«en,j.ona.L cureau or bi-anaaraa

Library, N.W. Bldg

NOV 3^&1 Referep

takelf rv.

PB 161610

Moulder laboratories

92c. 109

A COMPILATION OF THE PHYSICAL

EQUILIBRIA AND RELATED PROPERTIES

OF THE

HYDROGEN-HELIUM SYSTEM

BY

D. E. DRAYER AND T. M. FLYNN

U. S. DEPARTMENT OF COMMERCE

NATIONAL BUREAU OF STANDARDS
THE NATIONAL BUREAU OF STANDARDS

Functions and Activities

The functions of the National Bureau of Standards are set forth in the Act of Congress, March

3, 1901, as amended by Congress in Public Law 619, 1950. These include the development and

maintenance of the national standards of measurement and the provision of means and methods for making measurements consistent with these standards: the determination of physical constants and

properties of materials; the development of methods and instruments for testing materials, devices.

and structures; advisory services to government agencies on scientific and technical problems; in- vention and development of devices to serve special needs of the Government; and the development

of standard practices, codes, and specifications. The work includes basic and applied research,

development, engineering, instrumentation, testing, evaluation, calibration services, and various

consultation and information services. Research projects are also performed for other government

agencies when the work relates to and supplements the basic program of the Bureau or when the

Bureau's unique competence is required. The scope of activities is suggested by the listing of

divisions and sections on the inside of the back cover.

Publications

The results of the Bureau's work take the form of either actual equipment and devices or published papers. These papers appear either in the Bureau's own series of publications or in the journals

of professional and scientific societies. The Bureau itself publishes three periodicals available from

the Government Printing Office: The Journal of Research, published in four separate sections,

presents complete scientific and technical papers; the Technical News Bulletin presents summary

and preliminary reports on work in progress; and Basic Radio Propagation Predictions provides

data for determining the best frequencies to use for radio communications throughout the world.

There are also five series of nonperiodical publications: Monographs, Applied Mathematics Series,

Handbooks, Miscellaneous Publications, and Technical Notes. Information on the Bureau's publications can be found in NBS Circular 460, Publications of the

National Bureau of Standards ($1.25) and its Supplement ($1.50), available from the Superintendent

of Documents, Government Printing Office, Washington 25, D.C.
NATIONAL BUREAU OF STANDARDS

technical Ntote

June 1961

A Compilation of the

Physical Equilibria and Related Properties

of the

Hydrogen -Helium

System

by

Dennis E. Drayer

and

Thomas M. Flynn

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. Department of Commerce, Washington 25, D. C.

DISTRIBUTED BY

UNITED STATES DEPARTMENT OF COMMERCE

OFFICE OF TECHNICAL SERVICES

WASHINGTON 25, D. C.

Price $ 1.25

11

Contents

Page

List of Tables

List of Figures

Abstract

1 . Introduction

1 . 1 Purpose

1.2 Organization

1 . 3 Scope

2. Survey of Literature

3. Discussion of Available Data

4. K-Factor Charts

5. Phenomena Index

5. 1 Hydrogen

5. 2 Helium

6. Properties Index

6. 1 Hydrogen

6. 2 Helium

7. Processes Index

7. 1 Hydrogen

7. 2 Helium

8. Bibliography of References

9. Appendix

in

ivv

1

1

1

1

2

2

4

9

10

11

12

13

15

17

18

19

20

49
Ill

List of Tables

Table Page

I Helium-Hydrogen Pressure-Concentration Data 50
IV

List of Figures

Figure Page

1. Regions Covered by Published Data 3

2. Helium-Hydrogen Vapor -Liquid Equilibria

Data: Helium K-Factors 5

3. Helium-Hydrogen Vapor -Liquid Equilibria

Data: Hydrogen K-Factors 6

4. Vapor -Liquid Equilibria

Helium-Hydrogen System 7

Abstract

Published data have been used to calculate K-factors for the

helium-hydrogen system over the range of 17.4 to 21.8 K and 2 to

32 atmospheres pressure. K-factors are presented graphically for

three isotherms over this range. A bibliography of approximately

290 references is also presented on related properties for this

system and for the pure components.

1

1 . Introduction

1 . 1 Purpose

Hydrogen is frequently found as a companion gas in helium

sources. If this helium is to be liquefied, a most rigorous purification is required to prevent blocking of the liquefier by solid impurities. The exacting design of such a helium purification system

requires a knowledge of the physical equilibria behavior of the hydrogen-helium system.

As an initial step in the study of the physical equilibria of the

hydrogen-helium system, a literature survey was made. This paper

presents the results of that survey, which includes the current knowledge of the vapor -liquid equilibria, and selected properties of the

pure components.

