Magnetocaloric materials for Room-temperature applications · PDF fileMagnetocaloric materials...
Transcript of Magnetocaloric materials for Room-temperature applications · PDF fileMagnetocaloric materials...
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19-11-2010
Challenge the future
DelftUniversity ofTechnology
Magnetocaloric materials for Room-temperature applicationsEkkes Brück, Fundamental Aspects of Materials and Energy, TNW
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2Magnetocaloric materials
Refrigeration
15% world energy consumption
Strong greenhouse gases
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3Magnetocaloric materials
Magnetic refrigeration:
External magnetic field changes temperature of magnetic material
No CFCs, permanent magnets, easy scalable, high efficiency, low noise
Important parameters!
ΔT temperature change
ΔS entropy change
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4Magnetocaloric materials
spins lattice
Basic magnetocalorics
E
Two energy reservoirs
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5Magnetocaloric materials
E
Basic magnetocalorics
spins lattice
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6Magnetocaloric materials
Develop energy-efficient refrigerator, operated in field of permanent magnet.
→ modern magnets ≤ 2.5 tesla
→ refrigerator regenerator design
→ Layered beds to increase T span
→ cycle frequency (power)
→ efficient heat-exchangers
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7Magnetocaloric materials
2001 Model magnetic refrigerator
C. Zimm, Astronautics Co.
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8Magnetocaloric materials
1.5T
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9Magnetocaloric materials
Chubu and Toshiba Refrigerator 2003
(Gd, Dy) metal
Rotating magnet
0.76 T
Cooling power
60 W
T span 20 K
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10Magnetocaloric materials
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11Magnetocaloric materials
Okamura 2005, 2007
560 W @ 1.1T
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12Magnetocaloric materials
Magnetocaloric airconditioner
Sari et al 2007
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13Magnetocaloric materials
Tura & Rowe 2009
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14Magnetocaloric materials
T (C0)
T (C
0 )
Increased T span with layered bed containing different materials with tailored Tc
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15Magnetocaloric materials
Multimaterial regenerator
Rowe & Tura Int.J.Ref. 2006
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16Magnetocaloric materials
Gd foil0.8 (P)48.8reciprocatingApril 2003Grenoble, FranceLab. d’Electrontechnique
Grenoble
Gd1-xDyx layered bed0.76 (P)1060rotaryMar. 4, 2003Yokohama, JapanChubu Electric/Toshiba
Gd1-xDyx layered bed0.6 (P)2740reciprocatingOct. 5, 2002Yokohama, JapanChubu Electric/Toshiba
Gd spheres; Gd5(Si,Ge)4 pwdr.b1.4 (P)23?reciprocatingMarch 4, 2003Nanjing, ChinaSichuan Inst. Tech./
Nanjing University
Gd spheres1.5 (P)2095rotarySept. 18, 2001Madison, Wisconsin, USAAstronautics
Gd & Gd1-xTbx layered bed2 (S)142reciprocatingJuly 2001Victoria, British Columbia
Canada
University of Victoria
Gd spheres4 (S)21100reciprocatingSummer 2000Yokohama, JapanChubu Electric/Toshiba
Gd foil0.95 (P)5?rotaryMay 2000Barcelona, SpainMater. Science Institute
Barcelona
Gd spheres5 (S)10600reciprocatingFeb. 20, 1997Madison, Wisconsin, USAAmes Laboratory/ Astronautics
Regenerator
Material
Magnetic Fielda
µ0H(T)
Max.
T
(K)
Cooling
Power
(W)
TypeAnnouncement
Date
LocationName
aMagnetic field source: S = superconducting magnet; P = permanent magnetbActual composition Gd5(Si1.985Ge1.985Ga0.03)
Room-temperature magnetic refrigerators
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17Magnetocaloric materials
11 prototypes 2009
Frequ. Power ΔT magn. mater.
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18Magnetocaloric materials
Giant MCE materials
1990 FeRh (Nikitin et al.)1997 Gd5Si2Ge2 (Percharsky & Gschneidner Jr.)1998 RCo2 (Foldeaki et al. )2000-2002 La(Fe,Si)13 (Hu et al., Fukamichi et al.) 2001 MnAs1-xSbx (Wada et al.)2002 MnFe(P,As) (Tegus et al.)2003 Co (S1-xSex)2 (Yamada & Goto)2005 NiMnSn (Krenke et al.)2009 MnCoGeB (Trung et al.)
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19Magnetocaloric materials
0 1 2 3 4 50.0
0.5
1.0
1.5
2.0
2.5
M (
B/f.u
.)
B (T)
at 310 K
MnFeP0.46As0.54
For example
Magnetization processes
Materials with field induced first order phase transition.
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20Magnetocaloric materials
La(Fe,Si)13 compounds
Cubic CaZn13 type of structure stabilized by addition of 10% Si(Kripyakewich et al. 1968)Invar type of behavior and unusual magnetic transition(Palstra et al 1983)Difficult to obtain single phase.
Gutfleisch et al 2004Meltspun almost single phase
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21Magnetocaloric materials
Concentration dependence of Curie temperature and moment
Palstra et al. 1983
Tc increase with dilution
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22Magnetocaloric materials
LaFe13 system
APL Zhang et al 2000Fujieda et al 2002
MCE decrease with dilution
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23Magnetocaloric materials
PRB Fujita et al 2003
Tc increase with hydrogen!
Sharp transition maintained!
