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The effects of silica and water on the viscosity of hydrous quartzofeldspathic melts
F. HOLTZ,1,* J. ROUX,1 S. OHLHORST,1,2 H. BEHRENS,2 AND F. SCHULZE2
1
CRSCM-CNRS, 1A rue de la férollerie, 45071 Orléans, France
2
Institut für Mineralogie, Universit;ät Hannover, Welfengarten 1, 30167 Hannover, Germany
ABSTRACT
The viscosities of hydrous melts (0.65 to 2.8 wt% H2O) with quartzofeldspathic com-
positions corresponding to Ab, Ab74Qz26, and Ab48Qz52 (mole proportions calculated on the
basis of eight oxygen atoms; Ab 5 NaAlSi3O8, Qz 5 Si4O8) have been determined between
980 and 1375 8C at pressures between 190 and 360 MPa using the falling sphere technique.
The use of large bubble-free hydrous glass cylinders (placed in internally heated pressure
vessels) previously prepared and already containing markers and platinum spheres allows
falling distances up to several centimeters to be measured with a precision of 650 to 200
mm. This results in a precision of 615% relative or less for most viscosity data (610%
relative or less if the temperature is known within 65 8C).
For a water content of 2.8 wt% H2O, viscosity increases with increasing Qz content. In
the investigated viscosity range, no significant deviation from Arrhenian behavior is ob-
served and the activation energy of viscous flow increases slightly with decreasing water
content of the melt (for Ab). Combining the experimental data obtained in this study with
data for a haplogranitic composition investigated previously by Schulze et al. (1996) shows
that the viscosities, and hence, the activation energies of viscous flow are similar for
compositions with the same atom ratio (Si 1 Al)/(H 1 Na 1 K) (SA/HNK). Thus, melt
viscosity is constant if Al, charge balanced by Na or K, is exchanged with Si 1 H (H
incorporated as OH or H2O). The viscosities (in dPa·s) of all investigated hydrous haplo-
granite compositions with water contents ranging between 0.7 and 8.2 wt% H2O can be
calculated to better than 60.15 log units using the expression:
logh 5 21.8 1 [940 1 5598·(SA/HNK)0.3774]·1/T
where T is expressed in Kelvin and varies from 1073 to 1650 K.
TABLE 2. Water content of starting hydrous glasses used for the settling distance(s) of the sphere(s) after the quench.
the viscosity determinations and water contents of The latter was measured with a microscope (see above)
glasses after the viscosity determinations using the position of the marker, considered to be static,
Ab Ab Ab75Qz25 Ab50Qz50 and that of the spheres before and after the experiments
Sample 0.65% H2O 2.8% H2O 2.8% H2O 2.8% H2O (Table 3). Several runs were performed at different P-T
step 2 experiments conditions with the same glass cylinder, thus allowing
end A of cylinder 0.65 3.06 3.55 2.82 determination of melt viscosities using the same sample
step 2 experiments
end B of cylinder 0.62 2.61 2.53 2.82 at different conditions. After each experiment, the plati-
after step 4 experiments num capsule was opened, the falling distance was mea-
end A of cylinder 0.65 2.83 2.72 2.72
after step 4 experiments
sured, the glass cylinder was turned upside down (so that
end B of cylinder ND 2.87 2.92 2.81 the platinum spheres were falling back in the opposite
average H2O content direction from the previous experiment), and sealed again
of the melt* 0.65 2.85 2.82 2.77
in a new platinum capsule for the next experiment.
Note: All analyses were performed by Karl Fischer titration (see preci- The viscosity, h (in dPa·s or poises), is derived from
sion in text). Ends A and B refer to the two ends of the cylinders. The
analyses were performed from glass pieces collected after the hydration the equation
experiments (step 2 experiments, see text) and after the viscosity exper-
iment (after step 4 experiments). ND 5 not determined. h 5 2·g·Dr·r2·Cf /9·v (1)
* The average H2O content is calculated from the determinations made
after the experiments.
where r is the radius (cm) of the sphere, g the acceleration
due to gravity (cm/s2), Dr the density (g/cm3) difference
between that of the platinum sphere (21.45) and of the
hydrous glass cylinders with a perfect cylindrical shape melt, Cf the Faxen correction, and v the settling velocity
and a diameter of 4 mm. One sample is slightly more Qz- of the spheres (cm/s). The mathematical expression for
rich than expected (Ab75Qz25, Table 1), and two are slight- Cf is given by Shaw (1963, Eq. 2), Dingwell (1987, Eq.