1. 2 Organization

The information is presented in three principal parts: (1)

physical equilibria with major emphasis on vapor -liquid equilibria;

(2) properties related to physical equilibria; and (3) a bibliography of

references. Some discussion is presented with Part (1). The information of Part (2) is presented in tabular form showing the reference

where important data are to be found. Part (3), the Bibliography,

lists the references alphabetically by author.

1 . 3 Scope

A literature search, as summarized in NBS Technical Note

No. 56, revealed most of the pertinent data. Such data were

abstracted, and presented in the form of K-factor charts, and as a bibliography of references for related areas of interest. The areas

searched are presented in the above reference and will not be enumerated here. Generally speaking, the literature was searched

extensively and includes articles published up to I960. This report

does, however, include additional references obtained from a search

of Volumes 1 through 5 of the series "Advances in Cryogenic Engineering".
2

2. Survey of Literature

Only one reference was found relating to the vapor -liquid

equilibria for the helium-hydrogen system. This reference, Smith

(247), presented pressure-concentration data for three temperatures,

17.4°, 20.4° and 2l.8°K.

No related physical data are actually presented in this paper;

only the references for such material are listed. Other areas so

covered include adsorption phenomena, purification processes, solubility relationships, density and compressibility data, thermodynamic

and transport properties, P-V-T data, critical constants, virial

coefficients, analytical techniques and various processing references.

Such material for the pure components as well as for mixtures of

helium and of hydrogen is included in many cases.

The P-T region explored by Smith (247) is shown in Figure 1.

(The data needed to prepare the P-T diagrams for hydrogen and

helium were taken from Johnson (134), Scott et al. (243) and Keesom

(151)).

3. Discussion of Available Data

Admittedly, the data presented herein cover only a narrow

o o temperature range: namely, from 17.4 to 21.8 K. However, for

this system one could expect the data, at best, to vary over a narrow

range. Complete data would extend roughly from the triple-point

temperature of hydrogen (13.9 K) to the critical temperature (33.0 K).

The difficulties of investigating this system completely are obvious.

The treatment given the original data of Smith (247) consisted

of making appropriate calculations to arrive at K-factors for each

component. (In some cases it was necessary to supplement the

tabulated data of Smith with P-x and P-y values from his various

plots). K is defined as y/x; where y is the mole fraction of a component in the vapor phase and x is the mole fraction of that component

in the liquid phase. K-factors were calculated for each component at a given temperature and pressure. Initially a plot of K versus P

(total pressure) was prepared for each component. The data did show

some scatter, especially for helium K-factors. The best smooth

curve was drawn through the plotted points and this curve was then

transferred to another plot (Figure 4).
100

40

10

Q.

</» o

E

LlI q:CO

CO

LU

ocQ.

0.4

0.1

.04

.01

/ H,

L 1

2 MELT

CURVE

1 MELTING

/ CURVE

1

C-H2M

•3C-M?

r

TP-H2

15 20

TEMPERATURE, °K

25 30 35

Figure 1. Regions Covered by Published Data
It should be noted that the 20. 4 and 21.8 K isotherms for

helium cross at approximately 10 atmospheres. Since the Boyle

point of helium is near 20 K, one would expect a reversal of the gas

solubility in that region. This is in fact shown by the data.

It is not the purpose of this article to make a test of the data

for thermodynamic consistency. Smith does treat his data from

several thermodynamic viewpoints.

4. K-Factor Charts

Figures 2 and 3 are plots of the K-factors for helium and for

hydrogen, respectively. Figure 4 shows the curves for both helium

and hydrogen as taken from Figures 2 and 3. In Figure 4, helium

K-factors are above the line K = 1 and those for hydrogen are below.

If the data extended to higher pressures, the isotherm could be

expected to close at the high-pressure end. Such closure would occur

at the line K z 1. This line thus represents the locus of the plait

points.

Figure 4 permits the calculation of the vapor and liquid phase

equilibrium composition at a given system temperature and pressure.

After obtaining the individual K-factors, one simply substitutes into

the following series of equations:

K

x z y1 /x1 (1)

K

2

= y

2

/x

2

(2)

x

x + x

2

= 1.0 (3)

v

1 + y

2

- l.o (4)

The subscripts refer to the components, helium and hydrogen. As an

example, at T = 20.4 and P = 20 atm

^e = 37

^Z

= 0. 094
X/A = X
3

cr W

cr ^ ft

i O

o w> § 2

7 ffi

•m ret >—• <-> a; a)

