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Article history: Magnetic refrigeration (MR) at room temperature is an emerging technology and shows real potential
Received 16 May 2012 to enter conventional markets. The principle of MR obeys the magnetocaloric effect (MCE), which is
Received in revised form based on the effect caused by a magnetic eld on the materials that bear the property of varying the
20 September 2012
magnetic entropy, as well as its temperature, when varying the magnetic eld. This article revises the
Accepted 23 September 2012
MCE, its theory and thermodynamics. It discusses the properties that must be met by the magneto-
Available online 16 October 2012
caloric materials as well as those most suitable for room temperature MR and those displaying a
Keywords: promising future. Finally, a presentation and description of the Carnot, Brayton, Ericsson, AMR and
Magnetocaloric effect cascading MR cycles is given with a view to establishing selection criteria based on their performances.
Refrigerating cycle
& 2012 Elsevier Ltd. All rights reserved.
Brayton
Ericsson
AMR
Cascade
Contents
1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 74
2. The MCE theory . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 75
2.1. Thermodynamics of the MCE. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 76
2.2. First order and second order phase transitions. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 77
2.2.1. First order phase transitions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 77
2.2.2. Second order transitions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 78
2.3. Inuence of temperature on the MCE . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 78
3. Materials for MR. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 78
3.1. Materials for room temperature MR . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 78
4. MR thermodynamic cycles . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 79
4.1. Carnot cycle . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 79
4.2. Brayton cycle . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 79
4.3. Ericsson cycle . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 80
4.4. Cascade magnetic cycles . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 80
4.5. Active magnetic regenerator cycle (AMR) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 80
5. Practical considerations for the application of cycles . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 81
6. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 81
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 82
1. Introduction
n
Corresponding author. Tel.: 34 981 167000x4233; fax: 34 981 167100. Ozone layer depletion still continues despite measures to
E-mail addresses: j.romero.gomez@udc.es (J. Romero Gomez),
protect the ozonosphere in the atmosphere and the ecological
fereiro@udc.es (R. Ferreiro Garcia),
alberto.demiguel@udc.es (A. De Miguel Catoira), environment: the treaty system of ozone layer protection agreed
m.romero.gomez@udc.es (M. Romero Gomez). in the Vienna Convention for the Protection of the Ozone Layer
1364-0321/$ - see front matter & 2012 Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.rser.2012.09.027
J. Romero Gomez et al. / Renewable and Sustainable Energy Reviews 17 (2013) 7482 75
(1985); Montreal Protocol on Substances Depleting the Ozone prototypes have been carried out, Yu et al. [15], with most
Layer (1987) and amendments to the Montreal Protocol have magnetic refrigerator prototypes using a regenerating cycle based
provided the schedule to reduce the use of CFCs (chlorouoro- on AMR.
carbons) [1]. On the other hand, the traditional technology of In this article, the thermodynamic cycles based on the MCE
steam compression refrigeration is close to reaching its technical principle are revised with the aim of establishing selection criteria
boundaries in achieving further improvements in energy and as on the basis of the expected performance for room temperature
exergy efciency, as well as its use of gases with ozone depletion refrigeration technology. First, the theory related with the MCE
and global warming potential [2]. Therefore, scientists and engi- and its associated thermodynamics are described in detail. In the
neers have begun in recent years to explore new technologies for same way, the properties of the magnetocaloric materials needed
cooling such as thermoelectric cooling [3], thermoacoustic refrig- to full performance requirements, as well as the most suitable
eration, absorption refrigeration [4,5], adsorption refrigeration [6] materials for MR at room temperature, including those that
and magnetic refrigeration. exhibit a promising future, are described. This article is organised
Refrigeration systems exploit a materials entropy change due so that in Section 2 the basic theory of MCE and the associated
to the variation of an external parameter as well as the pressure thermodynamics is described. In Section 3, suitable MR materials
or magnetisation to absorb and release energy. Conventional that full the conditions to be applied as MR as well as their
cooling systems (compression based cycles) are based on the betting characteristics have been depicted. In Section 4, the
elastocaloric effect (ECE). This is dened as the absorption or available thermodynamic cycles applicable to MR are described.
emission of heat due to the change in pressure on a material In Section 5, a discussion regarding the practical considerations
(working uid) in a process where the magnetic eld is not about MR cycles is carried out. The article ends with appropriated
applied. Moreover, in the refrigeration technologies based on the conclusions on the described topics.
MCE, the magnetocaloric effect can be dened as the absorption
or emission of heat when a magnetocaloric material is subjected
to a change of a magnetic eld in a process where the pressure 2. The MCE theory
has no inuence.
