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VAPOR PRESSURES OF ORGANIC COMPOUNDS

IN THE RANGE BELOW ONE MILLIMETER OF

MERCURY

U. S. DEPARTMENT OF COMMERCE

NATIONAL BUREAU OF STANDARDS
[E NATIONAL BUREAU OF STANDARDS

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NATIONAL BUREAU OF STANDARDS

technical ^lote

70

OCTOBER 1960

VAPOR PRESSURES OF ORGANIC COMPOUNDS IN THE

RANGE BELOW ONE MILLIMETER OF MERCURY

E. E. Hughes arid S. G., Lias

NBS Technical Notes are designed to supplement the Bureau's regular publications program. They provide a means for making available scientific data that are of transient or limited interest. Technical Notes may be

listed or referred to in the open literature. They are for sale by the Office of Technical Services, U. S. Depart- ment of Commerce, Washington 25, D. C.

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Price 75 cents

Vapor Pressures of Organic Compounds in the

Range B^low One Millimeter of Mercury.

By

E. E. Hughes and S. G. Lias

Data for vapor pressures less than one millimeter of

mercury for over three hundred organic compounds have been

collected. The values are presented in tabular form. No

attempt has been made to evaluate the reliability of these

data except where several investigators have studied the same compound over the same pressure range. A brief discussion of the methods and instruments which have been used

to measure low vapor pressures is included.

1. Introduction

Comparatively few determinations of the saturation vapor pressures

of pure organic compounds have been made in the pressure region below one millimeter of mercury. Vapor pressures greater than this have been

thoroughly studied and available data have been rather completely tabulated [87,101]. No such comprehensive collection of the data has been

made for compounds with lower vapor pressures, probably because of the

lack of data and because of the difficulty of assessing the reliability

of the few methods suitable for measuring these low pressures. The

following table is a collection of available published data. No attempt

has been made to evaluate the reliability of these data, except in the

few cases where several investigators have studied the same compound

over the same pressure range.

A brief discussion of the methods and instruments which have been

used to measure low vapor pressures precedes the table. The remarks on methods and recent developments supplement the review of Ditchburn and

Gilmour [3^].

2. Methods and Instruments

2.1 Gas Saturation. - This method depends on measuring the quantity

of a volatile substance necessary to saturate a fixed volume of an indifferent gas. Usually the substance whose vapor pressure is to be determined is contained in a saturator held at a fixed temperature. An inert

carrier gas is passed through the saturator and the amount of material

removed from the saturator is determined. The partial pressure of the

substance, and consequently, its saturation pressure at the particular

temperature, can then be easily calculated.

The method is simple and has been used frequently for determining

low pressures [11,13]. There are, however, many sources of error and

great care in the design and use of the apparatus is essential. It is one of the few methods that can be used at low temperatures.
2.2 Mass Spectrometry. - Tickner and Lossing [104,105] have used

the mass spectrometer to measure vapor pressures of a number of compounds

at low temperatures. The instrument is empirically calibrated for each

compound. A saturator containing the substance at a fixed temperature

is connected to the instrument and the concentration of the substance

in the vapor space over the liquid is determined.

The major advantage of this method is that the presence of impurities can be easily recognized. Their effect can often be minimized by selection

of a mass number characteristic only of the substance being investigated.

Other instrumental methods, such as non -dispersive infrared spectrophotometry and gas chromatography, may be used in a similar way to measure the

vapor concentration, provided their sensitivity for the substance is

sufficiently high.

2.3 Effusion and Evaporation. - Knudsen [5^-57] showed that under

certain circumstances the rate at which a substance effuses through an

orifice is a function of the temperature, its molecular weight, and the

pressure drop across the orifice. Methods, based on some modification of

Knudsen' s method, have been the primary methods for determining the low

vapor pressures of many organic and most of the inorganic compounds.

These methods are simple, and the amounts of material and time required

are generally small.

The effusion method depends rather critically on certain dimensional

factors and, because of this, it has not been used at temperatures much

below room temperature. One requirement is that the orifice have a diameter less than one -tenth of the mean free path of the molecules of

the substance. At high temperatures and low pressures, diameters as large as a half centimeter have been used, but at low temperatures the

orifice must be considerably smaller. Small orifices are in reality

short tubes as compared with orifices of larger diameter, and the simple

laws of effusion through orifices no longer apply [88,109]. Clausing

[27,28] determined theoretically the effect of varying the ratio of the

length of tube to its diameter, but no thorough experimental study of

the validity of the "Clausing factors" has been published.

