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journal homepage: www.elsevier.com/locate/fluid

Ilya Polishuk ∗

Department of Chemical Engineering & Biotechnology, Ariel University Center of Samaria, 40700 Ariel, Israel

a r t i c l e i n f o a b s t r a c t

Article history: This study demonstrates that SAFT EOS models might exhibit the practically unrealistic and even non-

Received 30 May 2010 physical predictions due to the two factors, namely the temperature dependencies of a segment packing

Received in revised form 3 July 2010 fraction and the very high-polynomial orders by volume. The ﬁrst factor is responsible for predicting

Accepted 5 July 2010

the negative values of the heat capacities at very high pressures and the intersections of isotherms at

Available online 13 July 2010

high densities. The very high-polynomial orders of several SAFT EOS models result in prediction of the

additional stable unrealistic critical points and the pertinent ﬁctive phase equilibria. It is demonstrated

Keywords:

that the unrealistic phase splits might present the globally stable states established by the models, while

Equation of state

Statistical association ﬂuid theory

the VLE matching the experimental data might be in fact metastable. In addition, the excessive complexity

Phase equilibria of certain SAFT models might result in wrong prediction of auxiliary thermodynamic properties of the

Global stability experimentally available ﬂuid phases. The undesired predictions discussed in the present study arise

queries regarding the robustness and the over-all physical validity of the models under consideration in

their present forms. This study discusses the ways of removing the numerical pitfalls.

© 2010 Elsevier B.V. All rights reserved.

1. Introduction compounds. However the reasons of this behavior have not been

investigated with great details.

The EOS models based on the Statistical Association Fluid The- The comprehensive studies of Yelash et al. [12,13] have demon-

ory (SAFT) are among the most important approaches for modeling strated that the predictions of PC-SAFT [14] are affected by crossing

thermodynamic properties of pure substances and their mix- of isotherms, attributed to the temperature dependence of hard-

tures. The comprehensive reviews of different SAFT EOS models sphere diameter, and by appearance of practically unrealistic phase

are available elsewhere [1–5]. Based on the advanced molecular equilibria, attributed to the polynomial expression of the dispersion

approaches, the SAFT EOS models are expected to be robust and term. It has been concluded that the unrealistic phase behavior can

reliable in the entire thermodynamic phase space. However, thus be a problem when the model is applied to polymer solutions and

far several studies have reported some worrying results. polymer blends. The predictions of the excessive phase equilibria

In particular, Koak et al. [6] have investigated the effect of the for large variety of pure compounds exhibited by PC-SAFT have

Chen–Kreglewski (CK) [7] dispersion term on the pressure–volume been recently discussed in great details by Privat et al. [15].

behavior of two non-associating pure components predicted by the The aim of the present study was detection and investigation of

CK-SAFT of Huang and Radosz [8]. It has been demonstrated the P–v the numerical pitfalls exhibited by several popular SAFT EOS mod-

isotherms exhibit multiple volume roots at low temperatures and els necessary for further development of their consistent versions.

volumes, while the smallest practically unrealistic root is more sta-

ble than the realistic ones. It has been concluded that this behavior 2. Theory

appears to be inconsistent with the intention of the original theories

and it needs to be resolved (see also [9]). The SAFT EOS models treat the compressibility factor as a

In the paper discussing the numerical pitfalls introduced by the combination of terms representing different inter-molecular inter-

Soave-type ␣-functions in Cubic Equations of State [10] it has been actions:

demonstrated that the theoretically based models such as the SAFT

version of Huang and Radosz [8] and Johnson–Zollweg–Gubbins Z = Z repulsive + Z attractive + Z associative (1)

approach for the Lennard–Jones ﬂuids [11] exhibit the practically In most of the cases the ﬁrst two terms are the polynomial expres-

unrealistic predictions, namely the multiple critical points for pure sions by volume, which makes their general analytical investigation

relatively easy. The associative term includes logarithmical expres-

sions for the volume, which substantially hinders its analytical

∗ Tel.: +972 3 9066346; fax: +972 3 9066323. investigation. Hence the question of an over-all consistence of this

E-mail addresses: polishuk@ariel.ac.il, polishyk@bgumail.bgu.ac.il. term has been left outside the scope of the present study and it

0378-3812/$ – see front matter © 2010 Elsevier B.V. All rights reserved.

doi:10.1016/j.ﬂuid.2010.07.003

Author's personal copy

Table 1

Phenomena of the multiple critical points generated by the non-associative SAFT

EOS models considered in the present study.

