International Journal of Refrigeration 29 (2006) 566–578

www.elsevier.com/locate/ijrefrig

A computationally effective formulation of the thermodynamic

properties of LiBr–H2O solutions from 273 to 500 K over
full composition range
J. Pátek*, J. Klomfar
Institute of Thermomechanics, Academy of Sciences of the Czech Republic, Dolejškova 5, CZ 182 00 Prague 8, Czech Republic
Received 4 January 2005; received in revised form 22 September 2005; accepted 10 October 2005
Available online 4 January 2006

Abstract

A set of computationally efficient formulations of thermodynamic properties of LiBr–H2O solutions at vapor–liquid

equilibrium is presented in the form of explicit separate functions of temperature and mixture composition. The set includes
pressure, density, isobaric heat capacity, enthalpy, and entropy. The description of these properties is valid from 273 K or from
the crystallization line up to 500 K in temperatures and for mixture composition from 0 to 75 wt% of LiBr in the solution. The
equations are based upon a body of experimental data that have been critically assessed. Gaps in the database are shown to give
experimenters orientation for future research. The structure of the equations guarantees an explicit transition to the properties of
pure water for lithium bromide concentration approaching zero. The uncertainties associated with correlation are estimated to
be G0.5% for density, G2.1% for pressure and G2% for isobaric heat capacity. The uncertainty in values of enthalpy is
estimated to be G10 kJ kgK1 and G0.03 kJ kgK1 KK1 for entropy. Values of the particular properties generated by the
representative equations are provided to assist with the confirmation of computer implementation of the calculation procedure.
q 2005 Elsevier Ltd and IIR. All rights reserved.

Keywords: Absorption system; Water-Lithium bromide; Calculation; Thermodynamic properties; Aqueous solution

Formulation permettant le calcul des propriétés thermodynamiques

des solutions de LiBr-H2O pour une plage allant de 273 à 500 K
et une gamme complète de compositions
Mots clés : Système à absorption ; Eau-bromure de lithium ; Calcul ; Propriétés thermodynamiques ; Solution aqueuse

1. Introduction

The development in the field of refrigeration, cooling

* Corresponding author. Tel.: C420 266 053 163; fax: C420
2858 4695.
E-mail address: patek@it.cas.cz (J. Pátek).
0140-7007/$35.00 q 2005 Elsevier Ltd and IIR. All rights reserved.
doi:10.1016/j.ijrefrig.2005.10.007
and heat transforming systems based on absorption cycles
has attained its own internal dynamic in the last decade. The
most common combinations of working fluid/absorbent for
 J. Pátek, J. Klomfar / International Journal of Refrigeration 29 (2006) 566–578 567

Nomenclature
Symbols RMS root mean square relative deviation (%),
cp molar isobaric heat capacity (J molK1 KK1) RMSZ 100½ð1=NÞSðzexp =zcal K1Þ2
1=2
g molar Gibbs free energy (J molK1)
Subscripts
H enthalpy (J)
c at the critical point
H partial enthalpy of water in solution (J molK1)
cal calculated
h molar enthalpy (J molK1)
exp experimental
M molar mass (kg molK1)
g superheated vapor states of pure water
m mass (kg)
l subcooled liquid states of pure water
N number of points
LiBr lithium bromide
n amount of substance (mol)
p isobaric
p pressure (Pa)
s denotes a state on the vapor-pressure curve
DHvap molar enthalpy of evaporation (J molK1)
t at the triple point
DHdil molar enthalpy of dilution (J molK1)
w water
S entropy (J KK1)
S partial entropy of water in solution Physical constants and characteristic properties of H2O
(J KK1 molK1) and LiBr
s molar entropy (J molK1 KK1) Molar mass
T temperature (K) MLiBr 0.08685 kg molK1
T0 constant (K). Eqs. (3)–(5) MH2 O 0.018015268 kg molK1
V volume (m3) Critical point of pure water
V partial volume of water in solution (m3 molK1) Tc 647.096 K
v molar volume (m3 molK1) pc 22.064!106 Pa
w mass fraction (wZmLiBr/(mLiBrCmw)) 9c 17,873 mol mK3 (322 kg mK3)
x molar fraction (xZnLiBr/(nLiBrCnw)) Triple point of pure water
9 molar density (mol mK3) Tt 273.16 K
0
saturated liquid state pt 611.657 Pa
MR mean relative deviation (%), 9t0 55,496.8 mol mK3 (999.789 kg mK3)
MRZ ð100=NÞSðzexp =zcal K1Þ