The Knudsen method depends ultimately on determining the mass flow

of the substance through the orifice. In the simplest methods, the substance is contained in a small crucible which is covered with a lid

pierced with an orifice of known diameter. The mass of material lost

from the crucible during a measured time interval is determined by weighing the crucible or by collecting the effused material. The weight loss can be conveniently followed by suspending the crucible from a micro

balance [16,17,76,106]. Instead of measuring the mass effusing, it is

possible to measure the force exerted by the effusing vapor. The effusion

cell can be calibrated with a substance of known vapor pressure and the

vapor pressure of the unknown can be calculated from the reaction force

[9,69].
A recent technique for determining the vapor pressure of inorganic

substances depends on the "counting" of radioactive isotopes in the

vapor effusing from a Knudsen cell. This has been used only for inorganic substances [67].

Langmuir [59] nas proposed a modification of the Knudsen method

which can be used to determine very small vapor pressures. The vapor

pressure can be calculated from the rate of evaporation from a surface

of known area. This modification is more easily applied to metals and

other substances having very small vapor pressures, than to organic compounds.

2.4 Thermal Conductivity. - Delaplace [33] measured the thermal

conductivity of the vapor phase of a saturated system and related this

to the concentration of the substance. He reported pressures as low as one micron. His values agree fairly well with those of other investigators who have studied the same compounds over the same temperature

interval [15,105].

2.5 Boiling Point Methods. - Several methods are available in

which the boiling points of substances are measured at low pressures

[43, 45]. An inert and noncondensible gas is contained in the system at

low pressure. The evolution of vapor from the liquid being studied increases abruptly when the vapor pressure equals the pressure of the

residual gas. The method is accurate, but its use has been limited by

difficulties encountered in the design of suitable apparatus and in the

measurement of temperature.

2.6 Mechanical Methods. - McLeod gages and oil manometers are generally unsuitable for measuring condensible gases at low pressure,

although several excellent determinations of vapor pressure have been

reported [10, 15]. Oil manometers have limited use because of the significant vapor pressures of the manometri'c fluids and the solubility of

many substances in these oils. Several modifications have been reported

[11,44,62], but in general they can be used only at higher pressures.

These methods are particularly sensitive to errors caused by the

difference in temperature between the sample and the measuring instrument. The errors are often quite large and must be carefully evaluated.

A theoretical treatment of this effect, which may also affect other

methods, is presented by Liang [60,6l],

The Rodebush manometer measures the force required to lift a "lid"

which is subjected to the vapor pressure of a substance on one side and

to a high vacuum on the other [8,85,86].

Tube gages that operate like Bourdon tubes have been used for measuring very low pressures [49]. The deflection of the tubes, usually of

quartz, is quite small and is measured with a microscope.
2.

7

Dew Point Methods. - The temperature at which a substance

just begins to condense can be used to calculate its concentration in

the vapor phase. If its partial pressure in the vapor phase is known,

a determination of the "dew point" can be used to determine directly

the temperature at which the particular pressure corresponds to the

vapor pressure. Several applications of this method have been reported

[51,112], but the accuracy of the method is doubtful.

2.8 Measurement of Ion Currents. - Methods that depend on the

measurement of ion currents have long been used for measuring low pressures. The methods require an empirical calibration for each substance

and this restriction limits their use in determining vapor pressures

[42].

2.

9

Viscous Damping. - The rate of damping of a vibrating quartz

fiber can be related to the pressure of a gas in the system containing

the fiber [28,58]. Several applications of this method have been reported [1-7,25].

3. Table

3.1 Treatment of Data. - The saturation temperatures given in the

table were obtained either by direct calculation from logarithmic equations or by graphical interpolation of the data presented by the original

worker. The temperature range specified for a compound is approximately

the experimental range reported by the investigators. In most cases,

sufficient data were available to allow the calculation of at least three

points without exceeding the experimental pressure range by more than a half order of magnitude. In a few cases, data were reported at only one temperature. These have been included in the table with appropriate

otation.

