CN1170749A - Perovskite-like compound as high-temperature magnetic refrigerating working medium - Google Patents
Perovskite-like compound as high-temperature magnetic refrigerating working medium Download PDFInfo
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- CN1170749A CN1170749A CN96117013.1A CN96117013A CN1170749A CN 1170749 A CN1170749 A CN 1170749A CN 96117013 A CN96117013 A CN 96117013A CN 1170749 A CN1170749 A CN 1170749A
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- perovskite
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- magnetic refrigerating
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- 230000005291 magnetic effect Effects 0.000 title claims abstract description 34
- 150000001875 compounds Chemical class 0.000 title claims abstract description 15
- XEEYBQQBJWHFJM-UHFFFAOYSA-N Iron Chemical compound [Fe] XEEYBQQBJWHFJM-UHFFFAOYSA-N 0.000 claims abstract description 9
- 229910052742 iron Inorganic materials 0.000 claims abstract description 6
- 229910052746 lanthanum Inorganic materials 0.000 claims abstract description 5
- 229910052777 Praseodymium Inorganic materials 0.000 claims abstract description 4
- 229910052788 barium Inorganic materials 0.000 claims abstract description 4
- 229910052712 strontium Inorganic materials 0.000 claims abstract description 4
- 229910052684 Cerium Inorganic materials 0.000 claims abstract description 3
- 229910052784 alkaline earth metal Inorganic materials 0.000 claims abstract description 3
- 229910052791 calcium Inorganic materials 0.000 claims abstract description 3
- 229910052759 nickel Inorganic materials 0.000 claims abstract description 3
- 229910052688 Gadolinium Inorganic materials 0.000 claims description 9
- 239000000463 material Substances 0.000 claims description 7
- 238000005516 engineering process Methods 0.000 claims description 6
- 239000000126 substance Substances 0.000 claims description 6
- 229910052748 manganese Inorganic materials 0.000 claims description 4
- 239000000203 mixture Substances 0.000 claims description 3
- 229910052761 rare earth metal Inorganic materials 0.000 claims description 3
- 229910052692 Dysprosium Inorganic materials 0.000 claims description 2
- 229910052691 Erbium Inorganic materials 0.000 claims description 2
- 229910052693 Europium Inorganic materials 0.000 claims description 2
- 229910052689 Holmium Inorganic materials 0.000 claims description 2
- 229910052765 Lutetium Inorganic materials 0.000 claims description 2
- 229910052779 Neodymium Inorganic materials 0.000 claims description 2
- 229910052772 Samarium Inorganic materials 0.000 claims description 2
- 229910052771 Terbium Inorganic materials 0.000 claims description 2
- 229910052775 Thulium Inorganic materials 0.000 claims description 2
- 229910052769 Ytterbium Inorganic materials 0.000 claims description 2
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 2
- 229910052745 lead Inorganic materials 0.000 claims description 2
- 239000001301 oxygen Substances 0.000 claims description 2
- 229910052760 oxygen Inorganic materials 0.000 claims description 2
- 229910052700 potassium Inorganic materials 0.000 claims description 2
- 229910052701 rubidium Inorganic materials 0.000 claims description 2
- 229910052706 scandium Inorganic materials 0.000 claims description 2
- 229910052708 sodium Inorganic materials 0.000 claims description 2
- 229910052727 yttrium Inorganic materials 0.000 claims description 2
- 238000000034 method Methods 0.000 abstract description 2
- UIWYJDYFSGRHKR-UHFFFAOYSA-N gadolinium atom Chemical compound [Gd] UIWYJDYFSGRHKR-UHFFFAOYSA-N 0.000 description 6
- 229910052751 metal Inorganic materials 0.000 description 6
- 239000002184 metal Substances 0.000 description 6
- 239000011575 calcium Substances 0.000 description 4
- 238000001816 cooling Methods 0.000 description 4
- 239000007789 gas Substances 0.000 description 4
- 150000002500 ions Chemical class 0.000 description 4
- 238000005057 refrigeration Methods 0.000 description 4
- YCKRFDGAMUMZLT-UHFFFAOYSA-N Fluorine atom Chemical compound [F] YCKRFDGAMUMZLT-UHFFFAOYSA-N 0.000 description 3
