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Zinc isotope fractionation under vaporization processes and in aqueous solutions

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Abstract

Equilibrium Zn isotope fractionation was investigated using first-principles quantum chemistry methods at the B3LYP/6-311G* level. The volume variable cluster model method was used to calculate isotope fractionation factors of sphalerite, smithsonite, calcite, anorthite, forsterite, and enstatite. The water-droplet method was used to calculate Zn isotope fractionation factors of Zn2+-bearing aqueous species; their reduced partition function ratio factors decreased in the order \(\left[ {{\text{Zn}}\left( {{\text{H}}_{2} {\text{O}}} \right)_{6} } \right]^{2 + } > \left[ {{\text{ZnCl}}\left( {{\text{H}}_{2} {\text{O}}} \right)_{5} } \right]^{ + } > \left[ {{\text{ZnCl}}_{2} \left( {{\text{H}}_{2} {\text{O}}} \right)_{4} } \right] > \left[ {{\text{ZnCl}}_{3} \left( {{\text{H}}_{2} {\text{O}}} \right)_{2} } \right]^{ - } > {\text{ZnCl}}_{4} ]^{2 - }\). Gaseous ZnCl2 was also calculated for vaporization processes. Kinetic isotope fractionation of diffusional processes in a vacuum was directly calculated using formulas provided by Richter and co-workers. Our calculations show that in addition to the kinetic isotope effect of diffusional processes, equilibrium isotope fractionation also contributed nontrivially to observed Zn isotope fractionation of vaporization processes. The calculated net Zn isotope fractionation of vaporization processes was 7–7.5‰, with ZnCl2 as the gaseous species. This matches experimental observations of the range of Zn isotope distribution of lunar samples. Therefore, vaporization processes may be the cause of the large distribution of Zn isotope signals found on the Moon. However, we cannot further distinguish the origin of such vaporization processes; it might be due either to igneous rock melting in meteorite bombardments or to a giant impact event. Furthermore, isotope fractionation between Zn-bearing aqueous species and minerals that we have provided helps explain Zn isotope data in the fields of ore deposits and petrology.

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Acknowledgements

Y.L. and co-author are grateful for support from 973 Program Fund (No. 2014CB440904), Chinese National Science Fund Projects (Nos. 41530210, 41490635, 41403051).

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  1. School of Karst Science, Guizhou Normal University/State Engineering Technology Institute for Karst Desertification Control, Guiyang, 550001, China

    Jixi Zhang

  2. State Key Laboratory of Ore Deposit Geochemistry, Institute of Geochemistry, Chinese Academy of Sciences, Guiyang, 550081, China

    Jixi Zhang & Yun Liu

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Zhang, J., Liu, Y. Zinc isotope fractionation under vaporization processes and in aqueous solutions. Acta Geochim 37, 663–675 (2018). https://doi.org/10.1007/s11631-018-0281-8

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