Abstract:The advances which have taken place during the last four decades in the instrumentation and applications of thermal ionisation mass spectrometry (TIMS) particularly of relevance to nuclear science and technology are highlighted.
“…Highly precise and accurate isotopic measurements are urgently required in multiple scientific areas such as the redefinition of the SI units, geochemistry, environment, geology, agriculture, nuclear science, archaeology, etc. Multi‐collector thermal ionization mass spectrometry (MC‐TIMS) is one of the state‐of‐the‐art techniques for high‐quality isotope analysis because its sources of uncertainty are relatively small and well understood .…”
Section: Introductionmentioning
confidence: 99%
“…Unfortunately, in practice, the isotopic ratios obtained by TE‐TIMS are affected by various factors, including inconsistency in the loading of sample, ionization temperature fluctuations, filament deformation caused by successive heating, isotopic ion loss, peak tailing, etc . Due to our poor understanding of these factors, inconsistent opinions on which kind of filament to use and the influence of loading sample amount have been reported over the past two decades.…”
Section: Introductionmentioning
confidence: 99%
“…Due to our poor understanding of these factors, inconsistent opinions on which kind of filament to use and the influence of loading sample amount have been reported over the past two decades. Some groups believed that a single filament source was not suitable for TE‐TIMS due to the change in its temperature throughout the TE process, while other groups have used a single filament source for Ra, B, Re, and Pb analysis. There have also been different opinions on the influence of sample amount.…”
Rationale: An absolute method that does not require calibration is very important in several areas of isotope analysis due to the shortage of suitable certified reference materials (CRMs). As total evaporation thermal ionization mass spectrometry (TE-TIMS) theoretically overcomes mass fractionation through integrating the ion currents till the sample on the filament is completely exhausted, it could be an absolute method that does not require the use of CRMs for calibration. However, the lack of reliable method verification and reasonable uncertainty evaluation restricts its extensive application, and these effects need to be quantitatively evaluated.
Methods:A series of different amounts of strontium reference material SRM987 was deposited on both single and triple tantalum filament sources, and analyzed by TE-TIMS. The work function of the tantalum filament loaded with the sample was measured by ultraviolet photoelectron spectroscopy. In order to evaluate the change in ion transmission efficiency, we terminated the total evaporation process manually after running for a certain period of time, and recorded the ion beam intensity before and after this operation.
Results:The TE results obtained with the triple filament source agreed well with the reference values of SRM987, while the TE results obtained with the single filament source changed significantly with the amount of sample loading. The crucial effect factors on TE-TIMS, including ionization temperature fluctuation, variation of ion transmission efficiency and ion loss before data acquisition, were quantitatively assessed. These factors were used to correct the single filament TE results and the measurement uncertainty was quantitatively evaluated.
Conclusions:The reliability of strontium isotopic ratio measurement with triple filament TE-TIMS was verified. The mathematical model for correction of each crucial effect factor was successfully established, thus providing a feasible way for the correction of single filament TE-TIMS results.
“…Highly precise and accurate isotopic measurements are urgently required in multiple scientific areas such as the redefinition of the SI units, geochemistry, environment, geology, agriculture, nuclear science, archaeology, etc. Multi‐collector thermal ionization mass spectrometry (MC‐TIMS) is one of the state‐of‐the‐art techniques for high‐quality isotope analysis because its sources of uncertainty are relatively small and well understood .…”
Section: Introductionmentioning
confidence: 99%
“…Unfortunately, in practice, the isotopic ratios obtained by TE‐TIMS are affected by various factors, including inconsistency in the loading of sample, ionization temperature fluctuations, filament deformation caused by successive heating, isotopic ion loss, peak tailing, etc . Due to our poor understanding of these factors, inconsistent opinions on which kind of filament to use and the influence of loading sample amount have been reported over the past two decades.…”
Section: Introductionmentioning
confidence: 99%
“…Due to our poor understanding of these factors, inconsistent opinions on which kind of filament to use and the influence of loading sample amount have been reported over the past two decades. Some groups believed that a single filament source was not suitable for TE‐TIMS due to the change in its temperature throughout the TE process, while other groups have used a single filament source for Ra, B, Re, and Pb analysis. There have also been different opinions on the influence of sample amount.…”
Rationale: An absolute method that does not require calibration is very important in several areas of isotope analysis due to the shortage of suitable certified reference materials (CRMs). As total evaporation thermal ionization mass spectrometry (TE-TIMS) theoretically overcomes mass fractionation through integrating the ion currents till the sample on the filament is completely exhausted, it could be an absolute method that does not require the use of CRMs for calibration. However, the lack of reliable method verification and reasonable uncertainty evaluation restricts its extensive application, and these effects need to be quantitatively evaluated.
Methods:A series of different amounts of strontium reference material SRM987 was deposited on both single and triple tantalum filament sources, and analyzed by TE-TIMS. The work function of the tantalum filament loaded with the sample was measured by ultraviolet photoelectron spectroscopy. In order to evaluate the change in ion transmission efficiency, we terminated the total evaporation process manually after running for a certain period of time, and recorded the ion beam intensity before and after this operation.
Results:The TE results obtained with the triple filament source agreed well with the reference values of SRM987, while the TE results obtained with the single filament source changed significantly with the amount of sample loading. The crucial effect factors on TE-TIMS, including ionization temperature fluctuation, variation of ion transmission efficiency and ion loss before data acquisition, were quantitatively assessed. These factors were used to correct the single filament TE results and the measurement uncertainty was quantitatively evaluated.
Conclusions:The reliability of strontium isotopic ratio measurement with triple filament TE-TIMS was verified. The mathematical model for correction of each crucial effect factor was successfully established, thus providing a feasible way for the correction of single filament TE-TIMS results.
“…Monitoring nuclear material in facilities can be facilitated by field deployable mass spectrometers . Currently, the field of isotope ratio analysis relies heavily on multi‐collector inductively coupled plasma mass spectrometry (MC‐ICP‐MS; the workhorse of the nuclear material isotopic analyses) and thermal ionization mass spectrometry (TIMS; considered the “gold standard”) . While these instruments have clear benefits, neither is capable of being deployed in the field given their size and the strict operating parameters and the infrastructure that each requires for operation.…”
The LS-APGD/Orbitrap system, while still in the preliminary stages of development, offers highly accurate and precise isotope ratio results that suggest a potential paradigm shift in the world of isotope ratio analysis. Furthermore, the portability of the LS-APGD as an elemental ion source, combined with the small size and smaller operating demands of the Orbitrap, suggests that the instrumentation is capable of being field-deployable.
“…Mass spectrometry has long been recognized as one of the most sensitive methods for the characterization of long‐lived actinides, but these techniques have been used primarily for the quantification of isotopic ratios or the characterization of inorganic contaminants rather than the identification and quantification of specific inorganic complexes. Paper spray ionization mass spectrometry (PSI‐MS) and the closely related swab touch spray ionization mass spectrometry have recently gained attention as versatile, ambient ionization techniques requiring minimal sample preparation and sample consumption for the direct analysis of blood, urine, and environmentally collected chemical warfare agent simulants .…”
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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