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Peer-reviewedCC BY 4.0Atomic Spectroscopy

Direct Determination of ²⁰⁶Pb/²⁰⁴Pb and ²⁰⁸Pb/²⁰⁴Pb Ratios by Triple Quadrupole ICP-MS Without Pb Purification: Opportunities and Limitations for Source Tracing

Abstract

Lead stable isotope ratios 206 Pb/ 204 Pb, 207 Pb/ 204 Pb and 208 Pb/ 204 Pb are widely used to trace the origin of natural or artificial materials in geochemistry, environmental science and archaeology. Time consuming sequential column chemistry for purification of Pb are often necessary for preparing the analysis of Pb isotopes ratios with MC-ICP-MS, with a precision (uncertainties) reaching 0.001. However, such a high precision is not always necessary for source tracing when the end-members have significant different signatures. Here, 206 Pb/ 204 Pb, 207 Pb/ 204 Pb and 208 Pb/ 204 Pb ratios were analyzed for 7 certified reference materials (CRM: SL-1, RGM-1, MAG-1, BHVO-1, BCR-723, BCR-1 and BCR-2), including sediments and urban road dusts, using Triple Quadrupole Inductively Coupled Plasma Mass Spectrometry (TQ-ICP-MS) after conventional total digestion without sequential column chemistry. The solutions from the digestion were measured at four Pb concentrations (0.5, 1, 1.5 and 2 ng ml -1 ). Among 56 measurements on 33 SL-1 samples at a lead concentration of 2 ng ml -1 (sample digestion was realized between 2018 and 2024 while lead isotopic ratio measurements were conducted between 2022 and 2025), the first and third quartile of the uncertainties are 0.07 and 0.1 for 206 Pb/ 204 Pb, 0.05 and 0.09 for 207 Pb/ 204 Pb and 0.16 and 0.21 for 208 Pb/ 204 Pb. The 206 Pb/ 204 Pb and 208 Pb/ 204 Pb ratios obtained with TQ-ICP-MS can be especially useful for source tracing while uncertainties related to 207 Pb/ 204 Pb are in the same range of differences between terrestrial sources. This study employs TQ-ICP-MS to complement earlier ICP-QMS-based research, while also validating lead isotope ratio analysis using a larger set of certified reference materials (CRMs). In addition, the analytical protocol, spanning digestion and measurement over multiple years, enables an assessment of the long-term stability and reproducibility of the entire methodological workflow. We conclude that some studies can benefit from the simple and fast analysis of 206 Pb/ 204 Pb and 208 Pb/ 204 Pb ratios by TQ-ICP-MS with very small amount of additional works and investment, when potential end-members display sufficiently distinct isotopic signatures. Moreover, the here developed approach can be used to select samples which deserve more detailed geochemical analyses, lowering costs and environmental impacts.

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BibTeX
@article{xuyang2026direct,
  title = {{Direct Determination of ²⁰⁶Pb/²⁰⁴Pb and ²⁰⁸Pb/²⁰⁴Pb Ratios by Triple Quadrupole ICP-MS Without Pb Purification: Opportunities and Limitations for Source Tracing}},
  author = {Yangjunjie Xu-Yang and Sophie Ayrault and Delphine Thomas},
  journal = {Atomic Spectroscopy},
  year = {2026},
  month = nov,
  doi = {10.46770/as.2026.0047},
  url = {https://hal.science/hal-05851315v1},
  note = {CC BY 4.0},
}
RIS
TY  - JOUR
TI  - Direct Determination of ²⁰⁶Pb/²⁰⁴Pb and ²⁰⁸Pb/²⁰⁴Pb Ratios by Triple Quadrupole ICP-MS Without Pb Purification: Opportunities and Limitations for Source Tracing
AU  - Yangjunjie Xu-Yang
AU  - Sophie Ayrault
AU  - Delphine Thomas
PY  - 2026
DA  - 2026/11/04
JO  - Atomic Spectroscopy
DO  - 10.46770/as.2026.0047
UR  - https://hal.science/hal-05851315v1
AB  - Lead stable isotope ratios 206 Pb/ 204 Pb, 207 Pb/ 204 Pb and 208 Pb/ 204 Pb are widely used to trace the origin of natural or artificial materials in geochemistry, environmental science and archaeology. Time consuming sequential column chemistry for purification of Pb are often necessary for preparing the analysis of Pb isotopes ratios with MC-ICP-MS, with a precision (uncertainties) reaching 0.001. However, such a high precision is not always necessary for source tracing when the end-members have significant different signatures. Here, 206 Pb/ 204 Pb, 207 Pb/ 204 Pb and 208 Pb/ 204 Pb ratios were analyzed for 7 certified reference materials (CRM: SL-1, RGM-1, MAG-1, BHVO-1, BCR-723, BCR-1 and BCR-2), including sediments and urban road dusts, using Triple Quadrupole Inductively Coupled Plasma Mass Spectrometry (TQ-ICP-MS) after conventional total digestion without sequential column chemistry. The solutions from the digestion were measured at four Pb concentrations (0.5, 1, 1.5 and 2 ng ml -1 ). Among 56 measurements on 33 SL-1 samples at a lead concentration of 2 ng ml -1 (sample digestion was realized between 2018 and 2024 while lead isotopic ratio measurements were conducted between 2022 and 2025), the first and third quartile of the uncertainties are 0.07 and 0.1 for 206 Pb/ 204 Pb, 0.05 and 0.09 for 207 Pb/ 204 Pb and 0.16 and 0.21 for 208 Pb/ 204 Pb. The 206 Pb/ 204 Pb and 208 Pb/ 204 Pb ratios obtained with TQ-ICP-MS can be especially useful for source tracing while uncertainties related to 207 Pb/ 204 Pb are in the same range of differences between terrestrial sources. This study employs TQ-ICP-MS to complement earlier ICP-QMS-based research, while also validating lead isotope ratio analysis using a larger set of certified reference materials (CRMs). In addition, the analytical protocol, spanning digestion and measurement over multiple years, enables an assessment of the long-term stability and reproducibility of the entire methodological workflow. We conclude that some studies can benefit from the simple and fast analysis of 206 Pb/ 204 Pb and 208 Pb/ 204 Pb ratios by TQ-ICP-MS with very small amount of additional works and investment, when potential end-members display sufficiently distinct isotopic signatures. Moreover, the here developed approach can be used to select samples which deserve more detailed geochemical analyses, lowering costs and environmental impacts.
SN  - 0195-5373
ER  -