by volume phenomena

SSAFT [19] m = 1 5 No

SSAFT [19] m =/ 1 6 No

Original SAFT [21] m = 1 8 No

Original SAFT [21] m =/ 1 9 No

CK-SAFT [8] m = 1 13 Yes

CK-SAFT [8] m = / 1 14 Yes

Simpliﬁed PC-SAFT [24] m = 1 19 Yes

Simpliﬁed PC-SAFT [24] m =/ 1 24 Yes

Soft-SAFT [25] m = 1 Non-applicable, Yes

exponential

expression

Soft-SAFT [25] m =

/ 1 Non-applicable, Yes

exponential

expression

Fig. 3. CV of ethane predicted by SSAFT [19]: 100 bar, solid line; 9000 bar, dashed

line; and 䊉, experimental data [20].

= 0.74048 and C = 0.12. The numerator of Eq. (2) is the model’s

covolume, or the volume at the inﬁnite pressure. It can be seen that

Eq. (2) results in decrease of covolume with temperature. In other

words, as the temperature rises, the inﬁnite pressure is approached

at the smaller values of volume. As a result, at high-pressures

volume will decrease with temperature and the isotherms will

Fig. 1. Intersection of isotherms predicted by SSAFT [19] for ethane; ,, and ,

experimental data [20].

priate approaches for its general analysis.

The numerical pitfalls of the repulsive term are generated by the

temperature dependence of the reduced density . For example,

according to CK-SAFT of Huang and Radosz [8] it is given as:

3

V oo (1 − C exp[−3(uo /k)/T ]) Fig. 4. Intersection of isotherms predicted by SAFT of Chapman et al. [21] for ethane;

= (2)

V ,, and , experimental data [20].

Fig. 2. Lines of zero CV predicted by several versions of SAFT for ethane. Fig. 5. The 120 K isotherm of nitrogen predicted by CK-SAFT [8].

Author's personal copy

Table 2

Critical points predicted by CK-SAFT [8] for several pure compounds.

Argon 151.56 50.28 191.74 34125.4

Methane 192.17 48.15 242.85 32643.7

Carbon monoxide 136.45 39.16 146.75 26131.9

Ethane 320.61 60.24 254.59 46646.7

Carbon dioxide 320.71 92.50 311.20 63525.7

Water 725.95 422.88 682.38 166350.8

Fig. 6. The 120 K isotherm of nitrogen predicted by CK-SAFT [8] at high densities.

has been proven that any temperature dependency of the covol-

ume necessarily results in inﬁnite negative value of the isochoric

heat capacity at the inﬁnite pressure. It should be pointed out

that although CV < 0 is mathematically possible, it cannot actually

occur, since the mechanical stability limit will be violated before

Fig. 7. Two vapor pressure curves of pure nitrogen predicted by CK-SAFT [8]; 䊉, the thermal limit. This is because the mechanical limit represents

experimental data [23]. a response of higher-order than the thermal limit [17,18]. Con-

sidering a fact that the models with the temperature-dependent

intersect in contradiction with experimental facts. The same effect covolumes exhibit the negative CV under conditions of mechanical

is characteristic for other expressions of covolume exhibiting sim- stability, such predictions should be considered as non-physical.

ilar behavior. The latter phenomena might affect different models with the

Another serious drawback of the temperature-dependent covol- different degree of extend. While some models, such as the CK-

umes is the description of the caloric properties at high pressures, SAFT of Huang and Radosz [8], exhibit the negative isochoric heat

capacities at the extremely high pressures (the reason will be dis-

Fig. 8. Two-phase envelopes of pure nitrogen predicted by CK-SAFT [8]; 䊉, experi- Fig. 10. Departure Gibbs energy – pressure projection of nitrogen generated by

mental data [21]. CK-SAFT [8] at 150 K.

Author's personal copy

Table 3

Critical points predicted by CK-SAFT [8] with D29 = 0.

Argon 149.74 47.32 17.1 45041.2

Methane 189.87 45.32 22.53 44798.2

Carbon monoxide 135.78 38.27 16.02 43542.4

Ethane 320.29 59.97 29.15 86343.5

Carbon dioxide 319.87 91.31 45.87 144762.0

Water 721.06 409.18 60.88 260270.1

[19] for ethane. Fig. 2 presents the zero values of CV predicted

by several versions of SAFT for ethane. It can be seen that SSAFT

starts to predict the non-physical negative values at the low-

est pressures, which are still very high (14,900 bars and above).

