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Empirical Fundamental Equation of State for Phosgene Based on Molecular

Simulation Data

Article  in  Journal of Chemical & Engineering Data · September 2015

DOI: 10.1021/acs.jced.5b00266

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Empirical fundamental equation of state for
phosgene based on molecular simulation data

Gábor Rutkai and Jadran Vrabec∗

Lehrstuhl für Thermodynamik und Energietechnik, Universität Paderborn, 33098

Paderborn, Germany

E-mail: jadran.vrabec@upb.de

Phone: +49-5251/60-2421

Abstract

It is reported on an automatized empirical fundamental equation of state fitting

approach that is based on molecular simulation data. In total 400 state points are

sampled in the homogeneous fluid region for temperatures between 150 K and 700 K

up to a pressure of 550 MPa and a density of 17.6 mol·dm−3 . At each state point

six thermodynamic properties are calculated. These properties are different partial

derivatives of the Helmholtz energy divided by the temperature with respect to inverse

temperature and density. The present equation of state itself is also explicit in terms

of this thermodynamic potential, and it therefore allows for the calculation of all static

thermodynamic properties, including vapor-liquid equilibrium data, by differentiation

only. Phosgene is chosen as a candidate because of its industrial importance and the

poor availability of corresponding laboratory measurement data in the literature due

to its hazardous nature.

1
Introduction

There is a dire need for thermodynamic data in process engineering that cannot be satisfied
by experimental measurements alone. Even though the available experimental database is
in general increasing, it is obvious that traditional laboratory measurements are unable to
keep up with the demand of industry. An empirical equation of state (EOS) correlation is
an explicit relation between state variables and it can provide information for poorly inves-

tigated state points and properties by means of inter- and extrapolation schemes. The other
advantage of an EOS is that it can summarize and represent tabulated data; even up to a
level of accuracy where it can actually be used to calibrate experimental equipment. Such
EOS are often referred to as reference quality EOS. 1 The construction of a reference quality

EOS requires a large amount of experimental data, months or years of careful filtering of
these data, and complex non-linear fitting. Consequently, there are less than ten substances
privileged to have their own reference quality EOS correlations, such as water, 2 carbon diox-
ide, 3 or nitrogen. 4 For about 100 experimentally less studied substances, there are EOS

correlations available that cover a considerably narrower range of states and may have a sig-
nificantly lower accuracy than what is expected from a reference quality EOS. 1 Nonetheless,
several equations from this category still offer a reasonable extrapolation behavior both in
terms of states and thermodynamic properties for most process design purposes. For the
remaining pure compounds of industrial relevance, there are typically insufficient data avail-

able to support highly accurate EOS development; and the data availability is much worse
for mixtures. In any case, the most accurate and reliable EOS are regularly explicit empir-
ical correlations of a thermodynamic potential. 1 This is intentional, since thermodynamic
potentials play a special role in thermodynamics because they are different representations

of the fundamental equation of state (FEOS) of thermodynamics and they carry the same
information content. To be more specific, any other static thermodynamic property can be
obtained from a combination of the partial derivatives of the thermodynamic potential with
respect to its independent variables. These types of EOS are generally referred to as FEOS

2
correlations.
The problem of mapping the relevant fluid region of industrial interest with laboratory
measurements is associated with high financial costs, the often extreme thermodynamic con-
ditions, and the sometimes hazardous nature of the considered substance. The infamous

chemical weapon of World War I, phosgene (CCl2 O, CAS: 75-44-5) is a good example. Be-
ing extremely toxic, with a fatal level of around 100 ppm over minutes of exposure, 5 research
institutions and laboratories unsurprisingly prefer to abstain from this substance, let alone
systematically measure it. The available experimental data in the literature were measured
50 up to 100 years ago and essentially only consist of vapor-liquid equilibrium (VLE) data

(saturated liquid density, 6–10 vapor pressure, 6,10–13 enthalpy of vaporization, 10,13 and molar
isobaric heat capacity of the saturated liquid 9,10,13,14 ), with the exception of the relatively
recent measurements of the Wiltec Research Company that considered several state points
in the homogenous region in addition to vapor pressure and saturated liquid density. 15 Yet,

the estimated world production of phosgene reached 1.3 million tons in 1977 and 2.7 million
tons in 1996. 5 The production rate has increased in the last twenty years because phosgene
is used as an intermediate in numerous applications, including dye, pharmaceutical, agricul-
tural, and mainly polymer industry, in presumably suboptimal processes due to insufficient

thermophysical property data.

Molecular modeling and simulation has an advantage over experimental measurements that
it is not limited by extreme conditions (temperature or pressure) or the nature of the sub-
stance. Moreover, it is associated with considerably lower financial cost and has typically
a much faster response time. The predictive capability of molecular simulation is only de-

pendent on the underlying molecular model that represents the targeted substance. It is
generally accepted that atomistic molecular models can, and often do, provide reasonable
thermodynamic properties for state points, properties, or scenarios that were not considered
during the optimization of their parameters. Our previous findings with other substances

showed that molecular models tend to perform reasonably well when comparing various

3
Helmholtz energy derivatives from simulations with the available FEOS correlations that
are based on experimental data. The supplementary material of Ref. 16 contains numerous
examples. In fact, molecular models have evolved to a point when a seemingly notable
disagreement between a single laboratory measurement and the corresponding result from

molecular simulation does not immediately invalidate the latter. The strategy of using lab-
oratory data along with molecular simulation results has recently been employed to develop
FEOS for engineering purposes. 17
The properties of phosgene render the substance an ideal candidate for molecular modelling
and simulation and an effort of summarize and represent simulation data in the form of an

FEOS. The purpose of this work is to investigate a simple fitting approach that is able to
provide a reasonable FEOS correlation within extremely short notice and require essentially
no expertise once an adequate molecular simulation data set is available. Today, such a data
set can be generated within a few weeks on a couple of commodity computers.

Fundamental equation of state

Due to practical reasons, FEOS correlations are often explicit in terms of the thermodynamic
potential

ao (T, ρ) + ar (T, ρ)
α(τ, δ) = = αo (τ, δ) + αr (τ, δ), (1)
RT

with the molar Helmholtz energy a, the temperature T , the density ρ, the molar gas con-
stant R, the inverse reduced temperature τ = Tc /T , and the reduced density δ = ρ/ρc , in

which Tc is the critical temperature and ρc the critical density. The denominator renders
α dimensionless. Eq. (1) shows that α can be additively separated into an ideal αo and a
residual part αr . The ideal part αo (T, ρ) = αo (T ) + αo (ρ) by definition corresponds to the
value of α(T, ρ) when no intermolecular interactions are at work. 1 αo (T, ρ) has a trivial den-

sity dependence αo (ρ) = ln(ρ/ρref ) but a non-trivial temperature dependence. The latter is

4
often determined by spectroscopy or ab initio calculations. Although molecular models with
internal degrees of freedom are parametrized to describe αo (T ) properly, the residual part
αr (T, ρ) = α(T, ρ) − αo (T, ρ) is typically the target of molecular simulation. Accordingly,
αo and αr are correlated separately during FEOS development with different mathematical

functions.
For the present correlations, the ideal part was determined by integrating the isobaric heat
capacity of the ideal gas state

3
cop X (uk /T )2 exp(uk /T )
=4+ vk . (2)
R
k=1
[exp(uk /T ) − 1]2

This equation was fitted to the data of Giauque and Ott 14 for temperatures below 500 K
and the data of Stull and Prophet 18 for temperatures above 500 K (cf. Figure 1). The
obtained parameters are v1 = 3.22652, v2 = 1.23698, v3 = 1.51143, u1 = 874 K, u2 =
2344 K, and u3 = 445 K. Because the cop data from the literature are essentially derived from

quantum statistical calculations and cannot be directly validated by experimental results, an

uncertainty of ±1% can reasonably be assumed, although the literature data were reproduced
here within ±0.1%. In Figure 1, the deviation between the ideal part of the present FEOS
and the correlation of DIPPR has a local minimum of -1.6% at 130 K. It is likely that the

DIPPR correlation was not fitted to the corresponding literature cop values since the data of
Giauque and Ott 14 are missing from the database at present.
The integration of Eq. (2) yields

3
X
o
α (τ ) = ln δ + 3 ln τ + b1 + b2 τ + vk ln [1 − exp(−uk τ /Tc )] , (3)
k=1

where b1 = 8.3306265716, b2 = -3.401313711, while uk and vk are the same as those in Eq.
(2). The integration constants b1 and b2 were specified such that the enthalpy h = 0 kJ · kg−1
and the entropy s = 0 kJ·kg−1 ·K−1 at T0 = 298.15 K and p0 = 1 atm, and the corresponding
ideal gas density is ρ0 = p0 /(RT0 ).

5
The empirical formula that represents ar /(RT ) in this work consists of polynomial and
exponential terms 1

N Pol NExp
X X
r tk dk
α (τ, δ) = nk τ δ + nk τ tk δ dk exp(−δ lk ). (4)
k=1 k=NPol +1

Additional types of terms, e.g. Gaussian bell-shaped or non-analytic, 1 were not considered
here. The simultaneous optimization of the coefficients nk , the exponents tk , dk , lk , and the
number and type of terms requires complex non-linear fit algorithms. 1,19 Such an approach
is vital for developing reference type FEOS, and it also requires a substantial amount of

property data that goes through careful screening, which can easily take months or years
and demands considerable expertise. Naturally, the optimization of industrial processes
does not stay idle while FEOS are being developed. To provide a fast response time for
industrial needs, the problem of insufficient data and long development time has to be
tackled. An obvious solution to minimize the time requirement of FEOS fitting, is to use

recommendations from the literature for the functional form of the correlation, as well as
the values of the exponents tk , dk , lk that were simultaneously optimized for a number
of substances. There are a couple of such generalized parameter sets available: The 10-
and the two 12-term FEOS from Span and Wagner (one 12-term FEOS is intended for

polar and one 12-term FEOS for non- or weakly polar substances), 1,20 or the 14-term FEOS
from Sun and Ely are such correlations. 21 In addition to these, the Bender 22 (22-term)
and the MBWR 23 (40-term) correlations were also tested here, using their functional form
integrated to the Helmholtz energy representation according to Eq. (4). 1 With the present

data set, the MBWR equation showed the best performance, and it is therefore presented
in the following. Although the MBWR correlation has 40 terms, the parameter set of this
correlation (cf. table 1), unlike generalized parameter sets, was originally optimized for a
single substance (nitrogen) and the MBWR correlation in general is more likely to carry
numerical instability or poor extrapolation behavior when applied to considerably different

6
substances. However, the need of extrapolation can be avoided, if a consistent data set
containing a large number of thermodynamically non-redundant property information is
sampled at systematically distributed state points covering the entire fluid range of interest.
In contrast to laboratory work, molecular simulation renders such a data set feasible.

