ISSN 0016-7029, Geochemistry International, 2017, Vol. 55, No. 2, pp. 205–210. © Pleiades Publishing, Ltd., 2017.

Original Russian Text © A.L. Lebedev, V.L. Kosorukov, 2017, published in Geokhimiya, 2017, No. 2, pp. 171–177.

Gypsum Solubility in Water at 25°C

A. L. Lebedev* and V. L. Kosorukov
Faculty of Geology, Moscow State University, Moscow, 119991 Russia
*e-mail: aleb.104a@yandex.ru
Received November 12, 2015; accepted December 2, 2015

Abstract—The analysis of published data and our experimental results showed that the existing estimates of
gypsum solubility in water (C m↑ ) at 25°C range from 0.0147 to 0.0182 M. Such a scatter (more than 20%) is the
result of a combined influence of experimental conditions and ability of gypsum to form supersaturated solu-
tions. This influence appears most noticeable during gypsum dissolution in a dispersed state. Under such
conditions, equilibrium is determined with a precision of no better than ±4.5%; if a flat surface similar to nat-
ural one is dissolved, the (C m↑ ) value is characterized by the minimum scatter (±1%). According to experimental
data (25°C), the solubility of gypsum particles in water is inversely proportional to their size at r < 1 μm and is
r-invariant for larger grains. The invariance of (C m↑ ) at r > 1–5 μm is supported by the data of analytical cal-
culations using the approximate Ostwald–Freundlich equation. It is supposed that the difference of the con-
centrations of dissolved gypsum at the boundaries of the field of metastable state of gypsum-saturated
groundwater can be 1–5%. The results of our study can be used for the description of gypsum dissolution in
the models of mass transfer between gypsum-bearing rocks and groundwater.

Keywords: gypsum, distilled water, solubility, dispersed state, lithological varieties, metastable field, mass
transfer, groundwater
DOI: 10.1134/S0016702917010062

INTRODUCTION (Hardie, 1967). This scatter in C m↑ (~5%) is probably

During the solution of mass transfer problems in
groundwater, the computation of gypsum dissolution
is based on its equilibrium concentration. Using the
principles of chemical thermodynamics, equilibrium
solubility, i.e., the limiting amount of gypsum dis-
solved in water under given conditions, can be deter-
mined. Experimental values (pseudoequilibrium,
Levenshpil’, 1969) characterize only the end of gyp-
sum interaction with solution near the thermody-
namic equilibrium from either of two sides: from the
region of undersaturated solutions (C m↑ ) and from
supersaturated solutions (C m↓ ) . Therefore, the results
of mass transfer calculation in groundwater are largely
based on the equilibrium constraints (C m↑,C m↓ ) .
Most experimental studies on gypsum solubility in
water were conducted under static conditions at 25°C.
Synthetic or natural gypsum in the form of powder,
granules, or individual monocrystals was used. The
spontaneous reaction caused the dissolution process
to pass from the region of undersaturated solutions to
the region of gypsum saturation under the conditions
of open and closed (to air) systems. Equilibrium in the
solution was evaluated by the measurement of mainly
the concentration of Ca2+, C m↑ = 0.0149–0.0157 M
due to the gypsum ability to produce oversaturated
solutions (Budnikov, 1943). The C m↑ values obtained in
such a way can be considered only as minimum con-
straints, and the accurate values can be determination
at a similar transition from the region of supersatura-
tion (supersaturation → saturation, i.e., C m↓ ). Accord-
ing to an overview of Hardie (1967), the difference
between C m↓ and C m↑ for calcite, aragonite, and amor-
phous silica can be at least 5%.
Such metastable states (fields) are widespread in
hydrochemical systems (Krainov and Shvets, 1980).
There is no crystallization in a stable (undersaturated)
state. In a labile state (supersaturated solutions), crys-
tallization is inevitable. These states are separated by a
field of metastable states, in which the concentration
of solution is higher than or equal to equilibrium one,
and crystallization is practically impossible.
Investigations of the stability of supersaturated
solutions are usually focused on, first, the determina-
tion of experimental conditions affecting supersatura-
tion; second, the estimation of the degree of supersat-
uration as a function of particle size; and, third, the
calculation of the boundaries of the metastable region