ly peraluminous (Ab75Qz25 and Ab50Qz50, Table 1). 3), and Schulze et al. (1996, Eq. 2). The values of Cf and
of the density of the melt used to calculate the viscosities
Sample preparation for viscosity determinations (step 3) are given in Table 3. The Faxen correction used in Equa-
The glass cylinders with a diameter of 4 mm (15 to 18 tion 1 takes the effects of capsule walls into account (non-
mm long) were loaded into platinum capsules along with infinite medium), but not the possible effects of the ends
one or two platinum spheres and a platinum marker. Plat- of the capsule (see discussion). The density values that
inum powder was placed at the bottom of the capsule have been used were taken from studies of Behrens et al.
between a slice of glass and the cylinder to obtain a mark- (1996) for Ab glasses, and extrapolated from the studies
er perpendicular to the long axis of the cylinder. The plat- of Schulze et al. (1996) and Behrens et al. (1996) for the
inum sphere(s), surrounded by glass powder (collected Ab-Qz glasses. The small variations of the density due to
from the second step experiments), were placed at the top this extrapolation as well as those resulting from the ex-
of the capsule. Both the diameter and weight of the plat- trapolation of the density of glasses to that of melts do
inum spheres were determined before they were loaded not affect significantly the viscosity determination (Ding-
into the capsule. Only spheres that yielded the same di- well and Mysen 1985; Schulze et al. 1996). In one sample
ameter from both direct microscopic determination and (Ab50Qz50), one platinum sphere was extremely deformed
weighing were used. The capsule was sealed and then after the preparation experiment [lenticular shape with an
placed in an IHPV at the same P-T conditions as those axial ratio (c/a) of ;0.6]. On the basis of results of Kerr
planned for the viscosity determinations. Run times and Lister (1991), a correction factor of 0.9 (hmelt 5 0.9
ranged from 30 to 60 min. After the experiment, most of hdetermined) was applied to determine melt viscosity (Table
the spheres were still spherical. However, some became 3).
slightly ellipsoidal or lenticular, probably due to pressure In glass cylinders containing two spheres, two inde-
exerted at room temperature by the glass fragments on pendent viscosity determinations are obtained for each
the spheres (pressure is applied before heating up in the experiment using Equation 1. A third viscosity value can
experimental procedure). The positions of the platinum be calculated using the difference of the settling distances
marker and of the spheres within the translucent glass
of the two spheres. The latter determination does not re-
sample were determined using a microscope equipped
quire the existence of a marker and is given by the
with an automated x-y stage. Several determinations of a
equation:
distance (up to 10 mm) between two points showed a
variation of less than 5 mm. h 5 2·g·Dr·t·(r 2f ·Cfl 2 r 22·Cf2)/9·Dd (2)
Determination of viscosity (step 4) where t is the experimental duration (in seconds) and Dd
Viscosity experiments were performed by sealing the the difference of settling distances (d1-d2 in cm) between
glass cylinder (obtained from step 3) in a platinum cap- spheres 1 and 2 (r1, Cf1,, r2, Cf2, are the radii and Faxen
sule, holding it at the desired P and T, and determining corrections for spheres 1 and 2, respectively).
