JP4823516B2 - 複合ペロブスカイトよりなる断熱材料層 - Google Patents

複合ペロブスカイトよりなる断熱材料層 Download PDF

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JP4823516B2
JP4823516B2 JP2004513208A JP2004513208A JP4823516B2 JP 4823516 B2 JP4823516 B2 JP 4823516B2 JP 2004513208 A JP2004513208 A JP 2004513208A JP 2004513208 A JP2004513208 A JP 2004513208A JP 4823516 B2 JP4823516 B2 JP 4823516B2
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layer
heat insulating
thermal insulation
insulating material
layer system
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JP2005537203A5 (ja
JP2005537203A (ja
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ファッセン・ローベルト
シュヴァルツ−リュックゲ・ジークリート
ユンゲン・ヴァルフガング
シュテーファー・デトレフ
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フォルシュングスツェントルム・ユーリッヒ・ゲゼルシャフト・ミット・ベシュレンクテル・ハフツング
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    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/12—All metal or with adjacent metals
    • Y10T428/12493—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.]
    • Y10T428/12771—Transition metal-base component
    • Y10T428/12861—Group VIII or IB metal-base component
    • Y10T428/12944—Ni-base component
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y10—TECHNICAL SUBJECTS COVERED BY FORMER USPC
    • Y10T—TECHNICAL SUBJECTS COVERED BY FORMER US CLASSIFICATION
    • Y10T428/00—Stock material or miscellaneous articles
    • Y10T428/12—All metal or with adjacent metals
    • Y10T428/12493—Composite; i.e., plural, adjacent, spatially distinct metal components [e.g., layers, joint, etc.]
    • Y10T428/12771—Transition metal-base component
    • Y10T428/12861—Group VIII or IB metal-base component
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Description

【技術分野】
【０００１】
本発明は、複合ペロブスカイトで構成された断熱層に関する。
【背景技術】
