Canadian Journa canadien

Chemistry
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Volume 54 Number 21 November 1. 1976 Volume 54 numCro 2% 1 novembre 1974

Heat capacities of aqueous electrolytes: eight 1:l elee&sIytesand

AC: for ionizagon of water a&298 K
PREMPAUL SINGH,'EARLM . WOOLLEY,~
KEITH6 . MCCURDY,
A N D LOREN6 . HEPLER
Department of Chemistry, University of Lethbridge, Lethbridge, Alta., Canada T I K 3M4
Received April 29, 1976

PREMPAULSINGH,EARLM. WOOLLEY, KEITH6. MCCURDY, and LORENG. HEPLER.Can. J.

Can. J. Chem. 1976.54:3315-3318.

Chem. 54, 3315 (1976).

We have made measurements with a flow calorimeter leading to apparent molal heat
capacities of aqueous solutions of NaC1, HCI, KBr, KCI, KOH, NaBr, HBr, and NaOH at
298 K. Results have been used to derive apparent molal heat capacities of these electrolytes at
infinite dilution and thence AC,o = -215.2 +
4 5 K-1 mol-1 for ionization of H20(liq)
a t 298 K.
PREMPAULSINGH,EARLM. WOOLLEY,KEITHC. MCCURDYet LOREN6. HEPLER.Can. J.
Chem. 54,3315 (1976).
On a fait des mesures, B l'aide d'un calorimktre B Ccoulement, qui permettent de dkterminer
les capacitCs calorifiques molales partielles apparentes de solutions aqueuses de NaCl, HCI, KBr,
KC1, KOH, NaBr, HBr et NaOH a 298 K. O n a utilisC ces risultats pour en dCriver les capacitCs
calorifiques molales apparentes de ces 6lectrolytes a dilution infinie d'ou on a tirC que AC,o =
-215.2 f 4 5 k-I mol-I pour I'ionisation de HzO(1iquide) a 298 K.
[Traduit par le journal]

Introduction various systems. Although generali~ationscon-

cerning the usefulness of heat capacities are
It has been known since 1858 when Kirchhoff
about equally valid for solids, liquids, gases, and
(1) derived
solutions, difficulties in making the appropriate
111 (aa~/ar),= ac, measurements on solutions have severely in-
hibited such investigations.
that heat capacities are useful for classical Recent developments in calorinletry have
thermodynamic calculations. Following Ein- diminished some of the experimental difficulties
stein's (2) application of quantum theory and previously associated with measurement of heat
statistical thermodynamics to the theory of the capacities of dilute solutions. Nearly simul-
temperature dependence of the heat capacities of taneous increased interest in the properties of
simple solids, there have been many instances in aqueous solutions at temperatures other than
which heat capacities have been used in obtaining -298 K has provided new incentive for applying
information about the microscopic properties of calorimetry to investigation of heat capacities of
aqueous solutions with a view toward providing
'On leave from Department of Chemistry and Bio- thermodynamic properties that will be useful for
chemistry, Punjab Agricultural University, Ludhiana,
India.
calculations leading to knowledge of aqueous
*On leave from Department of Chemistry, Brigham systems at various temperatures.
Young University, Provo, Utah, U.S.A. In this paper we report the results of our heat
 CAN. 1. C K E M . VOL. 54. 1976

TABLE
1. Apparent molal heat capacities of aqueous electrolytes at 298 K*

Number of
4c O Concentration concentrations
Solute (9 K-I mol-1) B (eq. 2) ranae (m) investigated
NaCl
HCl
KC1
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KBr
KOH
NaOH
NaBr
HBr
*We use i values liere to indicate standard deviations. Limits on systematic uncertainties are dis-
cussed in the text.

capacity measurements on dilute aaueous solu- by careful addition of B ~ ( O H ) Zsolution to precipitate

2

tions of eight important 1 : 1 electroiytes( N ~ c ~ , barium carbonate. Five different stock solutions of KOH
A