30 HOLTZ ET AL.: VISCOSITY OF HYDROUS MELTS
TABLE 3. Experimental conditions and results of viscosity determinations in Qz-Ab hydrous melts
Experimental Sphere* Settling logh (exp) logh (exp) by logh (calc)
T (8C) P (MPa) duration(s) radius (mm) distance (mm) (dPa·s) difference† (dPa·s)
Ab—0.65 wt% H2O (Cf 5 0.869 for r 5 125 mm; Cf 5 0.861 for r 5 133 mm; d 5 2.36)
1275 360 33185 125 4.267 6 0.12 4.64 5.10 4.53
133 4.436 6 0.12 4.67
1325 360 6480 125 1.271 6 0.12 4.46 4.47 4.33
133 1.411 6 0.08 4.46
1375 340 10620 125 3.596 6 0.15 4.22 4.25 4.14
133 3.975 6 0.09 4.23
Ab—2.8 wt% H2O (Cf 5 0.874 for r 5 120 mm; d 5 2.33)
980 320 25170 120 1.30 6 0.08 5.01 4.91
1140 310 23480 120 7.47 6 0.30 4.22 4.15
1200 310 19980 120 10.65 6 0.30 3.99 3.91
Ab75Qz25—2.8 wt% H2O (Cf 5 0.890 for r 5 105 mm; Cf 5 0.872 for r 5 126 mm; d 5 2.34)
1115 280 42391 105 319 6 0.08 4.74 4.66 4.73
126 4.72 6 0.17 4.72
1200 290 19320 105 4.07 6 0.15 4.29 4.27 4.35
126 5.79 6 0.15 4.29
1307 290 4050 105 2.42 6 0.09 3.84 3.85 3.93
126 3.38 6 0.25 3.84
1307 280 7140 105 4.15 6 0.12 3.84 3.86 3.93
126 5.80 6 0.20 3.85
Ab50Qz50—2.8 wt% H2O (Cf 5 0.857 for r 5 136.5 mm; Cf 5 0.834 for r 5 159 mm; d 5 2.30)
1135 210 65795 136.5* 4.50 6 0.08 4.94* (4.77)† 4.97
159 6.84 6 0.08 4.93
1200 190 25980 136.5* 3.55 6 0.05 4.64* (4.54)† 4.70
159 5.15 6 0.05 4.65
1305 190 10650 136.5* 4.06 6 0.05 4.20* (4.03)† 4.24
159 6.17 6 0.05 4.18
Note: Cf, r, and d are the Faxen correction, sphere radius, and density, respectively, used for the determination of viscosities [logh(exp)]. The viscosity
calculated from Equation 4 is given for comparison [logh(calc)].
* The radii of the spheres indicated in the table are those determined before the experiments. The value of the experimentally determined viscosity
has been corrected by a factor of 0.9 to account for the lenticular shape of the sphere with an initial radius of 136.5 in composition Ab50Qz50 (see text).
† Viscosity values calculated from the settling difference of the two spheres, using Equation 2 (see text). This calculation does not take into account
the shape of the spheres; if one or both spheres is not strictly spherical, the viscosity value is erroneous.
EXPERIMENTAL AND ANALYTICAL TECHNIQUES tration and on the amount of water that is titrated. In this
Experimental apparatus study, the water content was determined with an absolute
precision of 60.15 wt% H2O.
All experiments at high P-T conditions were con-
The water contents at both ends of the hydrous glasses
ducted in two IHPV, equipped with high-temperature
synthesized in the second experimental step were almost
furnaces allowing temperatures up to 1400 8C to be
reached with temperature gradients of less than 10–15 identical for three samples, but one sample was not per-
8C along 30–40 mm long capsules (three PtRh6-
fectly homogeneous (Ab75Qz25, Table 2), which is prob-
PtRh30 thermocouples were positioned along the cap- ably the result of a heterogeneous distribution of water
sules). A detailed description of the pressure vessels within the glass powder before the synthesis of the hy-
and furnaces is given by Roux and Lefèvre (1992) and drous glasses. To reduce the water gradient along the
Roux et al. (1994). The experimental conditions for the sample, this glass was subsequently heated at 1250 8C
experiments designed to measure melt viscosities and 300 MPa for 4 h before the viscosity determination
(980–1375 8C, 190–360 MPa) and durations (67–1096 experiments. The identical viscosities obtained for two
min) are listed in Table 3. The heating rate between experiments at 1307 8C (Table 3), which corresponds to
800 8C and the desired temperature varied between 120 the first and last viscosity experiments conducted with
and 160 8C/min. The cooling rate between 1375 and sample Ab75Qz25 is evidence for a homogeneous distri-
900 8C was approximately 120 8C/min. bution of water in the melt during the viscosity experi-
ments. In addition, water contents at both ends of this
Water content of glasses glass sample analyzed after the last viscosity experiment
The water contents of the glasses were determined by are identical within error (Table 2). For the other samples,
Karl Fischer titration (KFT). This technique, also used no loss of water occurred during the experiments and wa-
for the determination of water solubilities, is described in ter contents determined before (after step 2 experiments)
detail by Behrens (1995) and Holtz et al. (1995). The and after the viscosity determinations (Table 2) were
relative precision depends mainly on the duration of ti- identical.
