The novel analysis of uranyl compounds by electrospray-ion mobility-mass spectrometry

Crawford, Christina L.; Fugate, Glenn A.; Cable-Dunlap, Paula; Wall, Nathalie A.; Siems, William F.; Hill, Herbert H.

doi:10.1016/j.ijms.2012.08.004

Cited by 16 publications

(16 citation statements)

References 44 publications

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“…) is one of the most common radioactive pollutants in the environment, and the concerns about its environmental effects and threats to human health have steadily increased over time [1][2][3][4]. Hence, there is an urgent need to precisely and rapidly monitor the content of uranyl ions in environmental aqueous settings, which has resulted in the rapid development of many different uranyl detection methods, such as colorimetric methods [5][6][7], fluorescence methods [8,9], mass spectrometry [10][11][12], and electrochemistry [13,14]. Due to its fast response, high sensitivity, and its successful application in the rapid trace analysis of biological molecules [15][16][17], organic pollutants [18][19][20][21][22], and heavy metal ions [23,24], SERS is expected to become an alternative technique for the detection of uranyl.…”

Section: Uranyl (Uo 2 2+mentioning

confidence: 99%

The contribution of photoinduced charge-transfer enhancement to the SERS of uranyl(VI) in a uranyl-Ag2O complex

Wang

Yang

et al. 2019

Science Bulletin

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Section: Uranyl (Uo 2 2+mentioning

confidence: 99%

The contribution of photoinduced charge-transfer enhancement to the SERS of uranyl(VI) in a uranyl-Ag2O complex

Wang

Yang

et al. 2019

Science Bulletin

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“…instrumental flexibility and variety of ionization techniques; including wide dynamic temperature regime; fast for operation and stage limited sample preparation steps, encompassing analysis in solutions, semi-liquid and solid state, makes mass spectrometry a method of choice for uranium speciation (Pajo et al 2001;Steppert et al 2012;Crawford et al 2012;Rutkowski et al 2011;Gresham et al 2011;Jennings et al 1989). Its applicability involves complex multicomponent homogeneous and heterogeneous environmental samples, including stages of the nuclear fuel cycle such as treatment of liquid wastes and/or dried fuel storage, where the assessment of uranium oxides reactivity [ 100-250°C is of considerable interest (He et al 2010;Lotnik et al 2001;Yusov and Shilov 2007;Kulyukhin and Kamenskaya 2010;Nagaishi et al 1998;Gorshkov et al 2001;Rios et al 2012).…”

Section: Introductionmentioning

confidence: 99%

Environmental modeling of uranium interstitial compositions of non-stoichiometric oxides: experimental and theoretical analysis

Ivanova

Spiteller

2015

Environ Geochem Health

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Study of uranium interstitial compositions of non-stoichiometric oxides UO2+x (x ∈ 0.1-0.02) in gas and condense phases has been presented, using various soft-ionization mass spectrometric methods such as ESI-, APCI-, and MALDI-MS at a wide dynamic temperature gradient (∈ 25-300 °C). Linearly polarized vibrational spectroscopy has been utilized in order to assign unambiguously, the vibrational frequencies of uranium non-stoichiometric oxides. Experimental design has involved xUO2.66·yUO2.33, xUO2.66·yUO2.33/SiO2, xUO2.66·yUO2.33/SiO2 (NaOH) and SiO2/x'NaOH·y'UO2(NO3)2·6H2O, multicomponent systems (x = 1, y ∈ 0.1-1.0 and x' = 1, y' ∈ 0.1-0.6) as well as phase transitions UO2(NO3)2·6H2O → {U4O9(UO2.25)} → U3O7(UO2.33) → U3O8(UO2.66) → {UO3}, thus ensuring a maximal representativeness to real environmental conditions, where diverse chemical, geochemical and biochemical reactions, including complexation and sorption onto minerals have occurred. Experimental factors such as UV-irradiation, pH, temperature, concentration levels, solvent types and ion strength have been taken into consideration, too. As far as uranium speciation represents a challenging analytical task in terms of chemical identification diverse coordination species, mechanistic aspects relating incorporation of oxygen into UO 2+x form the shown full methods validation significantly impacts the field of environmental radioanalytical chemistry. UO2 is the most commonly used fuel in nuclear reactors around the globe; however, a large non-stoichiometric range ∈ UO1.65-UO2.25 has occurred due to radiolysis of water on UO2 surface yielding to H2O2, OH(·), and more. Each of those compositions has different oxygen diffusion. And in this respect enormous effort has been concentrated to study the potential impact of hazardous radionuclide on the environment, encompassing from the reprocessing to the disposal stages of the fuel waste, including the waste itself, the processes in the waste containers, the clay around the containers, and geological processes. In a broader sense, thereby, this study contributes to field of environmental analysis highlighting the great ability of various soft-ionization MS methods, particularly, MALDI-MS one, for direct assay of complex multicomponent heterogeneous mixtures at fmol-attomol concentration ranges, along with it the great instrumental features allowing, not only meaningful quantitative, but also structural information of the analytes, thus making the method indispensable for environmental speciation of radionuclides, generally.

