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Parks, G.S., Manchester, K.E., Thermochem. Bull. I.U.P.A.C.

ACKNOWLEDGMENT No. 2, 8 (1956).

The author thanks B.F. Dodge of Yale University, New Pilcher, G., Pell, AS., Coleman, D.J., Trans.Famday SOC.

60, 499 (1964).

Haven, Conn., and W.M.D. Bryant of E. I. du Pont de Rossini, F.D., et al., U. S. Natl. Bur. Standards Circ. 461,

Nemours and Co., Inc., Wilmington, Del., for their sugges- 1947.

tions. Zbid., No. 500 (1952).

LITERATURE CITED Rossini, F.D., et al., “Selected Values of Physical and Thermo-

dynamic Properties of Hydrocarbons and Related

Barr-David, F.H., Dodge, B.F., J. Chem. Eng. Data 4, 107 Compounds,”(and supplements), A.P.I. Research Project 44,

(1959). Carnegie Press, Pittsburgh, Pa., 1953.

Berman, N.S., McKetta, J.J., J . Phys. Chem. 66, 1444 (1962). Shiffler, W.H., Holm, M.M., Brooke, L.F., Znd. Eng. Chem.

Beynon, E.T., Jr., McKetta, J.J., Zbid., 67, 2761 (1963). 31, 1099 (1939).

Buckley, E., Herington, E.F.G., Trans. Faraday Soc 61, 1618 Smutny, E.J., Bondi, A.A., J . Phys. Chem. 65, 546 (1961).

(1965). Stanley, H.M., Youell, J.E., Dymock, J.B., J . SOC.Chem.

Cope, C.S., A.I.Ch.E.J. 10,277 (1964). Ind. (London)53,205T (1934).

Cope, C.S., Dodge, B.F., Zbid., 5,lO (1959). Taft, R.W., Jr., Riesz, P., J . Am. Chem. SOC. 77, 902 (1955).

Dodge, B.F., “Chemical Engineering Thermodynamics,”

Chap. 11, McGraw-Hill,New York, 1944.

Eberz, W.F., Lucas, H.J., J . Am. Chem. SOC. 56, 1230 (1934).

Green, J.H.S., Trans. Faraday SOC. 59,1559 (1963).

Green, J.H.S., Quart. Revs. (London) 15, 125 (1961). RECEIVED for review September 24, 1965. Accepted April 6, 1966.

Janz, G. J., “Estimation of Thermodynamic Properties of Material supplementary to this article has been deposited as Docu-

Organic Compounds,” Academic Press, New York, 1958. ment number 8959 with the AD1 Auxiliary Publications Project,

Majewski, F.M., Marek, L.F., Znd. Eng. Chem. 30, 203 (1938). Photoduplication Service, Library of Congress, Washington 25,

Nicolini, E., Laffitte, P., Compt. rend. 229, pp.757, 935 (1949). D. C. A copy may be secured by citing the Document number and

Parks, G.S., Huffman, H.M., “The Free Energies of Some by remitting $1.25 for photoprints, or $1.25 for 35 mm. microfilm.

Organic Compounds,” A.C.S. Monograph No. 60, p. 124, The Advance payment is required. Make checks or money orders payable

Chemical Catalog Co., Inc., New York, 1932. to: Chief, Photoduplication Service, Library of Congress.

Tetrafluoromethane

Thermodynamic Properties of the Real Gas

Petroleum Research Center, Bureau of Mines, U. S. Department of the Interior, Bartlesville, Okla.

were determined a s functions of temperatures (0’ to 350’ C.) a n d molal density (0.75

to 11.0 gram-moles per liter) over a pressure range of 0 to 400 atm. The analytical

a n d graphical correlating techniques described h a v e produced results that reflect all of

the inherent accuracy of the basic data used, and in this sense the w l u e s given are

useful a s comparison standards.