205
206 LEBEDEV, KOSORUKOV

1 tration forms. In this paper, the C m↑ and C m↓ values are

2 presented in the molar scale.
3 The gypsum solubility is defined as the saturation
4 concentration of its solution under given conditions.
The boundaries of the field of metastable state are C m↑
and C m↓ values obtained under the conditions of the
undersaturation → saturation and supersaturation →
r > 2 μm r = 0.2–0.5 μm saturation transition, respectively.

SOLUBILITY OF DISPERSED GYPSUM

0.014 0.015 0.016 0.017 0.018 0.019
Solubility, mol/L
Fig. 1. Solubility of gypsum in water at 25°C, (4) calculated
and (1–3) measured under certain experimental condi-
tions. Dissolution of dispersed gypsum: (1) under the con-
ditions of C m↑ dependence on particle size, C m↑ = C m↑ (r),
and (2) under the conditions when such an effect is absent,
C m↑ ≠ C m↑ (r); (3) dissolution of a flat gypsum surface simi-
lar to natural one (unfilled symbols are C m↓ , and filled sym-
bols are C m↑ ). Solid horizontal lines are gypsum solubility
values under given conditions. Dashed vertical lines are the
boundaries of the range of most common C m↑ values deter-
mined under conditions 2.
on the basis of the general thermodynamic interpreta-
tion of this phenomenon (Khamskii, 1975).
This study is an attempt to interpret experimental
data on gypsum solubility in water for the determina-
tion of the boundaries of the field of metastable solu-
tion states. The goal of our study was to determined C m↑
and C m↓ values (25°C) for their use in constructing
models of mass transfer between gypsum-bearing
rocks and groundwater.
Based on the analysis of published data, we distin-
guished three intervals of parameters constrained by
experiments and one interval obtained by calculations
(1–4 in Fig. 1). Interval 4 (Fig. 1) was obtained from
the calculation of gypsum solubility in water using the
standard free energy of the reaction, activity coeffi-
cients, and solution ionic strength: 0.0151 M (Drever,
1982), 0.01525 (Raines and Dewers, 1997, using the
PHRQPTZ program), 0.0153 (Levchenko, 1950;
Zverev, 1967), and 0.0154 (Marshall and Slusher,
1966). The conditions of C m↑ and C m↓ determination for
intervals 1–3 are briefly characterized below.
In the available studies, data on gypsum solubility
in water (~2 g/L, 25°C) are expressed in weight,
molal, or molar concentrations. Given the small
amount of dissolved matter, changes in solution den-
sity can be ignored during the calculation of concen-
IN WATER (r < 1 μm)
There are only a few experimental investigations
of the influence of the size of gypsum particles on its
solubility in water. According to the most frequently
cited studies of Hulett (1901) and Dundon and Mack
(1923), the solubility of gypsum in distilled water
increases significantly at r < 1 μm, and the maximum
value 0.0182 M was observed at r = 0.2–0.5 μm
(C m↑ = C m↑ (r), 25°C, interval 1 in Fig. 1). An increase
in gypsum particle size to 2 μm depresses the solubil-
ity to 0.0153 M (25°C), when the solubility becomes
probably independent of the particle size, which is
supported by the data of Christoffersen and Christof-
fersen (1976): 0.0152–0.0153 M (25°C) at r = 50–
300 μm.
A lower C m↑ value of 0.0148 M was reported by
Sung-Tsuen Liu and Nancollas (1971) for solutions of
suspensions with r = 80–120 μm (25°C, distilled
water, 1 mL of suspension contained 74 mg of gypsum
crystals).
In the experiments of Kuznetsov et al. (1957), par-
ticle size fractions of 1000–500, 500–200, 200–90,
and <90 μm were blended with distilled water in gyp-
sum : water proportions of 1 : 10, 1 : 20, and 1 : 50.
Solutions with suspended particles prepared in such a
way were supersaturated by approximately 5% of gyp-
sum solubility (18°C), and the concentration of solu-
tion decreased in 1–2 h to a certain constant value,
and the supersaturation increased with decreasing
water : gypsum ratio. A similar effect was observed by
Dundon and Mack (1923).
Theoretical solutions are obtained on the basis of
considerations used for the deduction of the Ostwald–
Freundlich equation (known as the Thompson–Gibbs
effect or Gibbs–Kelvin equation). For a monocrystal
of arbitrary geometry in equilibrium with an electro-
lyte, this dependence can be expressed as (Enustun
and Turkevich, 1960)
log(a/ao) = (2/3(Mαδ))/(2.03RTpνχ), (1)
where a and a0 are the activities (defined as solubili-
ties) of a face with the characteristic size χ and an
infinitely large face, respectively; M is the molecular
mass of the crystal; α is the characteristic geometrical
coefficient; δ is the mean interface tension; R is the gas