- 239000011737 fluorine Substances 0.000 description 3
- 229910052731 fluorine Inorganic materials 0.000 description 3
- 238000005259 measurement Methods 0.000 description 3
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 description 2
- 229910002651 NO3 Inorganic materials 0.000 description 2
- NHNBFGGVMKEFGY-UHFFFAOYSA-N Nitrate Chemical compound [O-][N+]([O-])=O NHNBFGGVMKEFGY-UHFFFAOYSA-N 0.000 description 2
- 238000000975 co-precipitation Methods 0.000 description 2
- 239000002826 coolant Substances 0.000 description 2
- 239000012530 fluid Substances 0.000 description 2
- -1 nitrate Chemical class 0.000 description 2
- 239000011224 oxide ceramic Substances 0.000 description 2
- 229910052574 oxide ceramic Inorganic materials 0.000 description 2
- 150000003839 salts Chemical class 0.000 description 2
- 238000005245 sintering Methods 0.000 description 2
- 239000008207 working material Substances 0.000 description 2
- OYPRJOBELJOOCE-UHFFFAOYSA-N Calcium Chemical compound [Ca] OYPRJOBELJOOCE-UHFFFAOYSA-N 0.000 description 1
- 229910002180 La0.8Ca0.2MnO3 Inorganic materials 0.000 description 1
- 229910017034 MnSn Inorganic materials 0.000 description 1
- MUBZPKHOEPUJKR-UHFFFAOYSA-N Oxalic acid Chemical compound OC(=O)C(O)=O MUBZPKHOEPUJKR-UHFFFAOYSA-N 0.000 description 1
- 239000000956 alloy Substances 0.000 description 1
- 229910045601 alloy Inorganic materials 0.000 description 1
- 238000000498 ball milling Methods 0.000 description 1
- 230000006835 compression Effects 0.000 description 1
- 238000007906 compression Methods 0.000 description 1
- 239000002178 crystalline material Substances 0.000 description 1
- 230000007812 deficiency Effects 0.000 description 1
- 238000004134 energy conservation Methods 0.000 description 1
- ZPDRQAVGXHVGTB-UHFFFAOYSA-N gallium;gadolinium(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Ga+3].[Gd+3] ZPDRQAVGXHVGTB-UHFFFAOYSA-N 0.000 description 1
- 238000004519 manufacturing process Methods 0.000 description 1
- VIKNJXKGJWUCNN-XGXHKTLJSA-N norethisterone Chemical compound O=C1CC[C@@H]2[C@H]3CC[C@](C)([C@](CC4)(O)C#C)[C@@H]4[C@@H]3CCC2=C1 VIKNJXKGJWUCNN-XGXHKTLJSA-N 0.000 description 1
- 230000005298 paramagnetic effect Effects 0.000 description 1
- 239000002244 precipitate Substances 0.000 description 1
- 238000001556 precipitation Methods 0.000 description 1
- 238000005464 sample preparation method Methods 0.000 description 1
- 238000003980 solgel method Methods 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 230000009466 transformation Effects 0.000 description 1
Images
Classifications
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- H—ELECTRICITY
- H01—ELECTRIC ELEMENTS
- H01F—MAGNETS; INDUCTANCES; TRANSFORMERS; SELECTION OF MATERIALS FOR THEIR MAGNETIC PROPERTIES
- H01F1/00—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties
- H01F1/01—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials
- H01F1/012—Magnets or magnetic bodies characterised by the magnetic materials therefor; Selection of materials for their magnetic properties of inorganic materials adapted for magnetic entropy change by magnetocaloric effect, e.g. used as magnetic refrigerating material
- H01F1/017—Compounds
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B35/00—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products
- C04B35/01—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics
- C04B35/016—Shaped ceramic products characterised by their composition; Ceramics compositions; Processing powders of inorganic compounds preparatory to the manufacturing of ceramic products based on oxide ceramics based on manganites
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3205—Alkaline earth oxides or oxide forming salts thereof, e.g. beryllium oxide
- C04B2235/3208—Calcium oxide or oxide-forming salts thereof, e.g. lime
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3224—Rare earth oxide or oxide forming salts thereof, e.g. scandium oxide
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/02—Composition of constituents of the starting material or of secondary phases of the final product