KBr, KC1, KOH, NaBr, HBr, and NaOH) (B.D.H. Analar) were also prepared in this way. All of
these solutions were then standardized by titration as
at 298 K. Part of the motivation behind these described above,
Can. J. Chem. 1976.54:3315-3318.

measurements was simply to determine apparent Five HC1 (ACS reagent grade) solutions were standard-
and partial nlo]al heat capacities of these electro- ized against NaOH solutions prepared as above, while
lytes for subsequent thermodyrlamiccalculations, one HCI ~olutio" was standardized against HgO as
described by Kolthoff et al. (10). Stock solutions of HBr
More we are concerned with corn- were prepared and standardized similarly; all such solu-
bination of the results of this investigation to tions were stored in brown bottles and handled in a
obtain ACp0for ionization of water. partially darkened laboratory.

Experimental Results and Discussion

Most of our heat capacity measurements have been Our experimental results (compositions of
made with a Picker flow calorimeter that has been solutions, thermal data from calorimetric meas-
described in several publications (3-7) from the UniversitC
de Sherbrooke. Because the flow calorimeter measures
urements, and densities of solutions) have been
volumetric specific heats, we have also measured densities combined as previously described (3-7) to obtain
of all of our solutions as previously described (8). Calori- . ~ +c
apparent molal heat capacities ( c # ~ ) The
metrically measured volun~etricheat capaci:ies have been values so obtained are accurately represented by
combined with our densities and known compositions of equations of the form
solutions to obtain apparent lnolal heat capacities (+<.)as
described previously (3, 4) and subsequently modified (7).
Most of our calorimetric measurements were made with
flow rate about 0.6 cc/min. Heating rates were generally
set a t 100 mW. Measurements on solutions with concen- in which +,O represents the apparent molal heat
trations less than -0.15 mol/kg were made relative to capacity at infinite dilution. The coefficient of
water. Some measurements on more concentrated sclu- i d / ' is derived from the Debye-Hiickel theory
tions were also made relative to water, but most were and B is an adjustable parameter for each solute.
made relative to more dilute solutions.
A few heat capacity measurements on relatively con-
We list +CO and B values for each electrolyte in
centrated solutions were made with the 100 ml glass Table I , along with the concentration ranges of
calorimeter of the LKB 8700 system. solutions and statistical measures of the accuracy
Solutions of NaCI, NaBr, KCI, and KBr were prepared of fit of [2].
by weight from Fisher certified analytical reagents and Although our principal interest in this investi-
freshly degassed distilled water.
Five ditferent stock solutions of NaOH (B.D.N. Ana- gation has been the measurements on relatively
lar) were prepared at different times. Carbonate was dilute solutions in order to obtain +cOvalues, we
removed as described by Vogel (9). The resulting car-
bonate-free solutions were standardized against potassium 3Complete set of the actual experimental data is avail-
acid phthalate. All dilutions of these stock solutions were able, at a nominal charge, from the Depository of Un-
made with degassed water. published Data, C!STl, National Research Council of
One stock solution of NaOH was freed from carbonate Canada, Ottawa, Canada K:A 0S2.
 SlIiGW ET AE. 3317

have made a few measurements on more con- T a a ~ r2 ACpo values for tonlzatlon of
centrated solutions in order to obtain some IE20(I1q)at 298 K -
independent checks on the accuracy of the flow
calorineter. To this end we have used the LKB M+, X-
' c; 0
(J K-1 mol-1)
(non-flow) 8700 calorimetric system for measure-
ments leadifig to apparent molal heat capacities
of 1.0 and 3.2 nz NaCl solutions. Details of the
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method and results will be reported later; for