Fitting strategy and data set

The production of data sets by molecular simulation can be automatized and it is cheap.
Furthermore, the formalism proposed by Lustig 24,25 allows for the efficient generation of a
large amount of thermodynamically non-redundant information. From a single molecular
simulation run per state point, the method was designed to provide an arbitrary number of

Helmholtz energy derivatives

∂ x+y αr (τ, δ) x y∂
x+y r
α (T, ρ)
Arxy = τ x δ y x y
= (1/T ) ρ , (5)
∂τ ∂δ ∂(1/T )x ∂ρy

with x > 0 or y > 0. These are exactly the derivatives of the thermodynamic potential in
terms of which the FEOS is explicit, i.e. Eq. (1). Since α is a thermodynamic potential, any
other static thermodynamic property is a combination of its partial derivatives. The molar
internal energy u, pressure p, molar enthalpy h, molar Gibbs energy g, and molar isochoric

heat capacity cv are simple functions

u
= Ao10 (T ) + Ar10 , (6)
RT

p
= 1 + Ar01 , (7)
ρRT

 
1 ∂p
= 1 + 2Ar01 + Ar02 , (8)
RT ∂ρ T

7
  
1 ∂p
= 1 + Ar01 − Ar11 , (9)
ρR ∂T ρ

h
= 1 + Ar01 + Ao10 (T ) + Ar10 , (10)
RT

g
= 1 + Ar01 + Ao00 + Ar00 , (11)
RT

cv
= −Ao20 (T ) − Ar20 , (12)
R

while molar isobaric heat capacity cp , and speed of sound w are non-linear combinations of
derivatives

cp o r (1 + Ar01 − Ar11 )2
= −A20 (T ) − A20 + , (13)
R 1 + 2Ar01 + Ar02

Mw 2 (1 + Ar01 − Ar11 )2
= 1 + 2Ar01 + Ar02 − , (14)
RT Ao20 (T ) + Ar20

where M is the molar mass, Arxy = Arxy (T, ρ), and Aoxy = Aoxy (T, ρ) = (1/T )x ρy · ∂ x+y [αo (T ) +
αo (ρ)]/∂(1/T )x /∂ρy = Aoxy (T ) + Aoxy (ρ). Note that the ideal part

• Aoxy (T, ρ) = 0, for x > 0 and y > 0,

• Aoxy (T, ρ) = Aoxy (T ) + 0, for x > 0 and y = 0,

• Aoxy (T, ρ) = 0 + (−1)1+y , for x = 0 and y > 0.

A more complete list of thermodynamic properties can be found in Ref. 1

Most of the derivatives Axy cannot directly be measured in the laboratory. On the other
hand, it is possible to produce a simulation data set that contains explicitly Axy derivatives,

8
which is computationally convenient for FEOS correlation purposes: Each analytical deriva-
tive of Eq. (4) with respect to τ and δ provides an equation that is fitted to a result for Arxy
from simulation. The total set of such equations needs to be solved only for the parameters
nk if the functional form and the exponents tk , dk , and lk are specified (cf. Table 1). The

number of equations is much larger than the number of variables nk , thus the goal is to find
an optimal set of nk . This was done here with the algorithm for weighted multiproperty fits
of Hust and McCarty. 26
In total, five derivatives, Ar10 , Ar01 , Ar20 , Ar11 , Ar02 , as well as Ar00 were sampled using the
molecular simulation tool ms2 27 at 400 state points located in the homogeneous fluid region

(cf. Figure 2) so that 2400 thermodynamically non-redundant records were generated. At

each state point, 864 particles were equilibrated, and then sampled for two million produc-
tion cycles with NV T ensemble Monte Carlo simulations 28 (number of particles N, volume
V , and temperature T were held constant) using 16 processor cores per state point. The

electrostatic long-range correction was treated by the reaction field method. 29 The simula-
tions were based on the molecular model for phosgene of Huang et al. 30 that was optimized
to vapor pressure, saturated liquid density, and heat of vaporization data from experiment
between 270 K and 425 K. (The triple and critical point temperatures of phosgene are ap-

proximately 145 K and 455 K, respectively.). The model itself has no internal degrees of
freedom and consists of four Lennard-Jones sites, a point dipole, and a point quadrupole.
Details are given in the Appendix.
The statistical uncertainty of all simulation results was estimated with the method of Fly-
vbjerg and Petersen. 31 Note that the statistical uncertainty of a molecular simulation result,

by definition, cannot reflect any other factor than the inherent statistical nature of the sim-
ulation: At a given state point, M configurations on the molecular level are generated, and
for each configuration thermodynamic properties are sampled. The final result for a ther-
modynamic property is the average of M values, and the statistical uncertainty of the result

decreases as M increases.

9
Ar00 was determined by Widom’s test particle insertion 32 by inserting 3456 test molecules in
every production step. This method is associated with additional computational cost and
has well known difficulties at high density, namely, it leads to Ar00 values with a large statis-
tical uncertainty, both in absolute and relative terms. Because the statistical uncertainty of

the simulation results serves as the weight of the fitted property during FEOS correlation, 26
data with high uncertainties practically do not influence the fit. Consequently, Ar00 results
above 14 mol·dm−3 were discarded from the dense liquid region. The effect of removing
every Ar00 data from the fitting procedure was also assessed, which is discussed below.
An obvious problem when generating such a data set is how to avoid sampling the solid

and the two-phase regions. At first sight that seems to require some knowledge about the
location of these regions. However, using the following procedure, no prior knowledge about
the vapor-liquid equilibrium (VLE) or the solid-liquid equilibrium (SLE) is required:

1. Select two or three high temperature isotherms. Fit the FEOS to the simulation data

along these isotherms and calculate a preliminary VLE envelope from it.

2. Remove state points if they are in the vapor-liquid two-phase region. Add more state
points that are in the homogeneous fluid region.

3. Fit the FEOS to the extended set of state points, and calculate an updated VLE

envelope. It is advised to keep a somewhat safe distance from the vapor-liquid two-
phase region, because it is not guaranteed that the FEOS yields the VLE envelope
that exactly corresponds to the molecular model.

4. Repeat steps (1) to (3) until the VLE envelope does not change significantly any more.

In case that a few state points accidentally remain in the vapor-liquid two-phase region, they
likely do not significantly influence the overall fit quality if there is a sufficient number of
other points sampled in the homogeneous fluid region. Nonetheless, the goal is to remove
such state points. State points close to the solid state can be identified by monitoring the

10
mean square displacement of molecules from their initial positions. If the mean square dis-
placement for the entire duration of the simulation is practically zero, then the state point
is likely located very close to the solid state, and it should be removed.
Three iterations of this procedure are illustrated in Figure 2. Tests, considering other sub-

stances, indicate that the procedure requires about 3-6 iterations. For this iterative state
point selection, the calculation of the VLE from the FEOS is essential and it is described in
the Appendix.

Results and discussion

According to the database of the Design Institute for Physical Properties (DIPPR), 33 the
critical temperature of phosgene is Tc = 455 K ±3% and its critical density is ρc = 5.25
mol·dm−3 ±10% based on the currently available experimental data. The present FEOS
correlation locates the critical point at Tc = 462.88 K and ρc = 5.5916 mol·dm−3 using the
method described in the appendix. The coefficients of the correlation fitted to the data at

400 state points from molecular simulation are listed in Table 1. The FEOS yields the critical
pressure pc = 6.459 MPa; the corresponding value from DIPPR database is pc = 5.674 ±5%
MPa.
Statistical comparisons in the following are based on the relative and absolute deviation that

are defined here for a given property X as

(XDATA − XFEOS )
RDEV(X) = 100 , (15)
XDATA

and

ADEV(X) = |XDATA − XFEOS |, (16)

11
respectively.