- C04B2235/30—Constituents and secondary phases not being of a fibrous nature
- C04B2235/32—Metal oxides, mixed metal oxides, or oxide-forming salts thereof, e.g. carbonates, nitrates, (oxy)hydroxides, chlorides
- C04B2235/3224—Rare earth oxide or oxide forming salts thereof, e.g. scandium oxide
- C04B2235/3227—Lanthanum oxide or oxide-forming salts thereof
-
- C—CHEMISTRY; METALLURGY
- C04—CEMENTS; CONCRETE; ARTIFICIAL STONE; CERAMICS; REFRACTORIES
- C04B—LIME, MAGNESIA; SLAG; CEMENTS; COMPOSITIONS THEREOF, e.g. MORTARS, CONCRETE OR LIKE BUILDING MATERIALS; ARTIFICIAL STONE; CERAMICS; REFRACTORIES; TREATMENT OF NATURAL STONE
- C04B2235/00—Aspects relating to ceramic starting mixtures or sintered ceramic products
- C04B2235/70—Aspects relating to sintered or melt-casted ceramic products
- C04B2235/74—Physical characteristics
- C04B2235/76—Crystal structural characteristics, e.g. symmetry
- C04B2235/768—Perovskite structure ABO3
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- Engineering & Computer Science (AREA)
- Chemical & Material Sciences (AREA)
- Ceramic Engineering (AREA)
- Manufacturing & Machinery (AREA)
- Materials Engineering (AREA)
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- Power Engineering (AREA)
- Hard Magnetic Materials (AREA)
- Soft Magnetic Materials (AREA)
Abstract
the high temperature magnetic refrigerating working medium features its perovskite-like compound general formula of R1-xAxMO3 where R is RE elements La, Ce, Pr, etc. or their combination; A is alkali earth metal elements and large-ion radius low-valence elements Ca, Sr, Ba, etc. or their combination; M is Mn or its combination with other iron family elements Fe, Ni, Co, etc.; the content 3 -delta of O depends on technological process; X is 0.2-0.6; and the proportion among R, A, M reaches normal subtraction proportion.
Description
The present invention relates to perovskite-like compound as high-temperature magnetic refrigerating working material and making thereof.
Magnetic cooling is a kind of economy, and is effectively pollution-free, and the cool mode of energy-conservation system is that the rerigerator of principle is compared with common gas compression, and it does not contain the influential fluorine of environment Lyons gas, and the undesirable gas compressor therefore can miniaturization, lightweight and microcomputer control.As far back as the thirties, people just adopt the paramagnetic salt successfully to obtain the utmost point low temperature of milli K magnitude as refrigeration working fluid, magnetic cooling is applied to high temperature (20-300K), especially room temperature, it is the target that people are pursued for many years, make high temperature magnetic cooling practicability, key is that development one class can (1～1.5T) has the material of great magnetic entropy variation, normally utilizes the magnetic entropy of ferromegnetism-paramagnetism phase transformation Curie temperature to change under the magnetic field that permanent magnet material produced.Gadolinium gallium garnet, RAl, the RNi of report are only applicable to below the 40K temperature at present, and room temperature magnetic cooling medium is still optimum with metal gadolinium and alloy thereof at present, and other Mn
3AlC, Ni
2The magnetic entropy of non-crystalline materials such as compound such as MnSn and FeZr only becomes half into the metal gadolinium.Yet the poor chemical stability of metal gadolinium, the rare high price of thing, and regulate and control certain Curie temperature, the prescription of temperature range is also difficult, because above deficiency is therefore far away from practicality.Generally adopting at present fluorine Lyons is the gas of the working medium cooling agent of having calmed the anger.Owing to forbidden fluorine Lyons in the world, it is imperative to develop harmless refrigeration working fluid and refrigeration mode.Magnetic cooling is pollution-free, high efficiency refrigeration mode, and key is to need suitable magnetic refrigerating working medium.