However it would not be surprising that these undesired phe-

Fig. 11. The minus departure Gibbs energy – pressure projection of nitrogen gen- nomena have an impact on modeling the experimentally available

erated by CK-SAFT [8] at 120 K. caloric data. In particular, Fig. 3 demonstrates that SSAFT substan-

tially underestimates the experimental CV data at 9000 bar, which

cussed below), irrelevant for most practical implementations, the should be explained by the behavior of the model at higher pres-

other ones might yield the non-physical predictions at much lower sures.

pressures [16].

The attractive terms of SAFT EOS models typically present poly- 3.2. SAFT of Chapman et al. [21]

nomials adjusted to the theoretical expressions, whose analytical

calculation is not always possible. As the polynomial order becomes Although this model has a relatively high-polynomial order (see

higher, the EOS models yield more solutions for the volume. The Table 1), the additional practically unrealistic solutions for the vol-

complex solutions and the solutions smaller than the covolume ume have not been detected. However the model is still affected by

should be considered as the “numerical noise” having no impact the temperature-dependent covolume. Fig. 4 depicts the intersec-

on the performance of the model. However, if the polynomial tion of isotherms predicted for ethane and Fig. 2 presents the zero

order and, consequently, the number of the solutions increases, values of CV .

the additional practically improbable real solutions bigger than

the covolume appear. Table 1 lists several popular SAFT EOS mod- 3.3. CK-SAFT of Huang and Radosz [8]

els, their polynomial order (when applicable) and appearance of

unrealistic volume solutions. In what follows let us consider the The polynomial order of this model is higher than in the previ-

particular models. ously considered cases (see Table 1) and analysis shows that it may

exhibit up to ﬁve real solutions for molar volume bigger than the

covolume. These multiple real solutions are not only excessive on

3. Results

the thermodynamic phase scene, but might also be dangerous like

the famous Chekhov’s gun (“If in Act I you have a pistol hanging on

3.1. Simpliﬁed SAFT (SSAFT) of Fu and Sandler [19]

the wall, then it must ﬁre in the last act” [22]).

Fig. 5 depicts the isotherm predicted by the Huang and Radosz’s

This model has the lowest polynomial order among the SAFT

version of CK-SAFT [8] for nitrogen at 120 K. The points A, B and C

models (see Table 1) and it does not exhibit the additional practi-

represent the realistic phase envelope matching the experimen-

cally unrealistic solutions for the volume. However the temperature

tal data (A is the vapor and C is the liquid solution), and the

dependence attached to its covolume still affects its robustness.

extrema ˛ and ˇ represent the spinodal. At the volumes lower that

C the isotherm should approach the inﬁnite pressure. However, as

Fig. 12. Two vapor pressure curves of pure ethane predicted by CK-SAFT [8]; , Fig. 13. Two-phase envelopes of pure ethane predicted by CK-SAFT [8]; , experi-

experimental data [20]. mental data [20].

Author's personal copy

Fig. 15. Globally stable phase diagram of methane predicted by SOFT-SAFT [25]; ,

experimental data [26].

pure compounds. Table 2 lists these critical points for certain pure

compounds.

Fig. 9 depicts the isotherm at 150 K of nitrogen. It can be seen

that this time it takes a conventional form (three solutions and

two extrema), although in total disagreement with experimental

facts. Fig. 10 presents the excess Gibbs energy – pressure projec-

tion for this isotherm. It can be seen that the stable, the metastable

(A = E − and A = E − ı) and the unstable (ı − D − ) parts exhibit

a robust behavior characteristic for phase equilibria in pure com-

pounds. Thus, there are no doubts regarding the stability of VLE-2

above the critical point 1.

However at the coexisting of two-phase equilibria the picture

Fig. 14. Departure Gibbs energy – pressure projection of ethane generated by CK-

SAFT [8]. becomes complicated (see Fig. 11; −G is used for creating the

logarithmic scale). Three facts can be observed:

noticed, SAFT exhibits ﬁve real solutions bigger than its covolume. 1. The VLE-2 take place at the conditions closer to the ideal gas state

It can be seen that the two excessive solutions (E and D) deform and, therefore, at the GE closer to zero than the VLE-1.

the thermodynamic phase space established by the model. As a 2. There are no phase equilibria between the liquid phases.

