ISSN 00014370, Oceanology, 2010, Vol. 50, No. 6, pp. 861–868. © Pleiades Publishing, Inc., 2010.

Original Russian Text © A.P. Nedashkovsky, M.G. Shvetsova, 2010, published in Okeanologiya, 2010, Vol. 50, No. 6, pp. 910–917.

MARINE
CHEMISTRY

Total Inorganic Carbon in Sea Ice

A. P. Nedashkovskya and M. G. Shvetsovab
a
Arctic and Antarctic Research Institute, ul. Beringa 38, St. Petersburg, 199397 Russia
b
Pacific Institute of Oceanology, Far East Division, Russian Academy of Sciences, ul. Baltiiskaya 43,
Vladivostok, 690041 Russia
Email: nealpa@mail.ru
Received February 3, 2009; in final form, March 17, 2009

Abstract—The method proposed for determining the total inorganic carbon (TC) concentrations in sea ice
(Arctic region, North Pole35 expedition) based on the measurement of the total alkalinity (TA) and the pH
in the melt waters without the CO2 exchange with the atmosphere is considered. It is shown that the TC/Sal
and TA/TC values through the entire ice section remain similar to these parameters in the subice water. The
surface snow and the uppermost ice layers are characterized by elevated TA/TC values, which indicate the
–
reaction Ca2+ + 2HC O 3 = ↓CaCO3 + ↑CO2 + H2O. The release of CO2 to the atmosphere due to the
decomposition of calcium hydrocarbonate is as high as ~20 mmol/m2. The meltwater of the examined ice is
undersaturated with CO2, which may result in a sink of atmospheric CO2 (~30 mmol/m2).
DOI: 10.1134/S0001437010060056

INTRODUCTION The ice samples were collected in line with the

The measurements of the total inorganic carbon
(TC) concentrations in sea ice have received insuffi
cient attention. They are usually limited to the deter
mination of the total alkalinity (TA), the main contri
bution to which is provided by carbonate ions [3, 7].
Experiments [8, 10, 11] demonstrated that the freez
ing of seawater and diluted water solutions with hydro
carbonates results in the formation of calcium ions,
which indicates the development of the following
reaction:
2+ –
Ca + 2HCO 3 = ↓CaCO 3 + CO 2 + H 2 O.
When reaction (1) proceeds in natural conditions
and the forming СО2 is removed from the reaction
medium, the formation of sea ice is accompanied by
the release of carbon dioxide into the atmosphere [2].
In this connection, the measurement of the total
organic carbon concentrations in sea ice is of interest
for the study of the carbon cycle in waters that serve as
a source for ice formation, particularly in the Arctic
Ocean and Antarctica.
MATERIALS AND METHODS
Samples of firstyear ice and the snow covering its
surface that were taken by the North Pole35 expedi
tion in the period of November 2007 to June 2008
served as the materials for this study. The general char
acteristics of the examined ice and the information on
the sampling sites are presented in Tables 1 and 2.
technique in [1]. Before the drilling, the snow from the
ice’s surface was collected using a polyethylene scoop
and was placed into a polyethylene container 20 l in
capacity. For obtaining the ice core, a ring corer (9 cm
in diameter) was used. The sampled core was packed
into an elastic polyethylene film and transported to the
field laboratory, where it was immediately sawed into
cylinders 5–10 cm thick, which were placed into spe
cial containers for determining the total inorganic car
bon concentrations.
The method of measuring the total inorganic car
(1) bon content in the sea ice is based on the measurement
of the total alkalinity and the pH in the meltwater,
which is obtained without gas exchange with the
atmosphere, and the subsequent calculation of the
total inorganic carbon concentrations in line with the
theory of the seawater carbonate system. The ice’s
melting without gas exchange with the atmosphere
was realized in the following manner. The ice sample
(0.5–0.6 kg) was placed into an hermetically sealed
container (a bucket with a cover with a volume of 1.1 l
and a height of 11 cm made of polystyrene), which was
filled with water through a hole in the cover using a
siphon tube. For better sealing, the upper part of the
container with the cover was encapsulated using
Scotch tape and then the container was turned over.
For filling the container, seawater with known TC, TA,
and Sal values and aggressive toward the possible
CaCO3 phase in the sea ice was used. The seawater was
preliminarily treated in the following manner. A poly
ethylene can (V = 15 l) was practically entirely (the air
remaining was ~ 0.1 l) filled with subice seawater. To

