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The Liquefaction of Gas

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 1

The Liquefaction of Gas

M. Z. Ahsan
(Ph.D Student, Roll No: 1015144006)

Bangladesh University of Engineering and Technology, Dhaka-1000, Bangladesh

Introduction

All physical experiments need low temperature (below room temperature) that involves the use of liquefied gases in
some way or other. So, the liquefaction is a method for production of low temperature. Generally, air, hydrogen and
helium gases are used to be liquefied for the purpose. With the aid of these three liquefied gases, experiments can be
carried out over the whole range from room temperature down to about 0.8 K. Besides, a special isotope of helium (He3)
is being used to produce low temperature of 0.3 K. There are two types of method available for large scale liquefaction
of air (hydrogen and helium gases). One is the internal work method and the other external work method. In both
methods, cooling is produced from the Joule-Thomson effect. The objective of this assignment is to discuss principles
and methods for the liquefaction of air (hydrogen and helium gases)

Joule – Thomson Effect

When fluid or gas passed in a pipe of uniform cross-sectional area through a controlled valve from higher pressure to
lower pressure region as shown in the figure-1, the volume of fluid or gas expands at the valve and work done against the
attraction forces of molecules. Since the system is kept thermally insulated from the environment, the energy required to
do this work comes from the internal energy of the fluid or gas confined in the pipe and ultimately reduces the
temperature of the system. This is called Joule-Thomson effect. The process of expansion of fluid or gas at the
controlled valve is known as throttling expansion, which is also an adiabatic expansion since no energy or heat allowed
in the system coming from the environment.

P1, v1, T1 P2, v2, T2

h1 h2

Figure-1: Throttling Process

Conditions of Cooling by Throttling expansion

There are certain conditions of cooling or heating for this throttling expansion. In order to understand these conditions
let us consider two sections; one in the upstream and the other in the downstream as shown in the figure-1. Since the
system is now adiabatic, so the enthalpy per unit mass before expansion and after expansion remains the same as:

ℎଵ = ℎଶ --------------------------------------------------------------------------------------------------------------(1)

If we keep p1 and T1 fixed in the section-I, then the enthalpy in the section-I will be fixed. This means that the
enthalpy is a function of pressure and temperature i.e. ℎଵ = ℎଵ (‫݌‬ଵ ܶଵ ). Now by keeping the controlled valve at different
positions, we can generate equal enthalpy state points of p and T after plotting those state points on the T-p graph, we
will get isenthalpic curve. By thus, setting the enthalpy at different values like ℎଶ , ℎଷ , ℎସ − − and so on, we will get set
of isenthalpic curves as shown in figure-2.
 2

TMax Inversion
߲ܶ
Curve ൬ ൰ =0
߲‫ ݌‬௛

Cooling
T Region
Isenthalpic
Curves

Heating
Region

TMin

p
Figure-2: A set of isenthalpic curves

From this set of isenthalpic curves, the following points are interesting to note to understand the conditions of cooling
and heating:

డ்
1. Some isenthalpic curves have both the positive and negative slopes i.e. the value of is positive for
డ௉
some state points and negative for some other state points. Further more for some isenthalpic curve the value of
డ்
is always negative as evident from the figure-2.
డ௉

2. The maximum value of state points on the isenthalpic curves found to be shifted rightwards for certain
maximum values of pressure and then shifted leftwards as depicted by red marks on the curves. The value of
డ்
ቀ ቁ at these maximum value state points for each isenthalpic curve is 0. The line joining these loci defines a
డ௉ ௛
parabolic curve, which is called inversion curve shown by dotted red line in the figure. The extrapolation of this
curve intercepts the T axis at two points. They are called maximum inversion temperature Tmax and minimum
inversion temperature Tmin respectively.

3. The inversion temperature curve separates p-T area into two regions; one is below this line, which is
cooling region and the other above the line called heating region. The inversion temperature of the gas or fluid
to be liquefied must lie between Tmax and Tmin and throttling pressure must be maintained accordingly.

డ்
4. To get maximum cooling, the pressure point must be set at the point, where ቀ ቁ = 0.
డ௉ ௛

5. The gas or fluid having inversion temperature above Tmax, the isenthalpic curve is always negative so it
is never possible to get cooling effect by throttling or Joule-Thomson expansion unless the inversion
temperature bring within the Tmin – Tmax range by any other means. For example helium has inversion
temperature -2400 C normal atmospheric pressure. So, it has to pre-cool before hand to bring its inversion
temperature below Tmax.
డ்
6. The slope ቀ ቁ is called the Joule-Thomson coefficient, denoted by ߤ௝ it can be derived from the
డ௉ ௛
thermodynamic potential. The enthalpy per unit mass basis can be written as:

݀ℎ = ݀‫ ݑ‬+ ‫ ݌݀ݒ‬-----------------------------------------------------------------------------------------------(2)

