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Title: Investigating calcite growth rates using a quartz crystal microbalance with dissipation (QCM-D)

Abstract

Calcite precipitation plays a significant role in processes such as geological carbon sequestration and toxic metal sequestration and, yet, the rates and mechanisms of calcite growth under close to equilibrium conditions are far from well understood. In this study, a quartz crystal microbalance with dissipation (QCM-D) was used for the first time to measure macroscopic calcite growth rates. Calcite seed crystals were first nucleated and grown on sensors, then growth rates of calcite seed crystals were measured in real-time under close to equilibrium conditions (saturation index, SI = log ({Ca 2+}/{CO 3 2–}/ K sp) = 0.01–0.7, where {i} represent ion activities and K sp = 10 –8.48 is the calcite thermodynamic solubility constant). At the end of the experiments, total masses of calcite crystals on sensors measured by QCM-D and inductively coupled plasma mass spectrometry (ICP-MS) were consistent, validating the QCM-D measurements. Calcite growth rates measured by QCM-D were compared with reported macroscopic growth rates measured with auto-titration, ICP-MS, and microbalance. Calcite growth rates measured by QCM-D were also compared with microscopic growth rates measured by atomic force microscopy (AFM) and with rates predicted by two process-based crystal growth models. The discrepancies in growth rates among AFM measurements andmore » model predictions appear to mainly arise from differences in step densities, and the step velocities were consistent among the AFM measurements as well as with both model predictions. Using the predicted steady-state step velocity and the measured step densities, both models predict well the growth rates measured using QCM-D and AFM. Furthermore, this study provides valuable insights into the effects of reactive site densities on calcite growth rate, which may help design future growth models to predict transient-state step densities.« less

Authors:
 [1]; ORCiD logo [2];  [3];  [3];  [4];  [1]
  1. Univ. of Houston, Houston, TX (United States)
  2. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  3. Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
  4. Univ. of California, Berkeley, CA (United States)
Publication Date:
Research Org.:
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Energy Frontier Research Centers (EFRC) (United States). Center for Nanoscale Control of Geologic CO2 (NCGC); Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)
Sponsoring Org.:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
OSTI Identifier:
1468246
Alternate Identifier(s):
OSTI ID: 1476622
Grant/Contract Number:  
AC05-00OR22725; AC02-05CH11231
Resource Type:
Accepted Manuscript
Journal Name:
Geochimica et Cosmochimica Acta
Additional Journal Information:
Journal Volume: 222; Journal Issue: C; Journal ID: ISSN 0016-7037
Publisher:
The Geochemical Society; The Meteoritical Society
Country of Publication:
United States
Language:
English
Subject:
58 GEOSCIENCES; Crystal growth rate; Calcite; Quartz crystal microbalance with dissipation; Step density; Step velocity

Citation Formats

Cao, Bo, Stack, Andrew G., Steefel, Carl I., DePaolo, Donald J., Lammers, Laura N., and Hu, Yandi. Investigating calcite growth rates using a quartz crystal microbalance with dissipation (QCM-D). United States: N. p., 2017. Web. doi:10.1016/j.gca.2017.10.020.
Cao, Bo, Stack, Andrew G., Steefel, Carl I., DePaolo, Donald J., Lammers, Laura N., & Hu, Yandi. Investigating calcite growth rates using a quartz crystal microbalance with dissipation (QCM-D). United States. doi:10.1016/j.gca.2017.10.020.
Cao, Bo, Stack, Andrew G., Steefel, Carl I., DePaolo, Donald J., Lammers, Laura N., and Hu, Yandi. Fri . "Investigating calcite growth rates using a quartz crystal microbalance with dissipation (QCM-D)". United States. doi:10.1016/j.gca.2017.10.020. https://www.osti.gov/servlets/purl/1468246.
@article{osti_1468246,
title = {Investigating calcite growth rates using a quartz crystal microbalance with dissipation (QCM-D)},
author = {Cao, Bo and Stack, Andrew G. and Steefel, Carl I. and DePaolo, Donald J. and Lammers, Laura N. and Hu, Yandi},
abstractNote = {Calcite precipitation plays a significant role in processes such as geological carbon sequestration and toxic metal sequestration and, yet, the rates and mechanisms of calcite growth under close to equilibrium conditions are far from well understood. In this study, a quartz crystal microbalance with dissipation (QCM-D) was used for the first time to measure macroscopic calcite growth rates. Calcite seed crystals were first nucleated and grown on sensors, then growth rates of calcite seed crystals were measured in real-time under close to equilibrium conditions (saturation index, SI = log ({Ca2+}/{CO32–}/Ksp) = 0.01–0.7, where {i} represent ion activities and Ksp = 10–8.48 is the calcite thermodynamic solubility constant). At the end of the experiments, total masses of calcite crystals on sensors measured by QCM-D and inductively coupled plasma mass spectrometry (ICP-MS) were consistent, validating the QCM-D measurements. Calcite growth rates measured by QCM-D were compared with reported macroscopic growth rates measured with auto-titration, ICP-MS, and microbalance. Calcite growth rates measured by QCM-D were also compared with microscopic growth rates measured by atomic force microscopy (AFM) and with rates predicted by two process-based crystal growth models. The discrepancies in growth rates among AFM measurements and model predictions appear to mainly arise from differences in step densities, and the step velocities were consistent among the AFM measurements as well as with both model predictions. Using the predicted steady-state step velocity and the measured step densities, both models predict well the growth rates measured using QCM-D and AFM. Furthermore, this study provides valuable insights into the effects of reactive site densities on calcite growth rate, which may help design future growth models to predict transient-state step densities.},
doi = {10.1016/j.gca.2017.10.020},
journal = {Geochimica et Cosmochimica Acta},
number = C,
volume = 222,
place = {United States},
year = {2017},
month = {11}
}

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