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You are on page 1of 13

B.-Z. Maytal

*

,1

, G.F. Nellis, S.A. Klein, J.M. Pfotenhauer

The University of Wisconsin-Madison, Madison, WI 53706, USA

Received 3 November 2005; accepted 8 November 2005

Abstract

This paper explores the potential of mixed coolants at elevated pressures for JouleThomson cryocooling. A numerical model of a

JouleThomson cryocooler is developed that is capable of simulating operation with mixtures of up to 9 components consisting of hydro-

carbons, non-ammable halogenated refrigerants, and inert gases. The numerical model is integrated with a genetic optimization algo-

rithm, which has a high capability for convergence in an environment of discontinuities, constraints and local optima. The genetic

optimization algorithm is used to select the optimal mixture compositions that separately maximizes following two objective functions

at each elevated pressure for 80, 90 and 95 K cryocooling: the molar specic cooling capacity (the highest attainable is 3200 J/mol) and

the produced cooling capacity per thermal conductance which is a measure of the compactness of the recuperator. The optimized cooling

capacity for a non-ammable halogenated refrigerant mixture is smaller than for a hydrocarbon mixture; however, the cooling capacity

of the two types of mixtures approach one another as pressure becomes higher. The coecient of performance, the required heat transfer

area and the eect of the number of components in the mixture is investigated as a function of the pressure. It is shown that mixtures with

more components provide a higher cooling capacity but require larger recuperative heat exchangers. Optimized mixtures for 90 K cryo-

cooling have similar cooling capacity as those for 80 K. Optimized compactness for 80 K is about 50% higher than can be achieved by

pure nitrogen. For 90 K, no mixture provides a more compact recuperator than can be achieved using pure argon. The results are dis-

cussed in the context of potential applications for closed and open cycle cryocoolers.

2005 Published by Elsevier Ltd.

Keywords: JouleThomson coolers (E); Gas mixture (B); Cycle optimization (E)

1. Introduction: open and closed cycles and mixed coolants

JouleThomson cryocoolers may be classied as either

open cycle (OC) or closed cycle (CC). Initially, OC cryoco-

olers were operated using pure coolants at elevated pres-

sures. However, from the beginning the development of

OC cryocoolers was accompanied by attempts to close

the cycle [14]. The characteristics of the two categories

are very dierent. The central element of the CC cryocooler

is its compressor, which is a bulky, unreliable, an expensive

part of the system, and the source of vibrations. It is there-

fore desirable to reduce the operating pressure in a CC

cryocooler in order to alleviate these problems and also

lower the consumption of energy as characterized by an

improvement in the cycle COP (thermodynamic coecient

of performance).

The OC cryocooler is used for radiation detectors [57],

cryosurgical probes [810], and space applications [11]. The

OC cryocooler is energized by a gas reservoir which has the

function of extending the available operating period.

Therefore, elevated pressure becomes a desirable feature

of an OC cryocooler as high-pressure storage results in

more gas stored in a gas reservoir of xed volume and

therefore increased operating time. In contrast to the CC

systems, COP is not a major concern for OC systems

because the compression process does not occur at the site

of cryocooling. Another feature of OC JouleThomson

cryocooling is fast cooldown. Even if only a short run time

is required it is still necessary to use a high operating pres-

sure in order to maintain the high rate of cooldown.

0011-2275/$ - see front matter 2005 Published by Elsevier Ltd.

doi:10.1016/j.cryogenics.2005.11.005

*

Corresponding author. Tel.: +972 4908 7570; fax: +972 4990 6100.

E-mail address: benmay@rafael.co.il (B.-Z. Maytal).

1

On leave from Rafael, Ltd., P.O. Box 2250, Haifa 31021, Israel.

www.elsevier.com/locate/cryogenics

Cryogenics 46 (2006) 5567

The potential for mixed coolants to enhance Joule

Thomson cryocooling has allowed a dramatic reduction

in the operating pressure as compared with the pressure

required by traditional pure coolants in a JouleThomson

cycle. Mixed refrigerants allow ecient operation using a

single stage compression process, which provides operating

pressures that are below 2.5 MPa. Furthermore, to enable

lubrication of the compressor, the candidate mixtures are

expected to dissolve some lubricant contamination in their

liquid phase at the cryogenic temperature. Viable and gen-

eral-purpose JouleThomson closed cycle cryocoolers with

high COPs and prolonged reliable run times, driven by sin-

gle stage lubricated compressors. are currently available

[1216] both with and without phase separators [17,18].

Much less attention has been devoted to the potential of

mixed coolants in the context of OC cryocoolers. Note that

the low-pressure mixtures that have been developed for CC

operation are not applicable, in general, for high-pressure

operation as operation at elevated pressure will prevent

them from reaching the cryogenic temperatures. On the

other hand, harnessing these mixtures in an OC cryocooler

at low pressure will exhibit an unacceptably lower cooling

capacity and increase the size of the required gas reservoir.

There are several reported studies on OC cryocooling

with mixtures at elevated pressure. At the moderate pres-

sure range of 10 MPa, Brodianski et al. [19] demonstrated

experimentally the potential of mixtures to gain accelerated

cooldown. Brodianski demonstrated cooldown times with

mixtures that were eight times faster than could be

achieved using pure nitrogen at a similar volumetric ow

rate and pressure. Boiarski et al. [20] describes an experi-

ment with an open cycle regulated cryocooler fed through

two pressure vessels, each at 6.2 MPa to utilize the mixing

enthalpy. Chorowski [21] discussed open cycle operation

with mixtures of nitrogen with methane and nitrogen with

R-13 at pressures up to 14 MPa. Gong et al. [22] discussed

the use of nitrogen and hydrocarbon mixtures for acceler-

ating cooldown of open cycle JouleThomson cryocoolers.

Only a single analysis at higher pressures (up to 30 MPa)

has been reported: Maytal et al. [23] show how the cooling

capacity of a three component mixture can be optimized.

Little [24] used a 30 MPa mixed precoolant to accelerate

the cooldown of a nal nitrogen stage.

1

2 3

4

5

recuperator

evaporator

throttle

heat

load

gas

reservoir

or

compressor

high, operating

pressure

0.1 MPa

Q

P

system.