Technology of the present invention solves the chemical general formula that is achieved in that a kind of high-critical temperature magnetic refrigerating working medium material and has following class calcium petrochemical industry compound:
R
1-xA
xMO
3-δWherein: R is rare earth element La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Y, Sc etc. and combination; A is alkali earth metal and heavy ion radius Elements C a, Sr, Ba, Pb, Na, K, Rb etc. and combination thereof at a low price, and M is the combination of Mn or Mn and other iron family element ting Fe, Ni, Co etc.; O is an oxygen, and its content (3-δ) depends on technology, and X gets 0.1-0.9, and the proportioning of R, A, M three dvielements is near just dividing ratio: R: A: M=(1-x): x: 1 ± 10%.This compound can adopt sol-gel technology, chemical coprecipitation process, and the oxide ceramics prepared forms.
Characteristics of the present invention are that near the magnetic entropy change of perovskite-like compound room temperature can surpass the metal gadolinium, and chemical stability far is superior to the metal gadolinium, cheap, Curie temperature can change by composition artificially to be controlled, therefore be class ideal high temperature magnetic refrigerating working medium comparatively at present, can be applicable to the 20-400K warm area.
Fig. 1 is La
0.8Ca
0.2MnO
3And the Gd magnetic entropy becomes with the variation of temperature relation curve
Fig. 2 is La
0.67Ca
0.33MnO
3Magnetic entropy becomes with the variation of temperature relation curve
Fig. 3 is La
0.62Gd
0.05Ca
0.33MnO
3Magnetic entropy becomes with the variation of temperature relation curve
Fig. 4 is La
1-xR
xMnO
3Relation curve between Curie temperature of material (ordinate is represented absolute temperature) and the X (abscissa).[R＝Ca，Sr，Ba]
Fig. 5 is La
0.7-YPr
YSr
0.3MnO
3Be the Curie temperature (ordinate is represented absolute temperature) of material and the relation curve between the Y (abscissa).
Carry out proportioning by chemical formula, adopt salts such as nitrate, vitriol, colloidal sol-gel process decomposes about 200 ℃, and sintering is 8 hours in 600～300 ℃ of air atmospheres, its typical magnetic variation | Δ S
M| see figure (2) with the relation of temperature, near Curie temperature (260K), magnetic entropy becomes | Δ S
M|=4.3 (J/KgK), measurement magnetic field is 1.5T.The manufacture craft of another kind of perovskite-like compound high temperature mangneto working material is use coprecipitation technology, precipitates simultaneously by proportioning with oxalate or the nitrate of R, A, M, and precipitation medium is an ethanol, and its consumption is 10-20 times, and PH is 6-7.As for oxide ceramics technology is that sintering formed after corresponding oxide compound mixed ball milling in proportion.
Provide as Fig. 2 among the embodiment 2, near Curie temperature (260K), magnetic entropy becomes Δ S
M=4.3J/KgK, measurement magnetic field is 1.5T.
Provide as Fig. 3 among the embodiment 3, near Curie temperature (260K), magnetic entropy Δ S
MChange=4.3J/KgK, measurement magnetic field is 1.5T.
Embodiment 4
In order to obtain the magnetic working medium of required operation temperature area, on the one hand can be with other ion substitution perovskite-like compounds R
xA
1-xMO
3-δIn ion A or the content that changes A regulate and occupy a little, see figure (4); Can transfer Curie temperature by partly or entirely substituting the R ion on the other hand, see figure (5) with other rare earth ion.
Another embodiment as shown in Figure 3.
Claims (4)
1. high temperature magnetic refrigerating working medium material is characterized in that having the chemical general formula of following perovskite-like compound:
R
1-xA
xMO
3-δWherein: R is rare earth element La, Ce, Pr, Nd, Sm, Eu, Gd, Tb, Dy, Ho, Er, Tm, Yb, Lu, Y, Sc etc. and combination; A is alkali earth metal and heavy ion radius low price element, Ca, Sr, Ba, Pb, Na, K, Rb etc. and combination thereof; M is the combination of Mn or Mn and other iron family element ting (Fe, Ni, Co etc.); O is an oxygen, and its content (3-δ) depends on technology, and X gets 0.1-0.9, and the proportioning of R, A, M three dvielements is near just dividing ratio.
