JP2008135501A - 熱電変換材料 - Google Patents
熱電変換材料 Download PDFInfo
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- JP2008135501A JP2008135501A JP2006319695A JP2006319695A JP2008135501A JP 2008135501 A JP2008135501 A JP 2008135501A JP 2006319695 A JP2006319695 A JP 2006319695A JP 2006319695 A JP2006319695 A JP 2006319695A JP 2008135501 A JP2008135501 A JP 2008135501A
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- Compositions Of Oxide Ceramics (AREA)
Abstract
【解決手段】金属元素として、M1、M2AおよびM2B[ここで、M1はLa、Yおよびランタノイドからなる群より選ばれる1種以上の元素(M1A)を必須の元素とし、さらにアルカリ土類金属元素から選ばれる1種以上の元素(M1B)を含有してもよい元素であり、M2Aは、原子価が2価となり得る金属元素からなる群から選ばれる1種以上の元素であり、M2Bは原子価が4価となり得る金属元素からなる群から選ばれる1種以上の元素であり、M1、M2AおよびM2Bは相異なる元素である。]を有する複合金属酸化物であって、M1:M2A:M2Bのモル比が2:1:1であり、結晶構造がペロブスカイト型結晶構造である複合金属酸化物からなる熱電変換材料。
【選択図】なし
Description
すなわち、本発明は、下記の発明を提供する。
<1>金属元素として、M1、M2AおよびM2B[ここで、M1はLa、Yおよびランタノイドからなる群より選ばれる1種以上の元素(M1A)を必須の元素とし、さらにアルカリ土類金属元素から選ばれる1種以上の元素(M1B)を含有してもよい元素であり、M2Aは、原子価が2価となり得る金属元素からなる群から選ばれる1種以上の元素であり、M2Bは原子価が4価となり得る金属元素からなる群から選ばれる1種以上の元素であり、M1、M2AおよびM2Bは相異なる元素である。]を有する複合金属酸化物であって、M1:M2A:M2Bのモル比が2:1:1であり、結晶構造がペロブスカイト型結晶構造である複合金属酸化物からなることを特徴とする熱電変換材料。
<2>形状が焼結体であり、該焼結体の相対密度が60%以上である前記<1>記載の熱電変換材料。
<3>焼結体の表面の少なくとも一部が、ガス不透過膜でコーティングされている前記<2>記載の熱電変換材料。
<4>前記<1>〜<3>のいずれかに記載の熱電変換材料を有する熱電変換素子。
また、例えば、上記のLaの一部を上記の3価の金属元素で置換した場合、すなわち例えば、Laの40%をEuで置換したような場合には、(La0.6Eu0.4)2CuSnO6、(La0.6Eu0.4)2CuTiO6、(La0.6Eu0.4)2NiSnO6、(La0.6Eu0.4)2ZnSnO6、(La0.6Eu0.4)2ZnTiO6、(La0.6Eu0.4)2ZnZrO6、(La0.6Eu0.4)2Ba2Cu2Sn2O11、(La0.6Eu0.4)2Ba2Cu2Ti2O11、(La0.6Eu0.4)2Ba2Zn2Sn2O11、(La0.6Eu0.4)2Ba2Zn2Ti2O11、(La0.6Eu0.4)2Ba2Ni2Sn2O11となる。
本発明の熱電変換材料を焼結体の形状で用いる場合を例に挙げて、本発明の熱電変換材料を製造する方法について説明する。本発明の熱電変換材料は、複合金属酸化物からなり、該複合金属酸化物は、焼結により本発明における複合金属酸化物となる金属化合物混合物を焼結することにより製造することができ、すなわち、M1:M2A:M2Bのモル比が2:1:1となるように含有する金属化合物混合物を焼結することにより本発明の熱電変換材料を製造することができる。具体的には、対応する金属元素を含有する化合物を所定の組成となるように秤量し、混合した後に得られる金属化合物混合物を焼結することにより製造することができる。例えば、好ましい組成の一つであるY2CuSnO6で表される化合物は、Y2O3とCuOとSnO2を、Y:Cu:Snのモル比が2:1:1となるように秤量し、混合した後に得られる金属化合物混合物を焼結することにより製造することができる。
1.電気伝導度
焼結体試料を角柱状に加工し、銀ペーストで白金線を装着し、直流四端子法により測定した。測定は空気中で室温〜1073Kの範囲で温度を変化させながら行った。
2.ゼーベック係数
電気伝導度測定時と同様の形状に加工した焼結体試料の両端に、銀ペーストでR熱電対および白金線を装着して、焼結体試料の温度および熱起電力を測定した。測定は空気中で室温〜1073Kの範囲で温度を変化させながら行った。焼結体試料の片面にエアを流入したガラス管を接触させて低温部を作り、焼結体試料両端の温度をR熱電対で測定し、同時に焼結体試料の両端面間に生じている熱起電力(ΔV)も測定した。焼結体試料両端の温度差(ΔT)は、エアの流量を制御することで1〜10℃の範囲で制御し、ΔTとΔVの傾きからゼーベック係数の値(α)を算出した。
3.熱伝導度
真空中、室温で、レーザーフラッシュ法により焼結体試料の比熱および、熱拡散率を測定した。測定には真空理工株式会社製レーザーフラッシュ法熱伝導度測定装置TC−7000型を用いた。
4.構造解析
焼成品、焼結体資料の結晶構造は、株式会社リガク製X線回折測定装置RINT2500TTR型を用いて、CuKαを線源とする粉末X線回折法により分析した。
