TY - JOUR
T1 - A small-scale flow-through column system to determine the rates of mineral dissolution at high temperature and pressure
AU - Parthasarathy, Hariprasad
AU - Dzombak, David A.
AU - Karamalidis, Athanasios K.
N1 - Funding Information:
This project was funded by the Department of Energy, National Energy Technology Laboratory, an agency of the United States Government, through a support contract with URS Energy & Construction, Inc. Neither the United States Government nor any agency thereof, nor any of their employees, nor URS Energy & Construction, Inc., nor any of their employees, makes any warranty, expressed or implied, or assumes any legal liability or responsibility for the accuracy, completeness, or usefulness of any information, apparatus, product, or process disclosed, or represents that its use would not infringe privately owned rights. Reference herein to any specific commercial product, process, or service by trade name, trademark, manufacturer, or otherwise, does not necessarily constitute or imply its endorsement, recommendation, or favoring by the United States Government or any agency thereof. The views and opinions of authors expressed herein do not necessarily state or reflect those of the United States Government or any agency thereof.
Funding Information:
This project was performed as part of the National Energy Technology Laboratory's Regional University Alliance (NETL-RUA) under the RES contract DE-FE0004000 . We gratefully acknowledge Dr. Gregory Lowry of Carnegie Mellon University for his insights and helpful comments. We thank Drs. J. Alexandra Hakala and Karl Schroeder of the National Energy Technology Laboratory for reviewing the manuscript and Drs. Andy Wall, Brian Stewart and Rosemary Capo of the University of Pittsburgh for their help with arsenic analysis. We also thank Drs. Donald J. Rimstidt, Jeremy Fein and an anonymous reviewer for their helpful comments.
PY - 2013/9/16
Y1 - 2013/9/16
N2 - Mineral dissolution is a critical phenomenon in many geochemical systems, including those of geologic CO2 storage. It affects the mobilization, fate and transport of toxic metals in subsurface waters. A small-scale plug-flow system was designed and demonstrated for use in determining dissolution rates and simulating mineral-water interactions under a wide range of conditions, including high pressure (P, up to 300bar) and temperature (T, up to 120°C). The system enables rapid achievement of steady-state rates, and minimizes the experimental time to study such mineral-water systems. The performance of the system was evaluated through study of the oxidative dissolution of arsenopyrite (FeAsS (s)). Rates of arsenic release induced by dissolved Fe3+ (10-4M) in anoxic systems at 25°C and pressures of 1bar and 100bar were measured. The performance testing confirmed the ability to obtain reproducible results under the wide range of conditions tested, and to obtain similar results to certain benchmark cases, e.g., the FeAsS (s) dissolution rate of 10-8.09molAs/m2s at 25°C and 1bar was comparable to previously reported values. Potential mass-transfer limitations associated with the system were studied and results indicate such limitations can be avoided at flow-rates higher than 0.8mL/min.
AB - Mineral dissolution is a critical phenomenon in many geochemical systems, including those of geologic CO2 storage. It affects the mobilization, fate and transport of toxic metals in subsurface waters. A small-scale plug-flow system was designed and demonstrated for use in determining dissolution rates and simulating mineral-water interactions under a wide range of conditions, including high pressure (P, up to 300bar) and temperature (T, up to 120°C). The system enables rapid achievement of steady-state rates, and minimizes the experimental time to study such mineral-water systems. The performance of the system was evaluated through study of the oxidative dissolution of arsenopyrite (FeAsS (s)). Rates of arsenic release induced by dissolved Fe3+ (10-4M) in anoxic systems at 25°C and pressures of 1bar and 100bar were measured. The performance testing confirmed the ability to obtain reproducible results under the wide range of conditions tested, and to obtain similar results to certain benchmark cases, e.g., the FeAsS (s) dissolution rate of 10-8.09molAs/m2s at 25°C and 1bar was comparable to previously reported values. Potential mass-transfer limitations associated with the system were studied and results indicate such limitations can be avoided at flow-rates higher than 0.8mL/min.
UR - http://www.scopus.com/inward/record.url?scp=84880621339&partnerID=8YFLogxK
UR - http://www.scopus.com/inward/citedby.url?scp=84880621339&partnerID=8YFLogxK
U2 - 10.1016/j.chemgeo.2013.06.020
DO - 10.1016/j.chemgeo.2013.06.020
M3 - Article
AN - SCOPUS:84880621339
SN - 0009-2541
VL - 354
SP - 65
EP - 72
JO - Chemical Geology
JF - Chemical Geology
ER -