861
862 NEDASHKOVSKY, SHVETSOVA

Table 1. General characteristics of the examined ice

Core Date, H of ice, Number of the
H of ice, cm Coordinates Age of the ice, days
number month/day/year water, cm sampling site
10 12/22/2007 69 2.8 83°59.6′ N 1 30–40
98°57.4′ E
13 01/03/2008 10 1.2 84°53.4′ N 2 2
93°08.6′ E
15 01/06/2008 33 0.8 84°50.7′ N 2 4
91°52.2′ E
16 01/14/2008 55 1.8 85°05.5′ N 2 12
91°26.9′ E
18 01/25/2008 53 0.6 85°19.2′ N 3 11
80°47.6′ E
21 02/23/2008 82 2.2 85°36.4′ N 3 40
64°17.9′ E
25 03/22/2008 122 1.0 85°14.7′ N 1 120–130
51°02.2′ E
32 04/17/2008 4 0 84°22.3′ N 4 1
39°13.4′ E
36 04/28/2008 7 0 84°02.9′ N 5 2
31°28.2′ E
39 05/07/2008 144 1.8 84°44.2′ N 1 165–175
28°51.0′ E
42 06/07/2008 220 7.4 82°21.2′ N 6 Presumably >1 year
28°12.1′ E

the latter was added 30 ml of 0.2 M HCl and 3 ml of parameters, the total inorganic carbon content was
saturated HgCl2 solution. Table 3 presents some char then calculated. In this procedure, the quantity of СО2
acteristics of the carbonate system for the seawater in the gas phase that is formed in the container during
used for filling the container and for the liquid phase in the melting of the ice was taken into account (the СО2
the container after the ice’s melting. content in the gas phase was calculated as the equilib
rium one at the container’s temperature before the pH
The weight of the ice and the added seawater was measurement). The total inorganic carbon content,
determined using a GX2000 electronic balance the total alkalinity, and the salinity of the ice
(made by the A&D Company in Japan; the weighing (ТСic, TAic, and Salic) were calculated using the follow
accuracy was 0.01 g). After the complete melting of the ing formula:
ice (the next day), the pH value, the alkalinity, and the
salinity were measured in the container. Using these Sal cont – Sal w ( 1 – α ic )
Sal ic = 
, (1)
α ic
Table 2. Characteristics of the sampling sites TA cont – TA w ( 1 – α ic )
TA ic = 
, (2)
Number of the α ic
Characteristics of the ice sampling site
sampling site
( TC + ΔCO 2 ) cont – TC w ( 1 – α ic )
1 Ice field (>1 km across) formed ~1 km away TC ic = 
, (3)
from the camp in October of 2007 α ic
2 Ice in the icefree water area 5–10 m wide formed m ic
in the initial part of January 2008 near the camp α ic = 
, (4)
m ic + m w
3 Ice field (~1 km across) formed ~1 km away
from the camp in January of 2008 ( CO 2 ) gas
4 Ice in the icefree water area 5–10 m wide ΔCO 2 = 
, (5)
m ic + m w
formed on April 16, 2008, near the camp
–6
5 Ice in the icefree water area 5–10 m wide ( V gas × P ( CO 2 ) ) × 10
formed on April 26, 2008, near the camp ( CO 2 ) gas = 
 . (6)
22.4 × ( T/273 )
6 Ice massif ~1 km away from the camp formed
after the substantial reorganization of the ice The indices “ic,” “cont,” and “w” designate the ice,
fields in the station’s area. the container (the melted ice and seawater in the con

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 TOTAL INORGANIC CARBON IN SEA ICE 863

