Dissolution Amplification by Resonance and Cavitational Stimulation at Ultrasonic and Megasonic Frequencies
Abstract
Acoustic stimulation offers a green pathway for the extraction of valuable elements such as Si, Ca, and Mg via solubilization of minerals and industrial waste materials. Prior studies have focused on the use of ultrasonic frequencies (20-40 kHz) to stimulate dissolution, but megasonic frequencies (≥1 MHz) offer benefits such as matching of the resonance frequencies of solute particles and an increased frequency of cavitation events. Here, based on dissolution tests of a series of minerals, it is found that dissolution under resonance conditions produced dissolution enhancements between 4x-to-6x in Si-rich materials (obsidian, albite, and quartz). Cavitational collapse induced by ultrasonic stimulation was more effective for Ca- and Mg-rich carbonate precursors (calcite and dolomite), exhibiting a significant increase in the dissolution rate as the particle size was reduced (i.e. available surface area was increased), resulting in up to a 70x increase in the dissolution rate of calcite when compared to unstimulated dissolution for particles with d50 < 100 μm. Cavitational collapse induced by megasonic stimulation caused a greater dissolution enhancement than ultrasonic stimulation (1.5x vs 1.3x) for amorphous class F fly ash, despite its higher Si content because the hollow particle structure was susceptible to breakage by the rapid and high number of lower-energy megasonic cavitation events. These results are consistent with the cavitational collapse energy following a normal distribution of energy release, with more cavitation events possessing sufficient energy to break Ca-O and Mg-O bonds than Si-O bonds, the latter of which has a bond energy approximately double the others. The effectiveness of ultrasonic dissolution enhancement increased exponentially with decreasing stacking fault energy (i.e., resistance to the creation of surface faults such as pits and dislocations), while, in turn, the effectiveness of megasonic dissolution increased linearly with the stacking fault energy. These results give new insights into the use of acoustic frequency selections for accelerating elemental release from solutes by the use of acoustic perturbation.
Recommended Citation
R. A. Arnold and S. Dong and L. Tang and D. Prentice and M. Collin and J. C. Vega-Vila and A. Hernandez and E. C. La Plante and K. Ellison and A. Kumar and For full list of authors, see publisher's website., "Dissolution Amplification by Resonance and Cavitational Stimulation at Ultrasonic and Megasonic Frequencies," Journal of Physical Chemistry C, vol. 126, no. 7, pp. 3432 - 3442, American Chemical Society (ACS), Feb 2022.
The definitive version is available at https://doi.org/10.1021/acs.jpcc.1c10968
Department(s)
Materials Science and Engineering
International Standard Serial Number (ISSN)
1932-7455; 1932-7447
Document Type
Article - Journal
Document Version
Citation
File Type
text
Language(s)
English
Rights
© 2022 American Chemical Society (ACS), All rights reserved.
Publication Date
24 Feb 2022
Comments
The authors acknowledge financial support for this research provisioned by Department of Energy’s Advanced Research Projects Agency for Energy (ARPA-E: award number: DE-AR0001147), the U.S. National Science Foundation (DMREF-1922167), and the Electric Power Research Institute (EPRI).