Heteroepitaxial growth of cadmium carbonate at dolomite and calcite surfaces: Mechanisms and rates

Callagon, Erika Blanca R.; Lee, Sang Soo; Eng, Peter J.; Laanait, Nouamane; Sturchio, Neil C.; Nagy, Kathryn L.; Fenter, Paul

doi:10.1016/j.gca.2016.12.007

Heteroepitaxial growth of cadmium carbonate at dolomite and calcite surfaces: Mechanisms and rates

Journal Article · Sat Dec 10 00:00:00 EST 2016 · Geochimica et Cosmochimica Acta

DOI:https://doi.org/10.1016/j.gca.2016.12.007· OSTI ID:1372659

Callagon, Erika Blanca R. ^[1]; Lee, Sang Soo ^[2]; Eng, Peter J. ^[3]; Laanait, Nouamane ^[4]; Sturchio, Neil C. ^[5]; Nagy, Kathryn L. ^[6]; Fenter, Paul ^[2]

Univ. of Illinois, Chicago, IL (United States); Univ. of California, Los Angeles, CA (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)
Univ. of Chicago, Chicago, IL (United States)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Univ. of Illinois, Chicago, IL (United States)
Univ. of Delaware, Newark, DE (United States)

Here, the systematic variation of rates and the mechanism of cadmium uptake on the (104) surface of dolomite (CaMg(CO₃)₂) were investigated using in situ and ex situ atomic force microscopy (AFM), ex situ specular X-ray reflectivity (XR), and ex situ X-ray fluorescence (XRF). Selected experiments were performed on the calcite (CaCO₃) (104) surface for comparison. Aqueous solutions of CdCl₂, CaCl₂, and NaHCO₃, undersaturated with respect to calcite and supersaturated with respect to otavite (CdCO₃) and the (Cd_xCa_1-x)CO₃ solid solution, were reacted with dolomite surfaces for minutes to days. Calcite substrates were reacted with solutions containing 1-50 μM CdCl₂, and with no added Ca or CO₃. Thin carbonate films following the Stranski-Krastanov growth mode were observed on both substrates. Specular XR and XRF revealed the formation of nm-thick Cd-rich carbonate films that were structurally ordered with respect to the dolomite (104) plane. Epitaxial films adopted the calcite crystal structure with a d₁₀₄- spacing (3.00 Å) larger than those of pure dolomite (2.88 Å) and otavite (2.95 Å) indicating either a solid solution with x approximate to 0.5, or a strained Cd-rich carbonate with a composition near that of otavite. The growth rate r of this phase increases with the initial supersaturation of the solution with respect to the solid solution, beta max, and follows the empirical relationship, as determined from XRF measurements, given by: r = 10^{-4.88 ± 0.42} (β^{2.29 ± 0.24}_max - 1), (in units of atoms of Cd/Å²/h).The morphology of the overgrowth also varied with β_max, as exemplified by AFM observations. Growth at step edges occurred over the entire β_max range considered, and additional growth features including 3 Å high monolayer islands and ~ 25 Å high tall islands were observed when log β_max > 1. On calcite, in situ XR indicated that this phase is similar to the Cd-rich overgrowth formed on dolomite and images obtained from X-ray reflection interface microscopy (XRIM) reveal the existence of laterally variable Cd-rich domains.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Lab. (ANL), Argonne, IL (United States)

Sponsoring Organization:: National Science Foundation (NSF), Directorate for Geosciences Division of Earth Sciences (GEO/EAR); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22), Chemical Sciences, Geosciences, and Biosciences Division

Grant/Contract Number:: AC02-06CH11357; FG02-94ER14466

OSTI ID:: 1372659

Alternate ID(s):: OSTI ID: 1398653

Journal Information:: Geochimica et Cosmochimica Acta, Journal Name: Geochimica et Cosmochimica Acta Journal Issue: C Vol. 205; ISSN 0016-7037

Publisher:: The Geochemical Society; The Meteoritical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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