Representation of data in the homogeneous region

There are very few laboratory data available in the literature concerning the homogeneous
fluid region of phosgene. The Wiltec Research Company measured 20 pvT data points es-
sentially along four isotherms. 15 In those measurements, the phosgene sample was checked

by gas chromatography and a single peak was detected. The sample itself was obtained after
a single-stage distillation at 253.15 K from an initial sample that had a purity of > 99.0%.
The temperature was measured with a platinum resistance thermometer calibrated to a
NIST-traceable standard using the ITS-90 scale that had an accuracy of ±0.05 K, while the

pressure was measured with a Paroscientific pressure transducer having a NIST-traceable

calibration that had an estimated accuracy of ±0.03%. The density was estimated by first
filling an initially evacuated cell (300 cm3 ) with phosgene at 273.15 K, and then removing
phosgene increments and weighing them with a ±0.002 g accuracy as the temperature or the
pressure were gradually increased. The initial mass weighed to an accuracy of ±0.02 g plus

the removed phosgene content and the volume of the cell, which was determined through
multiple calibrations with water as a function of temperature and pressure, yielded the den-
sity. The results of those measuremens are listed in Table 2 along with the data from the
present FEOS correlation. The relative deviations between the laboratory data (for pressure

and density) and the present correlations increase in the vicinity of the critical point, but
exceed ±10% only once.
In a considerably more complex FEOS development effort for ethylene oxide, in which molec-
ular simulation data from the homogeneous region together with experimental VLE data were

used and during which the coefficients and the exponents of an empirical FEOS correlation
with polynomial, exponential, and Gaussian bell-shaped terms were optimized, the repre-
sentation of Arxy results was found to be as follows for the majority of state points: 17 Ar00
data were represented within ±5%, Ar10 within ±5%, Ar01 within ±6%, Ar20 within ±15%,

12
Ar11 within ±5%, and Ar02 within ±20%. According to Figure 3, the representation quality of
the present FEOS is predominantly better. However, a direct comparison is not entirely fair,
because the FEOS by Thol et. al. 17 considered experimental as well as simulation data and
even slight inconsistencies between the two may cause a deterioration in the representation

of both. Nonetheless, with the present FEOS, the majority of state points are represented
within ±2% for Ar00 , ±1.5% for Ar10 , ±2% for Ar01 , ±8% for Ar20 , ±3% for Ar11 , and ±5% for
Ar02 , which is mostly within the statistical uncertainty of the simulation runs. Deviations
with respect to potential simulation results close to the critical point may be higher than
these percentages. Especially in case of Ar02 , it is important to note that simulation results at

lower densities (below 4 mol·dm−3 ) are represented with seemingly large relative deviations.
However, many of those data are in fact reproduced within their statistical uncertainty. Fur-
thermore, at such low densities, large relative deviations are quite small in absolute terms.
The absolute deviation plots in Figure 4 support this statement. The dimensionless absolute

deviations shown there can be converted into SI units using Eqs. (1), (6), (7), (8), and (12):
For Ar00 , Ar10 , and Ar02 , 0.001 in dimensionless units translates to ≈ 2 J·mol−1 at 250 K and
≈ 6 J·mol−1 at 750 K. For Ar01 , 0.01 in dimensionless units is ≈ 0.3 MPa at 250 K and 16
mol·dm−3 . For Ar20 , 0.1 in dimensionless units is ≈ 0.8 J·mol−1 ·K−1 . The complete molecular

simulation data set along with the corresponding values from the present FEOS is provided
as supplementary material.
Finally, Figure 5 summarizes the performance of the FEOS in terms of usual thermodynamic
properties. With only a few exceptions, properties were represented as follows: within ±1.5%
for pressure, within ±3% for (∂p/∂ρ)T , within ±1.5% for (∂p/∂T )ρ , within ±1.5% for iso-

choric heat capacity, within ±2% for isobaric heat capacity, and within ±1.5% for speed of
sound, which is mostly within the statistical uncertainty of the simulation runs. However, de-
viations seem to be consistently larger very close to the triple point (above 17 mol·dm−3 and
below 175 K) for the isochoric and isobaric heat capacities, speed of sound, and (∂p/∂T )ρ .

Therefore, any information from the FEOS at this region should be treated with care.

13
Vapor-liquid equilibria and behavior of thermodynamic properties

VLE data from the present FEOS are predictions from homogeneous phase molecular simu-
lation data and the subsequent fitting procedure. According to Figure 6, the present FEOS

is fully consistent with the molecular model of phosgene as it predicts the VLE results from
dedicated molecular simulation runs accurately.
The performance in comparison with the experimental data can also be seen in Figure 6. The
saturated liquid density is represented within ±2%. The vapor pressure plot between 300

K and the critical temperature shows acceptable deviations from laboratory measurements
and their correlations. However, the deviation increases significantly below 300 K, although
it should be mentioned that the model was practically not fitted to experimental data below
270 K because the uncertainty of VLE simulations increases with decreasing temperature.

The large scatter of the vapor pressure simulation results can be clearly seen Figure 6 at low
temperatures. Noticeably, there is a deviation between DIPPR and the most recent measure-
ments by Jasperson et al. 15 with respect to vapor pressure that increases gradually (0.2%
at 260 K, 1.4% at 350 K, 5.0% at 440 K) approaching the critical temperature. According
to Jasperson et al., 15 the deviation is due the almost seventy year old measurements upon

which the DIPPR correlation is based involving outdated measurement methods, equipment,
and the presumably low purity of the sample. Nonetheless, the pressure values at the criti-
cal point by Wiltec and DIPPR agree within the reported uncertainty of the latter (±5%).
Enthalpy of vaporization data, which are questionable in general, are represented with −4%

and up to −8% deviation by the present FEOS. Literature data for the isobaric heat capac-
ity of the saturated liquid are available between 145 K and 280 K, which is essentially out
of the temperature range of the present model. Nonetheless, the experimental values are
represented with around +10% deviation. In light of the general trends shown in Figure 6,

it is advised to use the available correlations 15,33 instead of the present FEOS to obtain the
VLE data of phosgene.
Figure 7 shows the general physical behavior of the most important thermodynamic proper-

14
ties. The qualitative behavior of the thermodynamic properties is well-known. 19 In the T vs.
ρ diagram (Figure 7, top left) the rectilinear diameter is usually almost a straight line up to
the vicinity of the critical point where it may show a slight curvature. Here, the algorithm
employed to locate the critical density yields a value that causes a pronounced bend in the

rectilinear diameter approaching the critical temperature. We are unable to provide further
comments whether this bend is an artifact of the algorithm or it is really consistent with the
molecular model. However, a similar behavior has been observed in a previous work, other
earlier mentioned generalized FEOS that were fitted to a simulation based data set. 34
In the p vs. ρ plot (Figure 7, top right), the isotherms should converge, but not cross each

other at high temperature, pressure, or density. For the residual isochoric heat capacity crv
(Figure 7, mid left), the saturated liquid line should have a curvature and rise towards low
temperatures. In accordance with the speed of sound minimum at the critical point (Figure
7, mid right), the residual isochoric heat capacity should have a maximum there. Further-

more, the speed of sound should have a negative slope and no curvature at low temperatures
in the liquid phase. The second virial coefficient B (Figure 7, bottom left) should be negative
for low temperatures, cross the zero line once, and then approach zero after passing through
a maximum. B can be calculated for molecular models up arbitrary accuracy with sim-

ple numerical integration schemes. 35 The corresponding results agree well with the present
FEOS. The characteristic curves (Figure 7, bottom right) should be smooth with no unusual
curvature within the limits of the data set.

Interpolation performance: Effect of data set reduction

To apply the workflow presented here in practice, the computational bottleneck is carrying

out 400 molecular simulation runs with 3456 test molecule insertions in every production
step to calculate Ar00 . To test if such an effort is really necessary, a considerably smaller data
set was created by keeping every third state point (133 in total) along the isotherms of the
original one with 400 state points shown on Figure 2. After performing a new fit with the

15
133 state points and excluding Ar00 entirely from the fit, it was concluded that this serious
reduction barely affected the overall performance: The derivatives, including Ar00 , calculated
at the original 400 state points were represented with practically the same quality as before.
The corresponding figures, that are analogous to Figures 3, 4, and 5, showing the effect of

the reduction of the data set, are provided as supplementary material. The performance
with respect to VLE data and the experimental homogeneous data (Figure 6 and Table 2)
remained practically identical after the reduction.
The low importance of Ar00 values in the data set is not surprising. Its derivatives describe
the Helmholtz energy surface much more accurately then Ar00 itself when sampling about

400 state points. Furthermore, Ar10 (energy) and Ar01 (pressure) are the most well-behaved
properties from molecular simulation and fitting them with a high accuracy essentially guar-
antees a perfect match for Ar00 as well. These findings indicate that a similarly valuable data
set can be created even on a couple of commodity computers within a few days and without

considerable performance loss.

Conclusion

In this work, an empirical FEOS correlation was fitted to molecular simulation data and
serves predictive purposes. The underlying data set contains six properties at 400 state
points resulting in a set of 2400 thermodynamically non-redundant data points. These

thermodynamic properties along with the available experimental pressure and density data
in the homogeneous fluid region are represented well by the present FEOS. Furthermore, an
almost identical performance was achieved when the fitting procedure was repeated with a
considerably smaller and computationally less costly data set. Moreover, the VLE results of

dedicated molecular simulations were predicted accurately from the underlying homogeneous
data and the subsequent FEOS fitting. The VLE data from experimental measurements can
still be more accurately reproduced with existing experimental VLE only correlations 15,33

16
than with the molecular model of phosgene. The FEOS correlation of this work is provided
as supplementary material.
The workflow presented here was devised such that it requires very little human interaction
and almost no expertise while offering a fast response time. It was implemented into a

cloud computing environment that offers a web-based user interface to select state points
and the underlying molecular model. Simulation runs and FEOS fitting are carried out
automatically on dedicated high performance computers, and thus the effort requires no
computational resources from the user. Details will be published shortly.

Acknowledgments

The authors gratefully acknowledge financial support by Deutsche Forschungsgemeinschaft

under the grant VR6/4-1. This work was carried out under the auspices of the Boltzmann-
Zuse Society (BZS) of Computational Molecular Engineering. Access to hardware was given
by the High Performance Computing Center Stuttgart (HLRS) under grant MMHBF2. The
authors also would like to thank Monika Thol for her support in preparing figures and

setting up the ideal part of the FEOS, as well as Louis V. Jasperson for providing laboratory
measurement data in an electronic form.

Supporting Information Available

The supplementary material contains the complete underlying data set from molecular sim-
ulation along with the corresponding values from the present FEOS (including VLE data)

that can be used to verify computer implementation. The present FEOS is provided as
C++ code and an FLD file. The latter serves as input file for the software REFPROP 36
distributed by the National Institute of Standards and Technology. Additional figures are
also included that show the effect of data set reduction.

This material is available free of charge via the Internet at http://pubs.acs.org/.

17
Molecular model

The coordinates and parameters for the molecular model of phosgene are given in Table 3.