Table 3. Some parameters of the carbonate system in the seawater used for filling the container and in the liquid phase formed in the
latter after the melting of the ice (core 25). The pH, carbon dioxide pressure, and saturation degree with calcite are given for 15°C
Sample Sal, psu pH TA, mequiv/kg TC, mmol/kg P(CO2), μatm Calcite saturation, %
Seawater 34.15 6.88 1.860 2.136 7522 19
S.w. + snow 31.91 7.44 2.006 2.044 2177 70
S.w. + ice 0–5 cm 26.34 7.12 1.370 1.487 3329 21
S.w. + ice 5–10 cm 21.58 7.15 1.212 1.316 2856 17
S.w. + ice 10–20 cm 21.69 7.20 1.257 1.352 2676 20
S.w. + ice 30–40 cm 20.17 7.17 1.157 1.255 2677 16
S.w. + ice 50–60 cm 20.14 7.14 1.148 1.254 2850 15
S.w. + ice 70–80 cm 20.59 7.10 1.172 1.29 3134 14
S.w. + ice 90–100 cm 19.96 7.09 1.132 1.25 3119 13
S.w. + ice 112–122 cm 20.66 7.09 1.168 1.288 3179 14

tainer), and the water added to the container with the
ice, respectively. Sal, Ta, and TC are the salinity, the
total alkalinity, and the concentration of the total inor
ganic carbon measured in psu, mequiv/kg, and
mmol/kg, respectively. αic is the share of the ice in the
container; ΔСО2 is the correction for the carbon diox
ide contained in the gas phase that is formed in the
container during the melting of the ice (mmol/kg);
(СО2)gas is the quantity of carbon dioxide contained in
the gas phase (mmol); Vgas is the volume of the gas
phase (ml); and P(CO2) is the pressure of the carbon
dioxide (μatm), which is in the equilibrium state with
the liquid phase in the container at the temperature T
(degrees K).
Vgas = Vcont – (mic + mw)/d, where d is the density of
the liquid phase in the container accepted to be equal
to 1.
The Salic, TAic, and TCic calculated in line with the
system of equations (1–6) may be used for assessing
the carbon dioxide pressure in the water formed during
the melting of the ice.
The pH value was potentiometrically determined
in a closed (preventing the СО2 exchange with the
atmosphere) thermostated cell at a temperature of
15.0°С using an ESL4307 measuring electrode and
an EVL1M reference electrode (made at the plant for
measuring instruments in Gomel). The working vol
ume of the cell was ~10 ml. The reference electrode
was located in a saturated KCl solution placed into the
measuring cell only during the readings. For its cali
bration, firstclass buffer standards manufactured by
VNIIF3 and phosphate and tetraborate buffer solu
tions characterized by a pH of 6.857 ± 0.004 and 9.179 ±
0.004, respectively, at 25°C were used. The solutions
were prepared using deionized water free of dissolved
gases, which were removed by boiling. The measuring
cell was thermostated using an F12 electronic ther
mostat (Julabo, Germany) with an accuracy of 0.1°C.
The measuring cell was filled using a siphon tube.
The electromotive force of the cell was measured
using a SEVEN MULTI S80 converter (Mettler
Toledo, Switzerland) with an accuracy of 0.1 mV. The
pH was measured with an accuracy up to 0.01 pH unit.
The alkalinity was determined by the method of
direct titration by HCl (~0.02 M) during the CO2
blowing by air free of carbon dioxide and ammonia
(Bruevich’s method [5]). The air expenditure was
~1.3 l/min. The volume of the sample used for the
titration was 50 ml. For the calibration, a sodium car
bonate solution with an exact weight was used. The titra
tion was potentiometrically performed in an ATP02
autotitration cell (Akvilon, Moscow) using the auto
matic titration regime with the determination of the
equivalent point. The parameters of the regime were
the following: the drop volume was 0.01 ml, the pause
was 4–8 s, and the stabilization level of the electrode
potential was 0.2 mV. The initial acid dose V0 was
accepted in such a manner that its subsequent volume
added to by drops up to the equivalency point was at least
0.7 ml. The titration was conducted for 17–20 min up to
a pH of ~ 4.5. The equivalency point was determined
by the method of “manual processing” at pH = 5.5–
5.4. The determination accuracy of the equivalent vol
ume was 0.01 ml, which corresponds to an error of
0.004 meqiv/l in the alkalinity assessment.
In the calculations of the total inorganic carbon
contents, the components of the carbonate system, the
constants of the carbonic acid dissociation after
Mehrbach [6], the constant of the boric acid dissocia
tion after Yman [6], the СО2 dissolubility after Weiss
[12], and the calcite dissolubility after Millero [9] were
used.
The ice’s salinity was determined using a GM65
electric salimeter. For its calibration, seawater stan
dards (K15 = 1.00025 and K21 = –0.3254) prepared at
the Shirshov Institute of Oceanology of the Russian
Academy of Sciences were used. The measurements
were preceded by the testing of the consistency
between the temperature in the conductometric cell