Nomenclature

A heat transfer area (m

2

)

COP coecient of performance

COP

C

coecient of performance of the reversible cycle

of Carnot

h specic enthalpy (J/kmol)

Dh

T

integral isothermal JouleThomson eect, (J/

kmol)

Dh

T,PP

value of Dh

T

at T

PP

(J/kmol)

_ n molar ow rate (kmol/s)

NTU number of thermal units, U A= _ n c

P

P pressure (Pa)

P

OP

pressure at which a mixture was optimized (Pa)

s specic entropy (J/kmol K)

T temperature (K)

T

AMB

ambient temperature, gas inlet temperature (K)

T

B

normal boiling point (K)

T

M

melting/solidication temperature (K)

T

OP

ambient temperature at which a mixture was

optimized (K)

DT

PP

minimum temperature dierence along the recu-

perator (K)

Q total amount of rejected heat at the cryocooling

temperature (J)

_

Q cooling capacity, heat load (W)

_

Q

REC

recuperated enthalpy (W)

V volume of a gas reservoir (m

3

)

U overall heat transfer coecient (W/m

2

K)

_

W minimum compressing power (W)

y

i

molar fraction of component i

Subscripts

1 to 5 states along the thermodynamic cycle, Fig. 1

i index of any component in mixture

j index of the sections along the recuperator in the

numerical model

I number of components in mixture

H high (pressure or temperature) stream

L low (pressure or temperature) stream

OP state at which a mixture was optimized

Greek

q density (kmol/m

3

)

Abbreviations

min

y

(x) minimum value of (x) while changing parameter

y

OC open cycle

CC closed cycle

OM optimal mixture

56 B.-Z. Maytal et al. / Cryogenics 46 (2006) 5567

Longsworth [25] employed binary mixtures of nitrogen

and argon at 40 MPa for open cycle fast cooldown. How-

ever, these two components have similar boiling points

and therefore no thermodynamic advantage is expected.

Indeed the operating temperatures and rates of cooling

were intermediate between the values that could be

attained using either of the two pure components.

The intended contribution of the present study is an

investigation of the potential of mixed coolants to improve

the performance of high-pressure OC cryocooler applica-

tions at 80, 90 and 95 K as alternatives for nitrogen and

argon.

2. The model, optimization procedure and tools

The layout and notation associated with the modeled

JouleThomson cryocooler are indicated in Fig. 1. The

cryocooler includes a recuperative heat exchanger, throttle

(constant enthalpy expansion), and the evaporator (or load

heat exchanger). A numerical model using the Engineering

Equation Solver software [26] was developed to simulate

the steady state operation of this cycle. The details of the

numerical model are described elsewhere [27] in the context

of optimization of a low-pressure mixture composition.

The thermophysical properties of the components and their

mixtures were obtained using the NIST4 numerical code,

also known as SUPERTRAPP [28]. Up to 9 component

mixtures can be considered with constituents that include

various hydrocarbons, halo-carbonated refrigerants, and

inert gases.

The total recuperated enthalpy,

_

Q

REC

_ n

h

1

h

2

h

5

h

4

1

is carried in N equal parts by each section, j, along the

recuperator.

The heat load supported by the evaporator,

_

Q

_ n

h

4

h

3

2

matches the cooling capacity of the cycle which is the min-

imum departure between the low- and high-pressure iso-

bars in the Th plane at the temperature range, (T

B

, T

AMB

),

_

Q

_ n

min

T

hP

L

; T hP

H

; T min

T

Dh

T

Dh

T;PP

3

The allowable minimum temperature dierence (the pinch-

point temperature dierence), DT

PP

, is an input parameter

to the model which reects the nite real nature of the lim-

ited area recuperative heat exchanger,

DT

PP

minT

H

T

C

4

The required heat transfer area or thermal conductance

(U A)

j

of the jth section may be determined using the eec-

tivenessNTU relationship for a counter ow heat exchan-

ger. Other input parameters to the model include: the inlet

pressure and temperature of the mixture at state 1, (P

1

, T

1

),

the molar ow rate, _ n, the temperature of cryocooling, T

4

,

the species and their fractions, y

i

, and the outlet pressure,

P

5

, which was assumed to be 0.1 MPa for all of the results

presented here.

The minimum compressing power (corresponding to a

reversible and isothermal compression process) is,

_

W

min

_ n

T

1

s

5

s

1

h

5

h

1

5

which enables one to obtain the maximum possible coe-

cient of performance,

COP

_

Q

_

W

min

6

The solution for the temperature proles along the recu-

perator is obtained iteratively by adjusting the hot temper-

ature dierence, T

1

T

5

until the specied pinch-point

temperature dierence is achieved. For pure coolants, the

pinch-point occurs at the hot end and therefore the hot

temperature dierence coincides with DT

PP

.

The numerical model is integrated with a genetic opti-

mizing algorithm [29] implemented in Engineering Equa-

tion Solver that is characterized by a high capability for

nding the global optima of a target function even if the

function and/or its derivatives and constraints are non-

continuous. The genetic optimization algorithm is not

confused by local optima and converges to the global

one.

The scope of optimization is to maximize one of three

target functions: the cooling capacity, the coecient of per-

formance, or the compactness of the recuperator,

_

Q=U A. Computations are repeated after adjusting the

composition by the genetic optimizer for further improve-

ment of the objective function. Results are generated for

dierent values of: (a) high pressure, (b) number of species,

(c) ambient temperatures, and (c) cryocooling temperatures

(either 80 or 90 K).

The domain of the optimized-mixture compositions is

restricted by considerations of solidliquid equilibrium in

order to avoid clog formation at the throttle. A conserva-

tive approach was adapted in this regard; the freezing tem-

perature of the mixture, T

M

, was estimated according to

T

M

6

X

I

i1

y

i

T

M;i

7

and the choice of components for 80 K cryocooling was

restricted so that,

T

M

6 T

B

nitrogen 8

On the one hand, some rise of the boiling point of the mix-

ture may be expected, even if it is relatively small and re-

mains in the 80 K cryocooling range. On the other hand,

even a small presence of nitrogen, like a few percent, is ade-

quate for the mixture to reach the boiling point of nitrogen

B.-Z. Maytal et al. / Cryogenics 46 (2006) 5567 57

[30]. The condition guaranteeing a non-clogging operation

then is

T

3

PT

M

9

The optimized mixtures for 90 K cryocooling still employ a

substantial fraction of nitrogen as the lowest boiling point

specie. Therefore, their throttle exit remains at the same

temperature and the restriction (8) remains valid.

Optimizing the composition for maximum

_

Q= _ n may be

accomplished entirely in the Th plane. However, the inte-

gration along the recuperator serves to determine its size

and therefore allows optimization of the composition for

the most compact heat exchanger.

3. Specic cooling capacity

3.1. General scope

Two types of mixtures were examined for cryocooling at

80 K. The components of the rst type of mixtures are

mainly hydrocarbons and are selected from group I as

listed in Table 1. The second type of mixture contains

mostly halogenated derivatives of hydrocarbons which

are selected from group II listed in Table 1. Mixtures of

the rst type (group I components) are ammable whereas

mixtures of the second type (group II components) are not.

The composition of each mixture was optimized at a spe-

cic pressure, P

OP

, for maximum specic cooling capacity,

_

Q= _ n.

The lowest boiling point component for either of the

two groups is nitrogen. The components have to be chosen

so that their normal boiling points will be uniformly dis-

tributed over the entire temperature range from 80 to

300 K so that the occurrence of a pinch-point at some

intermediate temperature might be avoided; the pinch-

point constitutes the bottleneck (literarily, in the Th plan)

that xes the value of

_

Q= _ n that can be obtained. This

discussion is consistent with Littles [31] formulation of

the optimal mixture, namely, equidistant high and low-

pressure isobars in the Th plan.