The MCE was rst observed by Warburg [7] in 1881, but it was The MCE consists of a materials thermal response when
not until 1918 that Weiss and Picard [8] established the physical subjected to a magnetic eld change. It is an intrinsic property
principles that govern the MCE phenomenon, allowing the rst of all magnetic materials. It can be quantied as the reversible
application of the MCE to arise from the proposals of Debye [9] in change in temperature (DTad) in the material when the eld
1926, and Giauque [10], in 1927, of creating MR cycles in order to change takes place in an adiabatic process, or the reversible
reach temperatures below liquid helium. In 1933, Giauque and change of magnetic entropy (DSm) if the change in eld is brought
MacDougall [11] experimentally achieved a temperature value of about in an isothermal process. The relationship between the two
250 mK, with paramagnetic salts, overtaking the 1 K barrier for properties can be illustrated by a schematic diagram TS (Fig. 1).
the rst time. This diagram represents the thermal dependency of the entropy
The feasibility of MR at room temperature was introduced by of a magnetic system depending on the applied eld. The
Brow in 1976 through a magnetic refrigerator prototype working existence of MCE at temperature T0 may cause an adiabatic
in accordance with an Ericsson cycle with Gd material and a temperature change in the system DT ad T 1 T 0 or an isothermal
magnetic eld created by superconducting magnets [12]. change of magnetic entropy (DSm S1 S2 ). The rst occurs when
Pecharsky and Gschneidners discovery in 1997 [13] of materials the entropy is kept constant, while the second is produced when
with a remarkable magnetocaloric response at room temperature, the temperature is kept constant. Both DTad and DSm are char-
and the replacement of superconducting magnets with perma- acteristic values of the magnetocaloric effect, according to the
nent ones in 2001 by the Astronautics Cooperation in USA [14], initial temperature T0 and the value of change in the magnetic
sparked the interest of scientists, researchers and companies eld. With the increasing value of the external magnetic eld
around the world. Since then, numerous publications and patents change, the ordering of the magnetic spin increases and the
regarding magnetocaloric materials and magnetic refrigerator magnetic entropy is decreased.
76 J. Romero Gomez et al. / Renewable and Sustainable Energy Reviews 17 (2013) 7482
T
H1> H0 H1 H0
B
T1
C Sm=S Tad
T0
A
Fig. 2. Arrangement of magnetic spin system of an adiabatic sample before and
after applying a magnetic eld.
S1 S0 S
where the contribution to the total entropy ST is given by: dU TdSpdV m0 HdM 2
magnetic entropy of the magnetisation of the material, lattice where H is the intensity of the magnetic eld, p the pressure, V is
entropy caused by the vibrations of crystal lattice and electronic the volume of the sample, m0 the magnetic permeability of the
entropy of the materials free electrons (denoted as Sm, Sr, and Se, vacuum, and M the magnetic momentum of the sample. If the
respectively) [17]. The lattice and electronic entropy can be systems volume is not modied, dV0, Eq. (2) is expressed as:
considered independent from the magnetic eld and only depend
on temperature. The magnetic entropy, however, is highly depen- dU TdS m0 HdM 3
dent on both the magnetic eld and the temperature. rewriting Eq. (3), which contains extensive magnitudes, depend-
When applying a magnetic eld under adiabatic conditions in ing on specic values per unit mass it follows that:
a ferromagnetic sample (Fig. 2), the total entropy remains con-
stant during the process of magnetisation. Thus, when the du Tds m0 Hds 4
magnetic entropy is reduced, lattice and electronic entropy In this way, s is dened as the specic magnetisation (mag-
increase to compensate because of the spin lattice connections netic momentum per unit of mass). The total specic entropy
and vibrations. This causes a temperature increase (DTad) which change of the system expressed according to H and T can be
depends on the applied magnetic eld strength. When the represented as:
external eld is removed, the magnetic spin system returns to
ds @s=@TH dT @s=@HT dH 5
its original alignment by capturing energy from the lattice, which
decreases the thermal entropy and the sample returns to its The specic heat c of a substance under a constant state or
original temperature. parameter x can be dened as:
Individual magnetic moments align with the external eld,
cx dq=dTx 6
thereby decreasing the magnetic entropy of the sample and
maintaining the ST. If the magnetic eld is removed, the magnetic When the second law, dened by Eq. (7), is combined with
spin system returns to its original alignment together with the Eq. (6), the specic heat of the substance for an isobaric process
J. Romero Gomez et al. / Renewable and Sustainable Energy Reviews 17 (2013) 7482 77
and constant magnetic eld (CpH) can be dened as Eq. (8). magnetisation with temperature 9(@s/@T)H9 is large around the
phase transition involving a change of magnetisation in the
ds dq=T 7
material.