absorption systems are water/lithium bromide and ammo-
nia/water. The design and optimization calculations of
absorption cycles require computationally efficient formu-
lation of the thermodynamic properties of the working pair.
In the case of the lithium bromide–water system these
computations are usually conducted in the temperature
region above 273 and up to 500 K and at composition from
40 to 70 weight percent of LiBr in the solution [1].
Although significant improvements are being made in
predicting thermodynamic properties of pure fluids and
mixtures using theory based methods, more accurate
equations of state for calculating properties over wide
range of pressures and temperatures are to be developed by
correlation of selected experimental data. For the develop-
ment of such empirical formulations, the application of
linear optimization procedures and nonlinear multiproperty
fitting algorithm is state-of-art [9].
Modern equations of state are usually explicit in the
Helmholtz energy as a function of density and temperature
[9]. No formulation of the thermodynamic properties of the
LiBr–H2O system have been published in the form of
Helmholtz free energy similar to that of ammonia–water
system by Tillner–Roth and Friend [10]. Herold and
Moran [3] developed a description of the LiBr–H2O
solutions in terms of the Gibbs free energy. But all the
dependence of their Gibbs free energy on its variables in
states outside the vapor–liquid coexistence region is derived
solely from theory. All the available data on thermodynamic
properties of the LiBr–H2O system relate to states of vapor–
liquid equilibrium, no data for compressed liquid are
available. The gas phase of the system include practically
only pure steam; the vapour pressure of the LiBr is
negligible to the vapour pressure of H2O and the gaseous
mixture can be considered as pure steam.
In the studies published by various authors, the
formulation of McNeely [2] valid from 15 to 166 8C is
used most often. Other formulations [3–8] are used much
less frequently in cycle calculations, though some of them
were developed with intention to extend the region of
validity of the property description [4,5,7,8]. The formu-
lation by Herold and Moran [3] is the only one consistent
thermodynamically due to its form. All the others have the
form of a set of separate equations for pressure, density,
isobaric thermal capacity, enthalpy, and entropy of the
system at vapor–liquid equilibrium and, therefore, are
consistent only in the numerical sense.
568 J. Pátek, J. Klomfar / International Journal of Refrigeration 29 (2006) 566–578

The objective of the present study was to provide hðT; xÞ Z ð1KxÞh 0 ðTÞ
formulation of the thermodynamic properties of LiBr–H2O
X
30
ti
solutions in vapor–liquid equilibrium states valid over a Tc
broader range of parameters, from 273 K or from the C hc mi
ai x ð0:4KxÞ ni
; (4)
iZ1
T KT0
crystallization temperature (whichever is greater) up to
500 K in temperatures and over the full range of
compositions. The formulation should be based on all sðT; xÞ Z ð1KxÞs 0 ðTÞ
available experimental data, and it should approximate the
ti
correlated data within their experimental uncertainties. The X
29
Tc
C sc ai xmi ð0:4KxÞni ; (5)
formulation has the form of a set of explicit separate iZ1
T KT0
functions of temperature and composition.
In the present study, the partial enthalpy, partial entropy where T0Z221 K is a nonlinear parameter of the equations.
and partial volume of the water in the gas phase are In Eq. (1), the pressure p(T,x) is expressed in terms of the
approximated by the steam molar enthalpy hg(T,p), steam pure water saturation pressure ps(T) at shifted temperature
molar entropy sg(T,p) and steam molar volume vg(T,p). The q. As there exist direct casual connection between
required thermodynamic properties of pure steam, i.e. its thermodynamic properties of the system and the number
molar volume enthalpy, and entropy as well as their values density of its particles, it is natural from the physical point of
for saturated liquid water v 0 (T), h 0 (T), and s 0 (T) were view to use molar fraction x of the LiBr in solution (xZ
computed from the internationally agreed IAPWS formu- nLiBr/(nLiBrCnw)) and molar quantities for the description of
lation 1995 [11]. thermodynamic properties of the mixture. In comparison
with the description using LiBr mass fraction w, this choice
results in lower number of terms of the approximation
polynomial required to achieve given accuracy in given
2. Methodology region of validity of the property description. Specific
quantities and mass fraction w used in common compu-
tational practice are related to the molar quantities by the
2.1. Property equations and their fitting to data following relations:

In the present study, a separate approximating function is xMLiBr

wZ ; (6)
chosen for each quantity in a form that guarantees an xMLiBr C ð1KxÞMw
explicit transition to the property values of pure water for
lithium bromide concentration approaching zero. An w=MLiBr
analogical description of the limit of pure LiBr cannot be xZ ; (7)
w=MLiBr C ð1KwÞ=Mw
introduced here as at temperatures of interest the pure
lithium bromide does not exist in the liquid form. The
hðwÞ 1 hðxÞ
properties of saturated pure liquid water as a function of Z ; (8)
temperature are denoted by apostrophe (r 0 (T), cp0 ðTÞ, h 0 (T), J kgK1 xMLiBr C ð1KxÞMw J molK1
s 0 (T)) in Eqs. (1)–(5) whereas quantities describing the and similarly for density, entropy and isobaric heat capacity.
solution have no subscript (p(T,x), h(T,x) etc.). If a certain functional form fðT; x; aÞ
 has been selected
The resulting functions best reproducing the selected for a given property, experimental data on the property and
experimental data show the following form: experimental data for other properties related through
thermodynamic relations to it or its derivatives can be
X 8
ti
mi ni T
used to determine the unknown coefficients ai (expressed as
pðT; xÞ Z ps ðqÞ; q ZTK ai x ð0:4KxÞ (1) the vector a) by minimizing the following sum of squares:
iZ1
Tc
X
J Mj h
X i2
c2 Z fj zðjÞ ðjÞ
exp;i Kzcal ðTexp;i ; xexp;i ; aÞ
 ; (9)
X
2
ti jZ1 iZ1
T
9ðT; xÞ Z ð1KxÞ9 0 ðTÞ C 9c ai xmi ; (2)
iZ1
Tc where Mj is the number of data points used for the jth
property, zðjÞ
exp;i is the ith experimental value for the property
ðjÞ
and zcal;i is the value for the property calculated from the
equation for f with the parameter vector a at Texp,i and xexp,i.
cp ðT; xÞ Z ð1KxÞcp0 ðTÞ
The weighting factors fj are introduced to equalize the effect
X
8
ti of various properties on the regression matrix. The optimum
Tc
C cp;t ai xmi ð0:4KxÞni ; (3) set of regressors for the approximation function was selected
iZ1
T KT0 using a step regression method [12].
 J. Pátek, J. Klomfar / International Journal of Refrigeration 29 (2006) 566–578 569