The state, solid, or liquid, for which the data were collected is

indicated by the notation following the compound name. Melting points

are given only when the tabulated data pass through this point.

No attempt has been made to evaluate the methods, except in those cases where the data of several investigators concerning a single com- pound have disagreed. The final value selected was an average based on

the expected reliability of the several methods and the general care taken in selecting materials and in reporting data. The number of significant figures was chosen for uniformity and does not reflect the precision of the original measurements.

Original references were always consulted when available. In some instances, it was necessary to rely on information obtained from abstracts or from other sources. For some compounds, data of a particular

investigator are not included in the table, but the work is listed among

the references because of its interest.
3.2 Listing of Compounds. - Compounds are listed by empirical

formula. The order is determined first by the number of carbon atoms,

secondly, by the number of hydrogen atoms, and finally, by the symbols

of the remaining elements taken in alphabetical order. The names of

compounds are those recommended by the International Union of Pure and

Applied Chemistry (76a), except where the common name is preferable.

k. Acknowledgment

This work was supported by the Public Health Service of the Depart'

ment of Health, Education, and Welfare.
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6. References

1. Aihara, A., J. Chem. Soc. Japan, Pure Chem. Sect. 22/ 855-57 (1952).

2. Ibid., 74, 437-41 (1953).

5. Ibid!' 2E 492-94 (1955).

3. Ibid., S 631-34 (1953).

4. Ibid., 2fe 634-35 (1953).

6. Ibid., 26, 495-97 (1955).

7. Ibid., 22, 497-99 (1955).

8. Balson, E. W. , Trans. Faraday Soc., 43_, 48-53 (1947).

9. Ibid., j£, 54-60 (1947).

10. Balson, E.y., Adams, N.K., Ibid., 42* 417-19 (1951).

11. Balson, E.W., Denbigh, K.G., Adams, N.K., Ibid. 43_, 42-47 (1947).

12. Barker, J. T., Z. physik. Chenu, 2i, 235 "53 (1910).

13. Bent, H. E. , Francel, R.J. , J. Am. Chem. Soc. .70. 634-37 (1948).

14. Birks, J., Bradley, R.S. , Proc.Roy. Soc. (London), A198. 226-39 (1949).

15. Bourbo, P. S., J. Phys. (U.S.S.R. ), 2, 286-88 (1943).

16. Bradley, R.S. , Proc.Roy. Soc. (London), A205. .555-63 (1951).

17. Bradley, R.S., Bird, C.L., Jones, F., Nature, 178, 998-99 (1956).

18. Bradley, R;S. , Care, A.D. , J. Chem. Soc. , (195;$, I688-9O.

19. Bradley, R.S., Cleasby, T.G.,Ibid., (1953) 1681-84.

20. Ibid., (1953), 1690-92.

21. Bradley, R.S., Cotson, S. , Ibid., (1953) 1684-88.

22. Bradley, R.S., Shellard, A. P. .Proc.Roy. Soc. ( London). A198. 239-5I (1949).

23. Bright, N.F.H., J. Chem. Soc, (1951) 624-25.

24. Bright, N.F.H. , Carson, T. , Dyson, T. A., Research (London), 3_,l85-86

(1950).

25. Charnley, T. , Skinner, H. A. , J. Chem. Soc. , (1951) 1921-24.

26. Clausing, P., Ann. Physik, 12, 96I-89 (1932).

27. Ibid., Physica, % 65-8O (I929).

28. Coolidge, A. S. , J. Am. Chem. Soc, 4^, 1637-43 (1923).

29. Crooks, D. A., Feethan, F.M., J. Chem. Soc. , (1946) 899-9OI.

30. Crowell, T. I. , Jones, G.L. , J. Phys. Chem., 58, 666-67 (1954).

31. Dannenberg, H. , Bradley, T.F. , Evans, T.W#> Ind.Eng. Chem. .41.1709-11

(I949).

