Hydrothermal Experimental Data
Hydrothermal Experimental Data Edited by V.M. Valyashko
© 2008 John Wiley & Sons, Ltd. ISBN: 978-0-470-09465-5
Hydrothermal Experimental Data
Edited by
Vladimir M. Valyashko
A John Wiley & Sons, Ltd., Publication
This edition fi rst published 2008
© 2008 John Wiley & Sons, Ltd
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CD Table of Contents ix
Foreword xi
Preface xiii
Acknowledgements xv
1 Phase Equilibria in Binary and Ternary Hydrothermal Systems 1
Vladimir M. Valyashko
1.1 Introduction 1
1.2 Experimental methods for studying hydrothermal phase equilibria 3
1.2.1 Methods of visual observation 73
1.2.2 Methods of sampling 74
1.2.3 Methods of quenching 80
1.2.4 Indirect methods 82
1.3 Phase equilibria in binary systems 86
1.3.1 Main types of fl uid phase behavior 86
1.3.2 Classifi cation of complete phase diagrams 87
1.3.3 Graphical representation and experimental examples of binary phase diagrams 91
1.4 Phase equilibria in ternary systems 103
1.4.1 Graphical representation of ternary phase diagrams 103
1.4.2 Derivation and classifi cation of ternary phase diagrams 105
References 119
2 pVTx Properties of Hydrothermal Systems 135
Horacio R. Corti and Ilmutdin M. Abdulagatov
2.1 Basic principles and defi nitions 135
2.2 Experimental methods 136
2.2.1 Constant volume piezometers (CVP) 136
2.2.2 Variable volume piezometers (VVP) 137
2.2.3 Hydrostatic weighing technique (HWT) 138
2.2.4 Vibrating tube densimeter (VTD) 139
2.2.5 Synthetic fl uid inclusion technique 140
2.3 Theoretical treatment of pVTx data 140

4.5 General trends 221
4.5.1 Specifi c conductivity as a function of temperature, concentration and density 221
4.5.2 The limiting molar conductivity 222
4.5.3 Concentration dependence of the molar conductivity and association constants 223
4.5.4 Molar conductivity as a function of temperature and density 224
4.5.5 Conductivity in ternary systems 224
References 224
5 Thermal Conductivity 227
Ilmutdin M. Abdulagatov and Marc J. Assael
5.1 Introduction 227
5.2 Experimental techniques 228
5.2.1 Parallel-plate technique 228
5.2.2 Coaxial-cylinder technique 235
5.2.3 Transient hot-wire technique 239
5.2.4 Conclusion 241
5.3 Available experimental data 242
5.3.1 Temperature dependence 242
5.3.2 Pressure dependence 244
5.3.3 Concentration dependence 245
5.4 Discussion of experimental data 245
References 246
6 Viscosity 249
Ilmutdin M. Abdulagatov and Marc J. Assael
6.1 Introduction 249
6.2 Experimental techniques 252
6.2.1 Capillary-fl ow technique 253
6.2.2 Oscillating-disk technique 255
6.2.3 Falling-body viscometer 257
6.2.4 Conclusion 259
6.3 Available experimental data 260

sor, colleague and friend Ulrich Franck, but unfortunately,
he did not live to see the completion of an endeavor that he
had most arduously advocated. It is therefore with trepida-
tion that I, who consider myself at best as one of his many
disciples, act here as his substitute.
An immense amount of experimental material on water/
steam and aqueous systems has been obtained during the
past century, and even before, in laboratories around the
world, much of it not readily accessible. Especially during
the cold-war years, the International Association for Proper-
ties of Water and Steam (IAPS, later IAPWS) was among
the few international organizations in which experts in the
former Soviet Union actively participated. Franck, impressed
by the access IAPWS had to experimental data obtained
worldwide, repeatedly urged the organization to collect and
evaluate these data, bundling them in what he used to call
an Atlas.
This book presents evaluated experimental data acquired,
as well as some of the theoretical models developed, for
two-and three-component hydrothermal systems. These are
aqueous solutions containing both molecular and/or electro-
lytic solutes at high temperature and pressure, approaching
and exceeding water’s critical temperature. Hydrothermal
systems are ubiquitous, in the deep ocean and in the earth’s
crust, and of major importance in geology, geochemistry,
mining, and in industrial practices such as metallurgy and
the synthesis and growth of crystals.
The theoretical understanding of the phase behavior of
fl uid mixtures was developed in the second half of the 19
th

Russian organic chemist Vittorf (1869–1929) met Bakhuis
Roozeboom in Göttingen in 1904. Vittorf then used Bakhuis
Roozeboom’s phase theory and classifi cation as the basis
for his own 1909 book “Theory of Alloys in Application to
Metallic Systems”. From the late 1930s through the 1980s,
physical chemist Krichevskii and his many collaborators,
thoroughly familiar with the work of the Dutch School,
studied fl uid phase behavior and critical phenomena experi-
mentally, and discovered several predicted effects, such as
tricriticality, as well as gas-gas phase separation in both
nonaqueous and aqueous mixtures. Starting just after WWII,
thermal physicist Stirikovich, physical chemists Mashovetz
and Ravich, and geochemist Khitarov, began to explore
phase behavior and solution properties of aqueous systems
up to high temperatures and pressures.
Göttingen professors Nernst, Tammann, and Eucken had
built a physical chemistry laboratory for electrochemistry,
as well as for high-pressure phase equilibria studies and
calorimetry. It was there that Franck, a pupil of Eucken,
began his life’s work on the experimental exploration of the
properties of high-temperature, high-pressure aqueous solu-
tions of air constituents, acids, bases, and salts, studying
phase behavior as well as dielectric and electrochemical
properties. He and his disciples explored this fi eld through-
out the second half of the 20
th
century.
In the USA, just after WWI, geochemist Morey began
the fi rst phase equilibria studies in hydrothermal systems.
By the middle of the 20