result, two practically unrealistic extrema and ı appear (addi- 3. The liquid-2 (solution E) is more stable than the liquid-1 (solu-

tional details are shown in Fig. 6). Thus, two spinodal loci and tion C) and the VLE-1 at the pertinent pressure.

two-phase equilibria are generated simultaneously: the saturation

pressure 1 in the vicinity of experimental datum and the unrealistic The interpretation of Fig. 11 is not trivial because the prac-

saturation pressure 2 located at the deep vacuum. tically unrealistic phase behavior generated by the model under

Figs. 7 and 8 depict two vapor pressure lines and two-phase consideration cannot be explained by experimental facts. Let us

envelopes predicted by the CK-SAFT [8] for nitrogen. As discussed consider nitrogen at some point along VLE-1. As noticed, at such

previously [10], the model exhibits at least two critical points for conditions the liquid-2 (solution E) presents the most stable phase.

Author's personal copy

Fig. 16. Thermodynamic properties of methane [26] at high pressures as predicted by SOFT-SAFT [25]; 䊉, 100 bar; , 200 bar; , 500 bar; , 1000 bar; , 2000 bar; , 5000 bar;

, 10,000 bar.

Thus, according to CK-SAFT [8], at the conditions of VLE-1 and in be seen that yet at least some part of the realistic phase equilibria

the varying-volume vessel nitrogen is supposed to shrink into this (VLE-1 above LLVE) is globally stable. An explanation is provided in

highly compressed liquid. However even the microscopic increase Fig. 14.

of the vessel’s volume should result in a drastic fall of pressure In particular, it can be seen that at the T > TLLVE both VLE-1 and

(see Figs. 5 and 6) until appearance of VLE-2 at the deep vacuum. LLE do not face other phases with lower G at the pertinent pres-

Thus, the realistic VLE-1 is actually metastable and the unrealistic sures, and therefore both are globally stable. However, at T < TLLVE

VLE-2 represents the globally stable phase diagram established by the situation gets different. Yet vapor has lower G than LLE and

CK-SAFT [8]. liquid-2 has lower G than VLE-1. Thus, only the unrealistic VLE-

Table 2 shows that for some compounds CK-SAFT [8] gener- 2 is now globally stable. Remarkably, similar behavior has been

ates the realistic critical points at the temperatures higher than described by Privat et al. [15] for PC-SAFT. However it should be

the unrealistic ones. Figs. 12 and 13 depict the globally stable parts noticed that in the present case the numerical pitfalls signiﬁcantly

of the ethane’s phase diagram as predicted by CK-SAFT [8]. It can affect the accuracy of the model.

Author's personal copy

An artiﬁcial attempt of decreasing the polynomial order of CK- The very high-polynomial orders of several SAFT EOS mod-

SAFT [8] by considering the zero value for D29 might improve the els result in prediction of the additional stable unrealistic critical

situation (see Table 3). Remarkably, this practice does not affect the points and the pertinent ﬁctive phase equilibria. It is demonstrated

CK dispersion term radically. that the unrealistic phase splits might present the globally sta-

Finally, it should be pointed out that CK-SAFT [8] unavoidably ble states established by the models, while the VLE matching the

exhibits the numerical pitfalls characteristic for the previously con- experimental data might be in fact metastable. In addition, the

sidered simpler versions of SAFT. However since approaching the excessive complexity of certain SAFT models might result in non-

inﬁnity pressure at low temperatures is yet hindered by the unusual physical prediction of auxiliary thermodynamic properties of the

forms of its isotherms, CK-SAFT [8] generates the negative isochoric experimentally available ﬂuid phases. Thus, some SAFT EOS models

heat capacities at much higher pressures (see Fig. 2). should be re-evaluated while using fewer coefﬁcients. Investiga-

tion of the maximal equation orders free of the numerical pitfalls

3.4. PC-SAFT [14] is essential for further progress of SAFT.

In addition, it seems highly recommendable to make the seg-

The case of PC-SAFT [14] has been already investigated with ment packing fraction of SAFT models temperature-independent.