now it is suficient to state that results of these
"We ure i values here t o indicate standard
measurements and our measuremeats with the deviations. Limits o n systematic unceitaiotics arc
flow ca!orimeter (with caiculations done as discussed in the text.
described recently (7)) are in good agreement.
Further, these results for concentrated solutions MOH is in agreement with c $ = ~ ~- 126.8 3 K-I
are also in good agreement with heat capacities mol-I selected by Parker (12). For aqueous
measured by Cerutti (11). Thus we have con- NaOH we have +cO = - 102.1, -94.6, and
fidence in the accuracy as well as the sensitivity - 96.2 J K-l mol-I from Parker (12), Desnoyers
of the flow calorimeter. and co-workers (7, 15), and from our work,
We now turn to several com.parisons of our respectively.
+,O values with those reported by earlier in- Parker (12) has selected = -95.4 J K-I
Can. J. Chem. 1976.54:3315-3318.

vestigators. mol-I for aqueous NaBr. Desnoyers and co-

Parker (12) has reviewed earlier heat capacity workers (4, 7) have reported +cO= - 88.1 J K-I
measurements on aqueous NaCl and selected mol-I, in good agreement with our - 88.4 J K-I
+cO = -90.0 J K-I mol-I as the "best" value. mol-I.
Measurements of enthaipies of solution at differ- For aqueous HBr Parker (12) has selected
ent temperatures have led Criss and Cobble (13) +O , = - 141.8 J K-I mol-l, while our measure-
to +cO = - 79.1T. K-I mol-l. Flow calorimetric ments have led us to +,' = - 132.6 9 K-l mol-'.
measurements have led Picker et a]. (3) to One of the principal purposes of this research
$cO = - 82.4 J K-I mo!-I and Desnoyers and has been to obtain quantities that would permit
co-workers (4, 7) to +,O = -84.4 J K-I mol-I. calculation of ACpOfor ionization of water that
Our $cO = - 84.6 J K-' mol-I is in good agree- we represent by
ment with the latter two values and in fair
agreement with the value obtained by Criss and
Cobble (13). Because +CO = c: for a solute at infinite
Parker (12) has selected +cO = - 136.4 5 K-I dilution, we can combine our results from
mol-I for aqueous HCl. Enthalpy of solution Table 1 as follows to obtain the desired AC,O of
measurements have led Ahluwalia and Cobble ionization of water:
(14) to +,O = - 127.6, while flow calorimetric
measurements have led Desnoyers and co-
workers (4, 7) to +O, = - 124.1 J K - h ~ l - ~ .
Our +cO= - 127.2 J K-I mol-I for aqueous
HCl is in especially good agreement with one of Using our results from Table 1 with Cp0(H20)=
these values and fair agreement with another. 75.29 J K-'' rnol-I (16), we obtain the four semi-
For aqueous KC1 we have +cO= - 114.6 J independent ACpOvalues that are listed in Table
K-I mol-I from Parker (12) and - 114.2 J K-I 2. On the basis of all these results, we choose
mol-I from Desnoyers and co-workers (4, 7), in AG,O = - 215.2 0.8 J K-"01-I + as the best
excellent agreement with our - 114.1 J K-I value to be derived from our work. Here we have
+
mol-l. There is similar excellent agreement used to indicate the standard deviation; limits
between +cO = -120.1, -118.3, and -119.1 5 on systematic uncertainties are discussed below.
K-"01-I for aqueous KBr from Barker (12), Our assessment of uncertainties in the various
Desnoyers and co-workers (4, 7), and from our measured quantities and subsequent calculations
work, respectively. leading to cpc and values suggests that the
Our +CO = - 127.0 5 K-l mol-l for aqueous total uncertainty in each of these latter quantities
 3318 CAN. I. CHEM. VOL. 54. 1976

as listed in our Table I is about 5 3 J K-I mol-l. water at six temperatures from O to 50 'C.They
This estimate of total uncertainty is consistent have analyzed their results to obtain AC: =
with agreement of some of our results with -214 k 5 9 K-I mol-"or ionization of water at
related results of some other investigators al- 298 M, in excellent agreement with the new value
ready cited. Because all of our measurements and we have reported Inere.
calculations ieading r s bC0 values have been
carried out similarly, relative accuracies of our 1. 6. KIRCHHOFP. Ann. Pbys. (Z)103, 177 (1858).
2. A. EINSTEIN. Ann. Phys. 2Z9 180 (1907).
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results are better than indicated by the above