duced practical models for use in the fi eld.
On approaching the critical point, however, water’s
unusual dielectric and electrolytic properties diminish, its
compressibility increases hugely, and its behavior becomes
more like that of other, simpler near-critical fl uids. The
asymmetric solution model then becomes increasingly
strained. This message was brought home forcefully in the
early 1980s by the elegant experimental data of Wood and
coworkers on partial molar properties of the solute in dilute
electrolyte solutions near the water critical point. These
usually well-behaved properties exhibited divergences at
that critical point, while higher derivatives, such as the
partial molar heat capacity, displayed wild swings in water’s
critical region. When Wood et al. repeated the experiments
in the argon-water system, however, similar anomalies were
found, be it of the opposite sign and of smaller amplitude – a
sure sign that the effects they had seen were not electrolytic
in origin, but a general thermodynamic property of a dilute
near-critical mixture. In fact, in the early 1970s, Krichevskii
and coworkers had discovered the divergence of the
infi nite-dilution partial molar volume of the solute experi-
mentally, and explained it correctly.
Aqueous mixtures near and above the water critical point
can then be modeled by Van der Waals-like descriptions of
fl uid mixtures that treat the solvent and solutes equivalently
but ignore the charges. Franck and coworkers, for instance,
produced the phase separations observed in several binary
and ternary aqueous systems in the hydrothermal range
from simple Van-der-Waals type models.
A theory that combines in a unifi ed way the electrolytic

been extensively applied in a variety of fi elds of science and
technology, ranging from development of the chemistry of
solutions and heterogeneous mixtures, thermophysics, crys-
tallography, geochemistry and oceanography to industrial
and environmental applications, such as electric power gen-
eration, hydrothermal technologies of crystal growth and
nanoparticle syntheses, hydrometallurgy and the treatment
of sewage and the destruction of hazardous waste.
The available experimental data for binary and ternary
systems can be used as primary reference data, or as the
initial values for further refi nement, in order to obtain rec-
ommended values, particularly, the internally consistent
values that are used for thermodynamic calculations and
modelling of multicomponent equilibria and reactions.
However, the recommended values are derivatives and
largely depend on the method of treatment based on more
or less rigorous and varying models. Thus, a collection of
experimental data not only incorporates original informa-
tion from widely scattered scientifi c publications, it is fun-
damental and provides the foundation for modern and future
databases, and recommended values.
The main goals of this book are to collect, collate and
compile the available original experimental data on phase
equilibria and solution properties for binary and ternary
hydrothermal systems, to review these data, and to consider
the employed experimental methods and the ways these data
were refi ned/processed and presented.
The work on collecting hydrothermal experimental data
was started in the mid-1990s by Dr V. M. Valyashko (Kur-
nakov Institute of General and Inorganic Chemistry, Russian

original experimental values. The accompanying summary
tables, arranged in alphabetic order of the nonaqueous com-
ponents, list the temperatures, pressures and concentrations,
types of data and experimental methods employed in their
measurements, the uncertainty claimed by the authors as
well as the references (the fi rst author and the year of pub-
lication). The table code refers the reader to the original data
set in the appendices on the CD. The tables of experimental
data (with brief comments on each set of experimental
measurements) in the appendices are also arranged in alpha-
betic order of nonaqueous components. However, the order
of the systems in the appendices is usually not exactly the
same as in the summary tables. There are no subdivisions
in appendices, whereas in the summary tables the binary
and ternary systems are often placed in separate divisions
or subdivisions such as inorganic and organic compounds
or electrolytes, nonelectrolytes, acids, etc.
The text parts of the chapters, besides the general char-
acteristics of the available experimental data mentioned
above, usually contain several special topics and aspects of
material presentation.
Chapter 1 (Phase Equilibria in Binary and Ternary Hydro-
thermal Systems, V. M. Valyashko, Russia) contains a
description of the general trends of sub- and supercritical
phase behaviour in binary and ternary systems taking into
account both stable and metastable equilibria. A presenta-
tion of the various types of phase diagrams aims to show
the possible versions of phase transitions under hydrother-
mal conditions and to help the reader with the determination
of where the phase equilibrium occurs in p–T–X space, and

the literature.
xiv Preface
Special attention in Chapter 4 (Electrical Conductivity in
Hydrothermal Binary and Ternary Systems, H. R. Corti
(Argentina)) is paid to the procedures for obtaining infor-
mation on the thermodynamic properties of electrolytes
(including a determination of the limiting conductivity and
association constants) from the measured electrical conduc-
tivity of diluted solutions above 200 °C. However, the
behaviour of specifi c and molar conductivity in concen-
trated electrolyte solutions is also carefully discussed in the
chapter.
Chapters 5 and 6 (Thermal Conductivity and Viscosity,
I. M. Abdulagatov (Russia/USA) and M. J. Assael (Greece))
show not only the typical temperature, pressure and con-
centration dependencies of properties in hydrothermal
solutions, but also make a preliminary comparison of
various datasets for several systems to help the reader
choose which values to use. The empirical and semi-
empirical correlations which are necessary because of the
lack of theoretical background, employed in the reviewed
literature are also discussed.
Chapter 7 (Calorimetric Properties of Hydrothermal
Solutions, V. M. Valyashko (Russia) and M. S. Gruszkiewicz
(USA)), indicates the experimentally determined calorimet-
ric quantities of considerable current use, gives a brief
description of experimental methods for hydrothermal mea-
surements and contains a summary table with information
about the systems studied and the corresponding calorimet-
ric measurements.

I. Schmulovich, A. A. Slobodov, N. A. Smirnova, N. G.
Sretenskaya, M. A. Urusova, A. S. Viktorov, I. V. Zakirov,
V. I. Zarembo, A. V. Zotov (Russia), L. Z. Boshkov
(Ukraine), R. B. Dooley, A. H. Harvey, P. C. Ho, W. L.
Marshall, R. E. Mesmer, A. V. Plyasunov, J. M. Simonson,
R. H. Wood (USA).
Finally, I also would like to express my thanks to my wife
Luba and daughters Aliona and Katya for their constant
support and understanding.
Vladimir M.Valyashko
Moscow
1
Phase Equilibria in Binary and Ternary
Hydrothermal Systems
Vladimir M. Valyashko
Kurnakov Institute of General and Inorganic Chemistry, Russian Academy of Sciences, Moscow, Russia
1.1 INTRODUCTION
Defi ning the phase composition of the mixture at a certain
pressure and temperature is the fi rst step in any scientifi c
investigation and obligatory information for any practical
application of that mixture.
If the physical state of aqueous or any other systems at
ambient conditions can easily be determined, the phase
composition of the systems at high temperatures and
pressures should be specially studied using fairly complex
equipment.
Systematic scientifi c studies of infl uence of temperature
and pressure on a phase state of individual compounds
and mixtures were begun in the eighteenth century (D.
Fahrenheit, R. Reaumur, A. Celsius, M.V. Lomonosov, A.