The contribution of each additional component

becomes more signicant as its involvement bisects and

narrows a larger gap between the boiling points of other

components. Therefore, CF

4

, a non-ammable component,

is included in group I to narrow the wide gap (73 K)

between methane and ethane. Mostitski et al. [32] com-

mented in 1981 on the possibility of improving the e-

ciency of hydrocarbon mixtures by employing the

component CF

4

. Luo et al. [33,34] discussed the benet

of including CF

4

in comparison to mixtures of hydrocar-

bons only. Sometimes acetylene, C

2

H

4

, is also included in

order to bridge the gap between methane and propane

[35,36]. A dierent reason motivates the presence of argon

in the mixture. Argon has a signicantly larger integral

JouleThomson eect, Dh

T

, than nitrogen, in spite of hav-

ing a similar boiling point.

3.2. Hydrocarbon mixtures

Mixtures were optimized in which all 9 components in

group I were allowed. In addition, 3, 6, 7 and 8 component

mixtures were considered in which only some of the con-

stituents listed in group I were considered. The heat rejec-

tion temperature used for the optimization, T

OP

, was 290 K

for cryocooling at 80 K. The optimized

_

Q= _ n as a function

of the corresponding P

OP

are displayed in Fig. 2. Each

curve belongs to a specic group of components. These

curves do not describe a single mixture since each of the

points on a given curve represents a dierent composition

that is optimal for the specic pressure. Therefore, each

curve may be regarded as corresponding to a virtual cool-

ant that is referred to as the Optimized Mixture (OM) given

a set of components and operating condition. This view-

point is analogous to the pure coolants pressure dependent

Dh

T

(at ambient or inlet temperature) which reects the

highest attainable

_

Q= _ n. Note that Fig. 2 illustrates the cool-

Table 1

Two groups of candidate components to comprise optimized mixtures: the

hydrocarbons (I) and the halogenated hydrocarbons (II)

Group I T

B

[K] Group II T

B

[K]

Nitrogen N

2

77.2 N

2

77.2

Argon Ar 87.3 Ar 87.3

Methane CH

4

111.7 CH

4

111.7

R14 CF

4

145.1 CF

4

145.

Acetylene C

2

H

4

169.1 R23 190.0

Ethane C

2

H

6

184.5 R116 194.7

Propane C

3

H

8

231.2 R32 221.2

Isobutane C

4

H

10

263 R125 224.7

Isopentane C

5

H

12

300.6 R134a 246.8

0 10 20 30 40 50

0

500

1000

1500

2000

2500

3000

methane

7

6

3A

3B

8

argon

nitrogen

3C

9

Q n

J mol

290 K =

AMB

T

80 K

cryocooling

methane

7

6

3A

3B

8

argon

nitrogen

3C

9

[ ]

OP

P [MPa]

Fig. 2. Optimized specic cooling capacity of various hydrocarbon

mixtures (OM curves) as a function of the pressure of optimization. Each

curve indication represents the mixture by the number of its components.

Nitrogen, argon, and methane are shown for reference. (9) N

2

, A, CH

4

,

CF

4

, C

2

H

4

, C

2

H

6

, C

3

H

8

, C

4

H

10

, C

5

H

12

; (8) like 9 without C

2

H

4

; (7) like 8

without CF

4

; (6) like 7 without C

5

H

12

; (3A) N

2

, C

2

H

6

, C

3

H

8

; (3B) N

2

,

C

3

H

8

, C

4

H

10

; (3C) N

2

, CH

4

, C

2

H

6

.

58 B.-Z. Maytal et al. / Cryogenics 46 (2006) 5567

ing capacity,

_

Q= _ n , as a function of a mixtures optimiza-

tion pressure, P

OP

, but not the operating pressure, P.

Therefore it does not describe the cooling capacity

achieved during a discharge process of a gas reservoir.

Fig. 2 includes for reference the

_

Q= _ n (which is equivalent

to the Dh

T

(P)) for nitrogen, argon and methane. The com-

position of these pure refrigerants does not change with

pressure and therefore these are the corresponding dis-

charge curves. The use of nitrogen, argon, and methane

are appropriate for cryocooling at about 78 K, 88 K and

112 K, respectively. Note that the optimized mixtures have

higher

_

Q= _ n than argon at any pressure and even higher

than methane below 20 MPa.

Any optimized mixture that is obtained from a larger

group of components that contains as its basis a smaller

group of components must perform better than the original

mixture obtained from the smaller group. In other words,

the 9 component OM in Fig. 2 must perform better than

the 8 component OM which, in turn, must perform better

than the 7 component OM and so on. The reason is that

at any pressure, the domain of optimization of the original

OM is entirely included in the domain of the mixtures of

more components. Put another way, the optimization pro-

cedure always has the option to abandon the additional

components of the larger group, by reducing their molar

concentration, if necessary in order to obtain a larger

_

Q= _ n. Indeed, Fig. 2 shows that the various OM curves do

not intersect and the one with most components will exhi-

bit the highest

_

Q= _ n.

Synthesizing mixtures of 8 components with boiling

points distributed quite evenly along the entire range of

temperatures from 80 to 300 K provides the condence

that the optimization procedure does not require any

additional and intermediate components for further

enhancement of

_

Q= _ n. Therefore,

_

Q= _ n of this OM is

expected to be the envelope that encompasses any possible

hydrocarbon mixture or at least a very good approxima-

tion of this envelope. Indeed, Fig. 2 shows that the inclu-

sion of a 9th component, which in this case is C

2

H

4

, does

not elevate the performance noticeably at any optimization

pressure even though its boiling point bisects the 40 K gap

that otherwise exists between CF

4

and C

2

H

6

.

As observed in Fig. 2, the

_

Q= _ n curves of the OM exhibit

a peaking behavior with pressure that is similar to the Dh

T

of pure gases. However, the peak occurs at lower pressures

and is not related to the inversion of the JouleThomson

eect. The peaking pressure associated with the 8 compo-

nent OM clearly designates the highest attainable cooling

capacity,

_

Q= _ n, that can be achieved by any mixture at

any pressure. The highest value of

_

Q= _ n observed in this

study is 3180 J/mol for a heat rejection temperature of

290 K. The corresponding peak pressure is about 20 MPa

and its composition is listed in Table 2 (together with opti-

mized compositions at 10 and 40 MPa). However, notice

that the peak is relatively shallow and a cooling capacity

of nearly 93% of this optimal value may be reached at

7 MPa; albeit using a mixture with a dierent composition.

For nitrogen at a similar cryocooling temperature, the

cooling capacity

_

Q= _ n is 1200 J/mol at about 40 MPa and

for argon it is 1800 J/mol at 55 MPa.

