Experimental studies in high temperature aqueous chemistry at Oak Ridge National Laboratory Page: 1 of 12
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EXPERIMENTAL STUDIES IN HIGH TEMPERATURE AQUEOUS
CHEMISTRY AT OAK RIDGE NATIONAL LABORATORY
R. E. Mesmer, D. A. Palmer, J. M. Simonson, H. F. Holmes, P. C. Ho,
D. J. Wesolowski, and M. S. Gruszkiewicz
Chemical and Analytical Sciences Division, Oak Ridge National Laboratory,
P.O. Box 2008, Oak Ridge, Tennessee 37831
Abstract: Experimental research is conducted and models are developed in a long-
standing program at Oak Ridge on the aqueous chemistry at high temperatures of
broad classes of electrolytes emphasizing thermodynamics of reaction equilibria
and excess thermodynamic properties of electrolytes. Our experimental methods,
their capabilities, data analysis, and results will be summarized. The relevance of
the work to problems in power plants, natural and industrial processes as well as
basic solution chemistry and geochemistry are given. Progress in potentiometry,
electrical conductivity, flow calorimetry, and isopiestic research will be described.
The future in this field demands greater precision in measurements and significant
gains in our understanding of the solvation phenomena especially in the vicinity and
beyond the critical point for water. The communities who do research on scattering,
spectroscopy, and computer simulations can help guide these efforts through studies
at exteme conditions.
Aqueous chemistry is of great importance in many natural and technological applications involving high
temperatures, e.g., natural processes such as those geochemical processes of ore deposition, geothermal
reservoir behavior, and transport from hydrothermal oceanic vents. It is also of great importance to
industrial and technological applications such as steam generation in power plants, disposal of nuclear and
hazardous wastes, and in supercritical water oxidation of hazardous organic wastes. Water as a solvent
has challenged scientists from the beginning because of its molecular and solvation properties that lead to
large non-idealities for its solutions of most solutes. As a result much experimental data are required to
accurately describe the chemistry of even the simplest solutes especially due to the wide range of
temperature and pressure over which the liquid phase exists (critical point: 3740C, 221 bar).
A large database on the physical chemistry of water and its solutions has been generated at Oak Ridge
National Laboratory since the 1960's using a broad array of unique equipment yielding in excess of four-
hundred publications. This work has had substantial impact on many industrial processes as well as the
sciences of basic solution chemistry, thermodynamics, and geochemistry. The principal support for this
work has been from the Divisions of Chemical Sciences and Geosciences of the Office of Basic Energy
Science of DOE but in certain specialized areas support has come from the Division of Geothermal
Technology and the Office of Technology Development of DOE, the Electric Power Research Institute,
and from the Knolls Atomic Power Laboratory.
The authors wish to recognize at the outset the pioneering accomplishments of W. L. Marshall and C.F.
Baes, Jr. in this field at ORNL and to acknowledge that much of what has followed was built on the
foundation they laid.
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Mesmer, R.E.; Palmer, D.A.; Simonson, J.M.; Holmes, H.F.; Ho, P.C.; Wesolowski, D.J. et al. Experimental studies in high temperature aqueous chemistry at Oak Ridge National Laboratory, article, January 1, 1996; Tennessee. (digital.library.unt.edu/ark:/67531/metadc685715/m1/1/: accessed July 16, 2018), University of North Texas Libraries, Digital Library, digital.library.unt.edu; crediting UNT Libraries Government Documents Department.