, He
2
– CO
2
, He
2
– NH
3
and in
Ar – NH
3
mixtures (Krichevskii and Bol’shakov, 1941;
Krichevskii, 1952; Tsiklis, 1969), that confi rmed theo -
retical prediction of Van der Waals (Van der Waals and
Kohnstamm, 1927). It was shown that a separation of super-
critical fl uids can exist in the temperature range above the
highest critical temperature of the less volatile component.
Another important result obtained in the last century was
also connected with the critical phenomena. In 1926
Kohnstamm (Kohnstamm, 1926) pointed out the theoretical
possibility of fi nding a critical point ‘of second order’ in a
ternary liquid mixture – a point at which three coexisting
fl uid phases simultaneously become identical. In 1962–70
this point was confi rmed experimentally in two Russian
aboratories (of Prof. I.R. Krichevskii and Prof. R.V.
Mertslin) (Radyshevskaya et al., 1962; Krichevskii et al.,
1963; Myasnikova et al., 1969; Efremova and Shvarts, 1966,
1969, 1972; Shvarts and Efremova, 1970; Nikurashina
et al., 1971). In the 1970s such a type of phase transition,
called ‘a tricritical point’, was theoretically interpreted

2
NH) and ethylene (C
2
H
4
)) – p-chloroaniline (o-
xylidin (C
8
H
11
N), o-nitrophenol (C
6
H
5
NO
3
), m-chloronitro-
benzene (C
6
H
4
ClNO
2
)) (Smits, 1905, 1911; Buechner, 1906,
1918; Scheffer and Smittenberg, 1933).
However, the fi rst experimental studies of H
2
O – SiO
2
,

material synthesis, supercritical water oxidation for hazard-
ous waste destruction) and of fossil and nuclear power engi-
neering. The main volume of experimental data for aqueous
systems at high temperatures and pressures now available
was obtained during the past 50–60 years, whereas the most
precise measurements of hydrothermal solution properties
became possible only from the 1980s onwards (Wood,
1989).
Van der Waals and his school developed the ‘classical
approach’ to phase diagram derivation, in which phase
behavior of mixtures was established by investigation of the
behavior of thermodynamic functions (free energy) in p-V-
T-x space, calculated with the equation of state. Originally,
theoretical derivations of phase diagrams were done by a
topological method. After the main features of a geometry
of thermodynamic surfaces (p-V-T-x dependences of
Helmholtz or Gibbs free energy) were obtained from limited
calculations available at that time using the equation of
state. The following continuous transformations and combi-
nations of the geometrical features of the surfaces were
determined topologically as well as a derivation of topologi-
cal schemes of phase diagrams from the interplay of the
thermodynamic surfaces. As a result of such investigations
it was established that there is a limited number of various
types of fl uid phase diagram for binary systems. A topologi-
cal approach and knowledge of the regularities of phase
behavior and intersections of thermodynamic surfaces for
various phases (included the solid phase) permitted deriva-
tion of not only several types of fl uid phase diagrams but
also of the schemes of phase diagrams with solid phase

tion of phase equilibria with solid phases. To do so either
simultaneous investigation of two equations of state (for
liquid-gas and for solid phases) should be considered or the
usage of the topological method at the level of topological
schemes of phase diagram rather than at the level of thermo-
dynamic surfaces. Modern knowledge of phase diagrams
construction allows us to classify the main types of dia-
grams and to defi ne a few regularities of transformation of
one type of phase diagram into another.
This chapter reviews general characteristics of phase
behavior in sub- and supercritical binary and ternary aqueous
systems obtained in theoretical and experimental studies. It
starts with a brief presentation of the main experimental
methods employed to study the hydrothermal phase
equilibria.
The major body of the chapter provides an overview of
recent developments in our understanding of binary and
ternary phase diagram construction based on modern theo-
retical approaches to phase diagram derivation and on the
available experimental data. In case of binary system special
attention is drawn to the method of continuous topological
transformation of phase diagrams and to a demonstration of
systematic classifi cation of complete phase diagrams, which
describe all possible types of phase behavior in a wide range
of parameters. The main types of binary phase diagrams are
represented by topological schemes illustrated by experi-
mental results.
Methods of topological schemes for fl uid and complete
phase diagrams derivation and main features of phase
behavior at sub- and supercritical conditions for ternary

information (types of studied phase equilibria, experimental
methods, ranges of studied temperature, pressure and com-
position) about the experimental data obtained for one
system or several relevant systems from the publication(s)
and collected in Appendix 1.1.
1.2 EXPERIMENTAL METHODS FOR STUDYING
HYDROTHERMAL PHASE EQUILIBRIA
Over the years different experimental techniques at high
parameters of state were implied to study phase behaviors
(Tsiklis, 1968, 1976; Laudise, 1970; Ulmer, 1971; Jones
and Staehle, 1976; Styrikovich and Reznikov, 1977; Isaacs,
1981; Garmenitskiy and Kotelnikov, 1984; Zharikov et al.,
1985; Sherman and Tadtmuller, 1987; Ulmer and Barnes,
1987; Byrappa and Yoshimura, 2001; Hefter and Tomkins,
2003). The purpose of this review is to summarize existing
experimental methods for studing phase equilibria in
aqueous systems over a wide range of p-T-x parameters, to
describe briefl y major features of experimental procedures,
and to provide examples of the method related apparatus
along with their advantages and limitations.
Experimental methods could be considered as either ‘syn-
thetic’ and ‘analytic’ or static and dynamic (fl ow) methods.
In the ‘synthetic’ methods the phase transitions are studied
and the p-T parameters of phase transformations are recorded,
whereas the compositions of the coexistent phases are deter-
mined from the composition of initial mixture charged into
the cell. The ‘analytic’ methods determine compositions of
equilibrium phases directly at given temperature and pres-
sure, ignoring the study of phase transitions. The dynamic
(fl ow) methods are distinguished from the static ones by the