OCEANOLOGY Vol. 50 No. 6 2010

864 NEDASHKOVSKY, SHVETSOVA
H, cm
H, сm
40
0 10
40
80
80
120 120
160
160
200
0 4
200
0 20
Fig. 1. Vertical salinity variations in the examined ice. The inset shows the distribution of the salinity in cores 25, 39, and 42 (the
high salinity values in the snow at the ice’s surface are not shown). The snow’s thickness calculated for the meltwater is given in
the negative direction of the ordinate axis.
and the salimeter reading at the beginning of the expe
dition (October 2007). The testing was performed
using an F12 electronic thermostat (Julabo, Ger
many), which yields an accuracy of 0.1°С, and a mer
cury thermometer, which was verified at the Men
deleev AllRussian Institute of Metrology.
RESULTS AND DISCUSSION
Figure 1 demonstrates the vertical salinity varia
tions in the examined ice. Its distribution in all the
samples (except for core 42) is characteristic of young
and firstyear ice in this observation period [7]. The
maximal salinity was registered in the upper layer
including the surface snow (up to 80 psu). With its
growth, the ice becomes desalinated with the minimal
salinity being confined to its middle part. The sole
exception among the examined ice samples is core 39,
where the salinity of the snow and the upper ice layers
(ΔH = 10 cm) is lower as compared with that in the
underlying ice, which evidently indicates the onset of
the summer melting. The salinity distribution in core
25
39
42
8 12 16
Sal, psu
40 60 80
Sal, psu
42 is characteristic of ice already subjected to summer
melting. This is evident from the strongly desalinated
upper layer and the salinity minimum at a depth of
~130 cm [7].
Figure 2a demonstrates the correlation between the
total alkalinity and the salinity of the ice (data on all
the ice layers were used for constructing the plot).
As follows from the figure, all the measured values
are located near the straight line that crosses the origin
of the coordinates and whose incline is determined by
the TA/Sal value for the subice water. Notable devia
tions are observed for the surface snow, which is char
acterized by a higher TA/Sal value as compared with
that in the subice water, and the latter increases with
the snow desalination. Similar values were obtained by
the drifting SP34 station [4]. These data are consid
ered as an indirect indication that the thin snow layer
at the ice’s surface accumulates the calcium carbonate
phase. The main ice body is either free of reaction (1)
or the СаСО3 phase is removed together with the brine.
As a whole, the examined ice is characterized practi
cally by the same TA/Sal values as in the subice water.
OCEANOLOGY Vol. 50 No. 6 2010
 TOTAL INORGANIC CARBON IN SEA ICE
TA, mequiv/kg (а)
6
15
5
4 18
3 25
21 10
Subice water
2 39
0 20 40 60 80 0
Sal, psu
Fig. 2. Correlation of the total alkalinity (a) and the total inorganic carbon concentrations (b) in the examined ice samples with
the salinity. For comparison, data on the subice water layer are shown. The numbered data points designate the surface snow sam
ples with similar numbers.
Figure 2b demonstrates the correlation between the
total inorganic carbon concentrations and the salinity
in the examined ice. When constructing the plot, we
used the data obtained for the bedbybed sampled ice
core. In most cases, the data points coincide with the
straight line that crosses the origin of the coordinates
and whose incline is determined by the TC/Sal value
for the subice water. This means that the TC/Sal value
in the main ice body is practically the same as in the
subice water. This fact is consistent with the assump
tion that no reaction (1) occurs in the main ice body.
Otherwise, both the reaction (1) products (СаСО3 and
СО2) remain united and are removed together with the
brine.
Similar to the TA–Sal plot, notable deviations
from the straight line that crosses the origin of the
coordinates is observed for the surface snow. At the
same time, the TC/Sal value in the snow is lower as
compared with that in the subice water layer. This sup
ports the assumption that reaction (1) proceeds at the
ice’s surface with carbon dioxide released into the
atmosphere.
Figure 3a demonstrates the correlation between the
total alkalinity and the total inorganic carbon concen
trations in the examined ice. It is seen that the vertical
distribution of the TA/TC values is uniform except for
core 42: the TA/TC is equal to 1.07 ± 0.06 practically
through the entire ice section, which is well consistent
with its value in the subice water (1.069 ± 0.005). Only
in the snow at the ice’s surface does the TA/TC ratio
OCEANOLOGY Vol. 50 No. 6 2010
865
TC, mmol/kg (b)
15
3
Subice water
13
2 18
25 16
10
39
1 21
20 40 60 80
Sal, psu
increase to values close to 2. Such a TA/TC value
means that the СаСО3 represents the main form of the
inorganic carbon; i.e., reaction (1) in the snow at the
ice’s surface may proceed practically up to its comple
tion.
Figure 3b presents the calculated Р(СО2) values for
the water that is produced by the ice’s melting at 0°С
under conditions that the calcium carbonate is dis
solved. In all the samples, except for core 42, the СО2
pressure in the meltwater is substantially lower as com
pared with that in the atmosphere. The lowest СО2
pressure is characteristic of the snow and the upper ice
layer, which is explained by the release of the produced
СО2 into the atmosphere. For the young ice (cores 32,
34, and 36), the P(СО2) values are relatively high. This
is probably explained by the fact that the CO2 was not
yet released into the atmosphere. The high Р(СО2) val
ues observed in two layers of cores 10 and 16 represent
exceptions and probably resulted from measurement
errors. The obtained data imply that the meltwater
produced by the firstyear ice should consume atmo
spheric СО2, owing to which the ice melting should be
accompanied by a sink of carbon dioxide.
Before going into the discussion of the potential
physical factors responsible for the different parame
ters in the upper desalinated part of core 42 as com
pared with the general trend, it should be noted that
the TA and TC values, as well as their ratios, are char
acterized by large errors under low ice salinity and the
methods used. Unfortunately, the heavy ice conditions
866 NEDASHKOVSKY, SHVETSOVA