The three component mixtures N

2

C

2

H

6

C

3

H

8

and

N

2

C

3

H

8

C

4

H

10

develop maximum

_

Q= _ n of about 2620

J/mol and 2430 correspondingly, which is more than twice

that of pure nitrogen; these results are consistent with the

optimized peaking values obtained by Maytal et al. [23].

The mixture N

2

CH

4

C

2

H

6

reaches 2520 J/mol at about

45 MPa. Six components bring

_

Q= _ n closer to the envelope

represented by the 8 component OM and achieves a peak

cooling capacity of 2960 J/mol. There is essentially no dif-

ference in performance exhibited by the 7 and 8 component

OM in the high-pressure region, however the addition of

the 8th component (which is CF

4

) does improve

_

Q= _ n at

lower pressures.

The 7 and 8 component OMs are partially condensed at

the elevated pressures and the discussed temperature of

290 K which means at the inlet to the recuperator. How-

ever, the gas phase mass fraction is at least 90%. The pos-

sibility of enjoying higher

_

Q= _ n and COP by allowing a

coolant to stay in two-phase outside the recuperator was

previously mentioned in the literature in the context of

low-pressure mixtures for CC cryocoolers. Alexeev et al.

[15,37] and Boyarski et al. [38,39] compared the perfor-

mance of the two classes of Gas Refrigerant Supply

(GRS) and Liquid Refrigerant Supply (LRS). On the other

Table 2

Composition of mixtures (percent mole fractions) of 8 hydrocarbon components optimized at three values of P

OP

= 10, 20 and 40 MPa at 290 K for

maximum

_

Q= _ n

P [MPa]

_

Q= _ n [J/mol] N

2

A CH

4

CF

4

C

2

H

6

C

3

H

8

C

4

H

10

C

5

H

12

1.5 1464 54.1 3.4 10.5 12.1 5.2 5.2 0.0 9.5

3 2171 55.2 0.2 7.6 13.7 13.3 0.7 0.0 9.3

5 2751 60.4 0.1 5.0 11.1 11.6 0.8 3.0 8.0

7 2947 61.2 4.3 5.0 5.5 11.4 2.1 3.8 6.7

10 3080 64.6 2.0 9.8 1.7 9.0 5.0 0.6 7.3

20 3180 70.2 2.3 8.6 1.3 7.2 2.2 1.2 7.0

30 3070 74.6 0.0 7.4 2.5 6.2 2.0 1.0 6.3

40 2930 75.5 2.3 6.0 2.6 4.7 2.1 1.7 5.1

The highest attainable

_

Q= _ n value occurs at 20 MPa.

B.-Z. Maytal et al. / Cryogenics 46 (2006) 5567 59

hand, the ow of the two-phase might be heterogeneous

and therefore the performance will be aected by the

details in this ow regime.

The liqueed part of the 7 component OM includes a

substantial portion of the higher boiling point component,

which is isopentane. This component was removed for the

6 component OM and therefore the 6 component OM is

more likely to be in a single phase at the elevated pressure.

Notice that the performance of the 6 component OM is

only slightly worse than the 7, 8, or 9 component OM.

For instance, the 7 components OM at 20 MPa and

30 MPa, both at 290 K, are of two phases. Their gas phase

mass fractions are 90% and 97.5% correspondingly. On the

other hand, the 6 components OM at 25 MPa and 290 K is

of single phase. This mixture is mentioned in Section 10.1

for comparison and its composition is displayed in Table

5, optimized for 80 K cryocooling.

The composition of the OMs at elevated pressures, nom-

inally above 5 MPa, are not aected by the melting point

restriction and thus strongly fulll the inequality repre-

sented by Eq. (8). However, at lower pressures, this melting

point restriction becomes constraining and the optimized

compositions are on the boundary of this restriction and

Eq. (8) is fullled as an equality. The melting point restric-

tion therefore limits the share of higher boiling point com-

ponents in the mixture which in general also have higher

values of T

M

and Dh

T

[40]. Therefore, it might be that

the optimized

_

Q= _ n is underestimated at low pressures and

the actual values may be higher if the suppression of the

solidication point of the blend were accurately accounted

for. However, this issue was already discussed for low-pres-

sure mixtures for CC cryocoolers [23,41] and is not the

focus of the present study. Even though Table 2 displays

some compositions of OM at the lower pressure range gen-

erated by this study.

3.3. Halogenated hydrocarbon mixtures

The results of optimizing

_

Q= _ n for mixtures based on the

halogenated hydrocarbon refrigerants summarized as

group II in Table 1 are displayed in Fig. 3. The values of

_

Q= _ n for these OMs are smaller than can be achieved using

hydrocarbon components from group I (the 8 component

hydrocarbon envelope previously shown in Fig. 2 is also

shown in Fig. 3). The shortfall in performance is particu-

larly true in the low and intermediate pressure range; how-

ever, the performance of the halogenated hydrocarbons

approaches that of the hydrocarbons at pressures above

35 MPa.

The boiling points of the halogenated hydrocarbon

components are distributed less uniformly than those of

the hydrocarbons. Therefore, the inclusion of the 9th com-

ponent which is (the ammable) methane in order to nar-

row the 57 K boiling points gap between argon and R14

does somewhat enhance

_

Q= _ n at elevated pressures. At

50 MPa, the value of about 2500 J/mol for halogenated

hydrocarbon only becomes 2600 J/mol when including

methane. Another obstacle is the higher T

M

value that is

typical of the components in group II which causes these

OMs to be on the border of the solidication constraint

represented by Eq. (8) for most of the optimization pres-

sures. Consequently, it is not possible to include higher

boiling point components as much as would otherwise be

optimal from the standpoint of enhancing

_

Q= _ n. Refriger-

ants that are currently banned, such as R12, R13 and

R21, or an alternative substitute that has a similarly lower

T

M

value would close the gap between the OM based on

hydrocarbons and the synthetic refrigerants. The synthetic

refrigerant OM also exhibits a peaking behavior; the larg-

est

_

Q= _ n occurs at 35 MPa and the associated composition

is listed in Table 3 together with two other synthetic

OMs that are optimized at 20 and 45 MPa.

4. Coecient of performance of optimized mixtures

The COP at elevated pressure is another reection of the

improved cooling capacity of the OM. The COP as a func-

tion of optimization pressure is shown in Fig. 4 for mix-

tures optimized from the same groups of components

that are employed from the hydrocarbon category (group

I in Table 1) and discussed in the previous section in the

context of Fig. 2. The OMs with more components and

higher

_

Q= _ n also exhibit higher COP and the COP shows

the same peaking behavior with respect to pressure. How-

ever, the pressure associated with the highest COP is some-

what lower than the peak pressure associated with; this

behavior is similar to pure gases as discussed by Mann

et al. [42]. The curve associated with the 8 component

OM again represents an envelope that encompasses the

performance associated with other, partial groups of com-

ponents. This envelope has the signicance of representing

0 10 20 30 40 50

0

500

1000

1500

2000

2500

3000

Q n

[ ] J mol

290 K =

AMB

T

80 K

cryocooling

OP

P [MPa]

argon

nitrogen

8-HC

3-HC

8-HH

Fig. 3. Optimized specic cooling capacity of halogenated hydrocarbon

mixtures (OM curves) as a function of the pressure of optimization. For

reference are shown hydrocarbon mixtures, nitrogen and argon. Each

curve indication represents the mixture by the number of its components.

