Development of direct injection/ionization mass spectrometry methods for whole molecule characterization

Technical Report · Thu Sep 20 04:00:00 EDT 2018

DOI:https://doi.org/10.2172/1475269· OSTI ID:1475269

Wellons, M. ^[1]; Mannion, J. ^[1]; Shick, C. ^[1]; Hewitt, J. ^[1]; Lawrence, K. ^[1]; Swindle, A. ^[1]; Koby, S. ^[1]; Kuhne, W. ^[1]; Cody, C. ^[2]

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1. Savannah River National Lab (SRNL), Aiken, SC (United States)
2. JEOL USA Inc., Acworth, GA (United States)

Determining uranium isotopic and concentration information from environmental samples typically involves extensive chemical and physical processing prior to analysis. Harsh sample preparation results in the loss of the original uranium chemical speciation (i.e. what the uranium was bonded to/with when found in the environment) as well as the mixing of anthropogenic uranium with background material contained within the collection media (e.g. a swipe or soil). The objective of this work is to adapt a bioanalytical mass spectrometry technology called paper spray ionization mass spectrometry for the rapid analysis of intact uranium complexes. Soft ionization facilitates detection of whole molecule uranyl complexes including uranyl acetate, uranyl nitrate, and uranyl-tributylphosphate complex. Cotton swipe samples doped with a multi-element standard containing μg levels of U, Bi, Pb, Cd, Fe, and Zn were directly analyzed without purification, representing a major improvement over existing methods. Uranium quantitation is demonstrated using internal standards to obtain linear calibration curves. Limits of detection were determined to be approximately 100 ng for UO₂ and uranyl acetate through measurement of ppb level solutions. The development and qualification of PSI-MS techniques could lead to significant safeguards-related cost reduction and timeliness by facilitating the triage and queueing of swipe samples for more sensitive and time-consuming analyses.

• Research Organization: Savannah River National Lab (SRNL), Aiken, SC (United States)
• Sponsoring Organization: USDOE Office of Environmental Management (EM)
• DOE Contract Number: AC09-08SR22470
• OSTI ID: 1475269
• Report Number(s): SRNL-STI--2018-00520
• Country of Publication: United States
• Language: English

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