H, сm (а) H, сm (b)
–10 Subice water –10 36

10 10 32
42 10
30 30 42
16
50 50
70 70
90 90
110 110
130 130 Subice water
150 150
170 170
190 190
210 210

0 0.4 0.8 1.2 1.6 2.0 2.4 0 100 200 300 400 500
TA/TC P(CO2), μatm

Fig. 3. Parameters of the carbonate system in the sea ice. (a) The ratio between the total alkalinity and the total inorganic carbon
concentrations in the examined ice samples (mol/mol); (b) the carbon dioxide pressure calculated for the water produced by the
melted ice at 0°C. The numerals correspond to the core numbers.

in the area of core 42’s sampling prevented us from
obtaining additional ice samples.
The anomalous characteristics of core 42’s upper
part indicate high carbon dioxide contents in the liq
uid phase that produced the ice layer. It may be
assumed that the upper desalinated part of the ice sec
tion was formed due to the freezing of snow mixed
with water oversaturated with СО2. This may be
explained by the fact that such water becomes in equi
librium with the atmospheric СО2 before freezing, but
the subsequent oxidation of the organic matter iso
Based on the observations, the TC1 value may be
derived from the ice’s total alkalinity, since the TA/TC
value in the formed sea ice is equal to that in the subice
water layer (1.07). Then, TC1 = TAmeasured/1.07.
The total flux of СО2 released during the ice’s for
mation— F(CO2), mmol/m2—may be obtained by
summing the CO2 losses for all the ice layers:
n
F ( CO 2 ) = ∑ Δ ( CO ) .2 i (8)
i=1

lated from the atmosphere is accompanied by the
additional growth of the carbon dioxide pressure.
The obtained data allow the СО2 quantity released
into the atmosphere during the sea ice formation to be
assessed. For the ice layer with the thickness Н, the
equation is characterized by the following form:
ΔСО2 = 10 × (ТС1 – ТСmeasured) × d × H,
where ΔСО2 is the СО2 loss by the ice layer with the
thickness H (cm) per unit of the ice’s area (mmol/m2),
TC1 is the concentration of the total inorganic carbon
in the ice layer under the condition that no СО2 is
released (mmol/kg), TCmeasured is the observed concen
tration of the total inorganic carbon in the same ice
layer (mmol/kg), and d is the ice’s density (kg/dm3)
(for the snow at the ice’s surface, the thickness of
which is calculated for the meltwater, d is the water’s
density).
Figure 4 presents the results of these calculations.
The general trend of the F(CO2) variations, except for
core 18, is presented in the inset. The observed СО2
loss under Н = 0 is explained the fact that the snow’s
thickness is given, as was mentioned, with a negative
sign. The main СО2 loss is observed in the snow at the
ice’s surface and in the upper part of the core. There
(7) fore, the quantity of the released СО2 is practically
independent of the ice’s thickness. The obtained data
show that the formation of the firstyear ice during the
observation period lasting from January to the initial
part of May was accompanied by a CO2 release as large
as 20 ± 4 mmol/m2. According to [2], reaction (1) in
ice proceeds up to its completion. Our data provide no
grounds for such a conclusion: the ice layer 1 m thick
releases approximately 10% of the potential СО2.
The presented data on the concentrations of the
total inorganic carbon and the alkalinity in the first
year ice allow the potential quantity of СО2 that may

