X-ray-driven reaction front dynamics at calcite-water interfaces
Abstract
The interface of minerals with aqueous solutions is central to geochemical reactivity, hosting processes that span multiple spatiotemporal scales. Understanding such processes requires spatially and temporally resolved observations, and experimental controls that precisely manipulate the interfacial thermodynamic state. Using the intense radiation fields of a focused synchrotron X-ray beam, we drove dissolution at the calcite-aqueous interface and simultaneously probed the dynamics of the propagating reaction fronts using surface X-ray microscopy. Evolving surface structures are controlled by the time-dependent solution composition as characterized by a kinetic reaction model. At extreme disequilibria, the onset of reaction front instabilities was observed with velocities of >30 nanometers per second. As a result, these instabilities are identified as a signature of transport-limited dissolution of calcite under extreme disequilibrium.
- Authors:
- Publication Date:
- Research Org.:
- Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC)
- OSTI Identifier:
- 1355825
- Alternate Identifier(s):
- OSTI ID: 1234334
- Grant/Contract Number:
- AC05-00OR22725
- Resource Type:
- Published Article
- Journal Name:
- Science
- Additional Journal Information:
- Journal Name: Science Journal Volume: 349 Journal Issue: 6254; Journal ID: ISSN 0036-8075
- Publisher:
- American Association for the Advancement of Science (AAAS)
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 36 MATERIALS SCIENCE; X-ray microscopy; mineral/aqueous interfaces
Citation Formats
Laanait, N., Callagon, E. B. R., Zhang, Z., Sturchio, N. C., Lee, S. S., and Fenter, P. X-ray-driven reaction front dynamics at calcite-water interfaces. United States: N. p., 2015.
Web. doi:10.1126/science.aab3272.
Laanait, N., Callagon, E. B. R., Zhang, Z., Sturchio, N. C., Lee, S. S., & Fenter, P. X-ray-driven reaction front dynamics at calcite-water interfaces. United States. https://doi.org/10.1126/science.aab3272
Laanait, N., Callagon, E. B. R., Zhang, Z., Sturchio, N. C., Lee, S. S., and Fenter, P. Thu .
"X-ray-driven reaction front dynamics at calcite-water interfaces". United States. https://doi.org/10.1126/science.aab3272.
@article{osti_1355825,
title = {X-ray-driven reaction front dynamics at calcite-water interfaces},
author = {Laanait, N. and Callagon, E. B. R. and Zhang, Z. and Sturchio, N. C. and Lee, S. S. and Fenter, P.},
abstractNote = {The interface of minerals with aqueous solutions is central to geochemical reactivity, hosting processes that span multiple spatiotemporal scales. Understanding such processes requires spatially and temporally resolved observations, and experimental controls that precisely manipulate the interfacial thermodynamic state. Using the intense radiation fields of a focused synchrotron X-ray beam, we drove dissolution at the calcite-aqueous interface and simultaneously probed the dynamics of the propagating reaction fronts using surface X-ray microscopy. Evolving surface structures are controlled by the time-dependent solution composition as characterized by a kinetic reaction model. At extreme disequilibria, the onset of reaction front instabilities was observed with velocities of >30 nanometers per second. As a result, these instabilities are identified as a signature of transport-limited dissolution of calcite under extreme disequilibrium.},
doi = {10.1126/science.aab3272},
journal = {Science},
number = 6254,
volume = 349,
place = {United States},
year = {Thu Sep 17 00:00:00 EDT 2015},
month = {Thu Sep 17 00:00:00 EDT 2015}
}
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https://doi.org/10.1126/science.aab3272
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Works referenced in this record:
Calculation of initial and primary yields in the radiolysis of water
journal, March 1994
- Hill, M. A.; Smith, F. A.
- Radiation Physics and Chemistry, Vol. 43, Issue 3
A model of carbon dioxide dissolution and mineral carbonation kinetics
journal, September 2009
- Mitchell, Mark J.; Jensen, Oliver E.; Cliffe, K. Andrew
- Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 466, Issue 2117
Electron microscopy of specimens in liquid
journal, October 2011
- de Jonge, Niels; Ross, Frances M.
- Nature Nanotechnology, Vol. 6, Issue 11, p. 695-704
Kinetics of Water-Rock Interaction
book, January 2008
- Brantley, Susan L.; Kubicki, James D.; White, Art F.
- Springer New York, NY
Mechanisms of classical crystal growth theory explain quartz and silicate dissolution behavior
journal, October 2005
- Dove, P. M.; Han, N.; De Yoreo, J. J.
- Proceedings of the National Academy of Sciences, Vol. 102, Issue 43
Comprehensive Study of the Hydration and Dehydration Reactions of Carbon Dioxide in Aqueous Solution
journal, December 2009
- Wang, Xiaoguang; Conway, William; Burns, Robert
- The Journal of Physical Chemistry A, Vol. 114, Issue 4, p. 1734-1740
Sea Urchin Spine Calcite Forms via a Transient Amorphous Calcium Carbonate Phase
journal, November 2004
- Politi, Y.