Vapor-liquid equilibrium calculation

For locating the vapor pressure and the corresponding saturated vapor and saturated liquid
densities, an algorithm was chosen that is based on the method of Szalai et al. 37 Expanding
the chemical potential µ and the pressure p in a Taylor series around a known state point

(p0 , ρ0 ) yields

 
∂µ
µ = µ0 + (p − p0 ) + ... , (17)
∂p T

and

 
∂p
p = p0 + (ρ − ρ0 ) + ... . (18)
∂ρ T

Keeping the linear terms, using the relation (∂µ/∂p)T = (∂g/∂p)T = V /N = 1/ρ, that holds
for pure fluids, and applying the phase equilibrium conditions µL = µV and pL = pV = pv at
a given temperature leads to

1 1
µL0 + L
(pv − pL0 ) = µV V
0 + V (pv − p0 ), (19)
ρ0 ρ0

and

 L  V
∂p ∂p
pL0 + L
(ρ − ρL0 ) = pV
0 + (ρV − ρV
0 ) = pv . (20)
∂ρ T ∂ρ T

18
Eq. (19) yields the vapor pressure pv

(µL0 − pL0 /ρL0 ) − (µV V V

0 − p0 /ρ0 )
pv = , (21)
1/ρV 0 − 1/ρ0
L

and Eq. (20) provides the saturated densities ρL and ρV

pv − pL,V
L,V
ρ = 0
L,V
+ ρL,V
0 , (22)
(∂p/∂ρ)T

where the superscripts L and V stand for liquid and vapor, respectively. Note that the
variables in Eqs. (21) and (22), i.e. p0 , µ0 , and (∂p/∂ρ)T at state point (T, ρ0 ), that are

required to calculate pv and ρL,V are directly obtainable from the residual part of the FEOS
correlation (including µ0 , because the exclusively temperature dependent ideal part of the
total chemical potential cancels out in Eq. (19)). Naturally, increasing the number of terms
considered in the Taylor series up to arbitrary order would yield the vapor pressure and the
coexisting densities at a given temperature immediately. However, this might be an unre-

alistic expectation towards the FEOS correlation, because it would have to provide precise
values for the required derivatives (∂ 2 µ/∂p2 )T , (∂ 3 µ/∂p3 )T , ..., (∂ 2 p/∂ρ2 )T , (∂ 3 p/∂ρ3 )T ,... .
It is more suitable to find the VLE in finite steps applying Eq. (22) successively in an iter-
ative manner: At a given temperature T and densities ρL,V L,V L,V L,V
j , pj , µj , and (∂p/∂ρ)T are

calculated for step j. Substituting these values into Eq. (21) provides the vapor pressure pv
for step j, and since pv is known, Eq. (22) yields ρLj+1 and ρV
j+1 for step j + 1. Starting with

some initial ρL,V

0 , that must be in the homogeneous phase, the iterative process continues

until the criteria µLj − µV L V

j < d and pj − pj < d are satisfied for an arbitrarily small d. Upon

convergence, the saturated densities ρL,V

j = ρL,V and the vapor pressure pLj = pV
j = pv at

a given temperature are known. The VLE envelope itself can be obtained by locating the
saturated densities for a series of temperature values starting at Tmin < Tc . Eq. (22) ceases
to yield distinct coexisting densities if the critical temperature is exceeded. Consequently,
Tc and ρc can be determined up to an arbitrary numerical accuracy.

19
It has to be noted that when fitting Eq. (4) and just simply using some arbitrary values
for Tc and ρc in Eq. (4), the FEOS itself is unlikely to identify the very same values as the
actual critical temperature and critical density of the FEOS for which [∂p(Tc , ρc )/∂ρ]T =
[∂ 2 p(Tc , ρc )/∂ρ2 ]T = 0. In case these conditions are constrained at Tc and ρc , the FEOS

yields the critical point at Tc and ρc . If they are not constrained, the actual critical temper-
ature and density of the FEOS can still be determined by a simple iterative approach. One
iteration step consists of the following three substeps:

1. Perform the FEOS fit using Tci and ρic in Eq. (4).

′ ′
2. Determine the actual critical temperature Tc and density ρc of this fit.

3. Update the critical temperature and density used in Eq. (4) according to Tci+1 =
′ ′
λTc + (1 − λ)Tci and ρi+1
c = λρc + (1 − λ)ρic , where 0 ≤ λ ≤ 1 with typical values
between 0.1 and 0.5.

These substeps should be repeated until the critical temperature and density converge to

finite values, although it should be mentioned that convergence is not guaranteed. However,
a very rough guess for the initial values of Tc and ρc is perfectly satisfactory.

References

(1) Span, R. Multiparameter Equations of State: An Accurate Source of Thermodynamic

Property Data; Springer Verlag, Berlin, 2000.

(2) Wagner, W.; Pruss, A. J. Phys. Chem. Ref. Data 2002, 31, 387–535.

(3) Span, R.; Wagner, W. J. Phys. Chem. Ref. Data 1996, 25, 1509–1596.

(4) Span, R.; Lemmon, E. W.; Jacobsen, R. T.; Wagner, W.; Yokozeki, A. J. Phys. Chem.
Ref. Data 2000, 29, 1361–1433.

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 (5) Ryan, T.; Seddon, E.; Seddon, K.; Ryan, C. Phosgene: and Related Carbonyl Halides;
Topics in Inorganic and General Chemistry; Elsevier Science, Amsterdam, 1996.

(6) Paterno, E.; Mazzucchelli, A. Gazz. Chim. Ital. 1920, 50, 30–53.

(7) Germann, A. F. O. J. Phys. Chem. 1925, 29, 138–141.

(8) Davies, C. N. J. Chem. Phys. 1946, 14, 48–49.

(9) Timmermans, J. Physico-Chemical Constants of Pure Organic Compounds, Vol II ;

Elsevier, New York, NY, 1965.

(10) Braker, W.; Mossman, A. L. Matheson Unabridged Gas Data Book: A Compilation of

Physical and Thermodynamic Properties of Gases; Matheson Company, New Jersey,

NJ, 1974.

(11) Germann, A. F. O.; Taylor, Q. W. J. Am. Chem. Soc. 1926, 48, 1154–1159.

(12) Stull, D. R. Ind. Eng. Chem. 1947, 39, 517–540.

(13) Giauque, W. F.; Jones, W. M. J. Am. Chem. Soc. 1948, 70, 120–124.

(14) Giauque, W. F.; Ott, J. B. J. Am. Chem. Soc. 1960, 82, 2689–2695.

(15) Jasperson, L. V.; Wilson, G. M.; Wilson, L. C. Vapor Pressures, Critical Properties,
and High Pressure PVT Measurements on Phosgene; AIChE Spring Meeting, 1996.

(16) Rutkai, G.; Thol, M.; Lustig, R.; Span, R.; Vrabec, J. J. Chem. Phys. 2013, 139,
041102.

(17) Thol, M.; Rutkai, G.; Koster, A.; Kortmann, M.; Span, R.; Vrabec, J. Chem. Eng. Sci.
2015, 121, 87–99.

(18) Stull, D. R.; Prophet, H. JANAF Thermochemical Tables, 2nd ed., NSRDS-NBS 37 ;
U.S. Department of Commerce, Washington, D.C., 1971.

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(19) Lemmon, E. W.; Jacobsen, R. T. J. Phys. Chem. Ref. Data 2005, 34, 69–108.

(20) Span, R.; Wagner, W. Int. J. Thermophys. 2003, 24, 1–39.

(21) Sun, L.; Ely, J. F. Int. J. Thermophys. 2005, 26, 705–728.

(22) Bender, E. Equations of state exactly representing the phase behavior of pure sub-
stances. Proceedings of the Fifth Symposium on Thermophys. Prop., ASME, New York.
1970.

(23) Jacobsen, R. T.; Stewart, R. B. J. Phys. Chem. Ref. Data 1973, 2, 757–922.

(24) Lustig, R. Mol. Sim. 2011, 37, 457–465.

(25) Lustig, R. Mol. Phys. 2012, 110, 3041–3052.

(26) Hust, J.; McCarty, R. Cryogenics 1967, 7, 200–206.

(27) Glass, C. W.; Reiser, S.; Rutkai, G.; Deublein, S.; Koster, A.; Guevara-Carrion, G.;
Wafai, A.; Horsch, M.; Bernreuther, M.; Windmann, T.; Hasse, H.; Vrabec, J. Comput.
Phys. Commun. 2014, 185, 3302–3306.

(28) Frenkel, D.; Smit, B. Understanding Molecular Simulation: From Algorithms to Appli-

cations; Academic Press, Elsevier, San Diego, CA, 2002.

(29) Barker, J. A.; Watts, R. O. Mol. Phys. 1973, 26, 789–792.

(30) Huang, Y.-L.; Heilig, M.; Hasse, H.; Vrabec, J. AIChE J. 2011, 57, 1043–1060.

(31) Flyvbjerg, H.; Petersen, H. G. J. Chem. Phys. 1989, 91, 461–466.

(32) Widom, B. J. Chem. Phys. 1963, 39, 2808–2812.

(33) Rowley, R. L.; Wilding, W. V.; Oscarson, J. L.; Yang, Y.; ; Zundel, N. A.;
Daubert, T. E.; Danner, R. P. DIPPR Data Compilation of Pure Compound Prop-
erties: Design Institute for Physical Properties; AIChE, New York, NY, 2006.

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(34) Lustig, R.; Rutkai, G.; Vrabec, J. Mol. Phys. 2015, 113, 910–931.

(35) Hirschfelder, J. O.; Curtiss, C. F.; Bird, R. B.; Mayer, M. G. Molecular theory of gases
and liquids; Wiley New York, 1954; Vol. 26.

(36) NIST Reference Fluid Thermodynamic and Transport Properties Database.

http://www.nist.gov/srd/nist23.cfm.