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“…The identification of whole‐molecule uranium compounds was observed, and the quantification of uranium was possible through the addition of a gadolinium internal standard. As demonstrated previously with ESI‐MS, solvent selection for the analysis of actinide compounds can influence the type of ions formed due to solubility, chemical interactions between the solvent and formed ions, and the formation of adduct ions with solvent molecules . Water was found to be a poor solvent for uranyl and uranyl‐bearing complexes; therefore, the use of a methanol and water mixture improved the sensitivity for uranyl by several orders of magnitude compared with water alone.…”

Section: Resultsmentioning

confidence: 85%

“…The effects of solvent selection and differences between ESI‐MS and PSI‐MS spectra warrant further investigation. For example, solvent selection has been shown to affect ESI‐MS based on solubility and interactions with the analyte …”

Section: Conclusion and Summarymentioning

confidence: 99%

Rapid paper spray mass spectrometry characterization of uranium and exemplar molecular species

Coopersmith

Cody

Mannion

et al. 2019

Rapid Comm Mass Spectrometry

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Rationale:The ability to detect and quantify the presence of specific inorganic elements and complexes is essential for environmental monitoring and nuclear safeguards applications. In this work, paper spray ionization mass spectrometry was used for the rapid chemical and isotopic characterization of trace inorganic species collected on cotton swipe substrates. The direct analysis of cotton swipes using this ambient ionization technique led to fast sample analysis that retained original chemical information of the source material with minimal sample preparation.Methods: Mass spectra were collected with an atmospheric pressure ionization, high-resolution mass spectrometer for solutions containing uranyl acetate, uranyl chloride, uranyl nitrate, and uranyl tri-n-butylphosphate complexes. Gadolinium nitrate was used as an internal standard for the quantitative analysis of uranium. To demonstrate the ability to characterize inorganic contaminants in the presence of uranium, a multi-element inorganic standard containing U, Bi, Pb, Cd, Fe, and Zn was deposited onto cotton substrates and directly analyzed without purification.Results: All elements doped on the cotton substrate were detected with strong signal-to-noise ratios (ca 1000 for UO 2 + on multi-element doped swipes) and high integrated intensities (>10 5 counts) from collection periods of approximately 1 min.Limits of detection were determined to be approximately 94 ng for UO 2 + and uranyl acetate through the measurement of ppb level solutions. Conclusions:The rapid analysis of uranium and other inorganic-containing samples while still retaining original chemical information (e.g. uranyl complexation) was demonstrated. Qualitative detection and speciation were achieved in less than 1 min of analysis. For uranium isotopic quantitation, longer accumulations (>15 min) can be sustained to improve the accuracy of minor 235 U isotopic abundance measurements to approximately 1% error.

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The novel analysis of uranyl compounds by electrospray-ion mobility-mass spectrometry

Cited by 16 publications

References 44 publications

The contribution of photoinduced charge-transfer enhancement to the SERS of uranyl(VI) in a uranyl-Ag2O complex

The contribution of photoinduced charge-transfer enhancement to the SERS of uranyl(VI) in a uranyl-Ag2O complex

Environmental modeling of uranium interstitial compositions of non-stoichiometric oxides: experimental and theoretical analysis

Rapid paper spray mass spectrometry characterization of uranium and exemplar molecular species

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