tetrafluoromethane were determined a t the Bureau of Mines

Many of the numerical calculations were performed on a

digital computer; however, a combination of analytical and

as part of a larger program (8, 9) to evaluate P-V-T and graphical correlational methods was adopted to ensure full

intermolecular potential energy relationships as well as utilization of the inherent accuracy and precision of the

chemical thermodynamic properties for hydrocarbons, experimental results.

fluorocarbons, and mixtures of hydrocarbons and fluoro- Briefly, the approach to the correlations was as follows:

carbons. First, the temperature-dependent slopes of the experimental

The quantities presented in this paper are the contribu- isometric lines (aPjdT),,which appear in the integrands for

tions that originated in the intermolecular phenomenon or enthalpy and entropy (Equations 1 and 2 ) , were evaluated

nonideality of the gas. Thus, to obtain thermodynamic by fitting analytical functions to them, differentiating the

properties for the total or real gas, one must add to the analytic functions with respect to temperature, and adding

present values the contributions for the ideal gas at the graphically determined residuals. The integrals that con-

same temperature and at 1-atm. pressure. Spectroscopically tained ( a P / a T ) were then evaluated graphically. Location

based values of the ideal gas have been reported by of the zero density intercepts of the integrals, which usually

Nagarajan (13)and by McBride and coauthors (12). presents a problem, was accurately placed by a method

I n addition to providing useful information for various based on independently derived values of the second virial

direct engineering applications, the present values will coefficients and their first derivatives with respect t o tem-

qualify, when required, as standards in the sense that they perature.

reflect faithfully all of the trends that appear in the experi- Recently, Chari (7) calculated thermodynamic properties

mental data from which they were derived. Because the for the saturated liquid and gas, and the superheated gas.

computations are based directly on unsmoothed experi- However, his calculations for the super-heated gas were

mental compressibility values (8) measured a t even tem- based on unpublished values of the P- V -T properties, and

peratures and densities, the introduction of spurious trends it seemed best, therefore, not to make a serious attempt

from arbitrary smoothing of the basic data was prevented. at comparing those results with the currently derived ones.

THERMODYNAMIC RELATIONS

For ease in evaluating thermodynamic properties from

isometric data, the functions given for the real gas ( I , 4 )

were converted into forms having density p , as the primary

variable; thus,

and

G-Go= sp

T O

mdp+P/p-RT+RTlnRTp

P

(3)

degree mark as in HO, So, or @ is for the ideal gas at 1 atm.

and is, therefore, a function only of temperature and sub-

stance. I t is identical to the standard state used by the

American Petroleum Institute Research Project 44 on

P- V-T Properties (6).

Experimental values of P , T , and p used in evaluating

the thermodynamic functions were taken from Table I (8).

Although the derived values of the functions are tabulated

a t even values of the Celsius temperature scale, t , "C., all

calculations were made with the thermodynamic tempera-

ture scale T @), since thermodynamic derivatives were

shown (IO) to have small but significant error when com-

puted on the Celsius scale. The most recent definition 0" C.

= 273.15"K. was not used because much of the correlational

work was already completed on the basis of the older

definition (15).The effect on the slope of the isometric lines

is very small, about 0.00670, and can, therefore, be neglected

for most purposes.

The slopes, (dP/d7'),, of the isometric lines appearing in

the integrands of the enthalpy and entropy functions were

derived from the data by a technique that utilizes the

isometric representation of Beattie and Bridgeman (3). The

isometric representation was adapted, previously, to our

correlation of the thermodynamic properties of perfluoro-

cyclobutane (9). Some variations, described below, were

necessary to provide a more precise representation of the

tetrafluoromethane results. Following this method, one first

"straightens" the isometric lines (Figure 1)by adding to the

measured pressure, P , a quantity c ( A ~ ' / A T )V, /T kin which

the best values of c and k are determined for each isometric

by an iterative trial-and-error calculation. Differences in

d

Experimental isometric, P

TEMPERATURE

Figure 1. Schematic representation of original

and "straightened" isometric

m CD m w w m 3 m t- N m

i

pressure and temperature over the extremes of an iterated A comprehensive analysis of the way small experimental

isometric line are represented by Ap' and A T , respectively. and cdrrelational errors are translated to the final thermo-

