Extractive Electrospray Ionization Mass Spectrometry for Sensitive Detection of Uranyl Species in Natural Water Samples

Abstract

Ambient mass spectrometry has been increasingly applied for sensitive detection of trace organic compounds present in complex matrixes. In the real world, detection of trace amounts of inorganic species, particularly with speciation information, is of great significances. Herein a method based on extractive electrospray ionization (EESI) tandem mass spectrometry (MS/MS) has been established for rapid detection of radioactive inorganic species in natural water samples. Negatively charged uranyl acetate undergoes characteristic fragmentation in the gas phase, providing the fundamental chemistry for specific detection of uranyl species in complex matrixes without sample pretreatment. Under the optimized experimental conditions, uranyl species in various natural water samples were rapidly detected using multiple-stage EESI mass spectrometry. The mean time for each sample analysis was about 10 s. The limit of detection was about a few 10(-3) ng/L of uranium by utilizing the characteristic fragments obtained in the EESI-MS(3) experiments. The typical relative standard deviation (RSD) of this method was 6.9-8.1% for 8 measurements (S/N = 3). The dynamic response range was 10(-1)-10(3) ng/L for uranium in water samples. The isotope ratio of uranyl species was quantitatively detected using EESI-MS experiments. The results show that EESI-MS, a typical method initially developed for organic compound analysis, has promising perspectives for real time, online monitoring of inorganic species such as uranyl species in natural water samples.

Gas Phase Reactions of Ions Derived from Anionic Uranyl Formate and Uranyl Acetate Complexes

“…More , had previously been prepared in a Bbottom-up^approach by insertion of U + into NO in an ion-molecule reaction [28], our experiments demonstrated that the species can also be created in a CID reaction. Formation of the nitrido species by transfer of N from cyanide was confirmed using precursors labeled with -in a 3-D quadrupole ion trap has been reported [26,30], and the structure of the species has been determined using infrared multiple-photon photodissociation (IRMPD) spectroscopy [31]. However, the experiments reported here demonstrate that the chemistry of product ions from both systems can be explored more accurately in the 2-D LIT.…”

Reactive extractive electrospray ionization tandem mass spectrometry for sensitive detection of tetrabromobisphenol A derivatives

“…All the experiments were carried out using a linear trap quadruple mass spectrometer (LTQ-XL, Thermo Fisher Scientific, San Jose, CA) installed with a homemade EESI source, which was previously described in detail [26,[32][33][34][35]. The schematic illustration of EESI-MS is shown in Fig.…”

“…As reported in 2006, extractive electrospray ionization mass spectrometry (EESI-MS) was able to detect TNT in waste water, and trace atrazine in undiluted urine [26], showing promising applications in environmental studies. To date, EESI-MS has been applied to direct analysis of various samples, including exhaled human breath [27,28], skin [29], food [29][30][31], natural water [32], toothpaste [33], native proteins [34], etc. In this study, low ppb levels of TBBPA derivatives in waste water were detected for the first time with EESI-MS/MS.…”

Detection of trace levels of lead in aqueous liquids using extractive electrospray ionization tandem mass spectrometry

“…Most of EESI-MS studies have been carried out for the analysis of organic compounds, although the successful detection of uranium and its salts using EESI-MS has been reported [55]. In this study, EESI-MS was used for the fast and sensitive detection of trace levels of lead in aqueous liquid samples.…”