CN1170749A - 类钙钛石型化合物高温磁致冷工质 - Google Patents
类钙钛石型化合物高温磁致冷工质 Download PDFInfo
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- 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
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- 229910052748 manganese Inorganic materials 0.000 claims description 4
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- 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
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- 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
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- 239000002826 coolant Substances 0.000 description 2
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- 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
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- 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
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- H—ELECTRICITY
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- 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
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- 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
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Abstract
一种高温磁致冷工质材料，其特征是具有如下类钙钛石化合物的化学通式:R1－XAXMO3－δ，其中:R为稀土族元素La、Ce、Pr、Nd、Sm、Eu、Gd、Tb、Dy、Ho、Er、Tm、Yb、Lu、Y、Sc等以及组合;A为碱土金属元素及大离子半径低价元素,Ca、Sr、Ba、Pb、Na、K、Rb等及其组合;M为Mn或Mn与其它铁族元素(Fe、Ni、Co等)的组合;O为氧,其含量(3－δ)取决于工艺,X取0.2—0.6,R、A、M三类元素的配比接近正分比例。
Description
本发明涉及类钙钛石型化合物高温磁致冷工质材料及其制作。
磁致冷是一种经济，有效，无污染，节能的制泠方式，与通常气体压缩为原理的致冷机相比，它不含对环境有影响的氟里昂气体，不需要气体压缩机，因此可以小型化，轻量化与微机控制。早在30年代，人们就采用顺磁盐类作为致冷工质成功地获得毫K量级的极低温，将磁致冷应用于高温(20-300K)，尤其是室温，是人们多年来所追求的目标，要使高温磁致冷实用化，关键是研制一类能在永磁材料所产生的磁场下(1～1.5T)具有大磁熵变的材料，通常是利用铁磁性—顺磁性相变居里点的磁熵变化。目前报导的钆镓石榴石、RAl、RNi仅适用于40K温度以下，室温磁致冷工质目前尚以金属钆及其合金最合适，而其它的Mn3AlC、Ni2MnSn等化合物和FeZr等非晶材料的磁熵变仅为金属钆的一半。然而金属钆的化学稳定性差，物稀价昂，而且调节和控制一定居里点，温度范围的组方也较困难，由于以上不足，因此离实用较远。目前普遍采用氟里昂为工质的气体压气有致冷剂。由于国际上已禁用氟里昂，开发无害的致冷工质与致冷方式已势在必行。磁致冷是无污染、高效率的致冷方式，关键是需要合适的磁致冷工质。
本发明的技术解决是这样实现的，一种高临界温度磁致冷工质材料并具有下列类钙石化合物的化学通式：
R1-xAxMO3-δ其中：R为稀土族元素La、Ce、Pr、Nd、Sm、Eu、Gd、Tb、Dy、Ho、Er、Tm、Yb、Lu、Y、Sc等以及组合；A为碱土金属元素及大离子半径低价元素Ca、Sr、Ba、Pb、Na、K、Rb等及其组合，M为Mn或Mn与其它铁族元素Fe、Ni、Co等的组合；O为氧，其含量(3-δ)取决于工艺，X取0.1-0.9，R、A、M三类元素的配比接近正分比例：R∶A∶M＝(1-x)∶x∶1±10％。该化合物可采用溶胶-凝胶工艺，化学共沉淀工艺，以及氧化物陶瓷工艺制备而成。
本发明的特点是类钙钛石化合物在室温附近的磁熵变可超过金属钆，并且化学稳定性远优越于金属钆，价格低廉，居里温度可以通过成份变化进行人为控制，因此是一类目前较为理想的高温磁致冷工质，可应用于20-400K温区。
图1为La0.8Ca0.2MnO3及Gd磁熵变随温度的变化关系曲线
图2为La0.67Ca0.33MnO3磁熵变随温度的变化关系曲线
图3为La0.62Gd0.05Ca0.33MnO3磁熵变随温度的变化关系曲线
图4为La1-xRxMnO3材料的居里温度(纵座标表示绝对温度)与X(横座标)之间的关系曲线。[R＝Ca，Sr，Ba]
图5为La0.7-YPrYSr0.3MnO3为材料的居里温度(纵座标表示绝对温度)与Y(横座标)之间的关系曲线。
实施例1