X/A=M
1000

15 20

PRESSURE, otmospheres

25 30 35

Figure 4. Vapor -Liquid Equilibria Helium-Hydrogen System
8

Solving equations (1) - (4) gives

xTT = 0.0245; xTT = 0.9755 He H

2

y„ = 0.9083; y__ = 0.0917 He H

2

Other relationships involving K-factors, e.g. relative volatilities,

could also be easily calculated.
5.0

Phenomena Index

Phenomena

10

MAJOR COMPONENT

HYDROGEN

Category- Other Components References

Adsorption 9, 12, 59, 62,75,86, 126,

130, 133, 158, 159, 165,

166, 179, 180, 181, 188,

204, 218, 220, 221, 226,

249, 255, 257

Carbon Dioxide 121

Nitrogen 135, 257

Phase Equilibria 91,92, 174, 224

Butane 203

Deuterium 170

Helium 247

Hydroc arbons 216, 234

Methane 71

Nitrogen 96, 217

Non- Polar Solvents 45

Paraffins 178

Water 14

Water -Nitrogen 14

Purification 56, 57,64, 122, 141, 149,

268

Nitrogen 268
Phenomena

11

MAJOR COMPONENT

HELIUM

Category- Other Components References

Adsorption 8,70, 80, 103, 129, 131,

132, 146, 155, 186, 189,

200, 237

Neon- Nitrogen 269

Phase Equilibria Ammonia 254

Argon 150

Carbon Dioxide 254

Hydrogen 247

Methane 94,95

Nitrogen 72,73, 93, 161

Propane 253

Purification 24,44, 175, 260

Neon 65

Nitrogen 72
12

6.0

Properties Index

Properties

13

MAJOR COMPONENT

HYDROGEN

Category Other Components References

Beattie -Bridge - man Constants 17, 54

Critical Constants 10,21, 68,84, 124, 134,

173, 225, 261

Density, Compressibility, Expansion2, 3, 6, 11, 13, 15, 16, 21,

31, 55, 60,68,99, 109,

110, 134, 139, 145, 167,

173, 185, 190, 191, 193,

225, 231, 235, 242,263,

271

Nitrogen 13, 15, 263

Equations of

State, Corresponding States 1, 17, 19,42, 54,83, 184,

240

Isotherms 20,48, 125, 144, 192, 195,

206, 207, 209, 241, 252,

258

Carbon Monoxide 241, 252

Helium 20

Nitrogen 258

Lennar d - Jone

s

Potentials 177

Thermodynamic

Properties

25, 26, 53, 55, 66, 68,74,

85,88,89, 107, 119, 128,

134, 136, 138, 152, 169,

171, 194, 225, 243,246,

248, 265

Carbon Monoxide 107

Nitrogen 107
14

Properties (Continued)

MAJOR COMPONENT

HYDROGEN

Category Other Components References

Transport

Properties

6, 18,42, 68, 104, 113,

120, 134, 198, 223, 225,

231, 236

Vapor Pressure 10,28, 31, 37, 39,43, 55,

68, 82,84, 99, 101, 105,

108, 115, 123, 134, 137,

140, 196, 197, 210, 225,

243, 245, 248, 262

Helium 90

Nitrogen 82

Virial Coefficients 162, 198, 199, 205, 238,

239

Carbon Dioxide 47
Properties

15

MAJOR COMPONENT

HELIUM

Category Other Com.ponentsf References

Beattie -Bridge - man Constants 17

Critical Constants 21,97, 111, 118, 134, 151,

173, 200, 225, 233,260,

266

Density, Compressibility, Expansion

2, 3, 16, 21, 22, 33, 100,

111, 118, 134, 151, 153,

167, 173, 200, 219,225,

231, 233, 260, 264

Carbon Di oxide 112

Carbon Monoxide 187

Equations of

State, Corresponding States

17, 27, 147, 168, 184, 240,

260

Isotherms 125, 142, 143, 156, 209,

264

Hydrogen 20

Thermodynamic

Properties

4, 22, 23, 63, 111, 134,

151, 152, 171, 186, 200,

225, 231, 260

Nitrogen 232

Transport

Properties

5, 51, 100, 104, 111, 113

118, 120, 134, 151, 200,

225, 231, 260

Vapor Pressure 29,41,61,97, 100, 111,

118, 134, 151, 196,200,

219, 225, 233, 260

Hydrogen 90

Virial Coefficients

36, 52, 106, 148, 154, 157,

160, 163, 164, 205
16

Properties (Continued)

