Fractionation of radiogenic Pb isotopes in meteorites and their components induced by acid leaching

In this study we test the possibility that radiogenic 207Pb/206Pb ratios (207Pb*/206Pb*) in meteorites can be fractionated during partial dissolution, and explore the consequences of this fractionation for Pb-isotope chronology of meteorites. We report the results of experiments tailored to detect Pb-isotope fractionation, induced by partial dissolution through acid leaching, in plutonic angrite Northwest Africa (NWA) 4801 and ungrouped achondrites NWA 10132 and Erg Chech (EC) 002. We also re-examine previously published U-Pb data for other achondrites and for Ca-Al-rich refractory inclusions (CAIs), to seek evidence of such fractionation. We observe that, in primitive achondrite NWA 10132, differences in 207Pb*/206Pb* ratios, corresponding to the age bias of ca. 1–2 Ma, exist between the 0.5 M hydrofluoric acid leachates of pyroxene or crushed rock, and the residues after such leaching. In angrite NWA 4801, similar acid treatment of pyroxene separates did not cause a resolvable age bias. In EC 002, three steps of partial dissolution in 0.2 M – 5 M HF caused irregular 207Pb*/206Pb* fractionation between leaching steps, and generally higher 207Pb*/206Pb* ratios in the residues than in HF leachates. These age biases were observed in leaching pairs with highly radiogenic Pb, and cannot be explained by mixing between radiogenic Pb, primordial Pb, and Pb introduced by terrestrial contamination. Instead, the observed isotope fractionation is attributed to the combined effects of the size difference between α-recoil tracks in the decay chains of 238U and 235U, and exsolution of primary pigeonite, leading to the formation of a lamellar structure consisting of augite and low-Ca pyroxene by either slow-cooling or subsequent metamorphic reactions. Where extensive acid leaching intended for removal of non-radiogenic Pb causes fractionation of radiogenic Pb isotopes, its detrimental effect can be reversed by performing a numeric recombination of partial leachate and residue data. Currently, it is unclear how common leaching-induced isotopic fractionation is in Pb-isotopic chronology to meteoritic materials. Acid leaching is an essential step for removal of non-radiogenic Pb in the precise Pb-isotopic dating of meteorites, which currently does not have viable alternatives. However, it is important to be aware of its possible side effects, and to continue search for new non-radiogenic Pb removal techniques that do not cause radiogenic 207Pb* and 206Pb* fractionation.