cpH T@s=@TH 8
2.2. First order and second order phase transitions
The dependence of the entropy in the magnetic eld can be
expressed in terms of magnetisation through a Maxwell relation:
Transition or phase change is the transformation of a system
@s=@HT m0 @s=@TH 9 from one phase to another. The main characteristic is an abrupt
Introducing Eqs. (8) and (9) into Eq. (5), the following expres- change in one or more physical properties. With regard to the
sion is obtained for the entropy: phase transition in magnetic systems, two transition modes are
given: rst order magneto-structural phase transitions and the
ds cpH =TdT m0 @s=@TdH 10 continuous phase or second order transitions.
The reversible change of temperature (DTad) that the sample
undergoes in an adiabatic process of magnetisation (process AB 2.2.1. First order phase transitions
of Fig. 1) is carried out satisfying Eq. (10) under the condition of In rst order transitions, there are two phases in equilibrium, so
ds0, yielding: the transformation is not instantaneous and they are linked to the
Z H1 presence of latent heat. They show a discontinuity in the volume, in
DT ad m0 T=cpH @s=@TH dH 11 the magnetisation and entropy, so that @M/@T and @S/@T are innite in
Ho
the transition temperature. The analysis of the magnetic entropy
Thus, the MCE sample can be quantied when the eld change and the MCE behaviour in rst order magnetic transitions was
variation takes place in an adiabatic process, according to: carried out by Pecharsky et al. [18]. Fig. 4 shows a TS diagram of a
Z H1 magnetic system experiencing a rst order transition with a transi-
MCEad m0 T=cpH @s=@TH dH 12 tion temperature of Tt0 for a zero eld (H0 0) and a transition
Ho
temperature of Tt1 for a H1 (H1 4H0) eld. For each isomagnetic curve
It must be taken into account that this equation is not as trivial of the entropy, depending on the temperature, there is a temperature
as it appears as the temperature itself is an implicit function of H at which there is an abrupt change in entropy. The vertical lines
given that the temperature will change due to adiabatic tempera- between the two isomagnetic curves correspond to an adiabatic
ture change as when altering the magnetic eld. This should be temperature change (DTad). The adiabatic temperature change
included when carrying out integration. The adiabatic tempera- achieves its peak values in the scale of temperatures ranging from
ture change can, of course, also be determined by direct measure- Tt0 and Tm (geometrically dened by the dotted lines). For Tm oToTt0,
ments of the samples temperature. adiabatic temperature changes decrease due to the abrupt change in
When the sample is subjected to a variation of the magnetic entropy.
eld in an isothermal process (dT0, process AC in Fig. 1), the The ferromagnetic materials displaying a rst order phase
reversible change in entropy DS is equal to the magnetic entropy offer an acute magnetocaloric response centred at its transition
change DSm. The specic entropy change Ds can be determined temperature, rapidly annulling itself in its vicinity [19]. Both are
from Eq. 10, establishing dT 0, resulting in the following expres- characterised, therefore, by higher values of DSm. There are,
sion: however, problems arising from the nature of this phase transi-
Z H1 tion such as [20]:
Ds Dsm m0 @s=@TdH 13
H0
existence of thermal and magnetic hysteresis
From Eq. (13), the MCE can be quantied if the eld variation changes in volume and thermal stress between the existing
is performed under an isothermal process. phases
Z H1 slow kinetic of rst order phase transitions that can inuence
MCEisot m0 @s=@TdH 14 or limit refrigerator performance.
H0
Tm
the magnetic eld variation is large
magnetisation changes rapidly with temperature, i.e., 9(@s/@T)H9
Tt0
is high.
the material has a low specic heat.
