TY - JOUR
T1 - Atomic Dislocations and Bond Rupture Govern Dissolution Enhancement under Acoustic Stimulation
AU - Tang, Longwen
AU - Dong, Shiqi
AU - Arnold, Ross
AU - La Plante, Erika Callagon
AU - Vega-Vila, Juan Carlos
AU - Prentice, Dale
AU - Ellison, Kirk
AU - Kumar, Aditya
AU - Neithalath, Narayanan
AU - Simonetti, Dante
AU - Sant, Gaurav
AU - Bauchy, Mathieu
N1 - Publisher Copyright:
© 2020 American Chemical Society.
PY - 2020/12/9
Y1 - 2020/12/9
N2 - By focusing the power of sound, acoustic stimulation (i.e., often referred to as sonication) enables numerous "green chemistry"pathways to enhance chemical reaction rates, for instance, of mineral dissolution in aqueous environments. However, a clear understanding of the atomistic mechanism(s) by which acoustic stimulation promotes mineral dissolution remains unclear. Herein, by combining nanoscale observations of dissolving surface topographies using vertical scanning interferometry, quantifications of mineral dissolution rates via analysis of solution compositions using inductively coupled plasma optical emission spectrometry, and classical molecular dynamics simulations, we reveal how acoustic stimulation induces dissolution enhancement. Across a wide range of minerals (Mohs hardness ranging from 3 to 7, surface energy ranging from 0.3 to 7.3 J/m2, and stacking fault energy ranging from 0.8 to 10.0 J/m2), we show that acoustic fields enhance mineral dissolution rates (reactivity) by inducing atomic dislocations and/or atomic bond rupture. The relative contributions of these mechanisms depend on the mineral's underlying mechanical properties. Based on this new understanding, we create a unifying model that comprehensively describes how cavitation and acoustic stimulation processes affect mineral dissolution rates.
AB - By focusing the power of sound, acoustic stimulation (i.e., often referred to as sonication) enables numerous "green chemistry"pathways to enhance chemical reaction rates, for instance, of mineral dissolution in aqueous environments. However, a clear understanding of the atomistic mechanism(s) by which acoustic stimulation promotes mineral dissolution remains unclear. Herein, by combining nanoscale observations of dissolving surface topographies using vertical scanning interferometry, quantifications of mineral dissolution rates via analysis of solution compositions using inductively coupled plasma optical emission spectrometry, and classical molecular dynamics simulations, we reveal how acoustic stimulation induces dissolution enhancement. Across a wide range of minerals (Mohs hardness ranging from 3 to 7, surface energy ranging from 0.3 to 7.3 J/m2, and stacking fault energy ranging from 0.8 to 10.0 J/m2), we show that acoustic fields enhance mineral dissolution rates (reactivity) by inducing atomic dislocations and/or atomic bond rupture. The relative contributions of these mechanisms depend on the mineral's underlying mechanical properties. Based on this new understanding, we create a unifying model that comprehensively describes how cavitation and acoustic stimulation processes affect mineral dissolution rates.
KW - acoustic stimulation
KW - activation energy
KW - atomic bond rupture
KW - mineral dissolution
KW - molecular dynamics simulations
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U2 - 10.1021/acsami.0c16424
DO - 10.1021/acsami.0c16424
M3 - Article
C2 - 33258375
AN - SCOPUS:85097740929
SN - 1944-8244
VL - 12
SP - 55399
EP - 55410
JO - ACS Applied Materials and Interfaces
JF - ACS Applied Materials and Interfaces
IS - 49
ER -