【０００２】
固定−およびフライング−ガスタービンの性能を増すために、今日ではより高いガス温度がかゝる機械では必要とされる。この目的のためにはタービンの構成要素には、一般にイットリウムで安定化された酸化ジルコニウム（ＹＳＺ）よりなる断熱層（ＷＤＳ）が設けられている。構造要素と断熱層との間にＭＣｒＡｌＹ合金（Ｍ＝Ｃｏ、Ｎｉ）またはアルミニド層よりなる中間層が主として構造要素の酸化防止に役立つ。この系では今日ではタービン構成要素の表面温度を１２００℃まで実現し得る。
【０００３】
しかしながら１３００℃以上に更に高めることは、今日までに使用される材料では、特にＹＳＺでは達成できない。プラズマ溶射または電子線蒸着により析出される酸化ジルコニウムは１２００℃以上の温度では相転換並びに促進された焼結工程を経て、運転中に層に損傷がもたらされ得る。断熱層が同じ熱伝導性でそして同じ層厚である場合には、高い表面温度は中間層および構造要素において更に高い温度になる。この温度上昇も同様に材料間の結合をますます劣化させもする。
【０００４】
この理由のから、断熱層の材料としての部分的に安定化された酸化ジルコニウムと交換し得る新たな材料が広く世界中で研究されている。
【０００５】
ドイツ特許出願公開第１００５６６１７号明細書（Ａ１）から、Ｌａ、Ｃｅ、ＰｒまたはＮｄをＡ−位置に有しそしてＥｒ、Ｔｍ、ＹｂまたはＬｕをＢ−位置に有する希土類ペロブスカイトを断熱層材料として使用することが公知である。このものは、材料次第で１８００℃以上、それどころか特に２０００℃以上でさえある高い溶融温度に特徴がある。材料がそれの溶融温度を達成することによってこの範囲まで、かゝる材料は層転移を生じないし、それ故に相応する目的にとって、特に断熱層として使用することができる。この上述のペロブスカイトの別の性質は一般に８．５×１０-6Ｋ-1より高い熱膨張係数である。更に断熱層として使用するためには２．２Ｗ／ｍＫより小さい熱伝導性も有利である。
【０００６】
これらの性質を持つペロブスカイトは、適合した熱膨張係数が温度を高めた際に両方の材料の間の機械的応力を低減しそして低い熱伝導性が構造要素の過熱を一般に防止するので、金属製構造要素での断熱層として特に良好に適している。
【０００７】
更に、一般式Ａ２＋（Ｂ２ １／３ ＋Ｂ５＋ ２／３）Ｏ３で表される複合ペロブスカイトは公知である。このペロブスカイトはそれの温度均一化効果およびそれの損失の少ない誘電体として役立つ能力のために多くの無線の通信装置において使用されることが公知である（Ｌ．Ｄｕｐｏｎｔ， Ｌ．Ｃｈａｉ，Ｐ．Ｋ．Ｄａｖｉｅｓ：“Ａ− ａｎｄ Ｂ−ｓｉｔｅ ｏｒｄｅｒ ｉｎ （Ｎａ１／２Ｌａ１／２）（Ｍｇ１／３Ｔａ２／３）Ｏ３Ｐｅｒｏｗｓｋｉｔｅｓ”； Ａ．Ｓ． Ｂｈａｌｌａ， Ｒ．Ｇｕｏ， Ｒ．Ｒｏｙ，“Ｔｈｅ ｐｅｒｏｗｓｋｉｔｅ ｓｔｒｕｃｔｕｒｅ − ａ ｒｅｖｉｅｗ ｏｆ ｉｔｓ ｒｏｌｅ ｉｎ ｃｅｒａｍｉｃ ｓｃｉｅｎｃｅ ａｎｄ ｔｅｃｈｎｏｌｏｇｙ”， Ｍａｔ． Ｒｅｓ． Ｉｎｎｏｖａｔ． （２０００） 第４巻、第３〜２６行）。
【０００８】
本発明の課題は、低い熱伝導性、高い熱膨張係数、高い焼結温度の要求と同時に良好な相安定性を１３００℃以上の温度まで満足する断熱層用の断熱材料を提供することである。更に本発明の課題は、かゝる断熱層を有する熱応力の掛かる要素に関する。
【課題を解決するための手段】
【０００９】
この課題は請求項１の特徴的構成要件を備えた断熱層用の断熱材料並びにこの断熱材料の、構成要素の表面の断熱層としての請求項４の用途によって解決される。有利な実施態様はそれぞれの従属形式の請求項に記載されている。
【００１０】
本発明の対象は、複合ペロブスカイト構造、２５００℃以上の融点、８×１０−６Ｋ−１より大きい熱膨張係数並びに１４００℃より高い焼結温度を有する断熱材料よりなる断熱層に関する。この断熱材料は更に、以下の一般式で表される複合ペロブスカイト構造に特徴がある：
Ａ１＋ｒ（Ｂ’１／３＋ｘＢ”２／３＋ｙ）Ｏ３＋ｚ
