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Title: New insights into Mn2+ and Mg2+ inhibition of calcite growth

Abstract

Impurity ion and isotope partitioning into carbonate minerals provide a window into the molecular processes occurring at the fluid-mineral interface during crystal growth. Here, we employ calcium isotope fractionation together with process-based modeling to elucidate the mechanisms by which two divalent cations with starkly contrasting compatibility, magnesium and manganese, inhibit calcite growth and incorporate into the mineral lattice. Calcite growth inhibition by Mg2+ is log-linear and KMg is on the order of 0.02–0.03 throughout the range of {Mg2+}/{Ca2+} studied here (0.01–2.6). Mn2+ exhibits much stronger log-linear growth rate inhibition at low Mn2+ concentrations (fluid {Mn2+}/{Ca2+} = 0.001–0.02). Mn2+ is readily incorporated into the calcite lattice to form a calcite-rhodochrosite solid solution, with large partition coefficients (KMn 4.6–15.6) inversely correlated to growth rate. For both Mn2+ and Mg2+, calcium isotope fractionation is found to be invariant with {Me2+}/{Ca2+} despite more than an order of magnitude decline in growth rate. This invariant Δ44/40Ca suggests that the presence of Mn2+ or Mg2+ does not significantly change the relative rates of Ca2+ attachment and detachment at kink sites during growth, indicative of a dominantly kink blocking inhibition mechanism. Because the partitioning behavior dictates that Mn2+ must attach to the surface significantly faster than Ca2+,more » attachment of Mn2+ is likely to be as a non-monomer species such as an ion pair or possibly a larger polynuclear cluster. We propose that calcite growth rate inhibition by Mn is determined by the kinetics of carbonate attachment at Mn-occupied kink sites, potentially due to slow re-orientation kinetics of carbonate ions that have formed an inner-sphere complex with Mn2+ at the surface but must reorient to incorporate into the lattice. We demonstrate that patterns in Mg2+ partitioning and inhibition behavior are broadly consistent with growth inhibition driven by slow Mg2+-aquo complex dehydration relative to Ca2+ but argue that this mechanism likely represents one endmember scenario, seen in Mg-calcite growth at low supersaturations and net precipitation rates. During growth at faster net precipitation rates, some portion of Mg2+ is likely incorporated as a partially hydrated or otherwise complexed species, but calcite growth remains significantly inhibited by the kinetics of CO32- attachment at Mg2+ kink sites. These findings suggest a hybrid classical/nonclassical growth mechanism whereby Ca2+ incorporates largely as a free ion at kink sites while Mn2+ and some portion of Mg2+ are incorporated via non-monomer attachment. This pattern may be generalizable; trace constituent cations with aquo-complex desolvation rates significantly slower than the mineral growth rate preferentially incorporate as a non-monomer species during otherwise classical crystal growth.« less

Authors:
 [1]; ORCiD logo [2];  [3]; ORCiD logo [3]
+ Show Author Affiliations
  1. Univ. of California, Berkeley, CA (United States)
  2. California Institute of Technology (CalTech), Pasadena, CA (United States)
  3. Univ. of California, Berkeley, CA (United States); Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Publication Date:
Research Org.:
Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
OSTI Identifier:
1994355
Grant/Contract Number:  
AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Geochimica et Cosmochimica Acta
Additional Journal Information:
Journal Volume: 334; Journal ID: ISSN 0016-7037
Publisher:
Elsevier; The Geochemical Society; The Meteoritical Society
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; magnesium; manganese; calcite; calcium isotope fractionation; kinetic isotope effect; trace element partitioning; nonclassical growth

Citation Formats

Mills, Jennifer V., Barnhart, Holly A., DePaolo, Donald J., and Lammers, Laura N. New insights into Mn2+ and Mg2+ inhibition of calcite growth. United States: N. p., 2022. Web. doi:10.1016/j.gca.2022.06.015.
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Mills, Jennifer V., Barnhart, Holly A., DePaolo, Donald J., & Lammers, Laura N. New insights into Mn2+ and Mg2+ inhibition of calcite growth. United States. https://doi.org/10.1016/j.gca.2022.06.015
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Mills, Jennifer V., Barnhart, Holly A., DePaolo, Donald J., and Lammers, Laura N. Mon . "New insights into Mn2+ and Mg2+ inhibition of calcite growth". United States. https://doi.org/10.1016/j.gca.2022.06.015. https://www.osti.gov/servlets/purl/1994355.
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@article{osti_1994355,
title = {New insights into Mn2+ and Mg2+ inhibition of calcite growth},
author = {Mills, Jennifer V. and Barnhart, Holly A. and DePaolo, Donald J. and Lammers, Laura N.},
abstractNote = {Impurity ion and isotope partitioning into carbonate minerals provide a window into the molecular processes occurring at the fluid-mineral interface during crystal growth. Here, we employ calcium isotope fractionation together with process-based modeling to elucidate the mechanisms by which two divalent cations with starkly contrasting compatibility, magnesium and manganese, inhibit calcite growth and incorporate into the mineral lattice. Calcite growth inhibition by Mg2+ is log-linear and KMg is on the order of 0.02–0.03 throughout the range of {Mg2+}/{Ca2+} studied here (0.01–2.6). Mn2+ exhibits much stronger log-linear growth rate inhibition at low Mn2+ concentrations (fluid {Mn2+}/{Ca2+} = 0.001–0.02). Mn2+ is readily incorporated into the calcite lattice to form a calcite-rhodochrosite solid solution, with large partition coefficients (KMn 4.6–15.6) inversely correlated to growth rate. For both Mn2+ and Mg2+, calcium isotope fractionation is found to be invariant with {Me2+}/{Ca2+} despite more than an order of magnitude decline in growth rate. This invariant Δ44/40Ca suggests that the presence of Mn2+ or Mg2+ does not significantly change the relative rates of Ca2+ attachment and detachment at kink sites during growth, indicative of a dominantly kink blocking inhibition mechanism. Because the partitioning behavior dictates that Mn2+ must attach to the surface significantly faster than Ca2+, attachment of Mn2+ is likely to be as a non-monomer species such as an ion pair or possibly a larger polynuclear cluster. We propose that calcite growth rate inhibition by Mn is determined by the kinetics of carbonate attachment at Mn-occupied kink sites, potentially due to slow re-orientation kinetics of carbonate ions that have formed an inner-sphere complex with Mn2+ at the surface but must reorient to incorporate into the lattice. We demonstrate that patterns in Mg2+ partitioning and inhibition behavior are broadly consistent with growth inhibition driven by slow Mg2+-aquo complex dehydration relative to Ca2+ but argue that this mechanism likely represents one endmember scenario, seen in Mg-calcite growth at low supersaturations and net precipitation rates. During growth at faster net precipitation rates, some portion of Mg2+ is likely incorporated as a partially hydrated or otherwise complexed species, but calcite growth remains significantly inhibited by the kinetics of CO32- attachment at Mg2+ kink sites. These findings suggest a hybrid classical/nonclassical growth mechanism whereby Ca2+ incorporates largely as a free ion at kink sites while Mn2+ and some portion of Mg2+ are incorporated via non-monomer attachment. This pattern may be generalizable; trace constituent cations with aquo-complex desolvation rates significantly slower than the mineral growth rate preferentially incorporate as a non-monomer species during otherwise classical crystal growth.},
doi = {10.1016/j.gca.2022.06.015},
journal = {Geochimica et Cosmochimica Acta},
number = ,
volume = 334,
place = {United States},
year = {Mon Jun 20 00:00:00 EDT 2022},
month = {Mon Jun 20 00:00:00 EDT 2022}
}
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