HOLTZ ET AL.: VISCOSITY OF HYDROUS MELTS 31
TABLE 4. Activation energies of viscous flow and pre-exponential coefficients determined from the experimental results
Ab Ab Ab75Qz25 Ab50Qz50
Sample 0.65% H2O 2.8% H2O 2.8% H2O 2.8% H2O
activation energy, Ea (kJ/mol) 210 (643) 165 (613) 193 (619) 187 (622)
logho (dPa·s) 22.41 (61.39) 21.86 (60.49) 22.55 (60.68) 21.99 (60.76)
Note: The error given in parentheses has been calculated considering that the viscosity is determined with a precision of 610% relative.
32 HOLTZ ET AL.: VISCOSITY OF HYDROUS MELTS
to 400 mm), and the radius of the glass cylinders smaller ically that identical viscosities are obtained as a function
(R 5 0.125 cm), resulting in Faxen correction values that of time.
were higher (thus increasing potential error in viscosity The technique employed in this study significantly
determinations). In the present study, the correction for minimizes the uncertainties resulting from measurement
the height of the cylinder (end effects of the capsule) of settling distances, and the determination of temperature
would result in a maximum variation of 0.015 log units becomes the most important source of error. The temper-
for the viscosity and can be neglected (see calculation in ature is known with a precision better than 610 8C. This
Shaw 1963). range takes into account both the temperature gradient
The major source of error in experiments based on the along the sample and the precision of thermocouples. The
falling sphere technique is generally considered to be the resulting effects on viscosity range between 68–11% rel-
precision of the settling distance of the spheres (e.g., ative, depending on the temperature (60.04–0.05 log
Shaw 1963). In this study, the positions of the sphere and units). Because all viscosity (step 4) experiments were
of the marker were determined without changing the fo- performed in the same IHPV, and because the maximum
cus of the microscope. The distance between the sphere temperature was always recorded in the central part of
and marker was measured six to ten times for three or the sample where the platinum spheres were located, tem-
more positions of the cylinder (obtained by rotation of perature readings are probably precise to 65 8C.
the cylinder), and an average settling distance of each The calculated maximum overall error for viscosity
sphere is given in Table 3. The maximum and minimum values obtained in this study is close to 615% relative if
values were used to calculate the error of the settling T is known within 610 8C. If T is considered to be con-
distance given in Table 3. In the case of long settling strained within 65 8C, a precision of 610% relative or
distances and for small variations (e.g., the experiment less is attained for most of the viscosity data reported in
with Ab50Qz50 at 1135 8C, sphere with r 5 159 mm), the Table 3 (viscosity calculated from the settling distance
precision of the viscosity can be as good as 60.0035 log between the marker and the sphere). It is emphasized that
units or 60.8% relative. For all other determinations, the the difference of density between glasses and melts, and
error of the viscosity due to the measurement of the set- the error of the determination of the radius of platinum
tling distance of at least one platinum sphere is , 66% spheres, have not been considered in the precision given
relative (corresponding to 60.025–0.03 log units), except above. These errors can be neglected for the determina-
for Ab-0.65 wt% H2O at 1325 8C with an error of 610% tion of the effect of T on the viscosity of a given com-
relative (60.05 log units). The uncertainties for most vis- position (the same glass cylinder with the same platinum
cosities are within 61–4% relative. In samples containing spheres are used).
two platinum spheres, the viscosity determinations could The precision of viscosity determinations in previous
be duplicated, and the variation resulting from the deter- studies is estimated to be 615% (Dingwell 1987; White
mination of the settling distance of each sphere is 7.1% and Montana 1990; Baker and Vaillancourt 1995). Baker
relative for one experiment and ,5% relative for all other and Vaillancourt (1995) performed duplicate experiments
experiments. for two experimental conditions and the determined vis-
The uncertainty in measuring the time of descent varies cosities differed by 21 and 5% relative, which is consis-
with the duration of the experiment. To calculate the ve- tent with an uncertainty of 615% relative. However, most
locity of the sphere, the beginning of the experiment was of their experiments were performed in piston cylinder
considered to be 10 8C under the set point. The end of apparatus with small capsules (3 mm in diameter and 3
the experiment was the moment at which power was to 4 mm long in some cases, Baker and Vaillancourt
turned off. If a correction of 2 min is applied, which takes 1995; Baker 1996), which increases potential error, es-
into account the heating and cooling time between the set pecially in the determination of the Faxen correction fac-
point and a temperature 120 8C below the set point. It tor (end effects of the capsule must be taken into account;
also takes into account the viscosity increases by 2% rel- e.g., Shaw 1963; Baker and Vaillancourt 1995). The
ative for experiments with durations of 6000 to 10 000 s marker and the metal spheres were placed in glass powder
(10.01 log units or less) and by 1% relative or less for and the viscosity experiments were conducted directly
experiments with durations longer than 19 000 s. The un- with this starting material (Dingwell 1987; Baker and
certainty is 2.8% relative for the shortest experiment Vaillancourt 1995). With this procedure, the initial rela-
(4050 s). tive position of spheres and markers is not constrained
The possible lag in the starting time of sinking of the and both can move during the loading of the capsule in
platinum sphere can be determined with experiments of the piston cylinder (glass powder is not a rigid medium).