2.2. Vapor pressure Eq. (14) are functions of the vapor–liquid equilibrium
pressure p(T,x) and temperature T. Therefore, the enthalpy
The functional form (1) to approximate the p(T,x) of dilution can be taken into account only in a sequence of
relation takes advantage of the empirical Dühring’s rule iteration steps.
according to which the boiling point T(p,x) of a strong water The partial volume of water in the solution V is given by
solution at constant composition is close to a linear function the molar density 9(T,x) of the solution:
of the boiling point of water Ts(p) at the same pressure. The  
1 x v9ðT; xÞ
corresponding inverse function is also linear: 
VZ 1C : (15)
9ðT; xÞ 9ðT; xÞ vx
Ts ðpÞ Z CðxÞTðp; xÞ C DðxÞ; (10)
and therefore, 2.3. Enthalpy
pðT; xÞ Z ps ½CðxÞT C DðxÞ
: (11)
Values of enthalpy H(T, p, nLiBr, nw) of the system
The functional form (1), not containing higher order consisting of nLiBr moles LiBr and nw moles of water are
terms in temperature, proved to be the only one satisfactory defined by differential
for approximation of the pressure derivatives with respect to


vH vH
temperature and composition required in mixture enthalpy dH Z dT C dp
vT p;nw vp T;nw
and entropy calculations. For temperatures q below the
triple point, the pressure of the saturated steam above

vH
subcooled liquid water was used, calculated from the C dn (16)
vnw T;p w
IAPWS 95 formulation.
To correlate the p(T,x) relation of the LiBr–H2O and by its reference value chosen by convention in an
solution, besides the data on the pressure, the experimental arbitrary reference state. The molar enthalpy h(T,x) of the
data on enthalpy of dilution of Lange and Schwartz [13] and liquid phase on the vapor–liquid equilibrium surface as a
Hasaba et al. [14] were used. The enthalpy of dilution is function of the LiBr molar fraction x is defined as:
defined as the change in enthalpy of the water after being 1
added to the solution: hðT; xÞ Z H½T; pðT; xÞ; nLiBr ; nw
: (17)
nLiBr C nw
DHdil Z H Khl : (12) Based on Eqs. (16) and (17) and standard thermodynamic
The partial enthalpy of water in mixture liquid phase H relations the temperature dependence of the molar enthalpy
can be calculated from Clausius–Clapeyron-like equation h(T,x) is given by the equation


which follows from the condition of phase equilibrium (i.e. vhðT; xÞ vh vpðT; xÞ
equality of chemical potentials of water in coexisting Z cp ðT; xÞ C ; (18)
vT vp T;x vT
phases):
where
 vpðT; xÞ :
H Z hg KTðvg KVÞ (13)

vT vh vvðT; xÞ
Z vðT; xÞKT : (19)
vp T;x vT
From Eqs. (12) and (13) temperature derivative of pressure
can be expressed as or, when expressed in terms of the molar density 9(T,x):


  
vp hg Khl KDHdil;exp vh 1 T v9ðT; xÞ
Z  : (14) Z 1C : (20)
vT x Tðvg KVÞ vp T;x 9ðT; xÞ 9ðT; xÞ vT
The temperature and pressure dependence of a quantity By derivating Eq. (17) with respect to nw a differential
related to the superheated liquid or superheated vapor states equation is obtained, after some manipulations, describing
of pure water are denoted by subscript l (h1, v1) or by the dependence of the enthalpy h(T,x) on the mixture
subscript g (hg, vg), respectively, in the present study. Partial composition x:
 H and S relates to the water in the solution.
quantities V;

vhðT; xÞ vh vpðT; xÞ
Thus, in the p-T-x relation fitting, the pressure itself hðT; xÞKx Z H Kx (21)
vx vp T;x vx
represents the property z(1) and the left hand side of Eq. (14)
represents the calculated values zð2Þ
cal of the property z
(2)
while To calculate values of the molar enthalpy h(T,x), the values
the right hand side represents the experimental values zð2Þ exp of of the right hand side of Eqs. (18) and (21) should be
the property. expressed from the experimental data. In particular, the
To calculate values of derivative (vp/vT)x from the partial molar enthalpy of water in the solution H is given by
values of enthalpy of dilution in dependence on temperature the Clausius–Clapeyron Eq. (13). An additional independent
T and composition x, some preliminary approximation of the information concerning H is provided by the enthalpy of
p(T,x) relation should be used as the pure water properties in dilution data through the relation (12).
570 J. Pátek, J. Klomfar / International Journal of Refrigeration 29 (2006) 566–578