32. Darkis, F.R., Vermillion, H.E., Gross, P.M., Ibid., ^2, 946-49 (1940).

33. Delaplace, R. , Compt. rend., 204. 493-95 (1937).

34. Ditchburn, R.W., Gilmour, J.C. , Rev.Mod.Phys. 13_, 310-27 (1941).

35. Edwards, G. , Trans. Faraday Soc, 46, 423-27 (1950).

36. Ibid., 42/ 152-54 (1953).

37. Filosofo, I., Merlin, M. , Rostagni, A., Nuovo Cimento, 2, 69 (1950).

38. Fouretier, G. , Taillade, M. , Compt. rend., 218. 787 -90 (1944).

39. Gardner, G.S. , Brewer, J.E., Ind. Eng. Chem. , 2£, I79-8I (1937).

40. Granovskaya, A. A., Vestnik Moskov. Univ., 2, No. 6, Ser.Fiz. -Mat. i

Estestven. Nauk. No. 4, 47-50 (1952).

41. Hammer, E. , Lydersen, A.L. , Chem. Eng. Sci. , 7, 66-72 (1957).

42. Hickman, K.C.D., J. Franklin Inst., 221, 383 -402 (1936).

43. Ibid., J. Phys. Chem., 3JL, 627-36 (1930).

44. Ibid., Rev. Sci. Instr. , £, 161-64 (1934).

45. Hickman, K.C.D. , Hecker, J.C, Embree, N.D. , Ind. Eng. Chem. , Anal. Ed.,

2, 264-67 (1937). 22
Hopke, E.R. , Sears, G.W. , J. Am. Chem. Soc. , JO, 38OI-3 (1948).

Ibid., J. Chem. Phys.,12, 1345-51 (1951).

Hoyer, H. , Peperle, W. , Z. Elektrochem. , 62, 61-66 (1958).

Ivin, K. J., Dainton, F. S. , Trans. Faraday Soc. , 45_, 32-35 (19^7 ).

Jantzen, E. , Erdmann,W. , Fette u. Seifen, ^4, 197-201 (1952).

Kapff, S.F. , Jacobs, P., Rev. Sci. Instr. , 18, 581-84 (1947).

Kaufman, M.H. , Whittaker, G. , J. Chem. Phys. , 24, 1104 (1956).

Klochkov, V.P., Zhur. Fiz. Khim. , 22, 1177 (1958).

Knudsen, M. , Ann. Physik, 28, 75 "150 (1909).

Ibid., 28, 999-1016 (1909).

Ibid., 2& 179-93 (1909).

Ibid., 21, 205-29 (1910).

Langmuir, I., J. Am. Chem. Soc, 105-27 (1913).

Ibid., Phys. Rev., 2nd Ser. , Vol. II, 329 (19*53

Liang, S. , J. Appl. Phys., 22, 148-53 (1951).

Ibid., J. Phys. Chem., 56, 660-62 (1952).

Linder, E.G., Ibid., 2£, 531 "35 (1931).

Lister, B.A.J. , McDonald, L. A. , Atomic Energy Research Estab.

(G. Brit. ) Report No. C/R 1122 (1955).

Littlewood, R. , J. Chem. Soc. ,(1957) 2419-20.

Majury, T. G. , Chemistry and Industry, (1956), 349-50.

Menzies, A. , J. Am. Chem. Soc, 42, 2218-21 (1920).

McKinley, J.D. , Vance, J.E. , J. Chem. Phys., 22, 1120-24 (1954).

Nelson, O.A., Smith, L.E. , J. Am. Chem. Soc. , 6^7 5055-57 (19^2).

Neumann, K. , Volker, E., Z. physik. Chem. A, 161. 33-45 (1932).

Nitta, I., Seki, S. , J. Chem. Soc. Japan, Pure Chem. Sect. , 69

85-87 (19^3).

Ibid., 62, 141-43 (19^).

Ibid., 62, 143-45 (1948).

Nitta, I., Seki, S. , Momotani, M. , Ibid., £L, 430-33 (1950).

Nitta, I., Seki, S. , Momotani, M. , Sato, K. , Ibid., 2i; 378-82 (1950).

Nitta, I., Seki, S. , Suzuki, K. , Bull. Chem. Soc. Japan, 24, 63-69 (I95I).

Parks, G. S. , Moore, G.E. , J. Chem. Phys. , 1£, 1151-53 (19^9).

Patterson, A.M., J. Am. Chem. Soc. , ^

39Q5-25 (1933).