この場合、ＡはＢａ、Ｓｒ、Ｃａ、Ｂｅよりなる群の少なくとも１つの元素を意味し、Ｂ’はＭｇ、Ｂａ、Ｓｒ、Ｃａ、Ｂｅよりなる群の少なくとも１つの元素を意味しそしてＢ”はＴａ、Ｎｂよりなる群の少なくとも１つの元素を意味する。場合によってはこの断熱材料は以下の式の組成を有していてもよい：
Ａ１＋ｒ（Ｂ’１／２＋ｘＢ”１／２＋ｙ）Ｏ３＋ｚ
この場合、ＡはＢａ、Ｓｒ、Ｃａ、Ｂｅよりなる群の少なくとも１つの元素を、Ｂ’はＡｌ、Ｌａ、Ｎｄ、Ｇｄ、Ｅｒ、Ｌｕ、Ｄｙ、Ｔｂよりなる群の少なくとも１つの元素をそしてＢ”はＴａ、Ｎｂよりなる群の少なくとも１つの元素を選択することができる。上記の両方の組成について化学量論から僅かにずれた化合物も、即ち−０．１＜ｒ、ｘ、ｙ、ｚ＜０．１の化合物が本発明の範囲に包含される。
【００１１】
本発明者は、ペロブスカイトの種類の他の多くの材料と相違して上記の断熱材料は、Ｂ’およびＢ”原子の層が化学量論に相応して交換されている層構造が、配列した状態で形成されていることを見出した。Ｂ−位置の３つ以上の原子もほぼ化学量論を維持している場合には可能であり、原子の混合物がＡ−位置にある場合も同様である。化学量論からの５％までの範囲内での僅かなずれは許容できる。
【００１２】
更に元のカチオンのイオン半径から著しくずれたイオン半径を有していない異カチオンを数％の量で添加することも可能である。
【００１３】
断熱材料は有利には８×１０-6／Ｋより多い高い膨張係数および低下した焼結傾向を有しているのが有利である。これらの材料の一般的な焼結温度は１４００℃以上である。
【００１４】
全ての断熱材料は１３５０℃以上までの高い相安定性を有している。これらのペロブスカイトの熱伝導性は、３Ｗ／ｍ／Ｋより小さい熱伝導性は特に低くかつ満足であるので、断熱材料として使用するのに特に有利である。
【００１５】
更に本発明の断熱材料の融点は一般に２０００℃以上であり、一部は２５００℃以上でさえある。更にこの種類の材料では、追加的に熱伝導性を低減するカチオン量間に中位いから大きいまでの差が発生する。
【００１６】
これらの全ての性質は上述の材料を断熱層材料として使用するのに非常に適するものとしている。
【００１７】
上述の断熱物質の群の特に有利な代表例はＢａ（Ｍｇ1/3 Ｔａ2/3 ）Ｏ3 である。特に適することが判っている他の化合物はＳｒ（Ａｌ1/2 Ｔａ1/2 ）Ｏ3 、Ｃａ（Ａｌ1/2 Ｎｂ1/2 ）Ｏ3 、Ｓｒ（Ｓｒ1/3 Ｔａ2/3 ）Ｏ3 またはＳｒ（Ｌａ1/2 Ｔａ1/2 ）Ｏ3 である。
【００１８】
これらの材料から製造される断熱層は一般に約３０００℃の融点および極めて低い焼結傾向を有している。
【００１９】
実施例：
以下の本発明の対象を実験的態様との関連で更に詳細に説明するが、本発明はこれらに限定されない。
【実施例１】
【００２０】
断熱材料の性質：
以下の組成を有する有利な断熱材料から得られる特に適する断熱層を
Ｂａ（Ｍｇ1/3 Ｔａ2/3 ）Ｏ3
最初にＢａＣＯ3 、ＭｇＯおよびＴａ2 Ｏ5 の固体反応によって製造する。この材料をプレス成形した後に、顕著な焼結収縮を生じることなく１６００℃で数時間焼結する。それ故にこの材料は、小さい焼結傾向が望まれる断熱層として使用するのに適している。これは断熱層として使用するのに必要とされる、材料の小さい焼結傾向を証明している。
【００２１】
同様にＳｒ（Ａｌ1/2 Ｔａ1/2 ）Ｏ3 またはＣａ（Ａｌ1/2 Ｔａ1/2 ）Ｏ3 をＡｌ2 Ｏ3 およびＴａ2 Ｏ5 およびＳｒＣＯ3 あるいはＣａＣＯ3 から製造することができる。一般に元素のバリウム、ストロンチウムおよびカルシウムは炭酸塩としてそして残りの元素は酸化物として混合物中にもたらすことができる。個々の化合物は上述の化学量論的組成に相応して選択する。次に固体反応によって所望のペロブスカイトを得る。上述した通り化学量論から僅かにずれた組成も原料の量を適切に選択することによって達成できる。
【００２２】
こうして製造されたＢａ（Ｍｇ1/3 Ｔａ2/3 ）Ｏ3 を用いてディレトメータ試験を実施する。図面にこの材料についての結果を示した。この断熱材料は１０００℃で１０．４×１０-6／Ｋの熱膨張を示す。この値は標準材料ＹＳＺに匹敵しそしてそれ故に断熱層として使用するのに同様に非常に適している。