GEOCHEMISTRY INTERNATIONAL Vol. 55 No. 2 2017

 GYPSUM SOLUBILITY IN WATER AT 25°C
constant; T is the temperature; p is the crystal density;
and ν is the number of ions formed at the dissociation
of one mole of the electrolyte.
Equation (1) can be used also in the case of a set of
particles. Enustun and Turkevich (1960) studied the
solubility of a mixture of SrSO4 crystals in water at
25°C and showed that the solubility of a mixture of
crystals of varying size is controlled by the finest frac-
tion. In the case of a population of geometrically uni-
form particles, α = p(SΣχ3)/(Σχ2), where S is the reac-
tion surface.
Calculations based on Eq. (1) indicate that gypsum
solubility in water increases significantly at r < 0.01–
0.1 μm and is practical size-invariant at r > 1–5 μm
(0.0151 M at 20°C; Baldin and Grushevskii, 1976; Sri-
kantan, 1949). However, at r < 1 μm, the reliability of
the calculated values of gypsum solubility is question-
able to a certain degree, because the current estimates
of δ values differ by several orders of magnitude. For
instance, δ = 12 erg/cm2 was obtained from data on
the formation of crystal nuclei (Ratinov and Ivanov,
1969), whereas the dissolution of small gypsum parti-
cles yielded δ values of 370 and 1050 erg/cm2 (Enustun
and Turkevich, 1960).
SOLUBILITY OF DISPERSED GYPSUM
IN WATER (r = 10–500 μm)
The following is the range of C m↑values based on the
data of 17 most comprehensive studies conducted
under the condition C m↑ ≠ C m↑ (r) at 25°C (interval 2,
Fig. 1): 0.0142 M (Voznesenskii and Biktimirov,
1957), 0.0147 (Nakayama and Rasnick, 1967), 0.0148
(Sung-Tsuen Liu and Nancollas, 1971), 0.0151 (Mar-
shall and Slusher, 1966), 0.01513 (Madgin and Swales,
1956), 0.0152 (Sturn, 1975; Christoffersen and Chris-
toffersen, 1976; Bock, 1961), 0.0153 (Bennett and
Adams, 1972; Hulett and Allen, 1902; Shternina,
1949; Levchenko, 1950), 0.01535 (Zdanovskii and
Spiridonov, 1967), 0.01536 (Shternina and Frolova,
1945), 0.0154 (Karazhanov, 1959), 0.0158 (Raines and
Dewers, 1997), and 0.0161 (Blok and Waters, 1968).
Natural or synthetic gypsum (r = 10–500 μm) was
used in these studies.
The distribution of these values is shown in the his-
togram of Fig. 2 (value of 0.0142 M obtained by
Voznesenskii and Biktimirov (1957) was rejected as
least reliable). The C m↑ scatter of ~9% (0.0147–0.0161 M,
Fig. 2) is probably due to the combined effect of exper-
imental conditions. The following characteristics were
used for their description: quantity and quality of reac-
tants, geometry of the reaction vessel, rate of solution
stirring, preparation of gypsum particles for experi-
ments, etc. However, only a “selective” quantitative
description of these parameters was given in most of the
GEOCHEMISTRY INTERNATIONAL Vol. 55 No. 2
207
10
Number of experimental studies
8
6
4
2
0
1.47 1.49 1.51 1.53 1.55 1.57 1.59 1.61
C↑m 102, mol/L
Fig. 2. Distribution of C m↑ values (r ~ 10–500 μm, 25°C).
publications. Therefore, it is impossible to determine
the dependence of C m↑ on particular characteristics.
The histogram of Fig. 2 appears almost symmetri-
cal. The mean value is C m↑ = 0.0153 (±4.5%) M. The
most frequent C m↑ values fall within the range 0.0151–
0.0154 M (25°C).
SOLUBILITY OF A FLAT SURFACE
OF LITHOLOGICAL GYPSUM VARIETIES
IN WATER
Interval 3 is composed of two segments defined by
C m↑ and C m↓ values (Fig. 1). Data for C m↑ were obtained
in previous investigations of the kinetics of gypsum
dissolution in water (Lebedev, 2015). Fifteen litholog-
