TY - JOUR
T1 - Isothermal Stimulation of Mineral Dissolution Processes by Acoustic Perturbation
AU - Wei, Zongsu
AU - Hsiao, Yi Hsuan
AU - Chen, Xin
AU - La Plante, Erika Callagon
AU - Mehdipour, Iman
AU - Simonetti, Dante
AU - Neithalath, Narayanan
AU - Pilon, Laurent
AU - Bauchy, Mathieu
AU - Israelachvili, Jacob
AU - Sant, Gaurav
N1 - Funding Information:
The authors acknowledge financial support for this research from the Department of Energy, Office of Fossil Energy via the National Energy Technology Laboratory (NETL: DE-FE0029825), The Anthony and Jeanne Pritzker Family Foundation, Department of Energy’s Nuclear Energy University Program (DOE-NEUP: DE-NE0008398), and the National Science Foundation (CAREER Award: 1253269, CMMI: 1562066). This research was conducted in the Laboratory for the Chemistry of Construction Materials (LC2) at UCLA. As such, the authors gratefully acknowledge the support that has made these laboratories and their operations possible. The contents of this paper reflect the views and opinions of the authors, who are responsible for the accuracy of the datasets presented herein, and do not reflect the views and/or policies of the funding agencies, nor do the contents constitute a specification, standard, or regulation. The authors also acknowledge Dr. Joseph King (ARPA-E, U.S. Department of Energy) for numerous stimulating discussions of dissolution amplification by acoustic perturbation.
Publisher Copyright:
© Copyright 2018 American Chemical Society.
PY - 2018/12/20
Y1 - 2018/12/20
N2 - On the basis of systematic experimental interrogation of the aqueous dissolution behavior of a large selection of minerals, whose dissolution rates vary by several orders of magnitude, this study demonstrates that acoustic perturbation yields an unprecedented enhancement in dissolution kinetics, which scales with the mineral's hardness and average bond energy. The dissolution enhancement produced is described by an Arrhenius-like formulation that reveals the energy imparted to the solute's surficial atoms by sonication. From an energy landscape perspective, it is highlighted that sonication perturbs surficial solute atoms from their equilibrium positions. As a result, upon contact with a solvent, sonicated atoms need a smaller amount of energy for dissolution to occur by bond rupture. Therefore, the activation energy of dissolution under sonication is consistently smaller than that under sonication-free conditions. Altogether, this study suggests that the enhancement in mineral dissolution over the course of acoustic perturbation under macroscopically isothermal conditions results from the excitation of the surficial atoms and is negligibly associated with temperature rise or surface area amplification as has been previously suggested.
AB - On the basis of systematic experimental interrogation of the aqueous dissolution behavior of a large selection of minerals, whose dissolution rates vary by several orders of magnitude, this study demonstrates that acoustic perturbation yields an unprecedented enhancement in dissolution kinetics, which scales with the mineral's hardness and average bond energy. The dissolution enhancement produced is described by an Arrhenius-like formulation that reveals the energy imparted to the solute's surficial atoms by sonication. From an energy landscape perspective, it is highlighted that sonication perturbs surficial solute atoms from their equilibrium positions. As a result, upon contact with a solvent, sonicated atoms need a smaller amount of energy for dissolution to occur by bond rupture. Therefore, the activation energy of dissolution under sonication is consistently smaller than that under sonication-free conditions. Altogether, this study suggests that the enhancement in mineral dissolution over the course of acoustic perturbation under macroscopically isothermal conditions results from the excitation of the surficial atoms and is negligibly associated with temperature rise or surface area amplification as has been previously suggested.
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U2 - 10.1021/acs.jpcc.8b08343
DO - 10.1021/acs.jpcc.8b08343
M3 - Article
AN - SCOPUS:85058943913
SN - 1932-7447
VL - 122
SP - 28665
EP - 28673
JO - Journal of Physical Chemistry C
JF - Journal of Physical Chemistry C
IS - 50
ER -