Citation: ZENG Kai, CHEN Huan-Wen, LUO Ming-Biao, ZHANG Hui, YU Wen-Ting. Rapid Identification of Uranyl Speciation in Solution by Electrospray Ionization Tandem Mass Spectrometry and Speciation Research of Uranyl Citrate[J]. Chinese Journal of Analytical Chemistry, ;2019, 47(3): 429-438. doi: 10.19756/j.issn.0253-3820.181575 shu

Rapid Identification of Uranyl Speciation in Solution by Electrospray Ionization Tandem Mass Spectrometry and Speciation Research of Uranyl Citrate

1.
Jiangxi Key Laboratory for Mass Spectrometry and Instrumentation, East China University of Technology, Nanchang 330013, China;
2.
Nanchang Key Laboratory of Quality and Safety Evaluation of Traditional Chinese Medicine, Nanchang Institute for Food and Drug Control, Nanchang 330012, China

Received Date: 5 September 2018
Revised Date: 21 December 2018

Fund Project: This work was supported by the National Natural Science Foundation of China (No. 21761001) and Postgraduate Innovation Foundation of East China University of Technology (No.YC2017-B082).

By regulating collision energy and mass-to-charge ratio, a rapid identification method for uranium-containing compounds from aqueous solutions was established by electrospray ionization tandem mass spectrometry. At high collision energy of 200 V in collision-induced dissociation mode, target ions were bombarded to generate product ions which were subsequently analyzed whether there was mass spectrum peak of[UO₂]⁺ (m/z 269.9), thus identifying the existence of uranium-containing molecules because[UO₂]⁺ was their basic functional group. Based on this method, 16 uranyl citrate and 5 inorganic uranyl speciation were identified in the citric acid-uranyl nitrate solution. Each uranyl group could bind a citrate anion tightly and complex weakly more than one citric acid molecule to form mono uranyl complex. Experiment result showed the following sequence of uranyl citrate complex bond energies:uranyl bond energy > citrate anion-uranyl bond energy > citric acid molecule-uranyl bond energy, and it was also found speciation of double-charged and double-uranyl ions, of which the fragmentation pathways needed further analysis. The method used in here unnecessarily required interpretation of mass spectra or standards of uranium, which would further demonstrate the utility of ESI-MS and its applicability to analyze uranyl-citrate speciation of environmental samples. It improved the identifying ability and efficiency of uranium speciation greatly, which provided reference significance for the study of other heavy metal organic speciation. Meanwhile, U(I) was split from[UO₂OH]⁺ by controlled particle collision, which provided a possible way to separate and purify uranium.
- Electrospray ionization tandem mass spectrometry,
- Uranyl cation,
- Identification,
- Speciation,
- Uranyl citrate,
- Uranium (I)
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