ical varieties represented by practically pure gypsum
were collected at the coastal zone of the Kama reser-
voir (P1ir) and from drill cores (10–70 m depths) at the
region of the Kafirnigan River (N1kf1, Tajik Republic).
Experiments were conducted in a periodically active
cell under continuous stirring of a thermostated solu-
tion (Fig. 3). In all the experiments, almost identical
C m↑ values of 0.0151 M (±0.5%, 25°C) were obtained;
they correspond to the lowest values from the main
database on gypsum dissolution in a dispersed state
(C m↑ ≠ C m↑ (r), Fig. 1).
For the determination of C m↓ , gypsum-saturated
solution was produced in the cell at 30°C and then
cooled to 25°C. The stabilization of Ca2+ concentra-
tion in the solution (C m↓ = 0.0152–0.0153 M, 25°C)
was observed within 2–3 h. The scatter of C m↑ , C m↓ , and
C m↓ – C m↑ values (~0.7%) was comparable with the error
of solution analysis.
2017
208 LEBEDEV, KOSORUKOV
4 related to gypsum dehydration and/or a change in the
1 grinding; see a review by Budnikov, 1943).
3 tion of solutions with large suspended crystals
2 experiments for the separation of fractions, particles
Fig. 3. Cartoon of the experimental setup: (1) thermostated
cell; (2) sample; (3) stirrer; and (4) recording instruments.
Long experiments (up to one year) were conducted
at ambient temperature with water preliminarily satu-
rated or unsaturated with air using hermetic glass
flasks without solution stirring and thermostating.
Gypsum samples with untreated and treated flat sur-
faces were used. During the chemical analysis of water
samples at t = 21.5°C, a precipitate of small transpar-
ent gypsum crystals of tabular shape was observed in
the solutions. In all the experiments, the difference in
Ca2+ concentration (C m↑ ≈ 0.0147 M) was no higher
than the precision of the chemical analysis of solution.
These values are ~1% lower than those obtained in
short experiments (2–3 h) at continuous solution stir-
ring and gypsum dissolution from a flat surface
(0.0149 M) at 20°C (Lebedev, 2015).
Thus, the influence of experimental conditions on
the solubility of a flat gypsum surface analogous to
natural one appeared to be insignificant. The experi-
ments with solution stirring and in stagnant water, at
durations from a few hours to one year, and with dif-
ferent sizes of reaction vessels and lithological charac-
teristics of natural gypsum yielded a scatter in C m↑ , C m↓ ,
and C m↓ –C m↑ of approximately 1%.
DISCUSSION
The widest range of experimental C m↑ values was
obtained under the conditions when the particle size of
dispersed gypsum affects its solubility (r < 1 μm, C m↑ =
C m↑ (r), Fig. 1). At r > 1 μm, the solubility is indepen-
dent of particle size, C m↑ ≈ 0.0153 ± 4.5% M at 25°C,
and the maximum solubility was reached at r < 0.2–
0.5 μm (0.0182 M, 25°C); i.e., an order of magnitude
decrease in particle size is accompanied by a solubility
increase by 16%. Such a degree of supersaturation was
obtained for particle sizes much larger than could be
GEOCHEMISTRY INTERNATIONAL
expected from calculations using Eq. (1), i.e., larger
than 0.01 μm. Perhaps, such elevated solubility is
structure of the surface layer of grains during their
mechanical treatment (crushing and grinding), which
resulted in the chemical activation of the reaction sur-
face (gypsum powder may lose up to 8% H2O during
This feature explains the temporary supersatura-
observed in the experiments of Kuznetsov et al.
(1957). Furthermore, since sieves were used in these
much smaller than 90 μm could appear in the solu-