Table 1
Sources of data on p-T-x relation of LiBr–H2O solutions at vapor–liquid equilibrium

Author(s) Year Experimental Range of values No. of data Deviation (%)

method points
Temperature Pressure (kPa) Mass fraction All Used RMS MR
(K) (wt%)
Tamman [15] 1885 Static still 298–373 1.7–102 4–58 115 87 1.33 0.23
Lannung [16] 1934 Static still 291 0.07–2.0 0.7–15 30 0 3.76 1.6
Pennington [17] 1955 Static still 405–427 98.8–100.1 50–60 10 10 1.01 0.00
Ebulliometry 353–417 13.5–72.1 50–60 25 25 1.80 0.33
Gas transport 303 0.3–1.1 50–61 11 11 1.73 K1.73
Löwer [18] 1960 Static still 273–403 0.08–265 0–70 185 178 1.98 K0.45
Boryta et al. [19] 1975 Static still 273–348 0.2–21 40–60 15 0 7.02 K5.44
Gas transport 298–448 0.2–84 40–70 17 0 6.40 K1.86
Sada et al. [20] 1975 Static still 348 11–38 35–46 6 0 18.23 9.67
Fedorov et al. [21] 1976 Static still 423–623 110–15,000 8–56 35 11 1.58 K1.12
Felli and Mattiucci 1979 Static still 298–366 0.2–26 40–50 8 0 7.80 K3.63
[22]
Matsuda et al. [23] 1980 Static still 273–345 0.05–7 44–58 119 119 2.91 K0.59
Renz [24] 1980 Static still 273–448 1.2–95 25–70 96 95 1.83 0.72
Iyoki and Uemura [25] 1989 Boilling-point 362–452 10–281 39–70 39 39 3.57 K0.36
Patil et al. [26] 1990 Differencial 303–343 0.4–29 15–58 40 0 4.76 1.91
static
Lenard et al. [27] 1992 Static still 398–483 112–785 44–65 24 24 1.31 0.41
Feuerecker et al. [5] 1993 Gas transport 318–462 4.5–180 40–75 78 78 1.79 1.32
Murakami et al. [28] 1993 Bubble-point 310–413 0.5–316 20–60 44 0 6.44 3.09

Thus the right hand side of Eq. (18) represents the calculated from pressure (Eq. (13)) or from the enthalpy of
experimental values zð1Þ (1)
exp of the property z , the right hand dilution (Eq. (12)). The left hand sides of Eqs. (18) and (21)
ðjÞ
side of Eq. (21) the experimental values of the property represent the calculated values zcalc of the respective
zð2Þ ð3Þ
exp or zexp in dependence whether the partial enthalpy is properties.
Table 2
Sources of data on 9-T-x relation of LiBr–H2O solutions at vapor–liquid equilibrium

Author(s) Year Experimental Range of values No. of data Deviation (%)

method points
Temperature Density Mass fraction All Used RMS MR
(K) (kg mK3) (wt%)
Kremers [29] 1858 Pycnometer 292 1117–1542 15–60 10 0 1.64 1.41
Röntgen and Schneider [30] 1886 Piezometer 291 1042–1089 6–12 2 2 0.11 K0.11
Heydweiller [31] 1909 – 291 1003–1243 0.4–26 7 7 0.86 K0.58
Baxter et al. [32] 1911 Pycnometer 298 998–1289 0.2–30 18 18 0.66 K0.28
Grufki [33] 1913 – 291 1028–1241 4–26 4 4 1.03 K0.75
Lübben [34] 1913 – 291 1030–1241 4–26 4 4 1.04 K0.77
Gropp [35] 1915 – 273–391 1423–1480 41 6 0 4.90 4.90
Baxter and Wallace [36] 1913 Pycnometer 273–343 998–1798 3–64 23 22 0.26 K0.13
De Block [37] 1925 – 289 1207–1700 25–62 3 0 1.22 1.10
Scott et al. [38] 1934 Pycnometer 308 1058–1721 8–60 11 11 0.28 K0.10
Scott and Bridger [39] 1935 Pycnometer 308 1139–1450 18–45 4 4 0.08 0.04
Löwer [18] 1960 Pycnometer 273–373 958–1900 0–70 152 137 0.50 0.17
Hasaba et al. [14] 1961 Pycnometer 273–353 1061–1705 10–59 28 27 0.56 K0.41
Bogatykh and Evnovitch 1965 Pycnometer 283–373 1288–1760 35–62 111 109 0.42 K0.15
[40]
Mashovets et al. [41] 1971 Pycnometer 213–273 1038–1556 5–50 23 6 0.63 K0.57
Lee et al. [42] 1990 Pycnometer 301–473 1378–1721 45–60 39 39 0.57 K0.25
Wimby and Berntsson [43] 1994 Vibrating tube 298–343 1100–1750 30–61 48 47 0.39 K0.14
Murakami [44] 2002 Vibrating tube 284–422 1003–1810 10–65 113 110 0.51 K0.09
 J. Pátek, J. Klomfar / International Journal of Refrigeration 29 (2006) 566–578 571

