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Title: X-ray-driven reaction front dynamics at calcite-water interfaces

Journal Article · · Science

The interface between minerals and aqueous solutions hosts globally important biogeochemical processes such as the growth and dissolution of carbonate minerals. 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/water interface and simultaneously probed the dynamics of the propagating reaction fronts using surface x-ray microscopy. Evolving surface structures were controlled by the time-dependent solution composition, as characterized by a kinetic reaction model. At extreme disequilibria, we observed the onset of reaction front instabilities with velocities of > 30 nanometers per second. These instabilities serve as a signature of transport-limited dissolution of calcite under extreme disequilibrium.

Research Organization:
Argonne National Laboratory (ANL), Argonne, IL (United States)
Sponsoring Organization:
USDOE Office of Science - Office of Basic Energy Sciences - Chemical Sciences, Geosciences, and Biosciences Division
DOE Contract Number:
AC02-06CH11357
OSTI ID:
1392060
Journal Information:
Science, Vol. 349, Issue 6254; ISSN 0036-8075
Publisher:
AAAS
Country of Publication:
United States
Language:
English

References (28)

Calculation of initial and primary yields in the radiolysis of water journal March 1994
A model of carbon dioxide dissolution and mineral carbonation kinetics
  • Mitchell, Mark J.; Jensen, Oliver E.; Cliffe, K. Andrew
  • Proceedings of the Royal Society A: Mathematical, Physical and Engineering Sciences, Vol. 466, Issue 2117 https://doi.org/10.1098/rspa.2009.0349
journal September 2009
Electron microscopy of specimens in liquid journal October 2011
Mechanisms of classical crystal growth theory explain quartz and silicate dissolution behavior journal October 2005
Comprehensive Study of the Hydration and Dehydration Reactions of Carbon Dioxide in Aqueous Solution journal December 2009
Sea Urchin Spine Calcite Forms via a Transient Amorphous Calcium Carbonate Phase journal November 2004
On Symmetry‐Breaking Instabilities in Dissipative Systems journal May 1967
In situ TEM imaging of CaCO3 nucleation reveals coexistence of direct and indirect pathways journal September 2014
Stable Prenucleation Calcium Carbonate Clusters journal December 2008
Microscopic Evidence for Liquid-Liquid Separation in Supersaturated CaCO3 Solutions journal August 2013
Full-field X-ray reflection microscopy of epitaxial thin-films journal October 2014
Comparative study of the kinetics and mechanisms of dissolution of carbonate minerals journal December 1989
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
Image contrast in X-ray reflection interface microscopy: comparison of data with model calculations and simulations journal October 2008
Spatial organization of the extracellular matrix regulates cell-cell junction positioning journal January 2012
Observation of subnanometre-high surface topography with X-ray reflection phase-contrast microscopy journal September 2006
Electron–Water Interactions and Implications for Liquid Cell Electron Microscopy journal September 2014
Theory of Radiation Chemistry. II. Track Effects in Radiolysis of Water journal June 1953
Dissolution kinetics of calcite, dolomite and magnesite at 25 °C and 0 to 50 atm pCO2 journal April 2005
Using Krylov Methods in the Solution of Large-Scale Differential-Algebraic Systems journal November 1994
NIH Image to ImageJ: 25 years of image analysis journal June 2012
Dissolution Kinetics of Calcite in 0.1 M NaCl Solution at Room Temperature: An Atomic Force Microscopic (AFM) Study journal January 2000
The Pulse Radiolysis of Deaerated Aqueous Carbonate Solutions. I. Transient Optical Spectrum and Mechanism. II. pK for OH Radicals 1 journal July 1966
Variation of Crystal Dissolution Rate Based on a Dissolution Stepwave Model journal March 2001
The Hydrated Electron: Properties and reactions of this most reactive and elementary of aqueous negative ions are discussed journal October 1964
Computer modelling of the radiolysis in an aqueous lithium salt blanket: Suppression of radiolysis by addition of hydrogen journal August 1990
Kinetics of Water-Rock Interaction book January 2008
Radiation Chemistry of Gases book January 1999

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Mechanisms and Dynamics of Mineral Dissolution: A New Kinetic Monte Carlo Model journal July 2019
Picoscale materials engineering journal September 2017
X-ray microscopy journal July 1965

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