Any difference between the pressure denoted by a "straight- dynamic function is involved and generally impossible to

ened" isometric and a straight line represented by q is give in numerical terms; but in some areas a t least, one

carried as a residual pressure, r. For tetrafluoromethane, can reasonably expect them to be magnified when reckoned

minimum values of the residual pressures were obtained for on a percentage basis. In the integrand of H - Ho, Equa-

all isometrics when It = 1.5. Thus, differentiation of the tion l, for example, the situation becomes most critical when

relationship the magnitude of the product T(aP / a T ),approaches that

P = q + r - C(AP'/AT),/VT" of the pressure. Near this point, the error in the integrand

(4) may be an order of magnitude greater than the error in

yielded an exact expression for the slope of the isometric (aPjaT),itself. Fortunately, the integration over density

line a t any data point, takes advantage of the cancellation of errors having oppo-

(dP/aT),= (aq/aT),+ (ar/aT), + 1.5c(Ap'/AT),/VTZ5 ( 5 ) site sign, a likely occurrence when the residual quantities

are taken into account. On the other hand, large systematic

Since the first and third terms on the right of Equation 5 errors are possible when thermodynamic functions are

were evaluated analytically, all errors arising strictly from calculated by analytical methods only, based on closed

imperfection in the analytical representation of the iso- equations of state that deviate consistently in one direction

metric data accumulated in the residual terms and were from the true slope (aPIaT), over fairly wide ranges

finally accounted for in a graphical evaluation of (ar/aT),. of density.

Consequently, the estimated percentage error in (aP/aT),

will be equal to the estimated percentage error in (ar/ a T ), INTEGRATION OF FUNCTIONS

multiplied by the ratio (ar/aT),/(aP/aT),.

By far the most difficult areas for determining (ar/aT), The integrals in Equations 1, 2, and 3 were determined

are a t the temperature extremities of the isometrics and by graphical integration with little or no introduction of

are, therefore, the areas where the largest purely correla- spurious errors from this operation. However, the entropy

tional errors are introduced. Thus, at both 0" and 350" C. values tabulated were obtained from (G - Q) = (H- ITo) -

the probable correlational error in ( a P / a T ) , varies from T ( S - S o )rather than from Equation 2 in order to preserve

<0.1% a t the lowest and highest densities to 0.3 to 0.4% numerical consistency between the values for ( S - So),

a t medium densities. For all densities at intermediate tem- (H - W )and , (G - G o ) .To make certain that no significant

peratures the correlational errors in ( a P / a T ) , are con- errors were introduced by the correlating techniques them-

siderably less than 0.1%. selves, comparisons were made of the entropies, (S - So)'s,

,015 I

Q-

k

?

a

2x

c

I

n

0 2 4 6 8 10

0 2 4 6

DENSITY, g-mole/liter D E N S I T Y , g-rnole/liier

Figure 2. Integrand from enthalpy function a t 75" C. Figure 3. Integrand from entropy function at 75" C.

-RTB

Table II. -(S - So)for the 75" Isotherm

1.5

Density,

G. Moles/ (G - G') -

Liter ( H -W ) / T Eq. 2 Dev., %

1 6.9188 6.9188 0

2 8.5526 8.5526 0

3 9.6148 9.6147 0.001

4 10.4445 10.4444 0.001

5 11.1505

~- ~. 11.1505 0

6 11.7833 ii.7833 o

I.o 7 12.3712 12.3710 0.002

8 12.9326 12.9324 0.002

9 13.4820 13.4817 0.002

10 14.0298 14.0295 0.002

11 14.5843 14.5841 0.001

were taken from a previous publications ( 8 ) .