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 TOTAL INORGANIC CARBON IN SEA ICE 867

F(CO2), mmol/m2
28

18 21
24
39

15
10
20 13

F(CO2)
25

16 20

15

10
25
12 5
16

0 40 80 120 160
H, сm

8
0 40 80 120 160
H, сm

Fig. 4. The CO2 loss per unit of the ice area depending on its thickness. The numerals correspond to the core numbers. The inset
shows the general variations depending on the ice’s thickness.

be consumed by the meltwater to be estimated. Under
the ice’s thickness of 1 m, the СО2 consumption
should be as large as ~50 mmol/m2. The resulting
effect of the sea ice’s formation (CO2 release of
~20 mmol/m2) and its subsequent melting (CO2 con
sumption of ~50 mmol/m2) should consist of a sink of
carbon dioxide (~30 mmol/m2). This result is satisfac
torily consistent with the estimates obtained for the
firstyear Arctic ice [4].
The CO2 released during the ice’s formation and its
consumption during the ice’s melting may be respon
sible for insignificant seasonal variations of the СО2
concentrations in the nearice atmospheric layer.
CONCLUSIONS
Using the method proposed for measuring the total
inorganic carbon concentrations in young and first
year sea ice, it is demonstrated that the ratio between
the total inorganic carbon contents and the salinity
observed in the subice water layer is preserved in the
forming sea ice cover.
The snow at the ice’s surface and the upper ice layer
become depleted in carbon dioxide due to the reaction
of the calcium hydrocarbonate decomposition accom
panied by СаСО3 and СО2 formation.
The density of the released CO2 flux during the
period lasting from the beginning of the ice’s forma
tion to its summer melting is estimated to be 20 ±
4 mmol/m2. This constitutes approximately 10% of
the potential CO2 quantity that could be released in
the case of the complete decomposition of the calcium
hydrocarbonate in the ice layer 1 m thick.
The water produced by melted firstyear sea ice is
sharply undersaturated with carbon dioxide. Conse
quently, the ice’s melting may result in a sink of atmo
spheric carbon dioxide, which is estimated to be as
large as ~30 mmol/m2.

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868
APPENDIX
The relative error in measuring the total inorganic
carbon content by the proposed method is largely
determined by the accuracy of the alkalinity and pH
measurements. Under such an assumption,
ΔTC ic ΔTC ( Alk ) +
ΔTC ( pH)⎞
 ≈ 2 ⎛ 
TC ic ⎝ TC ic
where ΔТС(Alk) is the error in determining the total
inorganic carbon concentrations in the container
related to the error in the alkalinity measurement, and
ΔТС(pH) is the error in determining the total inor
ganic carbon concentrations in the container related
to the error in the pH measurement.
Using the numerical method, it may be shown that,
in the interval of the pH = 6.8–7.2, ΔТС(Alk) ≈ ΔTA
and ΔTC(pH) ≈ 0.4(ΔpH).
Assuming that TCic (mol/kg) ≈ 0.07Salic and ΔpH =
ΔTC 0.2
0.01, we obtain ic ≈  .
TC ic Sal ic
For the relative error (TA/TC)ic, the value should be
Δ ( TA/TC )
0.3
as follows: ic ≈  .
( TA/TC ) ic Sal ic
The calculated estimates show that the proposed
method is applicable for young and firstyear ice not
yet subjected to notable desalination. In the case of
strongly desalinated annual ice, the relative error in
determining the total inorganic carbon concentrations
may be significant.
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