thermal fl uid composition and salt solubility in vapor by
measuring the intensity of radiation of aqueous solution
without sampling or quenching. There are several cases of
tentative experiments on solubility measurements of sul-
fi des (Ag
2
S, SnS and ZnS) at elevated temperatures (below
200 °C) (Olshanski et al., 1959; Nekrasov et al., 1982) and
in temperature gradient conditions (Relly, 1959). In some
cases the radioactive tracers are used only to determine the
concentration of samples obtained by the method of sam-
pling or quenching (Ampelogova et al., 1989). The experi-
mental studies of isotope partitioning in hydrothermal
systems (e.g. Shmulovich et al., 1999; Driesner and Seward,
2000; Chacko et al., 2001; Horita and Cole, 2004 etc.) are
relevant to isotope chemistry in aqueous reactions but do
not pursue the goal of phase equilibria determination and
will be not discussed in this chapter.
Certainly, this classifi cation is largely arbitrary and not
exhaustive because in reality experimental methods are
highly diversifi ed and often contain the combinations of
various techniques in one run. For instance, the measure-
ments using the visual cell with a movable piston (for chang-
ing the inner volume of the vessel and for separation of the
studied mixture from the pressure medium) (see Figure 1.1)
permit us to observe the phase transformation, to determine
the break points (corresponding to the phase transition) on
the pressure versus temperature isochore or on the pressure
versus volume isotherm for the known composition and to
sample the equilibrium phases at predetermined tempera-

th
column), pressure – Pressure (5
th

column), and composition – Composition (6
th
column). The numbers of tables with hydrothermal experimental data, located in the Appendix (
Tables), and the literature sources of that data
(Reference) are indicated in the 7
th
and 8
th
columns, respectively.
Although the tables in the Appendix contain only high-temperature data (usually starting from 200
°C and above), an information about the low-temperature data available from the
publications is indicated in the Summary table. The oblique (/) indicates and separates the low-temperature and high-temperatur
e values of properties or parameters represented in Table 1.1.
Non-aqueous components Phase equilibria Methods Temperature
Pressure Composition Tables REFERENCE
CH
4
(Methane) H-Fl Sampl 298/473; 518 K 1.3/3.2; 6.5 MPa 2.1 * 10
−4
/4.1 * 10
−4
–0.49/0.998 (CH
4
) mol.fr. ptx-CH
4
-7.1 Crovetto et al., 1982

1
-G
2
, which continuously transform one
into another with a small variation of pTx- parameters. Sometimes it is the more complex fl
uid equilibria (especially, in ternary system).
Immisc – immiscibility equilibria such as L
1
-L
2
; L
1
-L
2
-G; L
1
-L
2
-S etc. Cr.ph-critical phenomena
Methods:
Sampl – the method of fl uid phase sampling is used for determination of solution composition (static apparatus);
Flw.Sampl – the method of fl ow-sampling is used for determination of
solution composition (Flow-apparatus); Fl.inclus – the method of fl uid inclusions is used for phase equilibria studies in hydrothermal conditions, sometimes for determination not only the
types of phase equilibria, but the composition of phases at high temperatures also;
Isopiest – the method of isopiestic measurements is used for determination of the isopiestic molality
(molality at a known activity of water in aqueous solutions); Quench – the method of quenching is used to fi x the high-temperature equilibria by a fast cooling and to determine both the
hydrothermal equilibria and the composition of high-temperature phases; Wt-loss – the method of weight-loss of crystalls is used for measurements of solid solubility;
Vis.obs. – the method
of visual observations is used for determination of phase equilibria at elevated temperatures and pressures, sometimes – for de
termination the composition of phases; p-T, p-V, p-x, T-V, T-Cv,

mm = 10
6
mm; (- log m) is a negative decimal logarithm of molality, mol/L - molarity (moles of
solute per a liter of solution usually at room temperature), mass.% or mol.% - mass or mole per cent, mol.fr., mass.fr. or vol.fr. - mole, mass or volume fraction, ppm or ppb - parts per
million or parts per billion, or by the complex symbols, such as g/100g H
2
O; mmol/kg; mg/mL; cm
3
/100cm
3
H
2
O etc, which are the proper fractions where the numerator indicates the number
of units of solute and the denominator shows the number of units (usually one unit) of solution (or of solvent, if it is indic
ated). A designation of the units - g (gram), mol (mole), L (liter),
cm (centimeter) and the decimal prefi x - m (micro, 10
−6
), m (milli, 10
−3
), c (centi, 10
−2
), k (kilo, 10
3
), M (mega, 10
6
), G (giga, 10
9
)
Non-aqueous
components Phase equil Methods Temperature Pressure Composition Table REFERENCE

Ag in (HCl + H
2
) Soly Quench 200; 280 C SVP
(1.2–52) * 10
−5
(Ag); 0.0001–0.1 (HCl) m ptx-Ag + HCl-1.1 Kozlov and
Khodakovskiy,
1983
Ag in (HCl + KCl + H
2
) Soly Wt-loss;
Quench
450 C 500; 1000 bar 0.004–0.019 (Ag); 0.1 (HCl); 0.2 (KCl) m
ptx-Ag + HCl +
KCl-1.1
Tagirov et al., 1997
Ag in (HCl + NaCl + H
2
) Soly Quench 200 C SVP (5.6–50) * 10
−5
(Ag) 0.016–0.056 (HCl);
0.064–0.09 (NaCl) m
ptx-Ag + HCl +
NaCl-1.1
Kozlov and
Khodakovskiy,
1983
Ag in (HCl + NaCl) Soly Wt-loss;
Quench
350–500 C 500–2500 bar 0.0013–0.0246 (Ag); 0.02–0.25 (HCl);

x
Au
y
S
z
Soly Sampl 91/150; 250 C SVP (2–6)*10
−5
(Au); (2–6)*10
−7
(Ag); 0.5 (S); 0.002
(NaOH) m
ptx- Ag
x
Au
y
S
z
-1.1 Tagirov et al., 2006
(Ag + Cu) in HCl Soly Wt-loss;
Sampl
40/200–300 C SVP 5.8–3.54 (Ag); 2.8–0.72 (Cu) (−log m);
0.004–1.0 (HCl) m
ptx-Ag + Cu +
HCl-1.1
Xiao et al., 1998
(Ag + Cu) in (HCl +
NaCl)
Soly Wt-loss;
Sampl
40/200–300 C SVP 5.92–4.12 (Ag); 2.56–1.01 (Cu) (−log m)];