tion; this is indicated by a subsequent rapid decrease in
solution concentration, which can be explained only
by the growth of these smaller crystals. It is believed
that such growth of finely dispersed particles is charac-
teristic mostly of crystal hydrates (Enustun and
Turkevich, 1960).
The analytical solution on the basis of the Ost-
wald–Freundlich expression (Eq. 1) is approximate
because its derivation involved the assumption that
solutions can be described by ideal gas laws, and the
δ value is independent of particle size. Another unre-
solved issue is the influence of electric charge (Knapp
effect) and adsorption on the particle surface of any
active substances on the solubility of particles. This is
probably why the gypsum solubility in water calculated
using Eq. (1) is consistent with experimental data only
at r > 1 μm.
Adamson (1976) argued that a relation similar to
Eq. (1) is not theoretically justified and proved even
for the excess solubility of small ionic crystals in a dis-
persed state, although the method of experimental
determination of surface tension from solubility has
become rather widespread. For the dissolution of a
polymineralic surface of fractures and pores in gyp-
sum-bearing rocks in groundwater, such dependence
is only hypothetical. For instance, the C m↑ values
obtained for the dissolution of flat surfaces of different
lithological varieties of gypsum in water appeared to be
practically identical (Lebedev, 2015).
In lithological varieties with even micro-grained
textures, the fraction of particles with r < 1 μm is very
limited (Lebedev, 2015). During the dissolution of
rocks with such textures, a state of supersaturated
solution can probably be attained only for a short time
after which C m↑ approached gradually “normal” values
for given conditions; this was observed in the experi-
ments of Kuznetsov et al. (1957). Therefore, the
results of experiments on the dissolution of larger gyp-
sum grains (r > 10–500 μm) are most useful for the
solution of problems of mass transfer in groundwater.
Most of the investigations of gypsum solubility in
water (C m↑ , 25°C; Fig. 2) were performed under the
conditions when the solubility is independent of parti-
Vol. 55 No. 2 2017
 GYPSUM SOLUBILITY IN WATER AT 25°C
cle size, C m↑ ≠ C m↑ (r). In these investigations, the com-
position and stability of supersaturated solutions are
controlled by a combined effect of experimental con-
ditions. The influence of particular factors (i.e., gyp-
sum mass, solution volume, their proportion, geome-
try of the reaction vessel, intensity of solution stirring,
presence of insoluble admixture particles, preparation
of particles for the experiment, etc.) on C m↑ is
unknown. The most common solubility values
(0.0151–0.0154 M, Fig. 2) correspond to the results of
calculation (interval 4) and experimental data on the
dissolution of a flat gypsum surface (interval 3, Fig. 1).
Such a correspondence is probably due to a combined
effect of some common experimental features (factors
above).
The most important problem in the experimental
investigation of the solubility of finely dispersed parti-
cles is their preparation for experiments, i.e., prepara-
tion of fractions with a more or less uniform composi-
tion (both in particle shape and size). Under such con-
ditions, the true value of supersaturation or saturation
cannot be measured, because a monodispersed fraction
cannot be obtained (solution concentration changes
continuously). In fact, the measured values approach