- Science, Vol. 306, Issue 5699
On Symmetry‐Breaking Instabilities in Dissipative Systems
journal, May 1967
- Prigogine, I.; Nicolis, G.
- The Journal of Chemical Physics, Vol. 46, Issue 9
In situ TEM imaging of CaCO3 nucleation reveals coexistence of direct and indirect pathways
journal, September 2014
- Nielsen, M. H.; Aloni, S.; De Yoreo, J. J.
- Science, Vol. 345, Issue 6201
Stable Prenucleation Calcium Carbonate Clusters
journal, December 2008
- Gebauer, Denis; Völkel, Antje; Cölfen, Helmut
- Science, Vol. 322, Issue 5909
Microscopic Evidence for Liquid-Liquid Separation in Supersaturated CaCO3 Solutions
journal, August 2013
- Wallace, A. F.; Hedges, L. O.; Fernandez-Martinez, A.
- Science, Vol. 341, Issue 6148
Full-field X-ray reflection microscopy of epitaxial thin-films
journal, October 2014
- Laanait, Nouamane; Zhang, Zhan; Schlepütz, Christian M.
- Journal of Synchrotron Radiation, Vol. 21, Issue 6
Comparative study of the kinetics and mechanisms of dissolution of carbonate minerals
journal, December 1989
- Chou, Lei; Garrels, Robert M.; Wollast, Roland
- Chemical Geology, Vol. 78, Issue 3-4
The kinetics of calcite dissolution in CO 2 -water systems at 5 degrees to 60 degrees C and 0.0 to 1.0 atm CO 2
journal, February 1978
- Plummer, L. N.; Wigley, T. M. L.; Parkhurst, D. L.
- American Journal of Science, Vol. 278, Issue 2
Image contrast in X-ray reflection interface microscopy: comparison of data with model calculations and simulations
journal, October 2008
- Fenter, P.; Park, C.; Kohli, V.
- Journal of Synchrotron Radiation, Vol. 15, Issue 6
Spatial organization of the extracellular matrix regulates cell-cell junction positioning
journal, January 2012
- Tseng, Q.; Duchemin-Pelletier, E.; Deshiere, A.
- Proceedings of the National Academy of Sciences, Vol. 109, Issue 5
Observation of subnanometre-high surface topography with X-ray reflection phase-contrast microscopy
journal, September 2006
- Fenter, Paul; Park, Changyong; Zhang, Zhan
- Nature Physics, Vol. 2, Issue 10
Electron–Water Interactions and Implications for Liquid Cell Electron Microscopy
journal, September 2014
- Schneider, Nicholas M.; Norton, Michael M.; Mendel, Brian J.
- The Journal of Physical Chemistry C, Vol. 118, Issue 38
Theory of Radiation Chemistry. II. Track Effects in Radiolysis of Water
journal, June 1953
- Samuel, Aryeh H.; Magee, John L.
- The Journal of Chemical Physics, Vol. 21, Issue 6
Dissolution kinetics of calcite, dolomite and magnesite at 25 °C and 0 to 50 atm pCO2
journal, April 2005
- Pokrovsky, Oleg S.; Golubev, Sergey V.; Schott, Jacques
- Chemical Geology, Vol. 217, Issue 3-4
Using Krylov Methods in the Solution of Large-Scale Differential-Algebraic Systems
journal, November 1994
- Brown, Peter N.; Hindmarsh, Alan C.; Petzold, Linda R.
- SIAM Journal on Scientific Computing, Vol. 15, Issue 6
NIH Image to ImageJ: 25 years of image analysis
journal, June 2012
- Schneider, Caroline A.; Rasband, Wayne S.; Eliceiri, Kevin W.
- Nature Methods, Vol. 9, Issue 7
Dissolution Kinetics of Calcite in 0.1 M NaCl Solution at Room Temperature: An Atomic Force Microscopic (AFM) Study
journal, January 2000
- Shiraki, Ryoji; Rock, Peter A.; Casey, William H.
- Aquatic Geochemistry, Vol. 6, Issue 1, p. 87-108
The Pulse Radiolysis of Deaerated Aqueous Carbonate Solutions. I. Transient Optical Spectrum and Mechanism. II. pK for OH Radicals 1
journal, July 1966
- Weeks, James L.; Rabani, Joseph
- The Journal of Physical Chemistry, Vol. 70, Issue 7
Variation of Crystal Dissolution Rate Based on a Dissolution Stepwave Model
journal, March 2001
- Lasaga, A. C.
- Science, Vol. 291, Issue 5512
The Hydrated Electron: Properties and reactions of this most reactive and elementary of aqueous negative ions are discussed
journal, October 1964
- Hart, E. J.
- Science, Vol. 146, Issue 3640
Computer modelling of the radiolysis in an aqueous lithium salt blanket: Suppression of radiolysis by addition of hydrogen
journal, August 1990
- Elliot, A. John; McCracken, David R.
- Fusion Engineering and Design, Vol. 13, Issue 1