/0.013–0.059 (AgCl) m ptx-AgCl-1.1 Gavrish and
Galinker, 1955
AgCl Soly Quench 250; 300 C SVP 0.0025–0.0029 (AgCl) m ptx-AgCl-2.1 Zotov et al., 1985c
AgCl Soly Wt-loss;
Quench
450 C 500–1500 bar 0.008–0.05 (Ag) m
ptx-AgCl-3.1 Levin, 1993
AgCl Soly Sampl 300–360 C 41–183 bar 9.82–7.9 (AgCl) (−log mol.fr.) ptx-AgCl-4.1; 4.2 Migdisov et al.,
1999
AgCl in HCl Soly Sampl 100/200–350 C SVP 0.03 * 10
−4
/0.0007–0.125 (AgCl);
6.4 * 10
−5
–3.5 (HCl) m
ptx-AgCl +
HCl-1.1
Ruaya and Seward,
1987
AgCl in (HCl + NaCl +
NdCl
3
)
Soly Sampl 200; 300 C SVP 2.69–0.86 (Ag) (−log m);
0.03–1 (HCl + NaCl); 0–0.24 (NdCl
3
) m
ptx-AgCl +
H,Na,Nd/Cl-1.1
Gammons et al.,

1986
AgCl in KCl Soly Wt-loss;
Quench
300 C SVP 0.0051–1.35 (Ag); 0.025–6 (KCl) m ptx-AgCl +
KCl-1.1
Levin, 1991
AgCl in KCl Soly Wt-loss;
Quench
450 C 500; 1000 bar 0.041–0.22 (Ag); 0.46; 0.9 (KCl) m
ptx-AgCl +
KCl-2.1
Levin, 1993
AgCl in NaCl Soly Sampl 100/197–353 C SVP 2.2 * 10
−5
/5.3 * 10
−4
–0.256 (AgCl);
5 * 10
−5
–3 (NaCl) m
ptx-AgCl +
NaCl-1.1
Seward, 1976
AgCl in NaCl Soly Quench 300 C SVP 0.0021–0.334 (AgCl); 0.0001–3 (NaCl) m ptx-AgCl +
NaCl-2.1
Zotov et al., 1986
AgCl in NaCl Soly Wt-loss;
Quench
300 C SVP 0.005–0.86 (Ag); 0.025–7 (NaCl) m ptx-AgCl +
NaCl-3.1

Soly Wt-loss;
Quench
250 C SVP 0.01–0.03 (Ag); 0.2; 0.5 (NaCl);
0–1 (NaClO
4
) m
ptx-AgCl + NaCl
+ NaClO
4
-2.1
Levin, 1991
AgCl in (NaCl + NaClO
4

+ NaOH)
Soly Quench 200–300 C SVP 0.0038–0.093 (AgCl); 0.2; 0.5 (NaCl);
0–0.3 (NaClO
4
); 0–0.3 (NaOH) m
ptx-AgCl +
Na/Cl,ClO
4
,OH-1.1
Zotov et al., 1982
AgCl in NaClO
4
Soly Quench 250; 300 C SVP 0.0026–0.0054 (AgCl); 0.01–1 (NaClO
4
) m ptx-AgCl +
NaClO

AgI Soly Wt-loss 20/300–365 C SVP 1.4 * 10
−6
/0.0008–0.0029 (AgI) m ptx-AgI-1.1 Gavrish and
Galinker, 1955
AgI in NaI Soly Sampl;
Wt-loss
150/200;
250 C
SVP 5.6/4.2–1.2 (AgI) (−log m); 0.001–0.89 (NaI) m ptx-AgI + NaI-1.1 Gammons and Yu,
1997
AgNO
3
Soly Vis.obs. 112/173–198 C SVP 91.6/98–99.4 (AgNO
3
) mass.% ptx-AgNO
3
-1.1 Benrath et al., 1937
AgNO
3
LGE Vap.pr. 152/219 C SVP (2.53/3.3–21.2
bar)
8.4–89.6 (AgNO
3
) mol.% ptx-AgNO
3
-2.1 Geerlings and
Richter, 1997
Ag
2
O Soly Sampl 25/200–260 C SVP 0.0022/0.063–0.022 (Ag

S) mol.%
ptx-Ag
2
S + NaOH
+ H
2
S-2.1
Gammons and
Barnes, 1989
Ag
2
S in (NaOH + S) Soly Flw.Sampl 25/200–400 C 1/40–500 bar (0.01/0.02–8.5) * 10
−5
(Ag); 0–0.4 (NaOH);
0.014–0.12/0.18 (S) m
ptx-Ag
2
S + NaOH
+ S-1.1
Stefansson and
Seward, 2003a
Ag
2
SO
4
in D
2
SO
4
Soly Vis.obs. 25/195–234 C SVP 0.02/0.029–0.67 (AgSO

250 C
SVP 0.02/0.12–0.68 (AgSO
4
); 0.1–1 H
2
SO
4
m ptx-Ag
2
SO
4
+
H
2
SO
4
-1.1
Lietzke and
Stoughton, 1956
Ag
2
SO
4
in UO
2
SO
4
Soly Vis.obs. 36/197–259 C SVP 1.04/12.8–17.3 (Ag
2
SO

SO
4
); 0.1/0.41–1.35 UO
2
SO
4
m ptx-Ag
2
SO
4
+
UO
2
SO
4
-2.1
Lietzke and
Stoughton, 1960
AlOOH (boehmite) +
Buff
Soly Sampl 150/200;
250 C
100 bar 0.018/0.023–470/933 (AlOOH) mg/kg;
Buffer soln. (pH
25
= 1.17–9.44)
ptx-AlOOH +
Buff-1.1; 1.2
Bourcier et al.,
1993

2
H
4
O
2

+
C
2
H
3
O
2
Na-1.1
Castet et al., 1993
AlOOH (boehmite) in
(HCl + NaCl)
Soly Sampl 90/200–350 C SVP 6.8/6.54–4.96/3.56 (AlOOH) (−log m);
(1.05/1.35–105)
*
10
−
4
(HCl);
0–0.01/0.025 (NaCl) m
ptx-AlOOH +
HCl +
NaCl-1.1
Castetet al., 1993
AlOOH (boehmite) in