(8-HH) N

2

, A, R14, R23, R32, R134a, R116 and R125; (8-HC) N

2

, A,

CH

4

, CF

4

, C

2

H

6

, C

3

H

8

, C

4

H

10

, C

5

H

12

; (3-HC) N

2

, C

2

H

6

, C

3

H

8

.

60 B.-Z. Maytal et al. / Cryogenics 46 (2006) 5567

the highest achievable COP with a JT cycle with any mix-

ture at any pressure; Fig. 4 shows that for a heat rejection

temperature of 290 K, the maximum COP is 0.19 which is

50% of the COP that can be achieved by a reversible

Carnot cycle, COP

C

. The maximum COP is achieved at

an optimization pressure of only 5 MPa by a mixture of

a composition that is listed in Table 4 and includes about

60% nitrogen. One may compare it with the composition

of the mixture that optimizes

_

Q= _ n (which peaks at

20 MPa) that includes 70% nitrogen (Table 2). The peak

COP associated with pure nitrogen is about 0.07 and this

peak is reached at about 30 MPa. For argon 0.11 is the

peak COP which is achieved at about 40 MPa. Therefore,

not only is the COP of the OM doubled in comparison with

a pure substance but it is also achieved at one eighth of the

pressure. The halogenated hydrocarbon mixtures reach a

maximum COP of about 0.14 at a pressure of 32 MPa

for the same 290 K heat rejection temperature and 80 K

cryocooling temperature.

An alternative attempt was made to optimize directly

the COP (instead of the cooling capacity) as an objective

function for each pressure and it was found that the same

composition that maximizes

_

Q= _ n also maximizes the COP.

This result may be explained by the extremely weak depen-

dence of the compression work on the composition of the

mixture.

5. Temperature eect on optimized mixtures

The T

AMB

, of an operating mixture has to be considered

in reference to the temperature for which it was optimized,

T

OP

. There are three aspects associated with the inuence

of temperature on

_

Q= _ n for an OM. In general, the inuence

of ambient temperature becomes more sensitive at lower

pressures.

5.1.

_

Q= _ n dependence on T

OP

As the temperature for which the optimization is per-

formed, T

OP

, is raised,

_

Q= _ n degrades quite moderately.

Fig. 5 shows the 7 component OM, optimized at 290 and

at 333 K; these curves represent dierent mixtures as the

optimization conditions for each are dierent. At elevated

pressures, above 10 MPa, the dierence between the two

curves remains within 15%. The optimization procedure

compensates for the higher temperature by changing the

composition so that the concentration of the higher boiling

point components is increased. Therefore, it is possible to

optimize a mixture for operation at elevated temperature

with a relatively small sacrice of

_

Q= _ n.

5.2.

_

Q= _ n dependence on T

AMB

when T

AMB

> T

OP

The most evident situation is when T

AMB

= T

OP

(for

example, the curves where T

AMB

= T

OP

= 290 K and

T

AMB

= T

OP

= 333 K) so that the OM operates at the

Table 4

Composition (percent mole fractions) of 8 components optimized mixture that exhibits the peaking COP value of 0.19 at 290 K reached at the pressure of

5 MPa

N

2

A CH

4

CF

4

C

2

H

6

C

3

H

8

C

4

H

10

C

5

H

12

60.4 0.1 5.0 11.1 11.6 0.8 3.0 8.0

0 10 20 30 40 50

0

0.02

0.04

0.06

0.08

0.1

0.12

0.14

0.16

0.18

0.2

7

8

nitrogen argon

6

3A

3B

3C

COP

OP

P [MPa]

290 K =

AMB

T

80 K

cryocooling

7

8

nitrogen argon

6

3A

3B

3C

Fig. 4. Coecients of performance as a function of the pressure of

optimization (OM curves). The various hydrocarbon mixtures were

optimized for highest

_

Q= _ n. Each curve indication represents the mixture

by the number of its components. Nitrogen and argon are shown for

reference. (8) N

2

, A, CH

4

, CF

4

, C

2

H

6

, C

3

H

8

, C

4

H

10

, C

5

H

12

; (7) like 8

without CF

4

; (6) like 7 without C

5

H

12

; (3A) N

2

, C

2

H

6

, C

3

H

8

; (3B) N

2

,

C

3

H

8

, C

4

H

10

; (3C) N

2

, CH

4

, C

2

H

6

.

Table 3

Composition (percent mole fractions) of mixtures of 8 halogenated hydrocarbon components optimized at 3 values of P

OP

= 20, 35 and 45 MPa at 290 K

for maximum

_

Q= _ n

P [MPa]

_

Q= _ n [J/mol] N

2

A R14 R23 R116 R32 R125 R134a

20 2260 76.0 0.0 0.0 18.7 0.0 4.2 0.5 0.6

35 2700 73.5 3.6 7.9 6.6 0.2 3.8 0.5 3.9

45 2550 81.1 0.2 6.1 2.0 1.5 0.0 2.3 6.8

The highest attainable

_

Q= _ n value occurs at 35 MPa.

B.-Z. Maytal et al. / Cryogenics 46 (2006) 5567 61

temperature that it was optimized for. However, practically

the mixture must operate over a range of ambient temper-

atures that might be higher than T

OP

. Fig. 5 shows mix-

tures which were optimized at room temperature,

T

OP

= 290 K, but operate at an ambient temperature of

60 C so that T

AMB

= 333 K. In this case, the sensitivity

to the higher ambient temperature is much more pro-

nounced than if the mixture was optimized for operation

at 333 K (i.e., the performance for the OM with

T

AMB

= 333 K and T

OP

= 290 K is signicantly less than

the OM with T

AMB

= 333 and T

OP

= 333 K). The reduc-

tion in performance associated with operation at 333 K is

more than doubled at 50 MPa as compared with the

previous case where the mixture is optimized for high-

temperature operation; the reduction in performance is

even more dramatic below 30 MPa. Note that the local,

non-smooth behavior marked by X in Fig. 5 is not

expected but remains even when the components CF

4

and C

2

H

4

are added to the mixture.

5.3.

_

Q= _ n dependence on T

AMB

when T

AMB

< T

OP

Operation at an ambient temperature below the optimi-

zation temperature for an OM is not accompanied with a

signicant gain in

_

Q= _ n as it would be for a pure gas; instead,

the cooling capacity remains almost the same for any oper-

ating temperature T

AMB

that is below. Since optimized mix-

tures have two equidistant isobars of low and high pressure

in the Th plane, the case of lower T

AMB

is described by the

same isobars and the same separation in the h direction.