great details in the previous studies [12,13,15]. It should only be It could be argued that the temperature-dependent covolumes

noticed that the rescaled simpliﬁed PC-SAFT [24] does not exhibit result in numerical pitfalls outside the range of the model’s appli-

an improvement in comparison with the original version. Never- cability (extremely high pressures). However the very concept of

theless the fact that PC-SAFT, in spite of its very high-polynomial the model’s applicability is characteristic for empirical correlations

order, typically generates the unrealistic phase equilibria at rela- rather than theoretically based approaches. The latter ones are sup-

tively low temperatures [15] should not be neglected. Hence, the posed to be robust and reliable in the entire thermodynamic phase

undesired predictions yielded by PC-SAFT [14] are not expected to space. Moreover, it does not seem possible to cancel the numeri-

affect most of its practical implementations. One might anticipate cal contribution of the repulsive term to the residual isochoric heat

for problems just in certain cases [12,13]. In addition, the unre- capacity at high pressures by other model’s terms.

alistic phase equilibria could interrupt the high-pressure LLE in

asymmetric mixtures at high pressures. Moreover, the probability List of symbols

of numerical problems might increase with increasing the number C integration constant of CK-SAFT [8]

of compounds in a mixture. CV isochoric heat capacity

k Boltzmann’s constant

3.5. Soft-SAFT [25] P pressure

R universal gas constant

The Soft-SAFT [25] EOS is based on the T temperature

Johnson–Zollweg–Gubbins approach for the Lennard–Jones ﬂuids uo /k temperature-independent dispersion energy of interac-

[11]. The latter approach typically exhibits the additional artiﬁcial tion between segments

phase equilibria at the temperatures higher than CK-SAFT [8] (see V molar volume

for example [10]). The same could be concluded regarding the Voo temperature-independent segment volume of CK-SAFT

Soft-SAFT [25]. For example, for methane it predicts: Tc1 = 193.27 K, [8]

Pc1 = 50.97 bar, Tc2 = 320.64 K and Pc2 = 24371.8 bar. Fig. 15 depicts W speed of sound

the globally stable phase equilibria yielded by Soft-SAFT [25] for Z compressibility factor

methane. A total disagreement with the experimental facts is

evident. Greek letters

Fig. 16 demonstrates that Soft-SAFT [25] could be an incredi- reduced density

bly accurate model for describing the high-pressure densities, heat segment molar volume in a closed-packed arrangement

capacities and sound velocities. However it can be seen that the sig-

niﬁcant part of the Soft-SAFT’s [25] ﬂuid phase diagram is actually Subscripts

metastable because the artiﬁcial high-pressure phase split takes c critical state

place above the compound’s solidiﬁcation temperatures. In addi- r reduced property

tion, it predicts the negative values for the heat capacities and, as a

consequence, wrong results for the sound velocities below 100 K. It Abbreviations

would be tempting to ﬁnd a relation these two facts [17,18]. How- EOS equation of state

ever it can be seen (Fig. 16a) that Soft-SAFT’s [25] still predicts the SAFT statistical association ﬂuid theory

mechanical stability at the experimentally available ﬂuid range.

Thus, the current non-physical results could rather be explained Acknowledgment

again by the excessive complexity of the model under considera-

tion. Acknowledgment is made to the Donors of the American Chem-

ical Society Petroleum Research Fund for support of this research,

4. Conclusions Grant No. PRF#47338-B6.

This study demonstrates that the SAFT EOS models might exhibit References

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to the two factors, namely the temperature dependencies of a seg- [1] Y.S. Wei, R.J. Sadus, AIChE J. 46 (2000) 169–196.

[2] E.A. Müller, K.E. Gubbins, Ind. Eng. Chem. Res. 40 (2001) 2193–2211.

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orders by volume. In particular, the ﬁrst factor is responsible for [4] S.P. Tan, H. Adidharma, M. Radosz, Ind. Eng. Chem. Res. 47 (2008) 8063–8082.

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experimentally available data as well. 1718–1722.

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[7] S.S. Chen, A. Kreglewski, Ber. Bunsen-Ges. Phys. Chem. 81 (1977) 1048–1052. [18] M. Modell, R.C. Reid, Thermodynamics and Its Applications, 2nd ed., Prentice-

[8] S.H. Huang, M. Radosz, Ind. Eng. Chem. Res. 29 (1990) 2284–2294. Hall, NJ, 1983.

[9] N. Aslam, A.K. Sunol, Ind. Eng. Chem. Res. 45 (2006) 3303–3310. [19] Y.-H. Fu, S.I. Sandler, Ind. Eng. Chem. Res. 34 (1995) 1897–1909.

[10] H. Segura, T. Kraska, A. Mejia, J. Wisniak, I. Polishuk, Ind. Eng. Chem. Res. 42 [20] D. Bücker, W.A. Wagner, J. Phys. Chem. Ref. Data 35 (2006) 205–266.

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