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Title: Unraveling the Effects of Strontium Incorporation on Barite Growth—In Situ and Ex Situ Observations Using Multiscale Chemical Imaging

Abstract

Impurity ions influence mineral growth rates through a variety of kinetic and thermodynamic processes that also affect partitioning of the impurity ion between the solid and solution. Here, the effect of an impurity ion, strontium, on Barite (BaSO4) (001) growth rates was studied using a combination of high-resolution in situ microscopy with ex situ chemical imaging techniques. In the presence of strontium, $$\langle$$120$$\rangle$$ steps roughened and bifurcated. The overall Barite growth rate also decreased with increasing aqueous strontium-to-barium ratio ([Sr]/[Ba]aq) < 1. Analysis of the reacted solids using chemical imaging techniques indicated strontium incorporated uniformly across all step orientations into the Barite growth hillock for [Sr]/[Ba]aq < 1. However, at [Sr]/[Ba]aq > 5, steps with an apparent [010] orientation were expressed and growth in the [010] step direction led to an increase in the overall growth rate of the surface. Strontium became preferentially incorporated into the [010] step direction, rather than being homogeneously distributed. The [Sr]/[Ba]s in the newly grown solid was found to correlate directly with that of solutions at [Sr]/[Ba]aq < 5, but not for higher [Sr]/[Ba]aq. Solid composition analyses indicate that thermodynamic equilibrium was not achieved. However, kinetic transport modeling successfully reproduces the shift in growth mechanism.

Authors:
ORCiD logo [1]; ORCiD logo [2]; ORCiD logo [3]; ORCiD logo [3]; ORCiD logo [3];  [3];  [4];  [4]; ORCiD logo [1]; ORCiD logo [4]; ORCiD logo [1]
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Chemical Science Division
  2. Argonne National Lab. (ANL), Argonne, IL (United States)
  3. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
  4. Wright State Univ., Dayton, OH (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Argonne National Lab. (ANL), Argonne, IL (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES)
OSTI Identifier:
1470873
Alternate Identifier(s):
OSTI ID: 1491847
Grant/Contract Number:  
AC05-00OR22725; AC02-06CH11357
Resource Type:
Accepted Manuscript
Journal Name:
Crystal Growth and Design
Additional Journal Information:
Journal Volume: 18; Journal Issue: 9; Journal ID: ISSN 1528-7483
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; atom probe tomography; atomic force microscopy; kinetic process modelling; mineral growth mechanism; mineral-fluid interface; sequestration of toxic elements

Citation Formats

Weber, Juliane, Bracco, Jacquelyn N., Poplawsky, Jonathan D., Ievlev, Anton V., More, Karren Leslie, Lorenz, Matthias, Bertagni, Angela L., Jindra, Sarah A., Starchenko, Vitaliy, Higgins, Steven R., and Stack, Andrew G. Unraveling the Effects of Strontium Incorporation on Barite Growth—In Situ and Ex Situ Observations Using Multiscale Chemical Imaging. United States: N. p., 2018. Web. doi:10.1021/acs.cgd.8b00839.
Weber, Juliane, Bracco, Jacquelyn N., Poplawsky, Jonathan D., Ievlev, Anton V., More, Karren Leslie, Lorenz, Matthias, Bertagni, Angela L., Jindra, Sarah A., Starchenko, Vitaliy, Higgins, Steven R., & Stack, Andrew G. Unraveling the Effects of Strontium Incorporation on Barite Growth—In Situ and Ex Situ Observations Using Multiscale Chemical Imaging. United States. https://doi.org/10.1021/acs.cgd.8b00839
Weber, Juliane, Bracco, Jacquelyn N., Poplawsky, Jonathan D., Ievlev, Anton V., More, Karren Leslie, Lorenz, Matthias, Bertagni, Angela L., Jindra, Sarah A., Starchenko, Vitaliy, Higgins, Steven R., and Stack, Andrew G. Thu . "Unraveling the Effects of Strontium Incorporation on Barite Growth—In Situ and Ex Situ Observations Using Multiscale Chemical Imaging". United States. https://doi.org/10.1021/acs.cgd.8b00839. https://www.osti.gov/servlets/purl/1470873.
@article{osti_1470873,
title = {Unraveling the Effects of Strontium Incorporation on Barite Growth—In Situ and Ex Situ Observations Using Multiscale Chemical Imaging},
author = {Weber, Juliane and Bracco, Jacquelyn N. and Poplawsky, Jonathan D. and Ievlev, Anton V. and More, Karren Leslie and Lorenz, Matthias and Bertagni, Angela L. and Jindra, Sarah A. and Starchenko, Vitaliy and Higgins, Steven R. and Stack, Andrew G.},
abstractNote = {Impurity ions influence mineral growth rates through a variety of kinetic and thermodynamic processes that also affect partitioning of the impurity ion between the solid and solution. Here, the effect of an impurity ion, strontium, on Barite (BaSO4) (001) growth rates was studied using a combination of high-resolution in situ microscopy with ex situ chemical imaging techniques. In the presence of strontium, $\langle$120$\rangle$ steps roughened and bifurcated. The overall Barite growth rate also decreased with increasing aqueous strontium-to-barium ratio ([Sr]/[Ba]aq) < 1. Analysis of the reacted solids using chemical imaging techniques indicated strontium incorporated uniformly across all step orientations into the Barite growth hillock for [Sr]/[Ba]aq < 1. However, at [Sr]/[Ba]aq > 5, steps with an apparent [010] orientation were expressed and growth in the [010] step direction led to an increase in the overall growth rate of the surface. Strontium became preferentially incorporated into the [010] step direction, rather than being homogeneously distributed. The [Sr]/[Ba]s in the newly grown solid was found to correlate directly with that of solutions at [Sr]/[Ba]aq < 5, but not for higher [Sr]/[Ba]aq. Solid composition analyses indicate that thermodynamic equilibrium was not achieved. However, kinetic transport modeling successfully reproduces the shift in growth mechanism.},
doi = {10.1021/acs.cgd.8b00839},
journal = {Crystal Growth and Design},
number = 9,
volume = 18,
place = {United States},
year = {2018},
month = {7}
}

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Figures / Tables:

Fig. 1 Fig. 1: Step velocity $v$s dependence on ratio of aqueous barium and strontium cations [Ba]/[Sr]aq. ⟨120⟩ step velocities are given in green and show a decrease with increasing [Ba]/[Sr]aq. In red, [010] step velocities are given, which show an increase with increasing [Sr]/[Ba]aq. Fit functions for the ⟨120⟩ and [010]more » step growth are displayed. HAFM-images (a-c) show how strontium in solution affects barite hillock morphology. All images have roughly the same crystallographic orientation.« less

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