This separation denes

_

Q= _ n and therefore, in principle,

the cooling capacity should remain unchanged. However,

practically, the optimization process is not absolutely per-

fect and the two isobars are not completely equidistant.

For instance, the 7 component mixture that is optimized

at 20 MPa and T

OP

= 333 K exhibits

_

Q= _ n 2897 J/mol

when it is operated at 333 K. When the same OM is oper-

ated at lower temperatures, T

AMB

= 300, 290, 260, 240,

220 K, the corresponding calculated

_

Q= _ n values are 2866,

2872, 2865, 2872 and 2875 J/mol. These values are close

to the optimized value, 2897 J/mol, within 0.41%. The

small deviations reect the well-optimized nature of that

particular composition.

Based on this discussion, a reasonable strategy is to opti-

mize the mixed coolant for the highest probable operating

temperature, T

AMB

. The associated

_

Q= _ n will be somewhat

lower than the largest attainable, however, it will remain

almost the same value over the entire range of lower T

AMB

.

6. Recuperator sizing for optimized mixtures

The

_

Q= _ n values of previously discussed OMs were ideal

in the sense of fully utilizing an unlimited heat transfer

area. In order to obtain the required heat transfer area

associated with the various OMs, a minimum temperature

dierence between the recuperating streams of DT

PP

= 3 K

is assumed. The numerical model determines for each step

the required amount of thermal conductance and normal-

izes this thermal conductance, (U A)

j

against the local

minimum average capacity rate, _ n c

P;j

where,

c

P;j

minc

P;H

; c

P;L

10

In this way, the corresponding non-dimensional element of

heat exchanger size is expressed in terms of the Number of

Transfer Units, NTU

j

, for each element. The summation

of these local number of transfer units provides the total

NTU of the entire recuperator

NTU

X

N

j1

U A

j

_ n c

P;j

11

Fig. 6 displays the pressure dependence of the NTU de-

manded by some of the OMs with the same groups of com-

ponents that were previously discussed in comparison to

that of pure nitrogen and argon. In general, mixed coolants

even at elevated pressure are more demanding in terms of

NTU than pure nitrogen. This observation has been dis-

cussed elsewhere in the context of low-pressure mixtures

for CC cryocoolers [43]. The more ecient OMs in terms

of

_

Q= _ n and COP have more components and therefore pro-

vide a lower average temperature dierence between the

recuperating streams. This characteristic necessitates larger

overall thermal conductance, U A and therefore the asso-

ciated NTU becomes higher.

However, the physical sizes of the recuperators for

mixed coolants and pure nitrogen cannot be compared

on the basis of NTU. A signicant portion of both chan-

nels of mixed coolant recuperator includes two phase ow

while for nitrogen (and other pure gases) both channels

carry a single phase which is gas. The heat transfer coe-

cient in the former case is associated with boiling and

may be signicantly larger (by a factor of 23) than of pure

nitrogen. This counter aspect tends to reduce the physical

0 5 10 15 20 25 30 35 40 45 50

0

500

1000

1500

2000

2500

3000

argon

333 K

290 K

333 K

nitrogen

Q n

[ ] J mol

OP

T

333 K

290 K

333 K

290 K

333 K

X

80 K

cryocooling

290 K

AMB

T

0 5 10 15 20 25 30 35 40 45 50

0

500

1000

1500

2000

2500

3000

argon

333 K

290 K

333 K

nitrogen

[ ]

OP

P [MPa]

X

T

Fig. 5. The aect of elevating the temperature of optimization, T

OP

, and

the ambient temperature, T

AMB

, on cooling capacity as a function of the

pressure of optimization (OM curves) for 7 component mixtures. The

mixtures were optimized for highest

_

Q= _ n and include the 7 components,

N

2

, A, CH

4

, C

2

H

4

, C

2

H

6

, C

3

H

8

, C

4

H

10

, C

5

H

12

.

62 B.-Z. Maytal et al. / Cryogenics 46 (2006) 5567

size of the mixed coolant recuperator thus narrowing the

dierence between the physical sizes of the two.

7. Open cycle application

7.1. Discharge process of a reservoir

High-pressure coolants are traditionally applied to OC

cryocooler systems where a gas reservoir discharges

through the JouleThomson cryocooler. If the discharge

process occurs slowly, then the gas reservoir may be

regarded as isothermal during this process. As previously

discussed, the cooling capacity

_

Q= _ n as a function of pres-

sure for the 6 component OM of group I, as is shown in

Fig. 7, is not a description of a discharge process; each

point along this curve represents a dierent mixture com-

position. Fig. 7 shows the discharge process associated with

5 of these OMs for which the pressure of optimization,

P

OP

, is 50, 40, 35, 30 and 25 MPa; these curves are gener-

ated assuming an isothermal discharge process and the

instantaneous

_

Q= _ n are displayed as a function of pressure.

Each of these mixtures may also be examined at a higher

pressure than the one for which it was optimized. Note that

the values of

_

Q= _ n at any pressure dierent from the optimi-

zation pressure must lie below the envelope of OM. Fig. 7

shows the pressure dependence above and below P

OP

for

P

OP

= 25 MPa (only a short portion of the curve at higher

pressure is shown in order to avoid unnecessarily compli-

cating the gure).

The proper criteria for comparing the performance of a

mixture for an OC cryocooler would be the total refrigera-

tion provided at the payload, Q, per unit volume of the res-

ervoir. The ow demand is assumed to be ideal in the sense

of instantaneously matching the specic cooling capacity

and heat load (as described elsewhere [44] for pure cool-

ants) then,

Q

V

Z

P

F

P

I

Dh

T;PP

dq 12

from the initial high pressure, P

I

to the nal one, P

F

. To

accomplish this integration, one would need the density

dependence of

_

Q= _ n during the isothermal discharge pro-

cess, as shown in Fig. 8 for the same ve optimized mix-

tures that were previously described. Fig. 8 also shows

the P

OP

= 25 MPa OM at P > P

OP

. The area below these

curves represents the Q/V values for the various coolants.

The curve of P

OP

= 50 MPa exhibits some uctuations as

0 10 20 30 40 50

0

10

20

30

40

50

NTU

OP

P [MPa]

290 K =

AMB

T 80 K cryocooling

argon

nitrogen

8-HC

6-HC

3-HC

8-HH

=

PP

T 3K

290 K =

AMB

T

8-HC

6-HC

3-HC

8-HH

=

PP

T 3 K

Fig. 6. The required sizes of recuperators performing with DT

PP

= 3 K, as

a function of the pressure of optimization (OM curves). The mixtures were

optimized for highest

_

Q= _ n. Each curve indication represents the mixture by

the number of its components. Nitrogen and argon are shown for

reference. (8-HC) N

2

, A, CH

4

, CF

4

, C

2

H

6

, C

3

H

8

, C

4

H

10

, C

5

H

12

; (6-HC)

like 8-HC without CF

4

and C

5

H

12

(3-HC) N

2

, C

2

H

6

, C

3

H

8

; (HH) N

2

, A,

R14, R23, R32, R134a, R116 and R125.