5.焼結体の密度
焼結体試料の相対密度はアルキメデス法により算出した。
CuO(株式会社高純度化学研究所製)を3.074g、SnO2(株式会社高純度化学研究所製)を5.825g、La2O3(株式会社高純度化学研究所製)を12.593g、秤取し、ジルコニア製のボールを用い、湿式ボールミルにより20時間混合した。該混合物を空気中において1100℃で24時間保持して焼成し、得られた焼成品をジルコニア製のボールを用い、湿式ボールミルにより20時間解砕し、1軸プレス(成形圧は1000kg/cm2)により円盤状に成形し、得られた成形体を100%酸素雰囲気中において1100℃で24時間保持して焼結した。得られた焼結体(焼結体1、La:Cu:Snは2:1:1)のX線回折図形を図1に示す。図1より、焼結体1の結晶構造は、ペロブスカイト型結晶構造であることがわかった。また、焼結体1の焼結体密度は相対密度で95%であった。
CuO(株式会社高純度化学研究所製)を1.537g、SnO2(株式会社高純度化学研究所製)を2.912g、La2O3(株式会社高純度化学研究所製)を6.139g、CaCO3(宇部マテリアル株式会社製、CS3N−A(商品名))0.097g秤取し、実施例1と同様の方法で焼結体(焼結体2、La:Ca:Cu:Snは1.95:0.05:1:1)を作製した。焼結体2の粉末X線回折により、焼結体2の結晶構造はペロブスカイト型結晶構造であることがわかった。
CuO(株式会社高純度化学研究所製)を1.537g、SnO2(株式会社高純度化学研究所製)を2.912g、La2O3(株式会社高純度化学研究所製)を6.139g、BaCO3(日本化学工業株式会社製、LC−1(商品名))0.191g秤取し、実施例1と同様の方法で焼結体(焼結体3、La:Ba:Cu:Snは1.95:0.05:1:1)を作製した。焼結体3の粉末X線回折により、焼結体3の結晶構造はペロブスカイト型結晶構造であることがわかった。
CuO(株式会社高純度化学研究所製)を1.537g、SnO2(株式会社高純度化学研究所製)を2.912g、La2O3(株式会社高純度化学研究所製)を6.139g、SrCO3(SrCO3、堺化学株式会社製、SW−K)0.143g秤取し、実施例1と同様の方法で焼結体(焼結体4、La:Sr:Cu:Snは1.95:0.05:1:1)を作製した。焼結体4の粉末X線回折により、焼結体4の結晶構造はペロブスカイト型結晶構造であることがわかった。
CuO(株式会社高純度化学研究所製)を1.537g、SnO2(株式会社高純度化学研究所製)を2.767g、La2O3(株式会社高純度化学研究所製)を6.297g、MgO(和光純薬株式会社製)0.039g秤取し、実施例1と同様の方法で焼結体(焼結体5、La:Cu:Sn:Mgは2:1:0.95:0.05)を作製した。焼結体5の粉末X線回折により、焼結体5の結晶構造はペロブスカイト型結晶構造であることがわかった。
Claims (4)
- 金属元素として、M1、M2AおよびM2B[ここで、M1はLa、Yおよびランタノイドからなる群より選ばれる1種以上の元素(M1A)を必須の元素とし、さらにアルカリ土類金属元素から選ばれる1種以上の元素(M1B)を含有してもよい元素であり、M2Aは、原子価が2価となり得る金属元素からなる群から選ばれる1種以上の元素であり、M2Bは原子価が4価となり得る金属元素からなる群から選ばれる1種以上の元素であり、M1、M2AおよびM2Bは相異なる元素である。]を有する複合金属酸化物であって、M1:M2A:M2Bのモル比が2:1:1であり、結晶構造がペロブスカイト型結晶構造である複合金属酸化物からなることを特徴とする熱電変換材料。
- 形状が焼結体であり、該焼結体の相対密度が60%以上である請求項1記載の熱電変換材料。
- 焼結体の表面の少なくとも一部が、ガス不透過膜でコーティングされている請求項2記載の熱電変換材料。
- 請求項1〜3のいずれかに記載の熱電変換材料を有する熱電変換素子。
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TW096144707A TW200832768A (en) | 2006-11-28 | 2007-11-26 | Thermoelectric conversion material and thermoelectric conversion element |
CN200780043906XA CN101542762B (zh) | 2006-11-28 | 2007-11-26 | 热电转换材料和热电转换元件 |
PCT/JP2007/073262 WO2008066189A1 (fr) | 2006-11-28 | 2007-11-26 | Matériau de conversion thermoélectrique et élément de conversion thermoélectrique |
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JP2003008086A (ja) * | 2001-06-22 | 2003-01-10 | Idemitsu Kosan Co Ltd | 複合酸化物及びそれを用いた熱電変換素子 |
JP2006062951A (ja) * | 2004-07-27 | 2006-03-09 | Sumitomo Chemical Co Ltd | 熱電変換材料およびその製造方法 |
JP2006100683A (ja) * | 2004-09-30 | 2006-04-13 | Sumitomo Chemical Co Ltd | チタン酸化物熱電変換材料 |
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