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Title: 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 Lab. (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. https://doi.org/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 = {2015},
month = {9}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record
https://doi.org/10.1126/science.aab3272

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Cited by: 14 works
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