-1.1
Kuyunko et al.,
1983
AlOOH (boehmite) in
(NH
3
/NH
4
Cl + SiO
2
)
Soly Sampl 300 C SVP (86 bar) 5.9–4.26 (Al); 3.37–1.97 (Si) (−log m);
0.005–16.5 (NH
3
) m
ptx-AlOOH +
NH
3
/NH
4
Cl +
SiO
2
-1.1
Salvi et al., 1998
AlOOH (boehmite) in
(NH
4
OH + NH
4

4
Cl-2.1
Castet et al., 1993
8 Hydrothermal Experimental Data
Table 1.1 Continued
Non-aqueous
components Phase equil Methods Temperature Pressure Composition Table REFERENCE
123456
78
AlOOH (boehmite) in
(NaCl + HCl/NaOH)
Soly Potentio;
Sampl
100/203–290 C SVP-68 bar 7.3/6.5–2.0 (Al) (−log m);
pH = 1.7–8.5 (HCl/NaOH)
ptx-AlOOH-NaCl
+ HCl/NaOH-
1.1; 1.2; 1.3;
1.4
Palmer et al., 2001
AlOOH (boehmite) in
(NaCl + HCl/NaOH)
Soly Potentio;
Sampl
101.5/203–290 C SVP 7.2/6.9–2.4 (Al) (−log m);
pH = 2.2–8.3 (HCl/NaOH)
ptx-AlOOH-NaCl
+
HCl/NaOH-2.1
Benezeth et al.,

0.0025–0.009 (NaOH); 0.001–0.0075 (NaCl) m
ptx-AlOOH +
NaOH +
NaCl-2.1
Castet et al., 1993
AlOOH (boehmite) in
(NaOH + SiO
2
)
Soly Sampl 300 C SVP (86 bar) 2.44 (Al); 3.24 (Si) (
−log m); 0.004 (NaOH) m ptx-AlOOH +
NaOH +
SiO
2
-1.1
Salvi et al., 1998
AlO
2
H (diaspore) in
NaOH
Soly Sampl 250; 300 C SVP 8.3–33.7 (Al
2
O
3
); 6.4–22.9 (Na
2
O) mass.% ptx-AlO
2
H +
NaOH-1.1

Verdes et al., 1992
Al
2
O
3

(corundum) Soly Quench 380–420 C 25–49 MPa 0.00006–0.0009 (Al
2
O
3
) m ptx-Al
2
O
3
-1.1 Yalman et al., 1960
Al
2
O
3

(corundum) Soly Wt-loss 700–900 C 6–6.75 kbar 0.043–0.105 (Al
2
O
3
) mass.% ptx-Al
2
O
3
-2.1 Anderson and
Burnham, 1967

-4.1 Ganeev and
Rumyancev, 1974
Al
2
O
3

(corundum) Soly Wt-loss 666–700 C 2.5–20 kbar 2.7–139.4 (Al
2
O
3
) ppm ptx-Al
2
O
3
-5.1 Becker et al., 1983
Al
2
O
3

(corundum) Soly Sampl 400–720 C 730–3120 kbar 1.0–4.2 (Al) ppm ptx-Al
2
O
3
-6.1 Ragnarsdottir and
Walther, 1985
Al
2
O

3
) (−log mol/L); 0.1;
1 (AlCl
3
) mol/L
ptx-Al
2
O
3
+
AlCl
3
-1.1
Korzhinskiy, 1987
Phase Equilibria in Binary and Ternary Hydrothermal Systems 9
Non-aqueous
components Phase equil Methods Temperature Pressure Composition Table REFERENCE
123456
78
Al
2
O
3

(corundum) in
Ba(OH)
2
Soly Wt-loss 430; 600 C 1450 bar 2 (Ba(OH)
2
) m; Solid ph not Al

ptx-Al
2
O
3
+
CaCl
2
-1.1
Korzhinskiy, 1987
Al
2
O
3

(corundum) in
CaCl
2
Soly Sampl 198–600 C 625–2100 bar 2.83–3.99 (Al
2
O
3
) (−log m);
0.1 (CaCl
2
) m
ptx-Al
2
O
3
+

2
CO
3
-1.1
Barns et al., 1963
Al
2
O
3

(corundum) in
CsOH
Soly Wt-loss 430; 600 C 1450 bar 5.2; 5.7 (Al
2
O
3
) mass.%;
2 (CsOH) m
ptx-Al
2
O
3
+
CsOH-1.1
Barns et al., 1963
Al
2
O
3


O
3
+
HCl-2.1
Korzhinskiy, 1987
Al
2
O
3

(corundum) in HF Soly Wt-loss 430 C 1450 bar 7.8 (HF) m;
Solid ph [Al(OHF)
3
]
ptx-Al
2
O
3
+
HF-1.1
Barns et al., 1963
Al
2
O
3

(corundum) in
K
2
CO

3
) mass.%; 2–20 (KCl) m ptx-Al
2
O
3
+
KCl-1.1
Barns et al., 1963
Al
2
O
3

(corundum) in
KCl
Soly Wt-loss 800 C 6; 6.17 kbar 0.13; 0.15 (Al
2
O
3
) mass.%; 4.6 (KCl) m ptx-Al
2
O
3
+
KCl-2.1
Anderson and
Burnham, 1967
Al
2
O

+
KF-1.1
Yalman et al., 1960
Al
2
O
3

(corundum) in KF Soly Wt-loss 430; 600 C 1380; 1450 bar 2; 10 (KF) m;
Solid ph [K
3
AlF
6
]
ptx-Al
2
O
3
+
KF-2.1
Barns et al., 1963
Al
2
O
3

(corundum) in
KOH
Soly Wt-loss 430; 600 C 1450 bar 6.6; 6.9 (Al
2

O
3

(corundum) in
KOH
Soly Wt-loss 500–700 C 1.86–2.65 kbar 0.09–0.89 (Al); 0.1–1.0 (KOH) m ptx-Al
2
O
3
+
KOH-3.1
Pascal and
Anderson, 1989
Al
2
O
3