3. P. PICKER,P,-A. LEDCTG, P. R. PHILIP,arid J. E.
total uncertainties; we estimate that rntrrl uncer- DESNOYERS. 1. Chem. Therrnodyn. 3, 631 (1971).
tainties in differezces between any two of our 4. J.-L. FORTIER, P.-A. EEDUC,and J. E. D ~ N O Y E R S .
values are about 5 % 9 K-I moi-I. We there- J. Solution Chem. 3, 323 (1974).
fore estimate that the rota! uncertainty in oar 5. P~ PICKER. Can. Res. Dev. 1 1 (1974).
BCp0for ionization of water is i4 J K-"01-I. 6. 6. PERRON, J.-&. FORTIER,and J. E. DESNOYERS. J.
Chem. Thermodyn. 7, 1177 (1975).
Various previous investigations have led to 7. S. E. DESNOYERS, 6. DE VISSER,6. PERROW, and P.
ACP0 values for ionization of water at 298 K PICKER.J. Solution @hem. In press.
ranging from - 195 to -225 J K-I mol-4 as 8. P. PICKER,E. TREMBLAY, and C. JOLICOEUR. J. Solu-
recently reviewed and calculated (17, 18). Largely tion Chem. 3, 377 (1974).
9. A. I. VOFEL.A text-book of quantitative inorganic
on the basis of results from Parker (12), values at analysis. Longmans Canada, Ltd., Toronto. 1962.
the negative end of this range were selected 10. I. M. KOLTHOFF, E. B. SANDELE, E. J. MEEHAN, and
Can. J. Chem. 1976.54:3315-3318.

(17, 18) as the "'best" ones then available. We S. BRUCKEWSTEIN. Quantitative chemical analysis.
now suggest that these earlier values should be 4th ed. McMillan, New York. 1971.
replaced by our new BCP0= -215.2 9 K-I 11. P. J. CERUTTI.Ph.D. Thesis, University of South
Carolina, 1975.
mol-I (estimated i4 J K-I m ~ l - ~ ) ) . 12. V. B. PARKER. Thermal properties of aqueous uni-
univalent electrolytes. National Standard Reference
Data Series, National Bureau of Standards 2,
Acknow8edgments Washington, .D.C. 1965.
We thank the National Research Council of 13. C. M. CRISSand J. W. COBBLE. J. Am. Chern. Soc. 83,
3223 (1961).
Canada for support of this research and Brigham 14. J. C. AHLUWALIA and J. W. COBBLE.3. Am. Chem.
Young University for sabbatical leave support SOC.86, 5381 (1964).
to E.M.W. We also thank Professor 9. E. 15. G.PERRON, J. E. DESNOYERS, and F. J. MILLERO. Can.
Desnoyers for sending us a manuscript copy of 9. Chem. 53, 1134 (1975).
16. D. D. WAGMAN,W. PI. EVANS,V. B. PARKER,1.
his paper that is cited as ref. '7. HALOW,S. M. BAILEY, and R. H. SCHUMM. National
Bureau of Standards Technical Note 270-3. Washing-
NOTEADDED IN PROOF: ton, D.C. 1968.
G. Olofsson and I. Olofsson (University of 17. L.G. HEPLERand E. M. WOOLLEY. I n Water: a com-
Lund, Sweden) have recently informed us that prehensive treatise. VoP. 3. Edited by F. Franks.
Plenum Press, New York. 1973.
they have completed calorimetric measurements 18. G. OLOFSSON and L. G. HEPLER. J. Solution Chem, 4,
leading to the standard enthalgy of ionization of 127 (1975).
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