Hydration structure of the barite (001)–water interface: Comparison of x-ray reflectivity with molecular dynamics simulations
Abstract
The three-dimensional structure of the barite (001)-water interface was studied using in situ specular and nonspecular X-ray reflectivity (XR). Displacements of the barium and sulfate ions in the surface of a barite crystal and the interfacial water structure were defined in the analyses. The largest relaxations (0.13 Å lateral and 0.08 Å vertical) were observed for the barium and sulfate ions in the topmost unit cell layer, which diminished rapidly with depth. The best fit structure identified four distinct adsorbed species, which in comparison with molecular dynamics (MD) simulations reveals that they are associated with positions of adsorbed water, each of which coordinates one or two surface ions (either barium, sulfate, or both). These water molecules also adsorb in positions consistent with those of bariums and sulfates in the bulk crystal lattice. These results demonstrate the importance of combining high resolution XR with MD simulations to fully describe the atomic structure of the hydrated mineral surface. The agreement between the results indicates both the uniqueness of the structural model obtained from the XR analysis and the accuracy of the force field used in the simulations.
- Authors:
-
- Argonne National Lab. (ANL), Argonne, IL (United States)
- Univ. of Chicago, Chicago, IL (United States)
- Karlsruher Institute fur Technologie, Karlsruhe (Germany)
- Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
- Publication Date:
- Research Org.:
- Argonne National Laboratory (ANL), Argonne, IL (United States); Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States); The University of Chicago
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES)
- OSTI Identifier:
- 1364403
- Alternate Identifier(s):
- OSTI ID: 1376531; OSTI ID: 1508010
- Report Number(s):
- DOE-UCHICAGO-14466-2
Journal ID: ISSN 1932-7447; 135369
- Grant/Contract Number:
- AC02-06CH11357; AC05-00OR22725; FG02-94ER14466
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Physical Chemistry. C
- Additional Journal Information:
- Journal Volume: 121; Journal Issue: 22; Journal ID: ISSN 1932-7447
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; barite; interface; molecular dynamics simulations; x-ray reflectivity; 58 GEOSCIENCES; Synchrotron radiation
Citation Formats
Bracco, Jacquelyn N., Lee, Sang Soo, Stubbs, Joanne E., Eng, Peter J., Heberling, Frank, Fenter, Paul, and Stack, Andrew G. Hydration structure of the barite (001)–water interface: Comparison of x-ray reflectivity with molecular dynamics simulations. United States: N. p., 2017.
Web. doi:10.1021/acs.jpcc.7b02943.
Bracco, Jacquelyn N., Lee, Sang Soo, Stubbs, Joanne E., Eng, Peter J., Heberling, Frank, Fenter, Paul, & Stack, Andrew G. Hydration structure of the barite (001)–water interface: Comparison of x-ray reflectivity with molecular dynamics simulations. United States. https://doi.org/10.1021/acs.jpcc.7b02943
Bracco, Jacquelyn N., Lee, Sang Soo, Stubbs, Joanne E., Eng, Peter J., Heberling, Frank, Fenter, Paul, and Stack, Andrew G. Thu .
"Hydration structure of the barite (001)–water interface: Comparison of x-ray reflectivity with molecular dynamics simulations". United States. https://doi.org/10.1021/acs.jpcc.7b02943. https://www.osti.gov/servlets/purl/1364403.
@article{osti_1364403,
title = {Hydration structure of the barite (001)–water interface: Comparison of x-ray reflectivity with molecular dynamics simulations},
author = {Bracco, Jacquelyn N. and Lee, Sang Soo and Stubbs, Joanne E. and Eng, Peter J. and Heberling, Frank and Fenter, Paul and Stack, Andrew G.},
abstractNote = {The three-dimensional structure of the barite (001)-water interface was studied using in situ specular and nonspecular X-ray reflectivity (XR). Displacements of the barium and sulfate ions in the surface of a barite crystal and the interfacial water structure were defined in the analyses. The largest relaxations (0.13 Å lateral and 0.08 Å vertical) were observed for the barium and sulfate ions in the topmost unit cell layer, which diminished rapidly with depth. The best fit structure identified four distinct adsorbed species, which in comparison with molecular dynamics (MD) simulations reveals that they are associated with positions of adsorbed water, each of which coordinates one or two surface ions (either barium, sulfate, or both). These water molecules also adsorb in positions consistent with those of bariums and sulfates in the bulk crystal lattice. These results demonstrate the importance of combining high resolution XR with MD simulations to fully describe the atomic structure of the hydrated mineral surface. The agreement between the results indicates both the uniqueness of the structural model obtained from the XR analysis and the accuracy of the force field used in the simulations.},
doi = {10.1021/acs.jpcc.7b02943},
journal = {Journal of Physical Chemistry. C},
number = 22,
volume = 121,
place = {United States},
year = {Thu May 11 00:00:00 EDT 2017},
month = {Thu May 11 00:00:00 EDT 2017}
}
Web of Science
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