Table 3
Sources of data on cp-T-x relation of LiBr–H2O solutions at vapor–liquid equilibrium

Author(s) Year Experimental Range of values No. of data points Deviation (%)
method
Temperature (K) Mass fraction All Used RMS MR
(wt%)
Jauch [45] 1921 – 291 3–28 5 5 1.01 K0.68
Lange and Schwartz 1928 – 299 0–60 39 39 1.01 K0.66
[13]
Löwer [18] 1960 – 273–403 0–60 168 140 1.89 K0.27
Hasaba et al. [47] 1960 – 298–403 10–66 33 0 4.98 3.18
Iyoki and Uemura [46] 1989 Twin isothermal 335–424 44–65 64 41 2.55 K0.77
calorimeter
Jeter et al. [48] 1992 Drop calorimeter 335–424 44–65 64 0 5.34 K0.81

The molar enthalpy h(T,x) of the solution is determined  vpðT; xÞ ;

by the relations (21) and (18) up to an arbitrary linear
function of the mixture composition x. In common practice,
the term linear in composition x is usually selected so that
the enthalpy takes its zero value for the solution with
composition of 50 wt% of LiBr at temperature 273.15 K,
while the absolute term is given by the reference state of
pure water (Section 5).
To calculate partial derivatives of the enthalpy with
respect to temperature and composition, the density 9(T,x)
of the solution, pressure p(T,x), pure steam molar enthalpy
hg(T,p) and molar volume vg(T,p) in dependence on pressure
and temperature and the molar isobaric thermal capacity of
the solution cp(T,x) hould be known. Instead of experimental
data on isobaric heat capacity a set of values was used
calculated from the approximation (3) on a grid of points
covering the temperature-pressure region of interest.
It should be noticed, that the second term of the right side
of Eq. (18) represents, when compared to isobaric heat
capacity cp, a small correction not exceeding within the
region of interest several tenths of percent of the value of cp.
Similarly the value of the partial volume V of water in the
mixture liquid phase in the relation (13) does not exceed 2%
of the gas phase molar volume of water vg(T,p).
2.4. Entropy
Entropy s(T,x) of the LiBr–H2O solutions, in analogy to
the enthalpy, is determined up to an additive linear function
of composition by its derivatives:



vsðT; xÞ cp ðT; xÞ vs vp
Z C ; (22)
vT T vp T;x vT x



vs vs vpðT; xÞ
sðT; xÞKx 
Z SKx ; (23)
vx vp T;x vx
where for the partial entropy S of water in the solution
follows from the Clausius–Clapeyron equation
S Z sg Kðvg KVÞ (24)
vT
where


vs vvðT; xÞ
ZK ; (25)
vp T;x vT
and therefore,


vs 1 v9ðT; xÞ
Z : (26)
vp T;x 9ðT; xÞ2 vT
An additional independent information concerning the
partial entropy is contained in the experimental data on the
enthalpy of dilution:
DH g Kgv
S Z sl K dil C l : (27)
T T
The arbitrary additive linear function of composition is
chosen so that the entropy equals to zero for the mixture
composition wZ0.5 at temperature 273.15 K, while for
xZ0 is consistent with the reference state of pure water.
3. Data selection
Not all the original works provide sufficient comparable
evidence on which to base a judgement of the relative merits
of the various sets of results. To assess the quality of the
particular sets of experimental data, all the data for each
property (i.e. p-T-x, 9-T-x, and cp-T-x relation) were
preliminary fitted simultaneously with weights equal to the
reciprocal of the number of points in each set. In this way, the
effect of different number of data points contained in
particular data sets was canceled. Mean relative (systematic)
deviation of each particular data set provide an idea of how
the set is shifted as a whole with respect to the common
average values given by the resultant function. In this way the
experimental data were divided into two categories: primary
data employed in the development of the correlation and
secondary data with excessive systematic deviation and/or
excessively scattered, which were used only for comparison
572 J. Pátek, J. Klomfar / International Journal of Refrigeration 29 (2006) 566–578

Table 4 Table 6
Coefficients and exponents of Eq. (1) Coefficients and exponents of Eq. (3)

i mi ni ti ai i mi ni ti ai
2
1 3 0 0 K2.41303!10 1 2 0 0 K1.42094!101
2 4 5 0 1.91750!107 2 3 0 0 4.04943!101
3 4 6 0 K1.75521!108 3 3 1 0 1.11135!102
4 8 3 0 3.25430!107 4 3 2 0 2.29980!102
5 1 0 1 3.92571!102 5 3 3 0 1.34526!103
6 1 2 1 K2.12626!103 6 2 0 2 K1.41010!10K2
7 4 6 1 1.85127!108 7 1 3 3 1.24977!10K2
8 6 0 1 1.91216!103 8 1 2 4 K6.83209!10K4