(corundum) in
KOH
Soly Wt-loss 400 C 0.5–2 kbar (0.064–7.1)
*
10
−
2
(Al
2
O
3
); 0.001–0.1 (KOH) m ptx-Al

(corundum) in
MgCl
2
Soly Quench 600 C 2 kbar 2.3 (Al
2
O
3
) (−log mol/L); 1 (MgCl
2
) mol/L ptx-Al
2
O
3
+
MgCl
2
-1.1
Korzhinskiy, 1987
Al
2
O
3

(corundum) in
NH
4
OH
Soly Wt-loss 430–600 C 1450–2760 bar <2 (Al
2
O

O
3
+
Na
2
CO
3
-1.1
Yamaguchi et al.,
1962
10 Hydrothermal Experimental Data
Table 1.1 Continued
Non-aqueous
components Phase equil Methods Temperature Pressure Composition Table REFERENCE
123456
78
Al
2
O
3

(corundum) in
Na
2
CO
3
Soly Wt-loss 430; 600 C 1450 bar 4.9; 7.0 (Al
2
O
3

+
NaCl-1.1
Barns et al., 1963
Al
2
O
3

(corundum) in
NaCl
Soly Wt-loss 800 C 6.0 kbar 0.092 (Al
2
O
3
) mass.%; 0.90 (NaCl) m ptx-Al
2
O
3
+
NaCl-2.1
Anderson and
Burnham, 1967
Al
2
O
3

(corundum) in
NaCl
Soly Quench 600 C 2 kbar 2.3 (Al

O
3
(corundum) in
NaCl
Soly Wt-loss 800

C 10 kbar 0.001–0.02 (Al
2
O
3
) (m); 0–0.6 (NaCl) mol.fr. ptx-Al
2
O
3
+
NaCl-5.1
Newton and
Manning, 2006
Al
2
O
3

(corundum) in
NaOH
Soly Quench 380–420 C 25–49 MPa 0.00021–0.1975 (Al
2
O
3
); 0–0.5 (NaOH) m ptx-Al

3

(corundum) in
NaOH
Soly Wt-loss 400–600 C 140–2760 bar 2–31.5 (Al
2
O
3
) mass.%; 0.5–10 (NaOH) m ptx-Al
2
O
3
+
NaOH-3.1
Barns et al., 1963
Al
2
O
3

(corundum) in
NaOH
Soly Wt-loss 800; 900 C 6–6.13 kbar 0.64; 0.65 (Al
2
O
3
) mass.%; 0.113 (NaOH) m ptx-Al
2
O
3

477–663 10.4–337.2 MPa 0.05–0.8 (Ar) mol.fr.
ptx-Ar-4.1; 4.2 Wu et al., 1990
Ar LGE Sampl 307/454;
568 K
1.67/2.2; 9.7 MPa 0.027–52.12 (Ar) mol.% ptx-Ar-5.1 Crovetto et al., 1982
Ar in D
2
O H-Fl Sampl 297/461–584 K 1.32/2.7–13.28 MPa 0.04–53.8 (Ar) mol.% ptx-Ar + D
2
O-1.1 Crovetto et al., 1982
As
2
O
3

(claudetite) Soly Wt-loss 22/150–250 C SVP 0.21–1.2 (As) (log m) ptx-As
2
O
3
-1.1 Pokrovski et al.,
1996
As
2
O
3
; As
2
O
3
+ NaCl, in

2
O
3
+ HCl)
Soly Wt-loss;
Sampl
200–300 C SVP 2.33–0.49 (As) (−log m); 0–740 (As
2
O
3
) mg;
0; 0.01 (HCl) mol/L
ptx-As
2
S
3
+
HCl-1.1
Pokrovski et al.,
1996
Non-aqueous
components Phase equil Methods Temperature Pressure Composition Table REFERENCE
Phase Equilibria in Binary and Ternary Hydrothermal Systems 11
components Phase

equil Methods Temperature Pressure Composition Table REFERENCE
123456
78
As
2

2
O
3
; Cu-Cu
2
O)
ptx-Au-1.1; 1.2 Zotov et al., 1985b
Au in Cl
2
Soly Wt-loss 125/200–500 C 1 atm 0.08–9.54 (Au) mass. % (Wt-loss);
(Cl
2

+ H
2
O − gaseous stream)
ptx-Au + Cl
2
-1.1 Ogryzlo, 1935
Au in H
2
Soly Flw.Sampl 300–600 C 500–1500 bar (0.17–17.9)
*
10
−
7
(Au); 4 * 10
−
5
(H

Stefansson and
Seward, 2003c
Au in (HCl + NaCl +
H
2
)
Soly Flw.Sampl 300–500 C 500–1800 bar (0.049–6.65) 10
−
6
(Au); 0.104–0.975 (NaCl);
1 * 10
−
9
–0.586 (HCl); (0.04–7.9) * 10
−
4
(H
2
) m
ptx-Au + HCl +
NaCl + H
2
-1.1
Stefansson and
Seward, 2003c
Au in H
2
S Soly Sampl 143/197–352 C 18.4/31–214 atm 7.04–5.69 (Au) (−log m); 0.8–1.93 (H
2
S) m ptx-Au + H

) m; 0.036 (H
2
) bar
ptx-Au + H
2
S +
H
3
PO
4
+ H
2
-1.1
Benning and
Seward, 1996
Au in (H
2
S + H
3
PO
4
+
KH
2
PO
4
)
Soly Sampl 150/199.4–300.8 C 27/38–132 atm 7.8/7.24–6.13 (Au) (−log m); 0.73; 1.56 (H
2
S);

Au in (H
2
S + NaOH +
H
2
)
Soly Sampl 150/200–400 C 500–1500 bar 2.075–108.4 (Au) ppm; 0.0176–0.114 (S);
0.0023–0.037 (NaOH) m;
0.036–0.37 (H
2
) bar
ptx-Au + H
2
S +
NaOH + H
2
-1.1
Benning and
Seward, 1996
Au in (H
2
S + NaOH +
Na
2
SO
4
)
Soly Sampl 296.2–351 C 96.4–234 atm 1.9–1.44 (Au) (−log m); 0.9–1.5 (H
2
S);