(37) Szalai, I.; Liszi, J.; Boda, D. Chem. Phys. Lett. 1995, 246, 214–220.

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23
Figure 1: Isobaric heat capacity of the ideal gas state cop : - - correlation of DIPPR; 33
— present FEOS; ✷ data from the literature 14,18 (top). Relative deviations (RDEV) were
calculated by Eq. (15) (bottom).

24
Table 1: Parameters of Eq. (4). The exponents tk , dk , and lk were taken from the MBWR
correlation. 23 The coefficients nk were determined in the present work.

k tk dk lk nk
1 0 1 -0.095842094249538
2 0.5 1 3.060952615139520
3 1 1 -4.747603241620660
4 2 1 1.338877244191170
5 3 1 -0.703848906445479
6 0 2 0.130746087315180
7 1 2 -0.185421337994230
8 2 2 0.323226318151166
9 3 2 0.390419782002820
10 0 3 0.029302442911150
11 1 3 -0.042207175336127
12 2 3 -0.079579086717665
13 1 4 0.068455977731017
14 2 5 -0.065766198173309
15 3 5 0.014775785350582
16 2 6 0.020058202738120
17 2 7 -0.001302560740835
18 3 7 -0.002862077171645
19 3 8 0.000471671584767
20 3 0 -1.992569767335400
21 4 0 -0.072342927646866
22 5 0 0.004522322999102
23 3 0 2 1.992557973563120
24 4 0 2 0.072428420215191
25 5 0 2 -0.004564386771021
26 3 2 2 1.311876945126580
27 4 2 2 0.659818243382377
28 5 2 2 -0.343829613759978
29 3 4 2 0.560294166439144
30 4 4 2 0.096613261111098
31 5 4 2 0.048621442800266
32 3 6 2 -0.009280163441566
33 4 6 2 0.137750035189476
34 5 6 2 0.018998019880235
35 3 8 2 0.042226707042714
36 4 8 2 0.007823270710127
37 5 8 2 -0.023062729469879
38 3 10 2 -0.008317628227420
39 4 10 2 0.011568386045278
40 5 10 2 0.001358217519838

25
Table 2: Comparison of experimental pvT data 15 (EXP) from the homogeneous fluid region
with the present correlation (FEOS). Comparisons are also expressed in terms of relative
deviations (RDEV) calculated by Eq. (15). The third column lists the density from the
present FEOS at the temperature and pressure specified by the laboratory pvT data, while
the sixth column is the pressure from the present FEOS at the temperature and density
specified by the laboratory pvT data.

T /K ρ/mol·dm−3 RDEV(ρ) p/MPa RDEV(p)

EXP FEOS EXP FEOS
423.153 10.942 10.870 0.7 13.631 14.678 -7.7
423.150 10.674 10.618 0.5 10.397 11.054 -6.3
423.157 10.300 10.273 0.3 6.909 7.140 -3.3
423.161 9.876 9.898 -0.2 4.158 4.023 3.2
443.149 10.290 10.191 1.0 13.776 14.831 -7.7
443.144 9.884 9.806 0.8 10.335 10.947 -5.9
443.151 9.254 9.228 0.3 6.895 7.013 -1.7
443.156 8.819 8.855 -0.4 5.509 5.400 2.0
473.148 8.975 8.828 1.6 13.003 13.821 -6.3
473.176 8.307 8.171 1.6 10.328 10.770 -4.3
473.200 5.926 5.082 14.2 7.329 7.562 -3.2
473.200 2.551 2.347 8.0 5.688 5.922 -4.1
473.150 1.180 1.129 4.3 3.537 3.659 -3.4
498.136 7.938 7.729 2.6 13.817 14.587 -5.6
498.143 6.375 6.023 5.5 10.370 10.809 -4.2
498.132 4.472 4.033 9.8 8.522 8.924 -4.7
498.134 2.933 2.727 7.0 7.026 7.307 -4.0
498.134 2.058 1.954 5.1 5.743 5.942 -3.5
498.134 1.450 1.380 4.8 4.488 4.657 -3.8
498.134 1.024 0.982 4.1 3.427 3.547 -3.5

Table 3: Sigma (σ) and epsilon (ǫ) denote the length and energy parameter of the Lennard-
Jones (LJ) potential, respectively. kB is the Boltzmann constant. D denotes the dipole
moment of the point dipole and Q the quadrupole moment of the point quadrupole. All
coordinates are in principal axes with respect to the center of mass. The orientation of
the point dipole is defined with Euler angles: ϕ is the azimuthal angle with respect to the
x-y-plane and θ is the inclination angle with respect to the z-axis.
Site x/Å y/Å z/Å σ/Å ǫ · kB−1 /K θ/deg ϕ/deg D/Cm · 10−30 Q/Cm2 · 10−40
C 0 0.5049 0 2.815 10.62
O 0 1.7018 0 3.195 132.66
Cl 0 -0.4695 -1.4509 3.366 157.63
Cl 0 -0.4695 1.4509 3.366 157.63
Dipole 0 0.0845 0 90 90 3.341
Quadrupole 0 0 0 90 90 -12.098

26
Figure 2: State points located in the homogeneous fluid region were selected in three consec-
utive steps according to the method described in this section. After the third iteration, the
present data set contained 400 state points. The continuous curve delimits the vapor-liquid
two-phase region calculated at the current iteration.

27
Figure 3: Relative deviations (RDEV) calculated by Eq. (15) between molecular simulation
data of this work and the present FEOS. The comparisons include the entire data set of 400
state points from the homogeneous fluid region shown in Figure 2. Different symbols denote
different isotherms and the notation corresponds to the one in Figure 2. RDEV values that
exceed the vertical axis limits were placed on the borders of the axis, but the spread of error
bars of these points reflects the uncertainty with respect to their original locations. Error
bars are plotted only in one direction for better visibility.

28
Figure 4: Absolute deviations (ADEV) calculated by Eq. (16) between molecular simulation
data of this work and the present FEOS. Details are as in Figure 3.

29
Figure 5: Relative deviations (RDEV) calculated by Eq. (15) between molecular simulation
data of this work and the present FEOS. Details are as in Figure 3.

30
Figure 6: Relative deviations according to Eq. (15) between the present FEOS and data from
the literature: ✷ experimental data (saturated liquid density ρL , 6–10 vapor pressure pv , 6,10–13
enthalpy of vaporization ∆hv , 10,13 and molar isobaric heat capacity cp 9,10,13,14 ); N dedicated
VLE simulations of this work using the molecular simulation tool ms2 27 with the grand
equilibrium method, 38 864 particles in the liquid phase, around 500 particles in the vapor
phase, and with the gradual insertion technique 39 applied instead of Widom’s method 32 to
calculate the chemical potential below 300 K; — correlation of DIPPR; 33 - - correlation of
Jasperson et al. 15 The vapor pressure correlation of Jasperson et al. is exclusively based
on their own laboratory measurements and represents those data with very high accuracy:
±0.04% on average, where the representation of an individual value never exceeds ±0.17%.
Error bars are plotted only in one direction for better visibility.

31
Figure 7: Physical behavior of the thermodynamic properties p, w, crv , B (second virial
coefficient) as well as characteristic curves: JI - Joule inversion curve (Ar11 = 0); JTI - Joule-
Thomson inversion curve (Ar01 + Ar02 + Ar11 = 0); ID - ideal curve (Ar01 = 0); BL - Boyle curve
(Ar01 + Ar02 = 0); pv - vapor pressure. H dedicated second virial coefficient calculations of
this work; - - the critical temperature.