[31], Gd5Si2Ge2 and those related with the Gd5 (Si4 xGex) series
[32], the MnAs1 xSbx [33] series, and the La (Fe1 xCox) 11.9Si1.1 isothermal processes and can be illustrated in a TS diagram
series [34]. The Fe49Rh51 alloy has a high known MCE value of between two lines of constant eld (Fig. 6).
near room temperature but the high cost of Rh means that it can The magnetic refrigerant is partially magnetised (process 12),
only be considered for applications researching the cooling increasing its temperature adiabatically from Tcold to Th. Then the
capabilities of the materials. The Gd5 (Si4 xGex) and MnAs1 xSbx intensity of the applied magnetic eld is increased to complete
series are associated with rst order phase transitions, i.e., there magnetisation isothermally, making it necessary to remove the
are practical obstacles because of the nature of this transition (see refrigerant materials thermal insulation in order to allow the
above). However, the La (Fe1 xCox)11.9Si1.1 series is associated heat exchange with the heat transfer uid (process 23). In this
with second order phase transitions and its acquirement through process, the coolant keeps its temperature at constant, while the
powder metallurgical processes allow its production on an indus- uid absorbs the heat generated in the refrigerant due to the
trial scale [35]. The Curie temperature of compounds can be easily magnetisation. In process 34, the applied magnetic eld
adjusted by altering the content of Co. Approximately DTad of 2 K/T decreases and this lowers the temperature of the magnetic
can be reached. All this indicates that the compounds of the La refrigerant adiabatically, from Th to Tcold. Finally, the cycle is
(Fe1 xCox) 11.9Si1.1 series can become the room temperature completed when the material is completely demagnetised during
magnetocaloric materials of the future, despite possessing MCE process 41. In this process the magnetic refrigerant absorbs heat
properties inferior to that of Gd metal. from the uid, recovering the energy lost during demagnetisation.
To ensure the efcient performance of the system, the uid
rejects the absorbed energy of the magnetised coolant (process
4. MR thermodynamic cycles 23) to the hot source and absorbs energy from the cold source
(system to be cooled) that is transferred to the magnetic refrig-
In general, a magnetic refrigerator comprises: a magnetic erant in demagnetising process 41.
working material, a magnetising/demagnetising system, hot and
cold heat exchangers and a heat transfer system with a thermal
uid. The heat transfer uid is responsible for pumping the heat
between the working magnetic material and the hot and cold heat 4.2. Brayton cycle
exchangers. Depending on the working temperature, the transfer
uid may be a gas or a liquid. The general working principle of a Heat transfer in the Brayton cycle occurs differently from that
magnetic refrigerator is as follows: the working material (refrig- of the Carnot cycle. Heat transfer is performed in processes where
erant) absorbs heat from the load at a low temperature (the cold the magnetic intensity remains constant, thus obtaining higher
heat exchanger) and transfers it to the high temperature source temperature ranges and consequently a higher heat transfer
(hot end heat exchanger). As a result of the cyclical repetition of between the magnetocaloric material and the uid.
this process, the load is cooled. In magnetic refrigerators the An MR Brayton cycle with regeneration is shown in Fig. 7. The
working material is a magnetic material, which changes its cycle consists of four processes; two adiabatic and two where the
temperature and entropy under the effect of a magnetic eld. intensity of the applied magnetic eld remains constant.
The combination of thermodynamic processes of isothermal Considering the cycle operating processes shown in Fig. 7 from
magnetisation, (where the refrigerant is magnetised as the point 1, when the working magnetic material is at temperature T1,
temperature is kept constant: during this process the MCE it undergoes a temperature rise to T2 (process 12) caused by the
manifests itself as a change in entropy), adiabatic magnetisation MCE in the adiabatic magnetisation. Thus the material, in the
(where the coolant temperature increases due to an adiabatic presence of a constant magnetic eld, transfers heat to the hot
temperature change) and processes at a constant eld, allow the source (Qh), lowering its temperature to T2a. The additional cool-
achievement of magnetic refrigerators with different thermo- ing of T2a to T3 is achieved with the aid of the regenerator (process
dynamic cycles. 4a1). At point 3, the material undergoes an adiabatic demagne-
tisation (process 34), thus its temperature drops to T4. The
4.1. Carnot cycle magnetic material at temperature T4 exchanges heat (process
44a) with the cold source exchanger (Qc) absorbing heat so that
In MR cycles, the Carnot cycle can be considered as the its temperature increases to T4a. Finally, the regenerator transfers
reference cycle as it allows the direct study of manifestations of heat to the magnetic material, (process 4a1), thereby completing
the MCE to. The cycle consists of two adiabatic and two the cycle.
80 J. Romero Gomez et al. / Renewable and Sustainable Energy Reviews 17 (2013) 7482
T
H1> H0 H1 H0
T2 (2)
Qh
(2a)
T1,2a (1)
T3,4a (3)
(4a)
T4
(4)
Qc
S3,4 S1,2 S
Fig. 7. TS diagram of an MR Brayton cycle with regeneration. Fig. 9. Magnetic cycle cascade refrigeration cycle based on the Ericsson
magnetic cycle.
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