JP6022806B2 - ナノ粒子を含む三元熱電材料及びその製造方法 - Google Patents
ナノ粒子を含む三元熱電材料及びその製造方法 Download PDFInfo
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Description
本発明及び本発明に伴う多くの利点についてのより完全な理解は、以下の詳細な説明を添付の図面と関連して参照することでよりよく理解されることになるから、容易に得られるであろう。
本発明は、三元主族マトリックス材料とナノ粒子及び/又はナノ包接物(nanoinclusions)を含む熱電材料を包含する。ナノ粒子の代表例としては、式MO及び/又はM(ここで、Mは酸化状態2+又は金属形態の第2族又は第12族元素である)により表される物質の粒子が挙げられる。マトリックス材料は三元主族又はカルコゲナイド半導体材料であり、当該三元主族又はカルコゲナイド半導体材料は好ましくは元素Bi、Sb及びTeを含み、好ましくは式(BiSb)2Te3により表されるものである。半導体マトリックス材料は、テルル化ビスマスとさらなる元素(例えば、電気伝導率の増加をもたらす元素)の合金、あるいはバルクで明らかな熱電効果を示す他の材料であることができる。熱電材料としては、高い性能指数を有し、高い変換効率を有する熱電デバイスで使用できる材料が挙げられる。
「ナノ包接物」は、マトリックス材料全体に分散されたナノ粒子である。本発明においては、ナノ包接物は、熱電マトリックス全体に分散されたセラミックナノ粒子を指す。
本明細書において使用する「半導体」という用語は、ドープされた半導体を包含する。三元半導体は、少なくとも3種の主な金属を含み、半導体特性を示すバルク構造を有する材料である。
従来の熱電材料は、典型的には、バルクで1未満の無次元性能指数ZTを有し、任意のかかる材料を、本発明の例において、材料として使用することができる。
当該デバイスは、熱源10、第1の電気伝導層12、第1の熱電材料14、第2の熱電材料16、第1の電気接点18、第2の電気接点20、ヒートシンク22、及び電気リード線26を通じて熱電デバイスに接続された抵抗負荷24を含む。熱源(TH>TC)により熱が与えられた場合、電流は図3に示されている方向に生じる。従って、この熱電デバイスは、熱入力から電気出力を生成するゼーベック熱電デバイスである。
再び、無酸素環境中で、6.5mLの水と5.5mLの28%水酸化アンモニウム中に溶解された9.0153gの酒石酸アンチモンカリウム及び1.5395gのクエン酸ビスマスの溶液を480mLの水に加えた。酸化亜鉛ナノ粒子の水溶液を添加しながら反応溶液を激しく撹拌した。
反応溶液をフリットガラスフィルター(まだ無酸素)に通して濾過し、激しく撹拌されているアンチモン/ビスマス/酸化亜鉛溶液中に入れた。溶液をさらに20分間撹拌し、常に無酸素環境下に保った。溶液を、即座に遠心分離して固体析出物を単離するか、あるいは、沈降、デカント、次いで遠心分離して固体析出物を単離した。この析出物を、副生成物が除去されるまで、水、メタノール及び水酸化アンモニウムの溶液により洗浄した。
次に、析出物をメタノールで洗浄し、超音波処理にかけながら不活性ガス流下で乾燥させた。この乾燥粉末を、真空下で、100℃で15分間、200℃で20分間、最後に300℃で20分間加熱した。得られた粉末を、次に、385〜450℃の温度で、100MPaで1〜10時間のいずれかでホットプレス焼結させて熱電材料を形成した。
Claims (12)
- 水性媒体中の還元化合物の形態にある少なくとも1種の金属を前記水性媒体中の酸化化合物の形態にある少なくとも1種の金属と混合することを含み、
前記混合が、主族金属の少なくとも3種の異なる金属化合物を混合することを含み、
前記混合が、式MO(ここで、Mは周期表の第2族又は第12族元素である)により表される物質のナノ粒子の存在下で実施され、
前記水性媒体が有機溶剤、界面活性剤又は分散剤を含まない、熱電材料の製造方法。 - 前記混合前に、金属粉末の形態にある金属を1又は2種以上の還元剤と水中で反応させることにより少なくとも1種の還元金属化合物を形成することをさらに含む、請求項1に記載の方法。
- 前記混合により形成された析出物を、
水、又は
極性有機物質及び塩基を含むアルカリ性水性組成物、
により洗浄することをさらに含む、請求項1に記載の方法。 - 洗浄された析出物を乾燥させ、次に、
当該洗浄された析出物をプレス成形し、
洗浄されプレス成形された析出物を焼結して、ナノ粒子を含む焼結三元熱電材料を形成すること、
をさらに含む、請求項3に記載の方法。 - 還元金属化合物が、テルル金属を水性アルカリ性媒体中で水素化ホウ素ナトリウムと反応させることにより形成される、請求項1に記載の方法。
- 2種の異なる酸化金属化合物を含む水性組成物を還元金属化合物と混合することを含む、請求項1に記載の方法。
- 前記酸化金属化合物は、ハロゲン化物、アルコキシド、カルボン酸塩またはそれらの混合物のうちの少なくとも一つの形態である、請求項6に記載の方法。
- 前記熱電材料は、
主族金属の3種の異なる金属化合物の三元半導体マトリックス、及び
前記式MOにより表される物質のナノ粒子、
を含み、
前記ナノ粒子は前記三元半導体マトリックス中に均一に分散されており、
前記三元半導体マトリックスは、組成に関して均一である、請求項1に記載の方法。 - 前記半導体マトリックスが、Bi、Te及びSbを含む、請求項8に記載の方法。
- 前記三元半導体マトリックスが(BiSb) 2 Te 3 である、請求項8に記載の方法。
- 前記三元半導体マトリックスが(BiSb) 2 Te 3 を含み、(BiSb) 2 Te 3 の含有量が、三元半導体マトリックスの総質量に基づいて少なくとも50質量%の量の(BiSb) 2 Te 3 を含む、請求項9に記載の方法。
- 前記三元半導体マトリックスが(BiSb) 2 Te 3 であり、ナノ粒子がZnOナノ粒子である、請求項8に記載の方法。
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US13/094,479 US8419980B2 (en) | 2011-04-26 | 2011-04-26 | Ternary thermoelectric material containing nanoparticles and process for producing the same |
US13/094,479 | 2011-04-26 |
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JP6022806B2 true JP6022806B2 (ja) | 2016-11-09 |
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US9847470B2 (en) * | 2011-04-26 | 2017-12-19 | Toyota Motor Engineering & Manufacturing North America, Inc. | Method of producing thermoelectric material |
US10672966B2 (en) | 2011-05-27 | 2020-06-02 | Toyota Motor Engineering & Manufacturing North America, Inc. | Method of producing thermoelectric material |
US8641917B2 (en) * | 2011-12-01 | 2014-02-04 | Toyota Motor Engineering & Manufacturing North America, Inc. | Ternary thermoelectric material containing nanoparticles and process for producing the same |
US8834736B2 (en) * | 2011-12-01 | 2014-09-16 | Toyota Motor Engineering & Manufacturing North America, Inc. | Ternary thermoelectric material containing nanoparticles and process for producing the same |
KR101473750B1 (ko) * | 2013-04-30 | 2014-12-18 | 재단법인대구경북과학기술원 | Bi2TeySe3-y 나노화합물 열전재료의 제조방법 및 이에 따라 제조되는 나노화합물 열전재료 |
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US8419980B2 (en) | 2013-04-16 |
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US20120273735A1 (en) | 2012-11-01 |
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