按化学式进行配比，采用硝酸盐、硫酸盐等盐类，溶胶—凝胶工艺，200℃左右分解，600～300℃空气气氛中烧结8小时，其典型的磁变｜ΔSM｜与温度的关系见图(2)，在居里温度(260K)附近，磁熵变｜ΔSM｜＝4.3(J/Kg·K)，测量磁场为1.5T。另一种类钙钛石型化合物高温磁致工质材料的制作工艺是用共沉淀工艺，以R、A、M的草酸盐或硝酸盐按配比同时沉淀，沉淀介质为乙醇，其用量为10-20倍，PH为6-7。至于氧化物陶瓷工艺为相应的氧化物按比例混和球磨后烧结而成。
实施例1材料为图1所示，｜ΔSM｜＝4.2(J/Kg·K)，在居里温度(293K)附近。样品制备方法同上，其典型的磁熵变｜ΔSM｜与温度的关系见图(1)，在居里温度(230K)附近，磁熵变｜ΔSM｜＝5.5(J/Kg·K)测量磁场为1.5T。而金属钆的磁熵受在相同条件下：｜ΔSM｜＝｜4.2(J/Kg·K)其居里温度(293K)。
实施例2中如图2给出，在居里温度(260K)附近，磁熵变ΔSM＝4.3J/Kg·K，测量磁场为1.5T。
实施例3中如图3给出，在居里温度(260K)附近，磁熵ΔSM变＝4.3J/Kg·K，测量磁场为1.5T。
实施例4
为了得到所需工作温区的磁工质，一方面可以用其他离子替代类钙钛石化合物RxA1-xMO3-δ中的离子A或者改变A的含量来调节居点，见图(4)；另一方面可以通过用其它稀土离子部分或全部地替代R离子来调居里点，见图(5)。
另一实施例如图3所示。
Claims (4)
1.一种高温磁致冷工质材料，其特征是具有如下类钙钛石化合物的化学通式：
R1-xAxMO3-δ其中：R为稀土族元素La、Ce、Pr、Nd、Sm、Eu、Gd、Tb、Dy、Ho、Er、Tm、Yb、Lu、Y、Sc等以及组合；A为碱土金属元素及大离子半径低价元素，Ca、Sr、Ba、Pb、Na、K、Rb等及其组合；M为Mn或Mn与其它铁族元素(Fe、Ni、Co等)的组合；O为氧，其含量(3-δ)取决于工艺，X取0.1-0.9，R、A、M三类元素的配比接近正分比例。
2.根据权利1所述的类钙钛石化合物磁致冷工质，其特征是R取La，A取Ca，M取Mn，X取0.2-0.6。
3.根据权利要求1、2所述的高温类钙钛石型化合物磁致冷工质，其特征是R取La和Pr混合物。
4.根据权利要求1、2所述的高温类钙钛石型化合物磁致冷工质，其特征是R取La和Gd混合物。
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Cited By (5)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN100364923C (zh) * | 2003-11-13 | 2008-01-30 | 同济大学 | 一种温致发射率可逆变化材料 |
| WO2010003926A1 (en) * | 2008-07-08 | 2010-01-14 | Technical University Of Denmark | Magnetocaloric refrigerators |
| CN102134749A (zh) * | 2010-01-22 | 2011-07-27 | 中国科学院福建物质结构研究所 | 一种镝离子激活的钆镓石榴石新型激光晶体 |
| CN103014631A (zh) * | 2012-12-19 | 2013-04-03 | 河北师范大学 | 一种彩色Pr(Sr0.1Ca0.9)2Mn2O7薄膜的制备方法 |
| CN105112025A (zh) * | 2015-09-10 | 2015-12-02 | 南通大学 | 一种固体磁制冷材料、制备方法及磁制冷器 |
Family Cites Families (2)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| JPH074326B2 (ja) * | 1985-08-12 | 1995-01-25 | 船井電機株式会社 | パンの製造方法 |
| CN1033174C (zh) * | 1993-01-20 | 1996-10-30 | 北京科技大学 | 磁致冷机用磁性致冷材料及其制造方法 |
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Cited By (8)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN100364923C (zh) * | 2003-11-13 | 2008-01-30 | 同济大学 | 一种温致发射率可逆变化材料 |
| 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 (zh) * | 2008-07-08 | 2011-06-08 | 丹麦理工大学 | 磁致热致冷器 |
| CN102134749A (zh) * | 2010-01-22 | 2011-07-27 | 中国科学院福建物质结构研究所 | 一种镝离子激活的钆镓石榴石新型激光晶体 |
| CN103014631A (zh) * | 2012-12-19 | 2013-04-03 | 河北师范大学 | 一种彩色Pr(Sr0.1Ca0.9)2Mn2O7薄膜的制备方法 |
| CN103014631B (zh) * | 2012-12-19 | 2014-08-20 | 河北师范大学 | 一种彩色Pr(Sr0.1Ca0.9)2Mn2O7薄膜的制备方法 |
| CN105112025A (zh) * | 2015-09-10 | 2015-12-02 | 南通大学 | 一种固体磁制冷材料、制备方法及磁制冷器 |
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| CN1126801C (zh) | 2003-11-05 |
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