From the first law of thermodynamics, we know that

݀ܳ = ݀‫ ݑ‬+ ‫ݒ݀݌‬
ௗொ
Or, ܶ݀‫ ݑ݀ = ݏ‬+ ‫ݒ݀݌‬ [since, ݀‫= ݏ‬ ]
்

Or, ݀‫ ݏ݀ܶ = ݑ‬− ‫ ݒ݀݌‬------------------------------------------------------------------------------------------(4)

 3

Substituting ݀‫ ݑ‬from equation-4 into equation-3, we get

݀ℎ = ܶ݀ܵ − ‫ ݒ݀݌‬+ ‫ ݌݀ݒ‬---------------------------------------------------------------------------------(5)

డ௩
Or, ݀ℎ = ‫ܥ‬௣ ݀ܶ − ܶ ቀ ቁ ݀‫ ݌‬+ ‫݌݀ݒ‬
డ் ௣

డ௩
Or, ݀ℎ = ‫ܥ‬௣ ݀ܶ + [‫ ݒ‬− ܶ ቀ ቁ ]݀‫ ݌‬-----------------------------------------------------------------------(6)
డ் ௣

Equation-6 is known as differential Joule –Thomson effect.

At constant enthalpy, ݀ℎ = 0, , so equation – 6 can be written as:

డ௩
‫ܥ‬௣ ݀ܶ + ൤‫ ݒ‬− ܶ ቀ ቁ ൨ ݀‫ = ݌‬0
డ் ௣

డ௩
Or, ൤‫ ݒ‬− ܶ ቀ ቁ ൨ ݀‫ܥ = ݌‬௣ ݀ܶ
డ் ௣
డ௣ ଵ డ௩
Or, ቀ ቁ = ൤‫ ݒ‬− ܶ ቀ ቁ ൨
డ் ௛ ஼೛ డ் ௣
డ௣ ଵ డ௩
Therefore, ߤ௝ = ቀ ቁ = ൤‫ ݒ‬− ܶ ቀ ቁ ൨ -------------------------------------------------------------------(7)
డ் ௛ ஼೛ డ் ௣

From this equation-7, it can be said that for ideal gas the Joule-Thomson coefficient will always be zero, so it
can be cooled by throttling expansion, But for the real gas, the Joule-Thomson coefficient might be some value
either positive or negative depending on the initial pressure condition, so real gas can be cooled or heated
depending on the coefficient’s value.

Internal Work Method of Liquefaction

Principle of Operation

The essential of liquefaction using Joule-Thomson effect is diagrammatically described here with reference to figure-3.
In its operation, compressed gas enters the inner tube of heat interchanger, H at a pressure pA and temperature TA . It then
expands at the valve, V to a pressure pB and the temperature falls on account of the performance of internal works in
expanding the gas against the force of attraction between molecules in the gas as the system is kept heat insulated. The
cold expanded gas then passes up the outer tube and cooling the incoming compressed gas. This gas then leaves the
liquefier at pressure pB and temperature TB.. The cooler compressed gas again expands at the valve, V and thereby is
further cooled, and continued so on until the temperature at the lower end of the interchanger has fallen sufficiently to
liquefy. A part of the expanded gas will then be liquefied and collected at the flask C with temperature TC. This is the
principle of liquefaction of helium gas by differential Joule-Thomson effect or internal work.

pA TA
P B TB

Figure-3: Arrangement for understanding liquefaction principle by Joule-Thomson effect.

 4

Description of Helium Liquefier

The inversion temperature of helium is -2400 C. Kapitza first liquefied helium gas by pre-cooling it. In that helium
passed through a coil, which is surrounded by a bath containing liquid hydrogen boiling under reduced pressure. By thus
he was successful to cool helium to -2580C. With the advent of technology, many apparatus have been evolved. The
most used apparatus of liquefaction with the reference to figure – 4 is described here. In its operation, helium gas at a
pressure of 240 atm. enters the spiral tube at A and divides into two portions. One portion of helium gas passes through
the spiral tube S1 in E is cooled because it is surrounded by liquid hydrogen, boiling under reduced pressure. The other
portion of helium gas passing through the spiral tube S2 in F is cooled due to the outgoing cold helium gas. Similar
process takes place in spiral tubes S3 and S4 in E and F respectively. This process repeated and when the helium
temperature becomes sufficiently low i.e. below its inversion temperature, then the helium gas gets liquefied while
passing through the nozzle N due to differential Joule-Thomson effect. The outgoing helium gas is compressed again by
the compressor at P and fed back to the spirals S1 and S2 to continue its operation. The liquid helium is then collected at
the Dewar flask. The whole arrangement is surrounded by the Dewar flask to provide perfect heat insulation.