32
 Supporting Information to: Empirical fundamental equation of state for
phosgene based on molecular simulation data

Gábor Rutkai and Jadran Vrabec

Lehrstuhl für Thermodynamik und Energietechnik, Universität Paderborn, 33098

Paderborn, Germany

Corresponding author: Jadran Vrabec

E-mail: jadran.vrabec@upb.de
Phone: +49-5251/60-2421

Content: The complete underlying data set from molecular simulation along with the
prediction of the present FEOS (including VLE data) that can be used to verify computer
implementation. Additional figures that show the effect of data set reduction.
Figure S1. Relative deviations (RDEV) calculated between molecular simulation data of this
work and the present FEOS. The comparisons include the entire data set of 400 state points
from the homogeneous fluid region. However, the FEOS correlation that produced these
results used only 133 state points (every third state points along the sampled isotherms) and
no Ar00 values were considered in the fit. This FEOS correlation locates the critical point at Tc
= 462.98 K and ρc = 5.5358 mol∙dm-3. Different symbols denote different isotherms and the
notation corresponds that of Figure 2 of the manuscript. RDEV values that exceed the vertical
axis limits were placed on the borders of the axis, but the spread of error bars of these points
reflects the uncertainty with respect to their original locations. Error bars are plotted only in
one direction for better visibility.
Figure S2. Absolute deviations (ADEV) calculated between molecular simulation data of this
work and the present FEOS. Details are as in Figure S1.
Figure S3. Relative deviations (RDEV) calculated between molecular simulation data of this
work and the present FEOS. Details are as in Figure S1.
x y Temperature Density Arxy Statistical uncertainty of Arxy Arxy RDEV
from simulation from simulation from FEOS
(K) (mol ∙ m-3) (dimensionless) (dimensionless) (dimensionless)
0 0 250 3 -0.002499956 0.000012371 -0.002453118 1.87
0 0 250 4 -0.003315874 0.000012483 -0.003275884 1.21
0 0 250 5 -0.004159874 0.000013723 -0.004098742 1.47
0 0 250 6 -0.004998759 0.000015419 -0.004921691 1.54
0 0 250 7 -0.005795955 0.000017978 -0.005744680 0.88
0 0 250 8 -0.006619252 0.000019959 -0.006567812 0.78
0 0 250 9 -0.007483267 0.000020373 -0.007391034 1.23
0 0 275 7 -0.004638517 0.000013398 -0.004544810 2.02
0 0 275 9 -0.005931248 0.000014372 -0.005861272 1.18
0 0 275 11 -0.007280721 0.000016909 -0.007177827 1.41
0 0 275 13 -0.008610798 0.000018841 -0.008494555 1.35
0 0 275 15 -0.009880605 0.000018772 -0.009811416 0.70
0 0 275 17 -0.011191445 0.000020844 -0.011128370 0.56
0 0 275 19 -0.012587291 0.000021490 -0.012445497 1.13
0 0 275 21 -0.013816613 0.000025243 -0.013762718 0.39
0 0 275 23 -0.015208118 0.000024075 -0.015080113 0.84
0 0 275 25 -0.016464166 0.000025158 -0.016397600 0.40
0 0 300 9 -0.004838092 0.000011446 -0.004782714 1.14
0 0 300 10 -0.005373433 0.000013277 -0.005322316 0.95
0 0 300 20 -0.010770989 0.000016879 -0.010718558 0.49
0 0 300 30 -0.016186109 0.000023134 -0.016115423 0.44
0 0 300 40 -0.021599166 0.000026465 -0.021512883 0.40
0 0 300 50 -0.026928972 0.000029491 -0.026910912 0.07
0 0 300 60 -0.032379773 0.000031506 -0.032309582 0.22
0 0 325 10 -0.004516141 0.000009683 -0.004439105 1.71
0 0 325 20 -0.009027122 0.000016471 -0.008948665 0.87
0 0 325 30 -0.013538756 0.000018365 -0.013457546 0.60
0 0 325 40 -0.018030196 0.000022735 -0.017965727 0.36
0 0 325 50 -0.022517985 0.000024255 -0.022473185 0.20
0 0 325 60 -0.027000789 0.000025575 -0.026979981 0.08
0 0 325 70 -0.031535826 0.000028310 -0.031486094 0.16
0 0 325 80 -0.036128036 0.000032522 -0.035991528 0.38
0 0 325 90 -0.040606376 0.000034509 -0.040496260 0.27
0 0 325 100 -0.045103653 0.000033115 -0.045000351 0.23
0 0 325 13600 -3.499917628 0.010390050 -3.529568436 -0.85
0 0 325 13800 -3.511747973 0.013930233 -3.535358392 -0.67
0 0 350 100 -0.038218169 0.000031308 -0.038158415 0.16
0 0 350 140 -0.053503834 0.000036085 -0.053412036 0.17
0 0 350 160 -0.061201392 0.000040646 -0.061031388 0.28
0 0 350 180 -0.068769596 0.000041997 -0.068645835 0.18
0 0 350 200 -0.076305864 0.000044571 -0.076255355 0.07
0 0 350 220 -0.084025931 0.000049598 -0.083859996 0.20
0 0 350 240 -0.091645887 0.000053960 -0.091459799 0.20
0 0 350 260 -0.099172848 0.000059615 -0.099054737 0.12
0 0 350 280 -0.106795146 0.000054316 -0.106644871 0.14
0 0 350 13000 -2.943035620 0.005406058 -2.954652464 -0.39
0 0 350 13400 -2.953698891 0.008977849 -2.965519020 -0.40
0 0 350 13800 -2.974709693 0.011850852 -2.962733443 0.40
0 0 375 100 -0.032795112 0.000025326 -0.032757843 0.11
0 0 375 140 -0.045945363 0.000037151 -0.045841317 0.23
0 0 375 160 -0.052441745 0.000037150 -0.052374175 0.13
0 0 375 180 -0.059005800 0.000038837 -0.058901177 0.18
0 0 375 200 -0.065555815 0.000039790 -0.065422307 0.20
0 0 375 220 -0.071993789 0.000042429 -0.071937608 0.08
0 0 375 240 -0.078631813 0.000044411 -0.078447124 0.23
0 0 375 260 -0.085107611 0.000049550 -0.084950833 0.18
0 0 375 280 -0.091560496 0.000047631 -0.091448795 0.12
0 0 375 300 -0.098096070 0.000050934 -0.097940986 0.16
0 0 375 12200 -2.465378778 0.002388915 -2.470183174 -0.19
0 0 375 12600 -2.483358925 0.003167911 -2.488078259 -0.19
0 0 375 13000 -2.485701602 0.004372563 -2.495525057 -0.40
0 0 375 13400 -2.485972293 0.006550655 -2.491012571 -0.20
0 0 375 13800 -2.461195973 0.010583925 -2.472945034 -0.48
0 0 400 100 -0.028467299 0.000024005 -0.028394723 0.25
0 0 400 200 -0.056852050 0.000034075 -0.056682086 0.30
0 0 400 300 -0.084933810 0.000042152 -0.084817502 0.14
0 0 400 400 -0.113009109 0.000056384 -0.112803373 0.18
0 0 400 500 -0.140970437 0.000060988 -0.140641363 0.23
0 0 400 600 -0.168827008 0.000073449 -0.168332424 0.29
0 0 400 650 -0.182610880 0.000081743 -0.182122957 0.27
0 0 400 700 -0.196264162 0.000083118 -0.195876824 0.20
0 0 400 750 -0.210230425 0.000083955 -0.209593923 0.30
0 0 400 800 -0.223754425 0.000100788 -0.223274181 0.21
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0 2 425 900 0.007455888 0.005581814 0.011666438 -56.47
0 2 425 1000 0.004647034 0.006052238 0.014508047 -212.20
0 2 425 10200 2.882279418 0.085990840 2.974585924 -3.20
0 2 425 10600 3.622842894 0.078857390 3.725267468 -2.83
0 2 425 11400 5.855115100 0.113862527 5.754441726 1.72
0 2 425 12200 8.667875595 0.118184802 8.634222459 0.39
0 2 425 13000 12.261881878 0.127922227 12.498886795 -1.93
0 2 425 13800 17.431991540 0.149447197 17.469595343 -0.22
0 2 425 14600 24.171025851 0.191728344 23.783186395 1.60
0 2 425 15400 32.138067541 0.224709793 31.985882005 0.47
0 2 425 16200 41.766653010 0.257272312 43.124721659 -3.25
0 2 450 200 0.001102922 0.001004332 0.000572993 48.05
0 2 450 1000 -0.003922556 0.005296529 0.013669481 448.48
0 2 450 1800 0.054120197 0.009537797 0.047887065 11.52
0 2 450 2600 0.102881787 0.015468800 0.109712067 -6.64
0 2 450 8200 1.022221800 0.055638840 1.071624312 -4.83
0 2 450 9000 1.613053621 0.062264988 1.634890636 -1.35
0 2 450 9800 2.498279921 0.069732336 2.520805481 -0.90
0 2 450 10600 3.879762366 0.073158263 3.874532869 0.13
0 2 450 11400 5.895252115 0.097013190 5.868689429 0.45
0 2 450 12200 8.751363121 0.108210131 8.662586132 1.01
0 2 450 13000 12.430439053 0.132222461 12.379225924 0.41
0 2 450 13800 17.350740203 0.138003865 17.146451305 1.18
0 2 450 14600 23.152321547 0.170074549 23.214631639 -0.27
0 2 450 15400 30.898066149 0.207143224 31.117719180 -0.71
0 2 450 16200 40.886629047 0.230002456 41.823343263 -2.29
0 2 475 200 0.000309201 0.000928570 0.000541892 -75.26
0 2 475 1000 0.015024681 0.004670592 0.012807355 14.76
0 2 475 1800 0.050934594 0.008279067 0.043625120 14.35
0 2 475 2600 0.099539593 0.012915641 0.097108307 2.44
0 2 475 3400 0.178516374 0.016662803 0.169103268 5.27
0 2 475 4200 0.244878699 0.024958555 0.247484211 -1.06
0 2 475 5000 0.338924463 0.028599724 0.325357153 4.00
0 2 475 5800 0.358470406 0.024541181 0.415383741 -15.88
0 2 475 6600 0.441184503 0.038728661 0.551986909 -25.11