NaHS-1.1
Ogryzlo, 1935
Au in NaCl + NaOH +
H
2
Soly Flw.Sampl 300–450 C 500 bar (2.8–55.6) * 10
−
8
(Au); 0.51; 0.52 (NaCl);
0.11; 0.3 (NaOH); (3.56–3.78) * 10
−
5
(H
2
) m
ptx-Au + Na/
Cl,OH + H
2
-1.1
Stefansson and
Seward, 2003c
Au in (NaOH + buffer) Soly Quench 25/250 C SVP 0.4 * 10
−
9
/(0.3–9.1) * 10
−
7
(Au) mol/L;
pH = 7.7/9.2–14 (NaOH); Buff. (Fe
2

2
S Soly Quench 590 C 0.15 GPa 0.1 (Au) g/kg; (Na
2
S) ptx-Au +
Na
2
S-1.1
Fleet and Knipe,
2000
12 Hydrothermal Experimental Data
Non-aqueous
components Phase equil Methods Temperature Pressure Composition Table REFERENCE
123456
78
B(OH)
3
LGE Sampl 452–645 K SVP 0.0007–0.11 (B(OH)
3
) m ptx-B(OH)
3
-1.1 Kukuljan et al.,
1999
B
2
O
3
; HBO
2
Soly Vis.obs. −0.76/169–450 C SVP 0.33–100 (B
2

2
-2.1 Benrath, 1941
BaCl
2
Soly Vis.obs. 25/200–370 C SVP 37/50–0 (BaCl
2
) mass.% ptx-BaCl
2
-1.1 Benrath and
Lechner, 1940
BaCl
2
Soly Quench 426 C 273 kg/cm
2
0.04 (BaCl
2
) mass.% ptx-BaCl
2
-2.1 Gillingham, 1948
BaCl
2
Soly Therm. anal 209; 272 C SVP BaCl
2
* H
2
O ⇒ BaCl
2
* 0.5H
2
O ⇒ BaCl

5.2; 5.3; 5.4
Valyashko et al.,
1983
BaCl
2
LGE Vap.pr. 412/452.5–630 K 0.3/0.9–17.5 MPa 0.25–1.55 (BaCl
2
) m ptx-BaCl
2
-6.1 Matuzenko et al.,
1984
BaCl
2
LGE Vap.pr. 150/200–350 C 4.45/24–165 bar 0.1–1.45 (BaCl
2
) m ptx-BaCl
2
-7.1 Azizov and
Akhundov, 1995
BaCl
2
LGE;
Isop-m
Isopiestc. 383/474–524 K SVP 0.42–4.1 (BaCl
2
) m ptx-BaCl
2
-8.1 Holmes and
Mesmer, 1996b
BaF

2
-1.1 Benrath et al., 1937
BaSO
4
Soly Flw.Sampl 500 C 1000 bar 0.004 (BaSO
4
) mass.% ptx-BaSO
4
-1.1 Morey and
Hesselgesser,
1951b
BaSO
4
Soly Sampl 250 C SVP 0.5 * 10
−
5
(BaSO
4
) m ptx-BaSO
4
-2.1 Jones et al., 1957
BaSO
4
Soly Wt-loss;
Quench
100/200–600 C 1/15–2100 bar 3.0–10 (BaSO
4
) mg/kg H
2
O ptx-BaSO

(0.3–22) * 10
−
4
(BaSO
4
) mol/L
ptx-BaSO
4
+
CaCl
2
-1.1
Uchameishvili et
al., 1966
BaSO
4
in KCl soly Wt-loss;
quench
110/210–300 C SVP 0.025 (KCl); (0.34–0.8/1.1) * 10
−
4
(BaSO
4
)
mol/L
ptx-BaSO
4
+
KCl-1.1
Uchameishvili et

2
-1.1
Uchameishvili et
al., 1966
BaSO
4
in NaCl soly Wt-loss;
quench
95/200–370 C SVP 0.25–2.0 (NaCl);
(0.2–8.4) * 10
−
4
(BaSO
4
) mol/L
ptx-BaSO
4
+
NaCl-1.1
Uchameishvili et
al., 1966
BaSO
4
in NaCl Soly Wt-loss;
Quench
20/200–600 C D =
0.3–0.9/1.0 (g/cm
3
)
0.1/2.0 (NaCl) m;

+
NaCl-4.1
Blount, 1977
BaSO
4
+ UO
2
SO
4
soly Sampl 250 C SVP
0.13–1.3 (UO
2
SO
4
); (1.5–40) * 10
−
5
(BaSO
4
) m ptx-BaSO
4
+
UO
2
SO
4
-1.1
Jones et al., 1957
BaSrSO
4

4
-1.1
Koz’menko et al.,
1986
BeO in HF Soly Quench;
Wt-loss
300 C SVP (7 * 10
−
6
–2 * 10
−
3
) (BeO); 0.00027–0.013 (HF)
mol/L
ptx-BeO +
HF-1.1
Koz’menko et al.,
1985
Bi
2
O
3
Soly Quench;
Wt-loss
75/200;
300 C
SVP (0.03 1.96–23.6) * 10
−
4
(Bi) m ptx-Bi

HClO
4
-1.1
Kolonin and Laptev,
1982
Bi
2
O
3
in NaOH Soly Quench;
Wt-loss
300 C SVP (16–73) * 10
−
4
(Bi); 0.0001–5.1 (NaOH) m ptx-Bi
2
O
3
+
NaOH-1.1
Kolonin and Laptev,
1982
CF
4
H-Fl;
Immisc
Vis.obs. 587–669 K 26–200 MPa 1.2–5.8 (CF
4
) mol.% ptx-CF
4

NaCl-1.1
Smits et al., 1997a
CH
4

(methane) H-Fl Sampl 38/204.4;
237.8 C
1.4/2.76–69 MPa 0.04/19.2–94.6 (CH
4
) mol.% ptx-CH
4
-1.1 Olds et al., 1942
CH
4

(methane) H-Fl Sampl 150/200–360 C 50–1100 kg/cm
2
0.985/0.96–0.074 (CH
4
) mol.fr. ptx-CH
4
-2.1; 2.2 Sultanov et al.,
1971
CH
4

(methane) H-Fl Sampl 150/200–360 C 50–1100 kg/cm
2
1/1.24–193 (CH
4

4
-6.1 Gillespie, P.C.;
Wilson, G.M.,
1982