Perry, E. S. , Weber, W.H. , J. Am. Chem. Soc. ,71, 3726-30 (1949).

Perry, E.S. , Weber, W.H. , Daubert, B.F. , Ibid., jO, 3720-26 (1949)

Ratchford, W.P. , Rehberg, C.E. , Anal. Chem. , 21, 1W-7-19 (1949).

Redemann, C.E. , Chaikin, S.W. , Fearing, R. B. , J. Am. Chem. Soc. , JO,

631-33 (19^).

Ibid., JO, 1648-50 (1948).

Ibid., JO, 2582-83 (1948).

Redemann, C.E. , Chaikin, S.W. , Fearing, R.B. , Benedict, D. , Ibid.,

20, 637-39 (19^).

Redemann, C.E. , Chaikin, S.W. , Fearing, R.B. , Rotariu, G. J. , Savit, J.,

Van Hoesen, D. , Ibid., 22, 3604-7 (1948).

Rodebush, W.H. , Cooms, C.C. , Ibid., 4£, 1953 "55 (1927).

Rodebush, W.H., Henry, W.F., Ibid., ^2, 3I59-6I (1930).

Rossini, F.D. , Am. Petroleum Inst. Research Project 44.

Rossman, M.G. , Yarwood, J., J. Chem. Phys., 21, 1406-47 (1953).

23
89o Scott, T., MacMillan, D„ , Melvin, E.H., Ind. Eng. Chem.

,

kk, 172-75 (1952).

90o Sears, G.W. , Hopke, E.R., J.Phys. and Colloid Chem., ^2, 1137-42 (1948),

9lo Ibid., J. Am. Chem. Soc. , £L, l632 -3* (19*9).

92. Ibid., 21, 2575-76 (19*9).

93. Seki, S. , Suzuki, K. , Bull. Chem. Soc. Japan, 26, 209-13 (1953).

94. Serpinskii, V.V. , Voitkevich, S.A., Lyuboshits, N.Yu. , Zhur. Fiz.

Khim., §2, 1032-38 (1953).

95. Ibid., 28, 810-13 (195*).

96. Ibid., 28, 1969-7^ (195*).

97. Ibid., 22, 653-57 (1955).

98. Sklyarenko, S. I. , Markin, B. I. , Belyaeva, L.B. , Ibid., ^2_, 1916-21

99. Small, P., Small, K.W. , Cowley, P., Trans. Faraday Soc, 44, 810-16

(19*8).

100. Spizzichino, C. , J. recherches centre natl. recherche sci Labs

Bellevue (Paris), No. ^kj 1-24 (1956).

101. Stull, D.R., Ind. Eng. Chem., 2£, 517-50 (19*7).

102. Suzuki, K., Onishi, S. , Koide, T. , Seki, S. , Bull. Chem. Soc. Japan,

22, 127-31 (1956).

103. Swan, T. , Mack, E. , J. Am. Chem. Soc. , i£J_, 2112-16 (1925).

104. Tickner, A.W. , Lossing, F.P. , J. Chem. Phys. ,18, 148 (1950).

105. Ibid., J. Phys. and Colloid Chem., ^2, 733-40 (1951).

106. Ubbelohde, A.R., Trans. Faraday Soc, jk, 282-92 (1938).

107. Verhoek, F. , Marshall, A. , J. Am. Chem. Soc, 61, 2737-42 (1939).

108. Werner, A.C. , Ind. Eng. Chem. jj4, 2736-40 (1952).

109. Whitman, C.I, , J. Chem. Phys. 20, 161-64 (1952).

110. Williams, E.F., Ind. Eng. Chem., j£, 950-5* (1951).

111. Winstrom, L. , Rulp, L. , Ibid., JO, 2584-86 (19*9).

112. Wise, H. , Puck, T.T. , Failey, C.F. , J.Phys. and Colloid Chem., £ib

73^-41 (1950).

113. Zil'berman-Granovskaya, A. A., J. Phys. Chem. (U.S. S.R. ), 14, 759"67

(19^0).

114. Ibid., 3k, 768-73 (19^0).

115. Zil'berman-Granovskaya, A. A., Shugam, E.A., Ibid., 2k, 1004-6 (19*0).

24 USC0MM—DC
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