Precise isotope analysis of nanogram-level Pb for natural rock samples without use of double spikes

A simple technique has been developed for the precise analysis of lead isotope in natural rock samples by thermal ionization mass spectrometry (TIMS). Two-stage column chromatography, using 100 and 10 μl columns, was used to minimize the amounts of impurities in separated lead samples. This dramatically improved the reproducibility of mass fractionation during mass spectrometry using an ion emitter made of a mixture of silicic acid and phosphoric acid. This improvement made it possible to precisely determine the Pb isotopic compositions of very small sample sizes, employing “zero-time correction” for mass discrimination, without requiring a double-spike technique. Using the present method, analytical reproducibility of 208Pb/204Pb of 0.02% and 0.06% (2σ) was attained for 100 and 1 ng of Pb, respectively, separated from natural rock samples. Furthermore, we obtained a reproducibility of 0.06% (2σ) for 208Pb/204Pb for 10 ng of Pb separated from GSJ JP-1 (peridotite), in which the Pb concentration was 0.09 ppm. The measured isotope compositions of USGS standard rocks AGV-1 and BCR-1 were comparable with the published values using the double-spike technique. These observations suggest that our simple technique is reliable in terms of both accuracy and precision for the determination of the Pb isotopic compositions of natural rock samples irrespective of rock chemistry and sample sizes from 1 to 100 ng of Pb.