X-ray Raman scattering study of hydrothermal fluids: The ... · 1 X-ray Raman scattering study of...
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X-ray Raman scattering study of hydrothermal fluids: The case of aqueous
sodium chloride solutions
Mirko [email protected]
IXS 2019, Stony Brook28.6.2019
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Motivation - hydrothermal fluids in geology
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An important factor in the formation of magma and volcanic arcs
SubductionZone
USGS
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Motivation - hydrothermal fluids in geology
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An important factor in the formation of magma and volcanic arcs
Transport agent of energy and mass in the earth’s mantle Formation of ore deposits
ETH Zurichgeologyin.com
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Hydrothermal diamond anvil cell (HDAC)
Using a Bassett-type HDAC
Temperature range from -190 to 800°C and pressures up to 4 kbar
Using melting points of: azobenzene, sodium nitrate for temperature calibration with a precision of 1.5°C
Flushing the cell with Ar+H2 mixture to prevent oxidation of the metallic parts
Utilizing microscope camera for live-view of sample during measurements
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C. Schmidt, K. Rickers, Am. Min. 2003
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Alignment of diamonds with one sliding and one rotational disk
Using a laser drilled recess in one of the diamonds as sample chamber No gasket needed!
X-ray
Hydrothermal diamond anvil cell (HDAC)
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C. Schmidt, I. Chou
PtRh10
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XRS at the oxygen K-edge
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Ch. J. Sahle et al, PNAS, 2013
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XRS at the oxygen K-edge
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PreI
MainII
PostIII
J. Niskanen et al, Phys. Rev 2017; PNAS, 2019
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XRS at the oxygen K-edge
Spectral features are correlated to the local structural environment of the
probed oxygen atom
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J. Niskanen et al, Phys. Rev 2017; PNAS, 2019
PreI
MainII
PostIII
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XRS spectra of sodium chloride
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XRS spectra of sodium chloride
T
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XRS spectra of sodium chloride
Reduction in the total number of hydrogen bonded molecules
General loss of tetrahedrality with increasing temperature
T
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Hydrothermal H2O, NaOH and HCl solutions
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Ch. J. Sahle et al, J. Phys. Chem. B, 2017
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Hydrothermal H2O, NaOH and HCl solutions
Overall spectral changes are similar to NaCl solution
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Ch. J. Sahle et al, J. Phys. Chem. B, 2017
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Comparison experiment – calculation
11Ch. J. Sahle et al, J. Phys. Chem. B, 2017
K. Gilmore, Comput. Phys. Commun. 2015; OCEAN
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Quantitative comparison: experiment – calculation
Experimental trends are almost completely reproduced
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Extracted structural information
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Destabilizing effect of the dissolved salt ions on the water structure
Extracted structural information
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Destabilizing effect of the dissolved salt ions on the water structure
Formation of contact pair ions reduce the destabilizing effect Structural similarity to pure water increases
Contact ion-pairs
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Comparison of NaCl and H2O
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Comparison of NaCl and H2O
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Comparison of NaCl and H2O
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Comparison of NaCl and H2O
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Acknowledgments
Christian Schmidt
Christoph Sahle
Sandro Jahn
Christian Sternemann, Robin Sakrowski,Christian Albers, Metin Tolan
Max Wilke
Hlynur Gretarsson, Martin Sundermann
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Acknowledgments
Christian Schmidt
Christoph Sahle
Sandro Jahn
Christian Sternemann, Robin Sakrowski,Christian Albers, Metin Tolan
Max Wilke
Hlynur Gretarsson, Martin Sundermann
Thank you for your attention!
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Determination of thermodynamic conditions
RT
200°C
300°C
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1bar
21bar
1kbarModified from C. Schmidt, I. Chou6