TcZ647.096 K; RMSZ2.1%. cp,tZ76.0226 J molK1 KK1; TcZ647.096 K; T0Z221 K; RMSZ

0.98%.
purposes. The sources of the assessed sets of experimental
data together with their relative root mean square (RMS) properties generated by the resultant representative equations
deviation and mean relative (MR) deviation are listed in are provided in Table 9 to assist with the confirmation of
Tables 1–3. The experimental method and the temperature, computer implementation of the calculation procedure.
pressure and composition ranges covered by each data set are In Figs. 1, 3, and 5 the deviations of the data used in the
also indicated here. The number of points used for fitting is fitting procedure from the corresponding resultant represen-
given in the table for the primary data while for the secondary tative equation are depicted, while in the Figs. 2, 4, and 6
data it is equaled to zero. The results obtained for cp of the deviations for the rejected data are plotted. In Fig. 7 the
LiBr–H2O solutions by Feurecker et al. [5] were published resultant Eq. (1) for pressure is compared with the
only it the form of an approximation polynomial. As there is a
lack of experimental data on cp at high solution concen- Table 7
trations, a set of data generated from the Feurecker’s equation Coefficients and exponents of Eq. (4)
was used in this region for fitting purposes.
i mi ni ti ai
Within the present study, 30 experimental works have
been collected containing a total of 1904 data points on 1 1 0 0 2.27431!100
various thermodynamic properties of the LiBr–H2O sol- 2 1 1 0 K7.99511!100
utions. A body of 1449 of them were selected as the primary 3 2 6 0 3.85239!102
4 3 6 0 K1.63940!104
data used for fitting of the representative equations. For
5 6 2 0 K4.22562!102
comparison, let us mention that in the time when Tillner– 6 1 0 1 1.13314!10K1
Roth and Friend were developing their formulation of the 7 3 0 1 K8.33474!100
thermodynamic properties of ammonia–water mixtures [10] 8 5 4 1 K1.73833!104
they had at their disposal 61 experimental studies 9 4 0 2 6.49763!100
concerning various thermodynamic properties of the system 10 5 4 2 3.24552!103
both in two phase and single phase region and involving in 11 5 5 2 K1.34643!104
total 5559 data points. 12 6 5 2 3.99322!104
13 6 6 2 K2.58877!105
14 1 0 3 K1.93046!10K3
15 2 3 3 2.80616!100
4. Results
16 2 5 3 K4.04479!101
17 2 7 3 1.45342!102
The respective coefficients ai and exponents mi, ni and ti of 18 5 0 3 K2.74873!100
Eqs. (1)–(5) are given in Tables 4–8. The number of 19 6 3 3 K4.49743!102
significant figures given in the coefficients ai is necessary 20 7 1 3 K1.21794!101
and sufficient to obtain the stated accuracy. In the tables are 21 1 0 4 K5.83739!10K3
also given relative root mean square deviations for the total 22 1 4 4 2.33910!10K1
data set used for correlation. Values of the particular 23 2 2 4 3.41888!10K1
24 2 6 4 8.85259!100
Table 5 25 2 7 4 K1.78731!101
Coefficients and exponents of Eq. (2) 26 3 0 4 7.35179!10K2
27 1 0 5 K1.79430!10K4
i mi ti ai 28 1 1 5 1.84261!10K3
1 1 0 1.746 29 1 2 5 K6.24282!10K3
2 1 6 4.709 30 1 3 5 6.84765!10K3

TcZ647.096 K; rcZ17,873 mol mK3; RMSZ0.44%. hcZ37,548.5 J molK1; TcZ647.096 K; T0Z221 K.

 J. Pátek, J. Klomfar / International Journal of Refrigeration 29 (2006) 566–578 573

Table 8
Coefficients and exponents of Eq. (5)

i mi ni ti ai
1 1 0 0 1.53091!100
2 1 1 0 K4.52564!100
3 2 6 0 6.98302!102
4 3 6 0 K2.16664!104
5 6 2 0 K1.47533!103
6 1 0 1 8.47012!10K2
7 3 0 1 K6.59523!100
8 5 4 1 K2.95331!104
9 1 0 2 9.56314!10K3
10 2 0 2 K1.88679!10K1
11 2 4 2 9.31752!100
12 4 0 2 5.78104!100
13 5 4 2 1.38931!104
14 5 5 2 K1.71762!104
15 6 2 2 4.15108!102
16 6 5 2 K5.55647!104
17 1 0 3 K4.23409!10K3
18 3 4 3 3.05242!101
19 5 0 3 K1.67620!100
20 7 1 3 1.48283!101
21 1 0 4 3.03055!10K3
22 1 2 4 K4.01810!10K2
23 1 4 4 1.49252!10K1
24 2 7 4 2.59240!100
25 3 1 4 K1.77421!10K1
26 1 0 5 K6.99650!10K5 Fig. 1. Percentage deviations between the primary experimental
27 1 1 5 6.05007!10K4 data of the pressure p of vapor–liquid equilibrium and values
28 1 2 5 K1.65228!10K3 calculated from Eq. (1). (7) Tamman [15], (3) Pennington [17],
29 1 3 5 1.22966!10K3 (B) Löwer [18], (") Fedorov et al. [21], (,) Matsuda et al. [23],
(*) Renz [24], (C) Iyoki and Uemura [25], (6) Lenard et al. [27],
scZ79.3933 J molK1 KK1; TcZ647.096 K; T0Z221 K. (>) Feuerecker et al. [5].

