Dissolution Amplification by Resonance and Cavitational Stimulation at Ultrasonic and Megasonic Frequencies
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 mega sonic 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 mega sonic 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 mega sonic 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 mega sonic 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.
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 S. Srivastava and M. Bauchy and D. Simonetti and G. N. Sant, "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, Feb 2022.
The definitive version is available at https://doi.org/10.1021/acs.jpcc.1c10968
Materials Science and Engineering
International Standard Serial Number (ISSN)
Article - Journal
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24 Feb 2022
National Science Foundation, Grant DMREF-1922167