different durations. The effect of experimental duration An additional problem in some studies is that glasses
was tested for one condition (1307 8C for composition were not always prehydrated (water was added to the dry
Ab75Qz25) and the viscosities were found to be identical glass for the viscosity experiments of Baker and Vaillan-
after 4050 and 7140 s (Table 3). This was also observed court 1995; Baker 1996), and heterogeneous distribution
by Schulze et al. (1996) for Ab38Or34Qz28 (AOQ) melts. of water in the melt at the beginning of the experiment
Because of the long experimental durations (always may affect the velocity of the sphere.
.4000 s), it was not deemed necessary to test systemat- Consequently, compared with the technique designed
HOLTZ ET AL.: VISCOSITY OF HYDROUS MELTS 33
Comparison with previous models and implications for and Dingwell (1996). For albite melts with 2.8 wt% H2O,
the viscosity of natural felsic melts the calculated and experimental viscosities are almost
The most popular model used to predict the viscosity identical at 1200 8C. However, it can be noted that the
of natural hydrous silicate melts was proposed by Shaw model would fail in predicting adequately the temperature
(1972) and derived from the model of Bottinga and Weill dependence of the viscosity of albite melts. With decreas-
ing temperature from 1200 to 980 8C, an increase in the
(1972). Recently, several studies have emphasized that
viscosity of 1.24 log units is predicted, whereas the ex-
the model of Shaw (1972), and therefore also the exten-
perimentally determined viscosity increase is 1.02 log
sion of this model to peraluminous melts proposed by
units. This deviation is small but shows that the activation
Goto et al. (1997), underestimates the viscosity of water-
energy for viscous flow is significantly dependent on the
rich haplogranite melts and overestimates the viscosity of
anhydrous composition of granitic or rhyolitic melts. For
water-poor melts at geologically relevant temperatures
such compositions, a change of the anhydrous composi-
(e.g., Baker 1996; Dingwell et al. 1996; Schulze et al.
tion may cause a variation of 20 to 40 kJ/mol at high
1996). This is also observed for the Ab-Qz compositions
temperatures (900 to 1300 8C, e.g., Holtz et al. 1996).
investigated in this study (Fig. 4C). However, in the in-
This compositional effect, as well as the non-Arrhenian
vestigated viscosity range (logh 5 103.5 –105.5), the model
behavior of viscosity (e.g., Bottinga 1994), must be un-
of Shaw predicts the viscosity with a maximum error of
derstood and taken into account if the viscosities of rhy-
60.5 log units. The differences are expected to be more
olitic melts are to be predicted with a precision better than
pronounced for melts with viscosities higher than 105.5 that obtained from empirical models. The best empirical
poise and lower than 103.5 poise (Schulze et al. 1996). For model that has been proposed to date is that of Hess and
a given experimentally determined viscosity, the predict- Dingwell (1996) with a standard deviation of 0.46 log
ed viscosity for Ab75Qz25 melts is systematically higher units and a validity over a wide viscosity range.
than the predicted viscosity for Ab and Ab50Qz50 com-
positions (Fig. 4C). Although these variations are small ACKNOWLEDGMENTS
(0.2 log units), they suggest that the model of Shaw This research was supported by Procope (German-French collaboration
(1972) does not accurately predict the effect of changing programme no. 95023) and the European TMR project ‘‘In Situ hydrous
SiO2 content in hydrous haplogranitic melts. melt properties (proposal no. ERBFMRX CT 960063).’’ The manuscript
The model of Persikov et al. (1990) and Persikov has been improved by the comments of B. Mysen, M. Pichavant, and B.
Scaillet. The manuscript also benefited from reviews by D. Baker, Y. Bot-
(1991) requires that the proportions of hydroxyl groups tinga, J. Blencoe, and an anonymous reviewer.
and molecular H2O be known. This has been determined
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