experimental data obtained by Fedorov et al. [21] at higher
temperatures which were not used for fitting. In this way, it is
demonstrated, that the equation for pressure can be used for
extrapolation in temperature with defined uncertainty up to
623 K.
In Figs. 8 and 9 the deviations are shown of the
experimental values of isobaric heat capacity from values
calculated from the representative functions for enthalpy (4)
and entropy (5) using Eqs. (18) and (22). The isobaric heat
capacity computed from enthalpy reproduces the experi-
mental values of cp used in fitting of the equation for cp (3)
with relative root mean square deviation of 1.3%. The
similar deviation for entropy is equal to 1.2%. Langeliers
et al. [49] published a correlation of their unpublished
experimental data on cp of LiBr–H2O solutions valid from
about 423 to 523 K in temperatures and from 54 to 66 wt%
in composition. The deviations of the cp values computed
from the enthalpy (4) from the correlation [49] do not
exceed 2% for temperatures up to 480 K and 3% up to
500 K. The values of the pressure derivative with respect to
composition derived from the resultant molar enthalpy (4)
according Eqs. (13) and (21) reproduce the temperature
derivatives of the p(T,x) equation used for the enthalpy
calculation with relative deviation not exceeding 0.8%.
The maximum differences of enthalpy and entropy
calculated from the Eqs. (4) and (5) from the values

Table 9
Property values calculated from Eqs. (1)–(5) for validation of computer programs

x T (K) p (Pa) 9 (mol mK3) cp (J molK1 KK1) h (J molK1) s (J molK1 KK1)

0.05 300 3025.1805 54,148.9 69.931 1603.9 7.79057
0.05 450 835,097.47 48,984.9 74.047 12,189.0 36.5288
0.1 300 2286.4858 52,985.4 65.520 1445.1 7.66416
0.1 450 647,702.12 48,550.2 70.305 11,555.2 34.9553
0.3 350 2237.3986 47,826.4 66.597 9072.1 15.3214
0.4 450 43,075.149 45,941.8 70.294 21,024.4 33.3788
574 J. Pátek, J. Klomfar / International Journal of Refrigeration 29 (2006) 566–578

Fig. 2. Percentage deviations between the rejected experimental Fig. 3. Percentage deviations between the primary experimental
data of the pressure p of vapor–liquid equilibrium and values data of the density r of LiBr–H2O solutions and values calculated
calculated from Eq. (1). (,) Lannung [16], (6) Boryta et al. [19], from Eq. (2). (*) Röntgen and Schneider [30], (1) Heydweiller
(B) Sada et al. [20], (C) Felli and Mattiucci [22], (*) Patil et al. [31], (5) Baxter et al. [32], (7) Grufki [33], (3) Lübben [34], (4)
[26], (>) Murakami et al. [28]. Baxter and Wallace [36], (:) Scott et al. [38], (;) Scott and
Bridger [39], (B) Löwer [18], (,) Hasaba et al. [14], (!)
calculated from the property formulations of the other Bogatykh and Evnovitch [40], (") Mashovets et al. [41], (>) Lee
authors within their range of validity are listed in Table 10. et al. [42], (6) Wimby and Berntsson [43], (C) Murakami [44].
Based on these comparisons the uncertainties associated
Table 11
with correlation are estimated to be G10 kJ kgK1 for
Coefficients and exponents of Eq. (28)
enthalpy and G0.03 kJ kgK1 KK1 for the entropy.
i bi ai
1 1.0 K7.85951783
5. Description of thermodynamic properties of the pure 2 1.5 1.84408259
water substance at saturation 3 3.0 K11.7866497
4 3.5 22.6807411
5 4.0 K15.9618719
In the Eqs. (1) and (2) the IAPWS 95 [11] equations for
6 7.5 1.80122502
vapor pressure and liquid density of pure water at saturation
TcZ647.096; rcZ22.064!106 Pa.
Table 10
Maximum differences of values of enthalpy and entropy calculated Table 12
from Eqs. (4) and (5), respectively, from values calculated Coefficients and exponents of Eq. (29)
according to formulations of other authors
i bi ai
Author (Dh)max (kJ kgK1) (Ds)max
(kJ kgK1 KK1) 1 1/3 1.99274064
2 2/3 1.09965342
McNeely [2] 14 – 3 5/3 K0.510839303
Herold and Moran [3] 16 – 4 16/3 K1.75493479
Feurecker et al. [5] 4 0.016 5 43/3 K45.5170352
Chua et al. [8] 10 0.030 6 110/3 K6.7469445!105
Kaita [7] 8 0.012
rcZ17,873 mol mK3.
 J. Pátek, J. Klomfar / International Journal of Refrigeration 29 (2006) 566–578 575

Fig. 4. Percentage deviations between the rejected experimental data Fig. 5. Percentage differences between the experimental data of the
of the density r of LiBr–H2O solutions and values calculated from isobaric heat capacity cp of LiBr–H2O solutions and the values
Eq. (2). (,) Kremers [29], (6) Gropp [35], (B) de Block [37]. calculated from Eq. (3). (B) Jauch [45], (!) Lange and Schwartz
[13], (7) Löwer [18], (*) Iyoki and Uemura [46], (6) Feuerecker
et al. [5].
are used:
"
 #
Tc X
6
T bi "
 #
ps ðTÞ Z pc exp a 1K ; (28) X4
T bi
T iZ1 i Tc 0
h ðTÞ Z hc 1 C ai 1K ; (31)
iZ1
Tc
"
 #
0
X
6
T bi
9 ðTÞ Z 9c 1 C ai 1K : (29)
iZ1
Tc
Table 14
Equations for isobaric heat capacity, enthalpy, and entropy of Coefficients and exponents of Eq. (31)
pure water at saturation were newly developed in the present i bi ai
study based on data calculated from the IAPWS 95
1 1/3 K4.37196!10K1
formulation: 2 2/3 3.03440!10K1
X5