A
To Pump

S2 S1

F B E
C

S4 S3

Liquid Helium Liquid Hydrogen

Figure-4: Liquefaction apparatus

External Work Method of Liquefaction

Principle of Operation

Suppose a volume of gas, v1 enters the cylinder of an engine at a pressure P1. Then it expands adiabatically and
reversibly and doing work on some external system until the volume has increased to v2 and pressure has fallen to P2.
Then the total work done by the gas will be the difference in enthalpy before expansion and after expansion, which can
be expressed as:
௉
‫׬‬௉ ܲ݀‫ܪ = ݒ‬ଵ − ‫ܪ‬ଶ -------------------------------------------------------------------------------------------------(8)
భ
మ
 5

Accordingly the temperature has fallen from T1 to T2. Now if the state equation of the gas is as:

ܲ‫ = ܴܶ = ݒ‬൫‫ܥ‬௣ − ‫ܥ‬௩ ൯ܶ -------------------------------------------------------------------------------------------(9)

Where, ‫ܥ‬௣ ܽ݊݀ ‫ܥ‬௩ are the specific heat at constant pressure and volume respectively. Hence the total work done by the
gas can be expressed by using equation-9 as:

ܹ = ‫ܥ‬௣ (ܶଵ − ܶଶ ) = ‫ܪ‬ଵ − ‫ܪ‬ଶ -------------------------------------------------------------------------------------(10)

The final temperature will be as:

ംషభ
௉ ಴೛ ஼೛
ܶଶ = ܶଵ ቀ మቁ , where = ߛ -------------------------------------------------------------------------------------(11)
௉భ ஼ೡ

The temperature drop as calculated from equation-11 is greater than that obtained from the internal work method i.e.
from the Joule-Thomson or throttling process. So, external work method is more preferable for liquefaction of gas. The
application of this expansion engine to the liquefaction of gas forms the basis of the Claude and Heylandt methods.

Description of Claude and Heylandt methods of helium liquefaction

Figure-5 illustrates one type of Claude and Heylandt method for air liquefaction to produce low temperature down to 8
K. In its operation, air compressed to about 40 atm. passes through the heat interchanger I where it is cooled to 193 K by
the expanded gas. The gas then divides into two fractions; one fraction M passes through the heat interchanger II and the
other fraction (1-M) passes through the expansion engine, E. The gas expands in the engine E to pressure 1 atm. and does
external work and thereby cooled over there. This cooled gas then passes through the heat interchanger II and cools the
fraction M of the high pressure gas. The degree of expansion is so chosen that the temperature of the interchanger II and
III is considerably lower than the critical temperature but not as low as its normal boiling point. The fraction M is still at
high pressure and condenses in the interchanger II and III and after expansion to 1 atm. collects at L. A portion of the
liquid evaporates in the expansion valve through the valve and the vapors produced returns the the compressor via the
heat interchanger.

II

III

Figure-5: Claude Method for gas liquefaction

 6

Efficiency of Liquefier

Suppose a liquefier has reached to a steady state and is liquefying gas at a constant rate. A certain quantity of gas enters
the liquefier per second at a pressure pA and temperature TA. The gas expands to a pressure pB and temperature TB. Then
a certain fraction € is liquefied and collected at the bottom part of the liquefier at temperature TC. If the heat interchanger
is perfect then TB = TA. When the liquefier reached to the steady state condition, then we can equate the enthalpy of the
compressed gas entering the liquefier to the sum of the enthalpy of the liquid produced and that of the gas leaving the
liquefier. Accordingly if HA, HB and HC are the enthalpies per unit mass, then we get:

‫ܪ‬஺ = (1 − €)‫ܪ‬஻ + €‫ܪ‬஼

Or, ‫ܪ‬஺ = ‫ܪ‬஻ − €‫ܪ‬஻ + €‫ܪ‬஼

Or, €‫ܪ‬஼ − €‫ܪ‬஻ = ‫ܪ‬஺ − ‫ܪ‬஻

ுಲ ି ுಳ
Therefore, € = ------------------------------------------------------------------------------------------------------------(12)
ு಴ ି ுಳ

This fraction € is known as the efficiency of liquefaction

Conclusion

The production of low temperature is of great importance for experimental works to study the temperature dependent
parameters of the material. Liquid nitrogen generally used. Nowadays liquid helium is extensively used in the laboratory
for various temperature dependent measurements. So liquefaction of helium is one of the best options.. Joule-Thomson
effect has been utilized extensively for liquefaction of gases. Many methods so far have been evolved for this purpose.
Internal work method and external work method are the basis for the Claude and Heylandt method for the liquefaction of
gases. In the internal work method, the gas cools down by the performance of internal work against the force of
attraction between molecules when the gas expands adiabatically and irreversibly. On the other hand, the gas is cooled
down while the gas expanding adiabatically and reversibly, and doing some external works on to some other system.
This method is more favorable as because the drop of temperature is more as that of obtained from the internal work
method.

References

1. You Tube Lecture by Prof Dr. Shamol, Dept of Physics, MIT, India

2. Photo Copy Class Notes, provided from Dept of Physics, BUET, Dhaka, Bangladesh

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