0 10 20 30 40 50

0

500

1000

1500

2000

2500

3000

Q n

[ ] J mol

Optimized mixtures

discharge

25 30

35

40

50 MPa

argon

nitrogen

290 K =

AMB

T

80 K

cryocooling

curves

OP

P

50 MPa

P [MPa]

Fig. 7. Cooling capacity pressure dependence during isothermal discharge

process. The mixtures were optimized for highest

_

Q= _ n and include the 6

components: N

2

, A, CH

4

, C

2

H

6

, C

3

H

8

, C

4

H

10

: the dashed line for

P

OP

= 25 MPa is extended for P > P

OP

.

0 2 4 6 8 10 12 14 16 18

500

1000

1500

2000

2500

3000

Q n

[ ] J mol

Optimized mixtures

[ ] J mol

25

30

40

50 MPa

20

5

7

10

argon

nitrogen

80 K

cryocooling

10

290 K =

AMB

T

50

30

50

OP

P

discharge

curves

0 2 4 6 8 10 12 14 16 18

500

1000

1500

2000

2500

3000

Q n

[ ] J mol

[ ] J mol

50 MPa

10

290 K =

AMB

T

process. The mixtures were optimized for highest

_

Q= _ n and include the 6

components: N

2

, A, CH

4

, C

2

H

6

, C

3

H

8

, C

4

H

10

: the dashed line for

P

OP

= 25 MPa is extended for P > P

OP

.

B.-Z. Maytal et al. / Cryogenics 46 (2006) 5567 63

a function of q although the curve is smooth when shown

as a function of P; this seems to reect a diculty with the

numerical properties correlations rather than any real

behavior.

7.2. Examples

The OM for P

OP

= 40 MPa remains single phase in the

gas reservoir while discharging from P

OP

to 5 MPa. The

integral shown in Eq. (12) shows that this mixture provides

a gas reservoir volume specic refrigeration capacity of Q/

V = 22.1 kJ/L. Pure nitrogen for the same pressure range

discharge can provide only 10 kJ/L Furthermore, the cut

o pressure for pure nitrogen at a similar heat load would

be about 10 MPa (because of the lower specic cooling

capacity) therefore, the Q/V would be reduced to only

8.8 kJ/L.

The OM associated with P

OP

= 35 MPa becomes two

phase below about 11 MPa; this pressure may therefore

be considered to be the practical limit to the nal pressure

of the discharge process. Even so, the Q/V integral for the

OM associated with 35 MPa is 18 kJ/L from 35 MPa to

11 MPa, which is more than twice that of nitrogen at

40 MPa.

The OM associated with P

OP

= 50 MPa discharging

from a reservoir from 50 MPa to 10 MPa can provide Q/

V as high as 25 kJ/L. Nitrogen at the same pressure range

provides only 11.3 kJ/L.

Indeed, Q/V increases for higher P

OP

mixtures in the

case where the reservoir is assumed to be charged initially

to P

OP

. However, a gas reservoir may be charged to a

higher pressure than P

OP

in which case each of the OMs

shown in Fig. 8 have similar Q/V integrals. In this case,

the OMs with higher P

OP

are more likely to stay single

phase during the discharge process.

8. Closed cycle application

The

_

Q= _ n of OM of group I (Fig. 2) increase quite shar-

ply up to pressures of about 10 MPa where they have

achieved most of the cooling capacity that is possible,

about 3000 J/mol and close to 50% of COP

C

. This strong

pressure dependence at low pressures is characterized by

a slope of about 400 J/mol per 1 MPa. (The pressure

dependence for pure nitrogen is only 50 J/mol per

1 MPa). The strong pressure dependence encourages

designers to double or triple the pressure of a CC cryoco-

oler to about 2 or 3 MPa. This pressure increase would

require adding a single compression stage while remaining

in a moderate pressure range (below 10 MPa) but still

enjoy values of

_

Q= _ n and COP that are nearly equal to the

maximum attainable. This remains consistent with pub-

lished performance data [45] for CC cryocoolers at 2 and

5 MPa achieving

_

Q= _ n of about 5001000 J/mol and COP

of 2030% of COP

C

. The practice of using two stages of

compression was reported with pure nitrogen [46], hydro-

carbon mixtures [47] and synthetic refrigerants [48].

The COP and

_

Q= _ n of OMs do peak at dierent pressures

and therefore occur for dierent compositions. Operation

at the highest COP (which occurs at 5 MPa) is associated

with giving up about 15% of the highest attainable

_

Q= _ n

(which occurs at about 20 MPa). One may try to compro-

mise between these two working points by choosing an

intermediate pressure and composition.

9. Minimum size recuperator

In some applications, the main concern is to minimize

the size of the recuperator even if this means sacricing

_

Q= _ n. Such an example may be the miniature cryosurgical

probe [27,49,50] or any other case where the platform of

the cold end is very delicate.

9.1. Pure coolants

While maintaining a constant ow rate, one may make

the size of a the recuperator progressively smaller in terms

of its thermal conductance, U A so that it becomes more

compact; this reduction in conductance is associated with

some loss eectiveness and thus in

_

Q= _ n. The question as

to whether and to what extent this strategy pays o is

examined by the parameter of compactness,which is,

_

Q=U A, and has units of degrees Kelvin. Since

_

Q and

U A are proportional to _ n, their ratio is independent of

_ n and characterizes the recuperator itself. A larger

_

Q=U A represents a more compact heat exchanger as a

given cooling rate is produced by a smaller recuperator.

Fig. 9 illustrates the compactness parameter,

_

Q=U A

for pure nitrogen at 40 MPa and 290 K as a function of

the NTU. Note that initially, the cooling capacity

_

Q

decreases more slowly than U A therefore

_

Q=U A

increases. However, if U A becomes too small then

_

Q

2 3 4 5 6 7 8 9 10 11

0

1

2

3

4

5

6

7

8

NTU

40

40

35

35

30

30

25

25

20

20

15

15

10

10

5

5

3

3

PP

T =

PP

T =

Q

optimized

mixtures

nitrogen

290 K =

AMB

T

80 K

cryocooling

40 MPa

NTU

40

40

35

35

30

30

25

25

20

20

15

15

10

10

5

5

3

3

PP

T =

PP

T

U A

290 K =

AMB

T

Fig. 9. Optimized compactness parameter, as a function of the size of the

recuperator, for 7 component hydrocarbon mixtures including N

2

, A,

CH

4

, C

2

H

6

, C

3

H

8

, C

4

H

10

, C

5

H

12

in comparison to that of nitrogen. The

DT

PP

values for each size recuperator are noted along the curves.