【実施例２】
【００２３】
断熱層系（ＷＤＳ）の製造
実施例１と同様に固体反応によって製造されるＢａ（Ｍｇ１／３Ｔａ２／３）Ｏ３組成を有する断熱材料を噴霧乾燥によって更に粉砕し、次いで大気プラズマ溶射（ＡＰＳ）の様な熱溶射法によってＷＤＳ−系に加工する。この目的のためにニッケル−またはコバルト−ベース合金を（真空）プラズマ溶射によって最初にＭＣｒＡｌＹ（Ｍ＝Ｃｏ、Ｎｉ）中間層と一緒に設ける（この層の厚さ：約５０〜５００μｍ）。次いで大気プラズマ溶射（ＡＰＳ）によって本発明の材料よりなる断熱層を約５０〜３０００μｍの層厚で設ける。場合によっては、最初に標準ＷＤＳ材料のＹＳＺよりなる層を設けそして上側層として本発明の断熱材料、例えばＢａ（Ｍｇ１／３Ｔａ２／３）Ｏ３（ＢＭＴ）を析出させることによって二層断熱層も製造することができる。
【００２４】
使用した略字のリスト：
ＷＤＳ ＝ 断熱層
ＹＳＺ ＝ イットリウムで部分的に安定化した酸化ジルコン
ＡＰＳ ＝ 大気プラズマ溶射
ＰＶＤ ＝ 物理蒸着法
ＢＭＴ ＝ Ｂａ（Ｍｇ，Ｔａ）Ｏ3
【図面の簡単な説明】
【００２５】
【図１】図１は実施例１の断熱材料についてのディレトメータ試験の結果をグラフ化したものである。

Claims (6)

  1. 構造要素および該構造要素の表面に設けられた断熱層を有する層系であって、該断熱層が２５００℃以上の融点、８×１０−６Ｋ−１より大きい熱膨張係数並びに１４００℃より高い焼結温度を有する断熱材料よりなり、層系において、該断熱材料がＢａ（Ｍｇ１／３Ｔａ２／３）Ｏ３、Ｓｒ（Ａｌ１／２Ｔａ１／２）Ｏ３、Ｃａ（Ａｌ１／２Ｎｂ１／２）Ｏ３、Ｓｒ（Ｓｒ１／３Ｔａ２／３）Ｏ３又はＳｒ（Ｌａ１／２Ｔａ１／２）Ｏ３で表されるペロブスカイト構造を有することを特徴とする、上記層系。
  2. 断熱材料が式Ｂａ（Ｍｇ１／３Ｔａ２／３）Ｏ３で表されるペロブスカイト構造を有する、請求項１に記載の層系。
  3. 構造要素と断熱層との間に中間層の材料としてＭＣｒＡｌＹ合金（Ｍ＝Ｃｏ，Ｎｉ）を設けている、請求項２に記載の層系。
  4. 構造要素と断熱層との間に中間層の材料としてアルミニド層を設けている、請求項２に記載の層系。
  5. 請求項１〜４のいずれか一つに記載の層系を製造する方法において、以下の各段階
    − 断熱層の原料を炭酸塩および／または酸化物として上述の化学量論に相応して混合物として存在させ、
    − この混合物を固体反応に付し、その際に生じた断熱材料が相応する化学量論およびペロブスカイト構造を有し
    − こうして製造された断熱材料を構造要素の表面に適用する
    を含むことを特徴とする、上記方法。
  6. 固体反応後のペロブスカイトがＢａ（Ｍｇ１／３Ｔａ２／３）Ｏ３、Ｓｒ（Ａｌ１／２Ｔａ１／２）Ｏ３、Ｃａ（Ａｌ１／２Ｎｂ１／２）Ｏ３、Ｓｒ（Ｓｒ１／３Ｔａ２／３）Ｏ３又はＳｒ（Ｌａ１／２Ｔａ１／２）Ｏ３に従う組成を有するように断熱層用の混合物を製造する、請求項５に記載の方法。
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US20050260435A1 (en) 2005-11-24
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EP1513781B1 (de) 2006-05-17
US7468213B2 (en) 2008-12-23
DE10226295A1 (de) 2004-01-08
EP1513781B9 (de) 2007-02-28
US7585575B2 (en) 2009-09-08
US20090098390A1 (en) 2009-04-16
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ATE326439T1 (de) 2006-06-15

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