Hydrothermal atomic force microscopy observations of barite step growth rates as a function of the aqueous barium-to-sulfate ratio

Bracco, Jacquelyn N.; Gooijer, Yiscka; Higgins, Steven R.

doi:10.1016/j.gca.2016.03.009

Title: Hydrothermal atomic force microscopy observations of barite step growth rates as a function of the aqueous barium-to-sulfate ratio

Journal Article · Sat Mar 19 00:00:00 EDT 2016 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2016.03.009· OSTI ID:1376308

Bracco, Jacquelyn N. ^[1]; Gooijer, Yiscka ^[2]; Higgins, Steven R. ^[1]

Wright State Univ., Dayton, OH (United States). Dept. of Chemistry
Wright State Univ., Dayton, OH (United States). Dept. of Chemistry; Hogeschool Utrecht, Utrecht (The Netherlands). Inst. for Life Sciences and Chemistry

The rate of growth of ionic minerals from solutions with varying aqueous cation:anion ratios may result in significant errors in mineralization rates predicted by commonly-used affinity-based rate equations. To assess the potential influence of solute stoichiometry on barite growth, step velocities on the barite (001) surface have been measured at 108 °C using hydrothermal atomic force microscopy (HAFM) at moderate supersaturation and as a function of the aqueous barium:sulfate ratio (r). Barite growth hillocks at r ~ 1 were bounded by $$\langle$$120$$\rangle$$ steps, however at r < 1, kink site densities increased, steps followed a direction vicinal to $$\langle$$120$$\rangle$$, and the [010] steps developed. At r > 1, steps roughened and rounded as the kink site density increased. Step velocities peaked at r = 1 and decreased roughly symmetrically as a function of r, indicating the attachment rates of barium and sulfate ions are similar under these conditions. We hypothesize that the differences in our observations at high and low r arise from differences in the attachment rate constants for the obtuse and acute $$\langle$$120$$\rangle$$ steps. Based on results at low r, the data suggests the attachment rate constant for barium ions is similar for obtuse and acute steps. Based on results at high r, the data suggests the attachment rate constant for sulfate is greater for obtuse steps than acute steps. In conclusion, utilizing a step growth model developed by Stack and Grantham (2010) the experimental step velocities as a function of r were readily fit while attempts to fit the data using a model developed by Zhang and Nancollas (1998) were less successful.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1376308

Alternate ID(s):: OSTI ID: 1359156

Journal Information:: Geochimica et Cosmochimica Acta, Vol. 183, Issue C; ISSN 0016-7037

Publisher:: The Geochemical Society; The Meteoritical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 23 works

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