The first derivatives of the second virial coefficients with

respect to temperature, dB/dT, were calculated from the

differentiated equation of the Lennard-Jones [ n , m ] ( 11 )

statistical mechanical expression fitted to experimental B

values. Correlation of the second virial coefficient of tetra-

fluoromethane by the Lennard-Jones [ n , m ] potential with

I n = 500 and m = 6 will appear in a separate publication. T o

these calculated derivatives were added small graphically

determined temperature derivatives of the differences

between observed and calculated values of the second virial

coefficients according to the [500,6]potential. Values for the

derivatives of the third and fourth virial coefficients with

0 respect to temperature, dC/dT and dD/dT, were deter-

mined by graphical differentiation of experimental values of

the third and fourth virial coefficients, respectively.

Closed equations of state applied without the aid of a

residual term are notoriously unreliable for estimating

thermodynamic properties, particularly when a derivative

quantity is involved. For comparison with results obtained

by the present method, the enthalpies of tetrafluoromethane

were also calculated a t 20 selected points based on the

Redlich-Kwong (14) and the Benedict-Webb-Rubin ( 5 , 8)

0 2 4 6 8 IO

DENSITY, g-mole/liter

Figure 4. integrand from Gibbs energy function at 75"C.

deviation, 0.01%, was found for some points on the 09, 25",

and 30" isotherms. Results of a comparison for integer

values of the density on the 75" isotherm, given in Table 11,

are typical of most isotherms.

Characteristic behaviors of the integrands are illustrated

for a single temperature, 75" C. (Figures 2 , 3 , and 4) by solid

lines drawn through points calculated from experimental

values of P , T , p , and derived values of ( d P / a T ) These

0.

calculated from the second virial coefficients and/or their

first derivatives with respect to temperature.

Approximate values of the integrands, shown as dashed

lines, relate them to the virial equation of state,

third, and fourth virial coefficients, respectively. At zero

density, the integrands reduce to exact functions of the

second virial coefficients and their derivatives with respect

to temperature; a t densities above zero the integrands are

functions of an infinite series of virial coefficients and their

temperature derivatives. Successive approximations through

the fourth virial coefficient were calculated and plotted DENSITY, g - m o l e / l i t e r

to illustrate the various degrees of approximations that can

be expected from terminated virial expansions. Figure 5 . Enth.alpy, -(H - H")

The enthalpy and entropy data in Table I have been

plotted in Figures 5 and 6 to illustrate the internal con-

sistency of the derived values.

Values of the thermodynamic properties (H - P ) / T ,

( s p - s p , Ideal) ( s u -

f s u , ideal) (Gp - G p , ideal) (Gu - Gu, ideal)

7 9 9

and can be made available to interested parties upon

request.

NOMENCLATURE

B = second virial coefficient, ~ m . ~ / m o l e

c = aparameter

C = third vinal coefficient, cm.6/mole2

D = fourth vinal coefficient, ~ m . ~ / m o l e ~

G = molal Gibbs energy, cal. /mole

H = molal enthalpy, cal./mole

k = aparameter

m = value of attractive exponent in Lennard-Jones potential

function

n = value of repulsive exponent in Lennard-Jones potential

function

P = pressure, atm.

p‘ = “corrected” pressure, atm.

q = P+c(A~‘/AT)~/vT‘-~

r = residual pressure, atm.

R = gas constant = 0.0820544 liter atm./mole deg.

S = molal entropy, cal./deg. mole

T = thermodynamic temperature = 273.16 + (0.04106 - 7.363

x 10-9) ( t i l o o ) (tjioo - 1)

t, 0 C. = International Celsius temperature

V = molal volume, liter/g.-mole

y= activity coefficient = exp.[(G - G o ) / R T ] / P

p= molal density, g.-moleiliter

cal. = 4.12917 x lo-* liter atm. = 4.1840 joules

O = superscript indicating standard state

ideal = subscript indicating ideal gas state

LITERATURE CITED

0 1 2 3 4 5 6 7 B 9 1 0

DENSITY, g-mole/ltter Beattie, J.A., Chem. Reus. 44, No. 1, 141 (1949).

