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 UO2 + on multi-element doped swipes) and high integrated intensities (>105 counts) from collection periods of approximately 1 min. Limits of detection were determined to be approximately 94 ng for UO2 + 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.

中文翻译：

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铀和样例分子物种的快速纸喷雾质谱表征。

理由检测和定量特定无机元素和配合物的存在的能力对于环境监测和核保障应用至关重要。在这项工作中，纸喷雾电离质谱法用于对棉签基材上收集的痕量无机物进行快速化学和同位素表征。使用这种环境电离技术对棉签进行的直接分析导致了快速的样品分析，从而以最少的样品制备时间保留了原料的原始化学信息。方法用大气压电离高分辨率质谱仪收集含有乙酸铀酰，铀酰氯，硝酸铀酰和铀酰三正丁基磷酸酯络合物的溶液的质谱图。硝酸用作铀定量分析的内标。为了证明在铀存在下表征无机污染物的能力，将包含U，Bi，Pb，Cd，Fe和Zn的多元素无机标样沉积到棉质基质上，无需纯化即可直接进行分析。结果在大约1分钟的采集时间内，检测到所有掺杂在棉质基质上的元素具有很强的信噪比（多元素掺杂的擦拭物中UO2 +的信噪比约为1000）和高集成强度（> 105个计数）。通过测量ppb级溶液，确定了UO2 +和乙酸铀酰的检出限约为94 ng。结论证明了对铀和其他含无机样品的快速分析，同时仍保留了原始化学信息（例如，铀酰络合）。在不到1分钟的分析时间内即可完成定性检测和形态分析。对于铀同位素定量，可以持续更长的累积时间（> 15分钟），以将次要的235 U同位素丰度测量的准确性提高到大约1％的误差。