0 2 475 7400 0.754386771 0.046446829 0.781620552 -3.61
0 2 475 8200 1.135044620 0.055567898 1.155948511 -1.84
0 2 475 9000 1.774588866 0.059490472 1.741074432 1.89
0 2 475 9800 2.655280752 0.058993117 2.636872165 0.69
0 2 475 10600 4.138160974 0.079067947 3.983905724 3.73
0 2 475 11400 5.997959223 0.085390353 5.942398587 0.93
0 2 475 12200 8.556804372 0.101843708 8.656447586 -1.16
0 2 475 13000 12.200442849 0.117334575 12.241697930 -0.34
0 2 475 13800 16.926758290 0.130986425 16.831150244 0.56
0 2 475 14600 22.892238980 0.164316628 22.681825857 0.92
0 2 475 15400 29.940698410 0.207739340 30.309714146 -1.23
0 2 475 16200 39.235852338 0.211718611 40.608733077 -3.50
0 2 500 200 -0.000145259 0.000865814 0.000509723 450.91
0 2 500 1000 0.006587403 0.004860553 0.011992010 -82.04
0 2 500 1800 0.046413496 0.007974379 0.040134841 13.53
0 2 500 2600 0.085231432 0.012871893 0.087692903 -2.89
0 2 500 3400 0.154690628 0.016911309 0.151238040 2.23
0 2 500 4200 0.191293859 0.021756346 0.222997499 -16.57
0 2 500 5000 0.341429493 0.024730526 0.302418102 11.43
0 2 500 5800 0.445322020 0.028108237 0.406126186 8.80
0 2 500 6600 0.572985025 0.032379032 0.566653180 1.11
0 2 500 7400 0.800505203 0.040641036 0.823664328 -2.89
0 2 500 8200 1.202753254 0.047675048 1.221803361 -1.58
0 2 500 9000 1.863773342 0.057308585 1.823347301 2.17
0 2 500 9800 2.674241792 0.064135498 2.725822072 -1.93
0 2 500 10600 4.074604509 0.072869214 4.063999243 0.26
0 2 500 11400 5.927489705 0.088466156 5.986923291 -1.00
0 2 500 12200 8.526938930 0.094393058 8.626811134 -1.17
0 2 500 13000 11.841828537 0.117267289 12.094302076 -2.13
0 2 500 13800 16.316459237 0.126887935 16.526007803 -1.28
0 2 500 14600 22.686452684 0.156920289 22.180790729 2.23
0 2 500 15400 29.139113442 0.177863541 29.553668923 -1.42
0 2 500 16200 38.176244808 0.210063880 39.471019093 -3.39
0 2 550 200 0.000524256 0.000789975 0.000450613 14.05
0 2 550 1000 0.009989484 0.004023938 0.010598888 -6.10
0 2 550 1800 0.047647965 0.007689852 0.034932059 26.69
0 2 550 2600 0.084128936 0.010484055 0.075130168 10.70
0 2 550 3400 0.142250688 0.013799372 0.129354817 9.07
0 2 550 4200 0.187313919 0.019668344 0.195467426 -4.35
0 2 550 5000 0.273221619 0.019931202 0.280121225 -2.53
0 2 550 5800 0.432753314 0.026547749 0.403665495 6.72
0 2 550 6600 0.550393599 0.032938022 0.595605010 -8.21
0 2 550 7400 0.881200647 0.042165982 0.887669829 -0.73
0 2 550 8200 1.287148590 0.047760237 1.316690776 -2.30
0 2 550 9000 1.919797230 0.048695977 1.939666133 -1.03
0 2 550 9800 2.848155651 0.058190080 2.847956428 0.01
0 2 550 10600 4.256693702 0.069977387 4.163857315 2.18
0 2 550 11400 6.090602917 0.078747381 6.017621360 1.20
0 2 550 12200 8.485768835 0.084865710 8.524326678 -0.45
0 2 550 13000 11.764861414 0.104751665 11.788267391 -0.20
0 2 550 13800 15.819441508 0.119287019 15.949309499 -0.82
0 2 550 14600 21.549631477 0.147667045 21.261054427 1.34
0 2 550 15400 27.811643332 0.175073363 28.173664618 -1.30
0 2 600 200 0.001317242 0.000688871 0.000402631 69.43
0 2 600 1000 0.007380858 0.003320728 0.009534917 -29.18
0 2 600 1800 0.022530960 0.006078885 0.031421900 -39.46
0 2 600 2600 0.075268847 0.008833125 0.067678319 10.08
0 2 600 3400 0.117220983 0.012304246 0.117941317 -0.61
0 2 600 4200 0.191208424 0.016126132 0.183363122 4.10
0 2 600 5000 0.290158057 0.021414461 0.273942213 5.59
0 2 600 5800 0.424703115 0.023476819 0.410975744 3.23
0 2 600 6600 0.648146751 0.028483947 0.621664223 4.09
0 2 600 7400 0.944217841 0.033915390 0.933729707 1.11
0 2 600 8200 1.376184703 0.041837081 1.380309759 -0.30
0 2 600 9000 2.013695462 0.041535706 2.014705354 -0.05
0 2 600 9800 2.840322215 0.056095601 2.921656330 -2.86
0 2 600 10600 4.207831454 0.062029885 4.211692408 -0.09
0 2 600 11400 6.014023185 0.075262082 6.000299594 0.23
0 2 600 12200 8.409127730 0.088100517 8.390851365 0.22
0 2 600 13000 11.551434573 0.095721272 11.483421621 0.59
0 2 600 13800 15.650537303 0.117880569 15.417247284 1.49
0 2 600 14600 20.508813193 0.133904962 20.434363136 0.36
0 2 600 15400 26.760511351 0.166325967 26.941325580 -0.68
0 2 650 200 0.000891222 0.000715999 0.000365530 58.99
0 2 650 1000 0.007263706 0.002932551 0.008747356 -20.43
0 2 650 1800 0.031628258 0.005923474 0.029037304 8.19
0 2 650 2600 0.053511533 0.008412175 0.063144710 -18.00
0 2 650 3400 0.099628468 0.011955819 0.111956305 -12.37
0 2 650 4200 0.163439880 0.016912168 0.178664803 -9.32
0 2 650 5000 0.274561740 0.018965881 0.274794641 -0.08
0 2 650 5800 0.379848072 0.022763792 0.421439374 -10.95
0 2 650 6600 0.617997174 0.025920899 0.643988118 -4.21
0 2 650 7400 0.941493709 0.034947769 0.967971848 -2.81
0 2 650 8200 1.365210905 0.036193439 1.424593185 -4.35
0 2 650 9000 2.052648907 0.041522067 2.064193854 -0.56
0 2 650 9800 2.931701028 0.056861219 2.965212155 -1.14
0 2 650 10600 4.237817151 0.061351883 4.227837950 0.24
0 2 650 11400 6.068462031 0.071381053 5.955854664 1.86
0 2 650 12200 8.114745632 0.071478739 8.244060170 -1.59
0 2 650 13000 11.189040209 0.082948574 11.189006240 0.00
0 2 650 13800 14.851839778 0.101882978 14.926867684 -0.51
0 2 700 200 -0.000767211 0.000607374 0.000337379 143.97
0 2 700 1000 0.011677267 0.002754418 0.008172080 30.02
0 2 700 1800 0.026838017 0.005189647 0.027409791 -2.13
0 2 700 2600 0.069581384 0.007636675 0.060353121 13.26
0 2 700 3400 0.111101592 0.010258836 0.108909216 1.97
0 2 700 4200 0.167676130 0.013608987 0.177598876 -5.92
0 2 700 5000 0.300240981 0.017433412 0.278585294 7.21
0 2 700 5800 0.472716683 0.018342821 0.432305541 8.55
0 2 700 6600 0.680023834 0.024237389 0.662683542 2.55
0 2 700 7400 1.023591843 0.031105876 0.993929578 2.90
0 2 700 8200 1.421302377 0.037577976 1.456069929 -2.45
0 2 700 9000 2.106963255 0.045144578 2.096890423 0.48
0 2 700 9800 3.039161269 0.047517425 2.989098640 1.65
0 2 700 10600 4.173229934 0.058424862 4.224007736 -1.22
0 2 700 11400 5.838007587 0.064849613 5.895976078 -0.99
0 2 700 12200 7.982435911 0.078707909 8.093129436 -1.39
0 2 700 13000 10.990428899 0.082413296 10.908694875 0.74
0 2 700 13800 14.652227661 0.108879149 14.474382464 1.21
0 2 250 15030 34.846786255 0.397025522 35.126001629 -0.80
0 2 250 15040 34.896124291 0.358407321 35.286360731 -1.12
0 2 250 15050 34.809381577 0.360412233 35.447016784 -1.83
0 2 250 15060 35.423388506 0.331068386 35.607970540 -0.52
0 2 250 15800 48.723264021 0.363119472 48.562149178 0.33
0 2 250 15900 50.234326072 0.460788181 50.527578853 -0.58
0 2 250 15100 36.156092491 0.363010961 36.254797589 -0.27
0 2 250 15150 36.551798781 0.354417977 37.070266432 -1.42
0 2 250 15350 40.654601628 0.322055396 40.415307517 0.59
0 2 275 14440 25.752752284 0.257695743 25.952430361 -0.78
0 2 275 14450 25.485351957 0.255923443 26.078141532 -2.33
0 2 275 14460 25.693313937 0.298575042 26.204130141 -1.99
0 2 275 14470 26.069590048 0.254251172 26.330395570 -1.00
0 2 275 14480 26.187097071 0.245497860 26.456939556 -1.03
0 2 275 14520 27.344627948 0.252389293 26.965897228 1.39
0 2 275 14560 27.461616095 0.258374741 27.479321613 -0.06
0 2 275 14600 28.154907157 0.307971444 27.997238504 0.56
0 2 275 14875 31.617179075 0.268322296 31.683261412 -0.21
0 2 300 13830 19.036708896 0.210205146 19.009293409 0.14
0 2 300 13840 19.070599651 0.225226402 19.106374152 -0.19
0 2 300 13850 19.056420268 0.211121384 19.203721605 -0.77
0 2 300 13860 19.475807178 0.232869753 19.301334989 0.90
0 2 300 13870 19.183616530 0.224138783 19.399214132 -1.12
0 2 300 13880 19.386565036 0.223394553 19.497358264 -0.57
0 2 300 13890 19.361047607 0.225380036 19.595768435 -1.21
0 2 300 13935 20.179111297 0.217680509 20.041894604 0.68
0 2 300 13985 20.641014075 0.212989424 20.543877258 0.47
0 2 300 14020 20.748539808 0.237148449 20.899198296 -0.73
0 2 300 14370 24.824045918 0.246446252 24.631284644 0.78
0 2 325 13170 13.858097743 0.161852928 13.572069001 2.06
0 2 325 13180 14.205418003 0.171671612 13.644901835 3.95
0 2 325 13190 13.973515576 0.178455762 13.717979259 1.83
0 2 325 13200 13.851618203 0.184316737 13.791300781 0.44
0 2 325 13210 13.383694727 0.190052972 13.864865903 -3.60