64 B.-Z. Maytal et al. / Cryogenics 46 (2006) 5567

sharply decays and dominating

_

Q=U A which drastically

decreases. The maximum value of

_

Q=U A for nitrogen is

5.05 K and is obtained with a recuperator sized by an NTU

value of 5.5. The numbers along the curves in Fig. 9, from 3

to 40 K, represent the warm end temperature dierence

between the recuperating streams which is also the DT

PP

for pure nitrogen. For smaller recuperators, as NTU

decreases, DT

PP

grows and is accompanied by a growing

gap between the actual specic cooling capacity,

_

Q= _ n,

and the potential or ideal one, Dh

T

. The peak value of

_

Q=U A is associated with a DT

PP

of about 16 K and at

this point

_

Q= _ n is 781 J/mol which is still about 65% of Dh

T

.

9.2. Mixed coolants

Can the use of mixtures at elevated pressure make the

recuperator more compact? In order to explore the highest

attainable

_

Q=U A and the associated composition, the

following procedure was adapted. At a given pressure,

for any value of DT

PP

the numerical model was used to

optimize the composition of a 7 component mixture com-

posed of group I hydrocarbons in order to directly maxi-

mize the compactness factor

_

Q=U A. Increasing DT

PP

values from 3 to 40 K is accompanied by further reduction

of recuperator size. Similar to pure nitrogen, the

_

Q=U A

value for these optimized mixtures exhibits a peak value

that is shown in Fig. 9. It should be claried that each

locally optimized point along this curve and its associated

composition namely, maximizing

_

Q=U A while imposing

a DT

PP

value, does not have any specic signicance since

by letting larger DT

PP

the optimized

_

Q=U A may

increase. However, these points pave the road to the global

optimum, which is the peaking point of this curve.

At the same conditions of 40 MPa and 290 K, the high-

est value of the compactness factor is 7.1 K at a DT

PP

between 20 and 30 K and NTU of about 4. This is about

50% more compact than nitrogen and it occurs at a smaller

NTU. The composition at the peaking

_

Q=U A is about

70% of nitrogen with the remaining 25% made up of argon

and the rest of the hydrocarbons. The

_

Q= _ n is about 1120 J/

mol which is only about 1/3 of the maximum attainable

value by mixtures (when optimized for

_

Q= _ n and similar

to the highest value attainable for pure nitrogen under

the same conditions. This procedure was repeated for 30

and 50 MPa and the peak value of

_

Q=U A were found

to be smaller than for the 40 MPa shown in Fig. 9.

Longsworth [51] considered the compactness of recuper-

ators when operated with pure coolants and proposed the

parameter, Dh

T

=

_

Q

REC

= _ n, which is indeed,

_

Q=

_

Q

REC

.

Dobak and Radebaugh [49,50] modied this parameter

for mixtures so that it becomes Dh

T;PP

=

_

Q

REC

= _ n. This

parameter can be used to compare coolants based on their

potential to tolerate a smaller recuperator while operating

at very high eectiveness. It is derived solely through the

thermophysical properties and in the Th plane. However,

it cannot serve to determine absolute gures of required

NTU, as in the case of operation at low eectiveness, to

gain additional compactness.

10. Mixtures for 90 and 95 K

10.1. Cooling capacity

Components of hydrocarbons group (I) and haloge-

nated hydrocarbons group (II) (Table 1) were optimized

for maximum

_

Q= _ n while cryocooling at the somewhat ele-

vated temperature of 90 and 95 K. The resulting

_

Q= _ n values

are only slightly higher than was obtained for the OM for

80 K. The gain by tolerating 90 K or even 95 K instead of

80 K is minor and therefore one may deduce that there are

no OMs for 90 and 95 K. Equivalently, one may state that

OMs for 80 K are approximately the same as the OMs for

90 and 95 K as observed in Table 5 which summarizes the

OM composition as a function of cryocooling temperature.

The situation is similar for mixtures of halogenated

hydrocarbons. For instance, the optimized mixture for

90 K at 35 MPa has

_

Q= _ n of 2775 J/mol whereas when it

is optimized at 80 K (Table 3) it has

_

Q= _ n 2700 J/mol.

Radebaugh discussed [52] how much entropy is enough

for cryocooling at any temperature. In this sense, the

entropy of the 90 K OM is mainly assigned around 80 K

and, consequently, the temperature of absorbing the heat

load will vary from 78 K to 90 or 95 K.

The 90 K OM still contains more than 60% nitrogen and

less than 8% argon. The low concentration of argon may be

explained by its high T

M

and by the fact that the major

enhancement of

_

Q= _ n is due to the hydrocarbons.

While optimized mixtures for 80 K cryocooling were

compared with nitrogen, the mixtures optimized for 90 K

must be compared with argon. However, the small gain

at 90 K on the one hand, and the special position of argon

as a noble gas and thus a superior coolant for JouleThom-

son cryocooling [53], on the other, do somewhat attenuate

the benet associated with using a mixed-gas coolant. For

instance, let us compare with argon the optimized mixture

at 50 MPa, 290 K for 90 K cryocooling. Indeed the

_

Q= _ n is

2850 J/mol against 2100 for argon. However, while dis-

charging down to 10 MPa, the mixtures provide Q/V of

Table 5

Compositions (percent mole fractions) of optimized mixtures at 30 MPa, 290 K for cryocooling at 80, 90 and 95 K

T [K]

_

Q= _ n [J/mol] N

2

A CH

4

C

2

H

6

C

3

H

8

C

4

H

10

C

5

H

12

80 3072 70.5 5.6 8.7 5.2 2.6 1.3 6.1

90 3115 65.1 6.1 14.5 4.9 1.3 2.1 6.0

95 3229 62.1 7.6 15.1 5.7 1.2 2.4 5.9

B.-Z. Maytal et al. / Cryogenics 46 (2006) 5567 65

about 26.5 kJ/L while argon at similar conditions provides

21.8 kJ/L. Argon compensates its lower

_

Q= _ n by higher

density at elevated pressure (Fig. 8) so that its Q/V inte-

gral approaches that of the optimized mixtures to within

20%.

10.2. Recuperators compactness

The optimization of mixtures for maximum compact-

ness parameter,

_

Q=U A, for cryocooling at 90 K points

to pure argon as the best choice. In analogy to the discus-

sion for 80 K cryocooling in Section 9, at 40 MPa, and

290 K the highest value of

_

Q=U A for argon is 25.2 K.

It is more then three times larger than for the optimized

mixtures for 80 K. However, one should still recall that

argon cools down to 90 K instead of 80 K. The associated

_

Q= _ n is 1050 J/mol which is about 50% of the highest attain-

able value by pure argon.

This characteristic might explain the use of high pres-

sure, open cycle argon for miniature cryosurgical probes

[54,55]. In the view of the compactness analysis, the mixed

coolant probes for similar cryocooling temperature cannot

be as compact as that of argon at elevated pressure. Still

mixed coolants are used for cryosurgical probes [56,57]

though at higher cryocooling temperatures and lower

pressures.

Acknowledgement

This work was partially sponsored by the Oce of

Naval Research under contract N00014-03-1-0175.

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