. p., 2018. Web. doi:10.1007/S13361-018-1947-5.
Stipdonk, Michael J. Van,, Iacovino, Anna, & Tatosian, Irena. Influence of Background H{sub 2}O on the Collision-Induced Dissociation Products Generated from [UO{sub 2}NO{sub 3}]{sup +}. United States. doi:10.1007/S13361-018-1947-5.
Stipdonk, Michael J. Van,, Iacovino, Anna, and Tatosian, Irena. Sun . "Influence of Background H{sub 2}O on the Collision-Induced Dissociation Products Generated from [UO{sub 2}NO{sub 3}]{sup +}". United States. doi:10.1007/S13361-018-1947-5.
@article{osti_22776891,
title = {Influence of Background H{sub 2}O on the Collision-Induced Dissociation Products Generated from [UO{sub 2}NO{sub 3}]{sup +}},
author = {Stipdonk, Michael J. Van, and Iacovino, Anna and Tatosian, Irena},
abstractNote = {Developing a comprehensive understanding of the reactivity of uranium-containing species remains an important goal in areas ranging from the development of nuclear fuel processing methods to studies of the migration and fate of the element in the environment. Electrospray ionization (ESI) is an effective way to generate gas-phase complexes containing uranium for subsequent studies of intrinsic structure and reactivity. Recent experiments by our group have demonstrated that the relatively low levels of residual H{sub 2}O in a 2-D, linear ion trap (LIT) make it possible to examine fragmentation pathways and reactions not observed in earlier studies conducted with 3-D ion traps (Van Stipdonk et al. J. Am. Soc. Mass Spectrom. 14, 1205–1214, 2003). In the present study, we revisited the dissociation of complexes composed of uranyl nitrate cation [U{sup VI}O{sub 2}(NO{sub 3})]{sup +} coordinated by alcohol ligands (methanol and ethanol) using the 2-D LIT. With relatively low levels of background H{sub 2}O, collision-induced dissociation (CID) of [U{sup VI}O{sub 2}(NO{sub 3})]{sup +} primarily creates [UO{sub 2}(O{sub 2})]{sup +} by the ejection of NO. However, CID (using He as collision gas) of [U{sup VI}O{sub 2}(NO{sub 3})]{sup +} creates [UO{sub 2}(H{sub 2}O)]{sup +} and UO{sub 2}{sup +} when the 2-D LIT is used with higher levels of background H{sub 2}O. Based on the results presented here, we propose that product ion spectrum in the previous experiments was the result of a two-step process: initial formation of [U{sup VI}O{sub 2}(O{sub 2})]{sup +} followed by rapid exchange of O{sub 2} for H{sub 2}O by ion-molecule reaction. Our experiments illustrate the impact of residual H{sub 2}O in ion trap instruments on the product ions generated by CID and provide a more accurate description of the intrinsic dissociation pathway for [U{sup VI}O{sub 2}(NO{sub 3})]{sup +}. .},
doi = {10.1007/S13361-018-1947-5},
journal = {Journal of the American Society for Mass Spectrometry},
issn = {1044-0305},
number = 7,
volume = 29,
place = {United States},
year = {2018},
month = {7}
}