0 2 325 13220 14.089543303 0.166383469 13.938675481 1.07
0 2 325 13270 14.170391444 0.198476672 14.311381272 -0.99
0 2 325 13310 14.822882048 0.189476463 14.613932355 1.41
0 2 325 13365 15.262155739 0.185535044 15.036301780 1.48
0 2 325 13450 15.683861867 0.181560617 15.703523917 -0.13
0 2 325 13500 16.411842044 0.177639214 16.104207292 1.87
0 2 325 13850 19.329749848 0.212466890 19.079083553 1.30
0 2 350 12480 9.506077433 0.136736446 9.527264899 -0.22
0 2 350 12520 9.804690817 0.144867250 9.741166004 0.65
0 2 350 12560 9.789283960 0.158214932 9.958432941 -1.73
0 2 350 12600 10.289228222 0.148936227 10.179077509 1.07
0 2 350 12630 10.488517316 0.155256513 10.346784040 1.35
0 2 350 12660 10.475706407 0.147485875 10.516400989 -0.39
0 2 350 12690 10.529559991 0.156306578 10.687932441 -1.50
0 2 350 12725 10.945682653 0.149792411 10.890477374 0.50
0 2 350 12770 11.121735007 0.154368911 11.154738299 -0.30
0 2 350 12800 11.368544116 0.155744886 11.333320954 0.31
0 2 350 13100 13.286940643 0.144424937 13.225785769 0.46
0 2 375 11750 6.361076341 0.117227428 6.538718334 -2.79
0 2 375 11780 6.852003159 0.120937485 6.651734192 2.92
0 2 375 11785 6.841116466 0.106621407 6.670717987 2.49
0 2 375 11900 7.200209496 0.122213315 7.119122195 1.13
0 2 375 11950 7.526872574 0.149418011 7.321202313 2.73
0 2 375 11980 7.336724281 0.118481146 7.444548232 -1.47
0 2 375 12030 7.652274076 0.137609556 7.653648667 -0.02
0 2 375 12080 7.857557568 0.135753874 7.867186415 -0.12
0 2 375 12300 8.738608551 0.130130651 8.860359060 -1.39
0 2 375 12750 11.429770348 0.140810250 11.172349915 2.25
0 2 400 10850 4.090639075 0.102541013 4.079264385 0.28
0 2 400 10950 4.036279952 0.103226051 4.323476963 -7.12
0 2 400 11050 4.586135515 0.093404661 4.580179262 0.13
0 2 400 11150 4.951190885 0.108391034 4.849790817 2.05
0 2 400 11250 5.122417056 0.104393292 5.132721926 -0.20
0 2 400 11350 5.396892536 0.113073434 5.429371343 -0.60
0 2 425 9700 2.223815472 0.073241621 2.235453260 -0.52
0 2 425 9750 2.326637651 0.081289854 2.300568385 1.12
0 2 425 9800 2.377705820 0.081647793 2.367522740 0.43
0 2 425 9900 2.479352734 0.082167319 2.507119253 -1.12
0 2 425 10000 2.714503860 0.083253858 2.654589300 2.21
0 2 425 10100 2.787714100 0.077524047 2.810289635 -0.81
0 2 450 8000 0.955181830 0.049004887 0.968527487 -1.40
0 2 450 8100 0.980080350 0.053992142 1.018441146 -3.91
0 2 450 8200 1.022221800 0.055638840 1.071624312 -4.83
0 2 450 8600 1.392447945 0.072631252 1.320222181 5.19
0 2 450 8900 1.496505248 0.068643752 1.549323877 -3.53
0 2 450 9200 1.745962785 0.069516887 1.821205746 -4.31
0 2 450 9500 2.196055861 0.071006207 2.142499629 2.44
0 2 450 9800 2.498279921 0.069732336 2.520805481 -0.90
0 2 450 10100 2.825864336 0.057216644 2.964580906 -4.91
0 2 450 10400 3.557203965 0.077221058 3.482914894 2.09
0 2 225 15600 47.846591514 0.396744073 47.197883829 1.36
0 2 225 15700 48.804514799 0.452545773 49.252359249 -0.92
0 2 225 15800 51.213891148 0.479686698 51.350993086 -0.27
0 2 225 15900 54.207281567 0.466505407 53.501533729 1.30
0 2 225 16100 58.589259263 0.440866249 57.996111916 1.01
0 2 225 16300 63.248307144 0.538973956 62.825876326 0.67
0 2 225 16500 67.932150471 0.497423681 68.104255339 -0.25
0 2 200 16200 64.258036669 0.586287157 64.453393997 -0.30
0 2 200 16300 68.063830279 0.617035500 67.162812176 1.32
0 2 200 16400 70.012124167 0.525943610 69.965564506 0.07
0 2 200 16500 72.645727514 0.602586825 72.881745051 -0.32
0 2 200 16600 75.319516889 0.608795410 75.933822813 -0.82
0 2 200 16700 79.301107137 0.628962151 79.146677167 0.19
0 2 200 16800 82.027637884 0.688368037 82.547625156 -0.63
0 2 175 16800 89.574867059 0.885531155 88.974059546 0.67
0 2 175 16850 91.522942971 0.847646217 90.925295695 0.65
0 2 175 16900 93.568163952 0.763151531 92.932294321 0.68
0 2 175 16950 95.313607257 0.871212782 95.000600471 0.33
0 2 175 17000 95.058069792 1.117500983 97.136001285 -2.19
0 2 175 17050 100.701603837 1.003070774 99.344546576 1.35
0 2 175 17100 101.487836400 1.068677535 101.632527814 -0.14
0 2 150 17400 126.803392585 1.598534413 127.359119421 -0.44
0 2 150 17450 127.804251700 1.659894253 130.828109899 -2.37
0 2 150 17500 132.179265164 1.903456951 134.454351788 -1.72
0 2 150 17550 137.370803366 1.660055177 138.250695167 -0.64
0 2 150 17600 132.251950006 2.045181307 142.230406307 -7.55
 from simulation from FEOS
Temp. Sat. Vap. Dens. Stat. Uncert. Sat. Liq. Dens. Stat. Uncert. Press. Stat. Uncert. Ent. of Vap. Stat. Uncert. Sat. Vap. Dens. Sat. Liq. Dens. Press. Ent. of Vap.
-3 -3 -3 -3 -1 -1 -3 -3
(K) (mol ∙ m ) (mol ∙ m ) (mol ∙ m ) (mol ∙ m ) (Pa) (Pa) (J ∙ mol ) (J ∙ mol ) (mol ∙ m ) (mol ∙ m ) (Pa) (J ∙ mol-1)
250 12.099957 0.484403 15011.02616 1.700357 24897.302 996.725 26963.23069 3.96330587 11.52640872 15003.31856 23731.55708 26992.53356
260 17.705561 0.567295 14776.90373 1.800543 37758.41 1209.799 26433.75236 4.295067256 18.36867633 14771.67367 39161.02094 26462.39762
270 26.369287 0.581293 14543.00425 1.400852 58120.183 1281.219 25903.0735 3.55249725 28.09458391 14537.05969 61851.19134 25925.92069
275 33.371263 0.736066 14423.32611 1.901175 74624.273 1645.979 25629.05501 4.160377371 34.27358748 14418.47457 76595.51655 25654.26623
280 42.961201 0.86202 14300.37634 1.801786 97298.95 1952.311 25334.97015 4.004943851 41.46650233 14298.94482 94004.90761 25379.77133
290 59.375556 1.073815 14061.06418 1.904342 138205.943 2499.474 24790.239 3.976936176 59.3381807 14056.75363 138122.3511 24820.52818
300 84.590453 3.233996 13808.38288 1.955887 201354.008 7698.009 24227.76173 4.18986067 82.65793928 13809.84506 196973.4927 24244.62617
310 108.75562 2.5217 13553.54789 2.431967 265054.854 6145.787 23651.41602 5.199481826 112.4777335 13557.48633 273567.1164 23648.28512
320 153.705079 2.954904 13292.84907 2.172062 379664.539 7298.862 22996.81319 5.043338476 149.9700908 13298.821 371119.7321 23027.41605
325 170.152804 2.759142 13165.22063 2.15625 424629.999 6885.661 22708.6034 4.822965524 171.9993171 13166.81224 428810.5174 22706.39178
330 192.960774 2.74603 13026.09474 2.75584 485051.122 6902.776 22376.94831 5.947397003 196.4554083 13032.82877 493027.0646 22377.49834
340 257.165187 2.893544 12753.56285 2.599472 651377.769 7329.103 21667.11754 5.527430024 253.4432015 12758.27355 642840.177 21693.41756
350 328.816843 2.39168 12468.31228 3.671 837594.186 6092.32 20929.06193 7.880231058 322.6929946 12473.63478 824247.811 20969.24735
360 405.493139 2.563736 12168.21192 2.910976 1038945.629 6568.749 20176.47038 6.739635852 406.3043499 12177.01392 1041066.33 20197.94804
370 505.417288 2.2575 11850.78681 3.659257 1294447.439 5781.787 19342.50153 9.043757857 506.8525303 11866.00364 1297238.891 19370.93642
375 566.953131 2.552481 11691.68748 4.226281 1444920.215 6505.179 18894.29152 10.3458264 564.462407 11704.16616 1441352.236 18933.28333
380 627.09362 2.838732 11521.82048 4.677156 1594482.824 7217.918 18440.20708 11.45814383 627.5996541 11537.49846 1596846.42 18477.44716
390 773.859423 2.825178 11170.65464 5.504753 1946513.374 7106.261 17461.32189 13.77550559 772.8381845 11187.41025 1944135.251 17503.54035
400 959.904554 2.823261 10798.83056 6.575785 2359446.245 6939.578 16362.92912 18.22524274 948.482054 10810.21913 2343571.312 16430.47081
410 1172.739474 3.692777 10383.25594 8.150123 2810076.826 8848.501 15169.50638 24.13145487 1163.158726 10398.21716 2799941.986 15231.8156
420 1448.01003 5.016965 9922.078511 12.579339 3339616.996 11570.873 13784.48706 33.55742505 1430.418522 9940.113638 3318553.517 13867.93458
425 1597.251417 4.362228 9665.913014 10.844097 3615550.416 9874.373 13058.11061 34.99591881 1590.466106 9688.608505 3603092.24 13105.34121
430 1771.521698 6.610398 9403.888543 17.529346 3904728.847 14570.417 12262.55825 51.69438435 1773.775019 9418.09928 3905640.355 12273.92007
440 2234.161288 7.428685 8644.104725 28.668855 4568198.505 15189.463 10177.87967 74.68561986 2240.281894 8800.334252 4569296.354 10328.66527

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