 3 5/6
T bi T gi
K1.29582
cp0 ðTÞ Z cp;t ai 1K ; (30) 4 21/6 K1.76410!10K1
iZ1
Tc Tt
TcZ647.096 K; hcZ37,548.5 J molK1.
Table 13
Coefficients and exponents of Eq. (30) Table 15
Coefficients and exponents of Eq. (32)
i bi gi ai
1 0 0 1.38801 i bi ai
2 2 2 K2.95318 1 1/3 K3.34112!10K1
3 3 3 3.18721 2 1 K8.47987!10K1
4 6 5 K0.645473 3 8/3 K9.11980!10K1
5 34 0 9.18946!105 4 8 K1.64046

cp,tZ76.0226 J molK1 KK1; TcZ647.096 K; TtZ273.16 K. TcZ647.096 K; scZ79.3933 J molK1 KK1.

576 J. Pátek, J. Klomfar / International Journal of Refrigeration 29 (2006) 566–578
Fig. 6. Percentage differences between the rejected experimental
data of the isobaric heat capacity cp of LiBr–H2O solutions and the
values calculated from Eq. (3). (B) Hasaba et al. [47], (,) Jeter
et al. [48].
"
 #
0
X4
T bi
s ðTÞ Z sc 1 C ai 1K : (32)
iZ1
Tc
The functional forms by Pátek et al. [50] were used for
enthalpy and entropy. The exponents bi, gi and coefficients ai
of Eqs. (28)–(32) are given in Tables 11–15. The
approximation Eqs. (30)–(32) are valid at temperatures
from 273.16 to 500 K. They give property values with
deviation from the IAPWS 95 values less then 0.08% for cp,
Fig. 7. Percentage differences between the experimental data by
Fedorov et al. [21] at temperatures above 500 K and the values
calculated from Eq. (1). (B) 523 K, (,) 573 K, (6) 623 K.
Fig. 8. Percentage differences between the experimental data on
isobaric heat capacity and the values of cp calculated from Eq. (4)
according to the relation (18). (B) Jauch [45], (!) Lange and
Schwartz [13], (7) Löwer [18], (*) Iyoki and Uemura [46], (6)
Feuerecker et al. [5].
0.33 kJ kgK1 for enthalpy, and 0.001 kJ kgK1 KK1 for
entropy.
It should be mentioned that since the 5th International
Conference on the Properties of Steam in London in 1956,
the specific internal energy and specific entropy of the
saturated liquid at the triple point have been arbitrarily set
equal to zero. This yields for the specific enthalpy of the
saturated liquid at the triple point the value of
0.611872 J kgK1 ([11], p. 429).
6. Conclusion
A set of separate empirical equations describing
pressure, molar density, isobaric heat capacity, enthalpy,
and entropy for LiBr–H2O solutions has been developed
based upon a body of critically assessed experimental data.
A method based on linear optimization procedure and
multiproperty fitting was used to this purpose. Temperatures
at which the published experimental data on isobaric heat
capacity are available do not exceed 430 K. Similarly
experimental data on p-T-x relation at temperatures below
483 K were used for fitting of the p(T,x) equation used then
also for enthalpy and entropy calculations. It is estimated
 J. Pátek, J. Klomfar / International Journal of Refrigeration 29 (2006) 566–578
Fig. 9. Percentage differences between the experimental data on
isobaric heat capacity and the values of cp calculated from Eq. (5)
according to the relation (22). (B) Jauch [45], (!) Lange and
Schwartz [13], (7) Löwer [18], (*) Iyoki and Uemura [46], (6)
Feuerecker et al. [5].
that extrapolation of the equations in temperature up to
500 K without substantial loss of accuracy is justified by
their structure which guarantees an explicit transition to the
property values of pure water for lithium bromide
concentration approaching zero. In the case of the p(T,x)
equation, the validity of extrapolation was demonstrated by
comparison with experimental data at temperatures up to
623 K. The equations obtained for enthalpy and entropy are
consistent with the results of Feurecker et al. [5], Chua et al.
[8], Kaita [7] and Langeliers et al. [49] in their regions of
validity. The code in ANSI C implementing Eqs. (1)–(5) is
available from the authors on request.
Comparisons of available measurements on the thermo-
dynamic properties of the LiBr–H2O solutions have shown
that the amount of available experimental data is far less
valuable to establish a description of the thermodynamic
properties of the system than it might appear at a first glance.
Many of the available sets of VLE data are only of limited
value, because they show large scatter or systematic
deviations when compared to other data. The largest gap
in the data is clearly found at temperatures above 400 K
and at compositions above 60 wt% of LiBr in the solution.
No single phase data are available in the compressed
liquid region.
577
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