LaFe13 system with hydrogen
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24Magnetocaloric materials
260 280 300 320 3400
5
10
15
20
-S
(J/k
g K
)
T (K)
Gd metal LaFe11.4Si1.6H
LaFe11.4Si1.6H1.5 LaFe11.4Co0.5Si1.1 LaFe11.2Co0.7Si1.1
0-2T
Fujita et al Phys Rev B 67 (2003) Hu, et al, JAP 97 (2005)
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25Magnetocaloric materials
Field driven 1st order metamagnetictransition around 200 K .
La(Fe,Si)13 cubic above magnetic transition
cubic below
volume change 1.5%. Low Tc can be increased by addition of Cobalt or Hydrogen.
Hysteretic transition: stability of hydrogenation?mechanical stability?
Summary La(Fe,Si)13
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26Magnetocaloric materials
MnFeP1-xAsx
Hexagonal Fe2P type of structure
Bacmann, JMMM 1994
Space group:
P62m
Mn 3g sites
Fe 3f sites
P/As 1b&2c sites
_
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27Magnetocaloric materials
Sample preparation
Starting Fe2P, Mn2As3, Mn & P
mechanical alloying
sintering 1000oC
annealing 800oC
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28Magnetocaloric materials
Magnetization process near Tc
Field induced transition with small hysteresis
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29Magnetocaloric materials
Temperature dependence of Magnetization
Step-liketransition
first order
but very littlehysteresis
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30Magnetocaloric materials
Comparison of magnetocaloric effect in different materials
Entropy changeconcentrated inrelevant T interval Tegus et al. Nature 415
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31Magnetocaloric materials
285 290 295 300 305 310 3150
1
2
3
4
5B = 1.45 T
MnFeP0.45As0.55MnFeP0.47As0.53
Mn1.1Fe0.9P0.47As0.53
T ad
(K)
T (K)
Direct measurements MSU
Adiabatic temperature-change
Sample dependence need for careful preparation
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32Magnetocaloric materials
For active magnetic regenerator
0 1 2 3 cm
MnFePAs sintered
Extrudedgreen
Shaping of materials
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33Magnetocaloric materials
200 220 240 260 280 300 3200
10
20
30
40
50
60
70
M (A
m2 /k
g)
T (K)
1
2
3
Mn1.1Fe0.9P0.78Ge0.22
0.1 T
Virgin effect and large hysteresis
Arsenic has bad reputation in kitchen
Sample with Ge replacing As
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34Magnetocaloric materials
Sample with Ge replacing As
Melt-spinning
+ Ar gas pressure 1 atm.
surface speed of the wheel v = 40m/s+
ribbons were annealed for ± 10 min.+
Mn2-xFexP0.75Ge0.25 (x = 0.70, 0.76, 0.78, 0.80)+
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35Magnetocaloric materials
Small thermal hyteresis, Tc = 288 K
Large MCE observed at low operation field
Sample with Ge replacing As
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36Magnetocaloric materials
Challenges with Fe2P materials
As bad reputationGe expensiveSi or Al could be perfect
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37Magnetocaloric materials
MnFe(P,Si) first samples
Large hysteresis
50 100 150 200 250 3000
10
20
30
40
50
M(A
m2 /k
g)
T(K)
1st cooling heating 2ndcooling
B = 50 mTsweep rate 2K/min
MnFeP0.6Si0.4
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38Magnetocaloric materials
Toxic ingredients0.1 %Hex. – hex.150-340250-580
MnFe(P,As)(P, Ge, Si)
Fe corrosion sensitiveH uptake
1.5 %Cubic -cubic
200-330La(Fe,Si)13Hy
High purity Gdrequired
hysteresis
0.5 %Ortho. –monokl.
130-270Gd5Ge2+xSi2-x
CommentsVStruct.Tc
(K)Alloy
Comparison giant magneto-caloric materials
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39Magnetocaloric materials
Availability
60t?WW prod=90t, avail 10t
?GaNi0.501Mn0.227Ga0.258
4000
4000
unlimited
WW prod=90t, avail 10t
?
1000
Estimated
availability
7000tLaManganites
LaMnO3
22000tLaLathanum alloys
La(Fe13-xMx)
No limitation for an
industrial productionnone
Manganese alloys
Mn(As1-xSbx)
MnFe(P1-xSix)
140tGeGadolinium Silicon alloys
Gd4(Si1-xGex)5
1000tGdGd metal
Total availability of
MC material
Limiting
ingredient
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40Magnetocaloric materials
Classical Technology:
Temperature range < 200 °C not considered
Magnetocaloric Technology: 75% of Carnot Efficiency
High Temperature (600 °C)Permanent magnets XMC-materials X
Low temperature (<200 °C)Permanent magnets ✔MC-materials ✔Access to waste heat
Heat- to electric-power conversion
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41Magnetocaloric materials
dBTMTdTcTdSdQ p
Heat input → temperature changemagnetization change
2222
dtdB
RSNRIWelect
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42Magnetocaloric materials
Magnetocaloric power generation
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43Magnetocaloric materials
Stack of materials in generator
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44Magnetocaloric materials
Various machine concepts were developed in the past.Lack of suited magneto-caloric materials prohibited realization of these.The novel materials showing giant-magneto-caloric effects near and above RT can lead to realization.
Summary MC power generation
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45Magnetocaloric materials
People involved in project in Delft
• Senior scientists: Jürgen Buschow, Niels van Dijk• Pos docs: Lian Zhang, Luana Caron, Cam Thanh Dinh• PhD students: Thanh Trung Nguyen, Zhiqiang Ou, Huu Dung
Nguyen, Jose Leitao• Technician: Anton Lefering
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46Magnetocaloric materials
Thank you
?