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On the growth of witherite and its replacement by the Mg-bearing double carbonate norsethite: Implications for the dolomite problem

  • Michael Lindner EMAIL logo and Guntram Jordan
Published/Copyright: January 29, 2018
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American Mineralogist
From the journal American Mineralogist Volume 103 Issue 2

Abstract

Witherite [BaCO3] and norsethite [BaMg(CO3)2] are perceived as chemical and structural analogs of aragonite [CaCO3] and dolomite [CaMg(CO3)2], respectively. However, norsethite, unlike dolomite, readily precipitates from aqueous solutions at ambient conditions. This is of special interest as the dehydration barrier of Mg2+ may be a likely cause of the dolomite growth inhibition. The easiness of norsethite growth shows that the problem of dolomite formation is more complex. To attain a comprehensive understanding of the analog BaCO3-MgCO3 system and of the formation of ordered anhydrous Mg-bearing double carbonates, we investigated the fate and behavior of aqueous magnesium during growth of witherite.

Growth experiments were conducted on witherite seeds in mixed-flow reactors at 50 °C and various Mg-concentrations (0.25–2 mM Ba2+, 0–20 mM Mg2+, pH 7.8–8.5, ionic strength 0.1 M). At Mg:Ba ratios in solution smaller than 6:1, Mg2+ did not affect witherite growth kinetics. No significant amount of Mg2+ was incorporated. The rate constant k and reaction order n for witherite growth were determined for the first time (k = 0.65 ± 0.05 × 10-7 mol m-2 s-1; n = 1.3 ± 0.1; supersaturation Ω = IAP/Ks = 1–4, where IAP is the ionic activity product and Ks the solubility constant). The insensitivity of witherite growth kinetics to these levels of Mg is analogous to aragonite growth. The general absence of the formation of solid solutions in the entire BaCO3-MgCO3 system, however, is not shared by the CaCO3-MgCO3 system, for which it is well known that substitution in the sixfold-coordinated cation sites occurs extensively.

Mg:Ba ratios in solution larger than 12:1 led to a replacement of witherite by norsethite. This replacement also is in strong contrast to the CaCO3-MgCO3 system, where higher temperatures and/or much longer timescales are necessary to obtain dolomite. The replacement rate of witherite at 50 °C was estimated to be ~200 times faster than the analogous replacement of aragonite by dolomite observed over 7 years at even 60 °C (Usdowski 1989).

We speculate that the preferential formation of ordered norsethite over a solid solution is facilitated by the large difference in Mg2+ and Ba2+ ionic radii. Due to the presumably very high free energy of formation of the solid solution, ordering into distinct Ba- and Mg-layers is the only way to combine both cations within one phase. In the CaCO3-MgCO3 system, solid solution occurrence is common and effectively contributes to the inhibition of the formation of the ordered double carbonate dolomite over a wide range of conditions (cf. Arvidson and Mackenzie 1999).

Keywords: Carbonate growth kinetics; trace element incorporation; norsethite; barium mobility

Acknowledgments

Support by the Deutsche Forschungsgemeinschaft DFG (JO301/4-1) is gratefully acknowledged. We thank Karin Paschert and Salvatore Carrocci for assistance with SEM and titration measurements, respectively. Furthermore, the authors are grateful for the two anonymous reviews and the editorial handling by Daniel Hummer.

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Received: 2017-7-3
Accepted: 2017-10-16
Published Online: 2018-1-29
Published in Print: 2018-2-23

© 2018 Walter de Gruyter GmbH, Berlin/Boston

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https://doi.org/10.2138/am-2018-6232
Keywords for this article
Carbonate growth kinetics; trace element incorporation; norsethite; barium mobility

Articles in the same Issue

  1. Invited Centennial Article
  2. Secular change in metamorphism and the onset of global plate tectonics
  4. Laboratory and field characterization of visible to near-infrared spectral reflectance of nitrate minerals from the Atacama Desert, Chile, and implications for Mars
  6. Comparative compressional behavior of chabazite with Li+, Na+, Ag+, K+, Rb+, and Cs+ as extra-framework cations
  8. Petrology of “Mt. Shasta” high-magnesian andesite (HMA): A product of multi-stage crustal assembly
  10. Conversion of serpentine to smectite under hydrothermal condition: Implication for solid-state transformation
  12. On the growth of witherite and its replacement by the Mg-bearing double carbonate norsethite: Implications for the dolomite problem
  14. First measurements of OH-C exchange and temperature-dependent partitioning of OH and halogens in the system apatite–silicate melt
  16. Dissolution mechanisms of chromitite: Understanding the release and fate of chromium in the environment
  18. Textural and mineral chemical evidence for the cumulate origin and evolution of high-titanium basalt fragment 71597
  20. Tourmaline crystal chemistry
  22. (Ca-Y)-phosphate inclusions in apatite crystals from Archean rocks from the Barberton Greenstone Belt and Pilbara Craton: First report of natural occurrence
  24. A siltstone reaction front related to CO2- and sulfur-bearing fluids: Integrating quantitative elemental mapping with reactive transport modeling
  25. Minerals Matter
  26. Apatite: Following the movements of ancient humans and mastodons
  27. Letter
  28. Macroscopic electrostatic effects in ATR-FTIR spectra of modern and archeological bones
  30. New Mineral Names
  32. American Mineralogist thanks the 2017 reviewers
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