more or less closely true values and are considered
appropriate for practical applications (Khamskii, 1975).
Therefore, the range of C m↑ = 0.0147–0.0161 M (~9%,
Fig. 2) characterizes the precision of C m↑ determination
(~4.5%) at the dissolution of dispersed gypsum in water
under the condition C m↑ ≠ C m↑ (r).
Such an uncertainty of gypsum solubility determi-
nation (~4–5%) may appear insufficient for the solu-
tion of problems of mass transfer in gypsum-saturated
groundwater. For instance, the path length of solution
saturation in gypsum in a 0.1-cm wide fracture at a
flow rate of <10–1 m/s can increase by up to 30% in
response to a concentration increase by 1% (Lebedev
and Lekhov, 1999).
Under the conditions of the dissolution of a flat
gypsum surface similar to natural one, the influence of
experimental conditions on C m↑ appeared to be negligi-
ble. In such a case, the scatter of C m↑ values is compa-
rable with the accuracy of solution analysis. The data
shown in Fig. 1 (interval 3) were obtained in a single
study (Lebedev, 2015). Nonetheless, the insensitivity
of measured parameters to changes in experimental
conditions (both quantitative and qualitative) allows
us to consider these data as representative.
It is obvious that the boundaries of the field of
metastable states of gypsum-saturated solutions can-
not be determined from the data shown in Fig. 1. For
approximate estimates, the maximum difference of C m↑
and C m↓ can be considered similar to the precision of
the determination of the solubility of dispersed gyp-
GEOCHEMISTRY INTERNATIONAL Vol. 55 No. 2
209
sum in water under the condition C m↑ ≠ C m↑ (r), and the
minimum difference can be estimated from the data
obtained for the dissolution of the flat surfaces of lith-
ological varieties of gypsum. Similar data on the solu-
bility of some minerals in water were reported by Har-
die (1967). Thus, the C m↑ – C m↓ range is approximately
1–5%, depending on the certain “safety margin” for
the solution of mass transfer problems.
CONCLUSIONS
Most of the investigations of gypsum solubility in
water at 25°C provided C m↑ values, and there are almost
no data for C m↓ . Therefore, the filed of metastable states
of gypsum-saturated groundwater cannot be currently
determined from experimental data. Supposedly, the
difference of the concentrations of dissolved gypsum
at the boundaries of this field is 1–5%.
The estimates of gypsum solubility in water at 25°C
↑
(C m) range from 0.0147 to 0.0182 M. Such a scatter of
C m↑ values (more than 20%) results from a combined
effect of experimental conditions. Their influence is
most prominent for the dissolution of dispersed gyp-
sum and very weak for the dissolution of a flat surface
of lithological varieties of gypsum similar to natural
ones. In the latter case, the precision of C m↑ is up to
±1%, and it can be used for modeling mass transfer
between gypsum-bearing rocks and groundwater.
The reverse dependence of the solubility of gypsum
particles in water on their size was experimentally
established (25°C) at r < 1 μm. As the grain size
increases to r > 1 μm, C m↑ decrases to a constant value
under the given experimental conditions. The results
of theoretical calculations of C m↑ using the approximate
Ostwald–Freundlich equation are consistent with
experimental data only at r > 1 μm. In the case of a
polymineralic surface of fractures or pores, such
dependence is still hypothetical.
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Translated by A. Girnis
Vol. 55 No. 2 2017