MAJOR COMPONENT

HELIUM

Category- Other Components References

Carbon Dioxide

Nitrogen

46

172
17

7.0

Processes Index

Processes

18

MAJOR COMPONENT

HYDROGEN

Category Other Components References

Analytical 211

Carbon Dioxide - Oxygen -Carbon

Monoxide 79

Helium 247

Methane 114

Methane -Ethane 202

Nitrogen -OxygenHe Hum 270

Distillation 56, 57,76, 244, 251

Deuterium 77,78

Equipment 32, 34, 38, 58,98, 116,

127, 222, 228

Handling 34, 35, 176, 201, 210, 214,

222, 228, 230, 256

Heat Transfer 40, 227, 259

Helium 267

Manufacture 49, 66, 149, 208, 212, 256

Safety 35, 116
Processes

19

MAJOR COMPONENT

HELIUM

Category Other Components References

Analytical 50,87, 117, 213

Hydrogen 247

Nitrogen -OxygenHydrogen 270

Equipment 29, 67,98, 102, 183, 215,

250

Handling 30, 182, 214

Heat Transfer

Hydrogen

81, 229

267

Manufacture

Nitrogen

7, 24, 182, 183, 200

72
20

8.0

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77. Flynn, T. M. , Weitzel, D. H. , Timmerhaus, K. D. , Vander

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78. Flynn, T. M. , Timmerhaus, K. D. and Weitzel, D. H. Pilot

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99. Granet, I. Physical properties of hydrogen in convenient

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103. Greyson, J. and Aston, J. G. The heats of adsorption of

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%»
34

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128. van Itterbeek, A. The dependency of C /C on pressure for

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215. Peshkov, V. P., Zinoveva, K. N. and Filimonov, A. I. Helium-3 cryostats (in Russian)

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43

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44

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45

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48

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49

9.0

Appendix

50

TABLE I HELIUM-HYDROGEN

PRESSURE-CONCENTRATION DATA

Reference': Smith (247)

Temperature Pressure

atm

Liq uid Vapor K

Mole % He Mole % H Mole % He Mole % H He H

2 17.4 3. 27 0. 19 99.81 83.40 16. 60 439 0. 166

17.4 3. 27 0. 20 99.80 83. 50 16. 50 418 0. 165

17.4 5.65 0. 22 99.78 90. 10 9.90 410 0. 0992

17.4 5.65 0. 28 99.72 90. 80 9.20 324 0. 0923

17. 4 6. 53 0. 27 99.73 91.76 8. 24 340 0. 0826

17.4 9. 59 0. 45 99. 55 93.47 6. 53 208 0. 0656

17. 4 9.59 0. 51 99.49 93.41 6.59 183 0. 0662

17.4 14. 08 0.67 99. 33 94. 31 5.69 141 0. 0573

17.4 14.08 0.74 99.26 94.44 5. 56 128 0. 0560

17.4 21. 50 1.05 98.95 95. 04 4.96 90. 5 0. 0501

17.4 21. 50 1. 08 98.92 95. 02 4.98 88. 0. 0503

17.4 24. 35 1. 11 98.89 95. 16 4.84 85.7 0. 0489

17.4 24. 35 1. 15 98. 85 95. 21 4.79 82. 8 0. 048 5 20.4 4.29 0. 59 99.41 72.90 27. 10 124 0.273

20.4 6.94 0.87 99. 13 82. 50 17. 50 94.8 0. 177

20.4 12. 04 1. 53 98. 47 87. 20 12.80 56. 9 0. 130

20.4 17.41 2. 16 97.84 89. 00 11.00 41.2 0. 112

20.4 19.80 2.47 97. 53 90. 16 9.84 36.5 0. 101

20.4 23.81 2.77 97.23 90.70 9.30 32.7 0.0956

20. 4 24.83 2.95 97.05 90. 20 9.80 30.6 0. 101

20.4 24.83 2.97 97. 03 90. 20 9.80 30. 4 0. 101

20.4 25. 51 2.89 97. 11 90. 70 9. 30 31.4 0. 0958

20.4 27.62 3. 06 96. 94 90.40 9.60 29. 5 0. 0990

21.8 2.93 0. 18 99.82 61.3 *

* 38.7 341 0. 388

21.8 3.74 0. 34* 99.66* 65.8 34.2 194 0. 343

2J. 8 5.17 0. 52* 99.48* 71. 5 28. 5 138 0. 286

21. 8 5. 58 0.29 99.71 74.0 * 26.0 * 255 0. 261

21.8 10. 68 1.21 98.79 83. 6 16.4 69. 1 0. 166

21.8 10.68 1.36 98.64 83.7 16.3 61.5 0. 165

21.8 12.86 1.55* 98.45* 82. 2 17.8 53.0 0. 181

21.8 20.82 2.44 97.56 88.9 * 11.1 36.4 0. 114

21.8 26.26 3.06 96.94 87.4 12.6 28.6 0. 130

21.8 26.26 3. 13 96.87 87.2 12.8 27. 9 0. 132

21.8 30.41 3. 38* 96.62* 88.9 11. 1 26.3 0. 115

NOTE:

Values taken from Smith's Figures

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