Beattie, J.A., “Temperature, Its Measurement and Control

Figure 6. Entropy, -(S - So) Science and Industry,” Vol. 11, Chap. 5, p. 93, Reinhold,

New York, 1955.

equations of state. In general, the results indicated that Beattie. J.A.. Brideeman. O.C.. Proc. Am. Acad. Arts Sei. 63,

, I

a closed equation of state that had the ability to represent 229 (1928).

the P-V-T data over a given range of variables with an Beattie, J.A., Stockmayer, W.H., “Treatise on Physical

average deviation of less than 1%,would often, because of Chemistry,” Vol. 11, Chap. 2, H.S. Taylor and S. Glasstone,

large percentage errors in (aP/aT)p , produce numbers for eds., Van Nostrand, New York, 1951.

the enthalpy that deviated an order of magnitude greater Benedict, M., Webb, G.B., Rubin, L.C., J. Chem. Phys 8 ,

334 (1940).

over the same range of variables. Some individual points Canjar, L.N., Rossini, F.D., “Work of American Petroleum

were off by as much as 27%, Institute Research Project 44 on P- V-T Properties,” Conf.

Values for the thermodynamic properties, P, H - Ho, on Thermodynamic and Transport Properties of Fluids,

S - So, and G - Go, are presented in Table I, tabulated at sponsored jointly by British Institute of MechanicaI Engineers

the even densities and temperatures corresponding to the and International Union of Pure and Applied Chemistry,

original experimental data (8). In some cases the values London, England, July 1957.

are given to an extra significant figure to minimize uncer- Chari, N.C.S., Sc. D. dissertation, University of Michigan,

tainties in any subsequent calculations rather than to 1960.

indicate this degree of accuracy. Douslin, D.R., Harrison, R.H., Moore, R.T., McCullough,

As previously discussed, the methods have introduced J.P., J.Chem. Phys. 35,1357 (1961).

Harrison, R.H., Douslin, D.R., “Perfluorocyclobutane.

small uncertainties from (aP/aT),, dB/dT, and the graph- Thermodynamic Properties of the Real Gas,” U. S. Bur.

ical integrations. These uncertainties apply largely to the Mines Rept. Invest. 6475 (1964).

enthalpy and entropy functions because the free energy Keyes, F.G., J. Chem. Phys. 15,602 (1947).

functions are independent of ( a P / a T ) , and dB/dT. How- Lennard-Jones, J.E., Proc. Roy. SOC.(London), Ser. A 106,

ever, all calculations are dependent on the original data 463 (1924).

whose estimated maximum uncertainty is 0.03% at the McBride, B.J., Heimel, S., Ehlers, J.G., Gordon, S., “Thermo-

lowest temperature and pressure and 0.3% a t the highest dynamic Properties to 6000” K. for 210 Substances Involving

temperature and pressure. As noted in the original publica- the First 18 Elements,” NASA, SP-30Q1,156 (1963).

Nagarajan, G., Australian J. Chem. 15,566 (1962).

tion ( 8 ) , the values of “observed pressure” were corrected Redlich, O., Kwong, J.N.S., Chem. Reus. 44, 233 (1949).

for the partial pressure of mercury vapor adjusted a t each Stimsh, H.F., Am. J . Phys. 23,614 (1955).

pressure for the Poynting effect. The correction did not RECEIVED for review October 4, 1965. Accepted March 14, 1966.

include the van der Waals interaction of mercury vapor Work conducted in part under an Interservice Support Agreement

with tetrafluoromethane, but the inaccuracy introduced is between the Air Force Office of Scientific Research, Office of

probably within the range of the stated over-all uncertainty Aerospace Research, U. S. Air Forec, Project No. 9713, Task

of the P-V-T data. Thus, the thermodynamic properties No. 9713-02, and the Bureau of Mines, U. S. Department of the

are, possibly, subject to small but significant corrections Interior. Contribution 143 from the Thermodynamics Laboratory,

due to the van der Waals interaction. Bartlesville Petroleum Research Center, Bureau of Mines.

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