2. according to right 1 described perovskite-like compound magnetic refrigerating working medium, it is characterized in that R gets La, A gets Ca, and M gets Mn, and X gets 0.2-0.6.
3. according to claim 1,2 described high temperature perovskite-like compound magnetic refrigerating working mediums, it is characterized in that R gets La and Pr mixture.
4. according to claim 1,2 described high temperature perovskite-like compound magnetic refrigerating working mediums, it is characterized in that R gets La and Gd mixture.
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN96117013A CN1126801C (en) | 1996-07-12 | 1996-07-12 | Perovskite-like compound as high-temperature magnetic refrigerating working medium |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN96117013A CN1126801C (en) | 1996-07-12 | 1996-07-12 | Perovskite-like compound as high-temperature magnetic refrigerating working medium |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN1170749A true CN1170749A (en) | 1998-01-21 |
| CN1126801C CN1126801C (en) | 2003-11-05 |
Family
ID=5123957
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN96117013A Expired - Fee Related CN1126801C (en) | 1996-07-12 | 1996-07-12 | Perovskite-like compound as high-temperature magnetic refrigerating working medium |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN1126801C (en) |
Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN100364923C (en) * | 2003-11-13 | 2008-01-30 | 同济大学 | Temperature induced emissivity reversibly variable material |
| WO2010003926A1 (en) * | 2008-07-08 | 2010-01-14 | Technical University Of Denmark | Magnetocaloric refrigerators |
| CN102134749A (en) * | 2010-01-22 | 2011-07-27 | 中国科学院福建物质结构研究所 | Dysprosium ion activated gadolinium gallium garnet novel laser crystal |
| CN103014631A (en) * | 2012-12-19 | 2013-04-03 | 河北师范大学 | Method for preparing color Pr (Sr0.1Ca0.9)2Mn2O7 film |
| CN105112025A (en) * | 2015-09-10 | 2015-12-02 | 南通大学 | Solid magnetic refrigerating material, preparing method and magnetic refrigerator |
Family Cites Families (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH074326B2 (en) * | 1985-08-12 | 1995-01-25 | 船井電機株式会社 | Bread making method |
| CN1033174C (en) * | 1993-01-20 | 1996-10-30 | 北京科技大学 | Magnetic refrigerating material for magnetic refrigerator |
-
1996
- 1996-07-12 CN CN96117013A patent/CN1126801C/en not_active Expired - Fee Related
Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN100364923C (en) * | 2003-11-13 | 2008-01-30 | 同济大学 | Temperature induced emissivity reversibly variable material |
| WO2010003926A1 (en) * | 2008-07-08 | 2010-01-14 | Technical University Of Denmark | Magnetocaloric refrigerators |
| US20110126550A1 (en) * | 2008-07-08 | 2011-06-02 | Technical University Of Denmark | Magnetocaloric refrigerators |
| CN102089835A (en) * | 2008-07-08 | 2011-06-08 | 丹麦理工大学 | Magnetocaloric refrigerators |
| CN102134749A (en) * | 2010-01-22 | 2011-07-27 | 中国科学院福建物质结构研究所 | Dysprosium ion activated gadolinium gallium garnet novel laser crystal |
| CN103014631A (en) * | 2012-12-19 | 2013-04-03 | 河北师范大学 | Method for preparing color Pr (Sr0.1Ca0.9)2Mn2O7 film |
| CN103014631B (en) * | 2012-12-19 | 2014-08-20 | 河北师范大学 | Method for preparing color Pr (Sr0.1Ca0.9)2Mn2O7 film |
| CN105112025A (en) * | 2015-09-10 | 2015-12-02 | 南通大学 | Solid magnetic refrigerating material, preparing method and magnetic refrigerator |
Also Published As
| Publication number | Publication date |
|---|---|
| CN1126801C (en) | 2003-11-05 |
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