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CN1178204A - 热障涂层构件及其制作方法、使用该构件的燃气轮机零件 - Google Patents

热障涂层构件及其制作方法、使用该构件的燃气轮机零件 Download PDF

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CN1178204A
CN1178204A CN97118646.4A CN97118646A CN1178204A CN 1178204 A CN1178204 A CN 1178204A CN 97118646 A CN97118646 A CN 97118646A CN 1178204 A CN1178204 A CN 1178204A
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ceramic layer
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CN1073061C (zh
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浜田孝浩
高桥雅士
齐藤正弘
伊藤义康
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Abstract

热障涂层构件具有以下部分:由以Ni、Co及Fe中的至少一种为主要成分的高温合金形成的金属基材1;由覆盖在该金属基材1上的MCrAlY合金(M至少为Ni、Co及Fe中的一种)形成的中间层2;在该中间层2上形成的以稳定化氧化锆为主要成分的陶瓷层3。在陶瓷层3内,使熔点比氧化锆更高的陶瓷材料4复合化。

Description

热障涂层构件及其制作方法、使用该构件的燃气轮机零件
本发明涉及燃气轮机的转子叶片、定子叶片、燃烧器等高温零件，热障涂层构件及其制作方法。
近年来，在发电用燃气轮机领域，为了要求有效利用能源，以提高燃气轮机效率的研究开发正在积极进行。一般地说，燃烧器出口气体温度越高，相应地可提高该燃气轮机的发电效率，这一点是众所周知的。因此，作为提高燃气轮机效率的措施，谋求燃气轮机入口温度的提高被看作是很重要的。具体地说，对于燃气轮机的转子叶片、定子叶片、燃烧器等高温零件，以降低材料温度和提高耐热温度为目标的各种研究，讨论正在进行之中。
例如，作为降低材料温度的措施，为人所知的有在结构方面进行各种改进。例如采用薄膜冷却结构，阻隔来自于燃烧气体的热量；或采用喷射冷却结构，提高冷却特性；或采用回流结构，增大转子叶片以及定子叶片的冷却截面积。
另外，作为提高耐热温度的措施，可在材料方面进行各种改进。例如为提高高温强度，采用Ni、Co或Fe的超合金的高温材料的研制正在进行之中。但是，这种高温材料受到如下限制：在高温合金的特性方面，可以看到软化和再结晶等因素引起合金强度降低，在大约900～950℃以上的温度范围内几乎不能使用。
于是，作为其的改善措施，使用热障涂层(TBC：Thermal BarrierCoating)的技术正在受到关注。这种TBC就是在由高温合金(超合金)加工而成的金属基材上，涂覆氧化锆等热传导率低、化学性能稳定的隔热陶瓷层。一个用这种TBC形成的热障涂层构件的例子如图8所示。
图8所示的热障涂层构件采用具有以下部分的结构：以Ni、Co或Fe为主要成份的高温合金金属基材1；由涂覆在该基材1上的耐蚀，耐氧化性优良的MCrAlY(M是Ni、Co及Fe中的至少一种)合金形成的中间层2；在该中间层2上以稳定化氧化锆为主要成份的陶瓷层3。通过该陶瓷层3可抑制金属基材1温度的上升。其中：中间层2可保护金属基材1，并提高它与陶瓷层3的结合力。
据报道(如特开昭62-211387号公报等)：利用这样的热障涂层构件，例如厚度数100μm的隔热陶瓷层，可使金属基材的表面温度降低50～100℃。因此，如果把该热障涂层构件用在燃气轮机高温零件上，则可提高燃气轮机的运行气体温度而不会使金属基材温度上升，同时可进一步降低从燃烧气体一侧向冷却气体一侧流动的热流束，因此，这种热障涂层构件具有以下优点：除抑制金属基材的温度上升外，还可减少金属基材用冷却气体的流量。
但是，以前例子的热障涂层构件，在材料特性方面，陶瓷层的开裂和剥离等损伤现象很容易发生，此时隔热功能下降。金属基材温度上升，结果，在最坏的情况下有可能发生金属基体溶融、破坏这样的严重事件。在机器运转方面，这种事件的发生决不是所希望的。
于是，为防止这样的事态发生，各种改善措施被提了出来。这些措施着眼于产生陶瓷层开裂或剥离的主要原因，例如金属基材和陶瓷层之间的热膨胀系数差、中间层的氧化，腐蚀等。
例如，作为解决热膨胀差的措施，降低热应力的方法被提了出来，如在金属基材上涂覆陶瓷层后实施热处理。藉此可把压缩残余应力附加到热膨胀系数较小的陶瓷层上。此时陶瓷层在压缩残余应力场下使用，因而可降低起因于上述热膨胀系数差的开裂和剥离的发生。
另外，作为解决中间层氧化，腐蚀的措施，提高中间层耐蚀性的方法被提了出来。例如在中间层表面事先形成以Al为主要成份的氧化物层，以抑制氧侵入中间层内。在这种情况下，通过氧化物层可防止中间层内氧化，腐蚀的进行，起因于中间层氧化，腐蚀的陶瓷层的剥离可得到抑制。
但是，除了上述产生开裂和剥离等现象的主要原因外，往往由陶瓷层保护膜本身的反应烧结引起开裂的发生。关于它的解决办法，以前几乎没有注意和研究过。而且陶瓷层一般以采用热传导率低、化学性能稳定的Y2O3、MgO、CaO等来稳定的氧化锆(ZrO2)为主要成份，从降低热传导率的角度来考虑，把它作为含有大量气孔(多孔性)的结构，所以，当该陶瓷层产生反应烧结而变为气孔少的致密层时，产生热传导率增加、耐热性变差这样的问题也就可想而知了。
本发明对这样的问题进行了考虑，目的在于有效利用热障涂层的优点，这种热障涂层在金属基材上通过中间层形成以稳定化氧化锆为主要成份的陶瓷层，同时使由陶瓷层的反应烧结引起的裂纹降低，并抑制隔热性能的下降。
本发明为达到上述目的，采用种种材料进行了研究、实验，结果发现：作为以稳定化氧化锆为主要成份的陶瓷层抑制反应烧结的措施，使熔点比氧化锆更高的陶瓷材料在陶瓷层内复合是行之有效的，这样本发明便得以完成。
即本发明的热障涂层构件，其结构为：具有由高温合金形成的金属基材，该高温合金以至少一种Ni、Co及Fe为主要成份；在该金属基体上，通过由MCrAlY合金(M为Ni、Co及Fe中的至少一种)形成的中间层，形成了以稳定化氧化锆为主要成份的陶瓷层，其特征在于：上述陶瓷层是与熔点比氧化锆更高的陶瓷材料复合而成的。借助于该陶瓷材料，可抑制由陶瓷层的开裂引起的隔热性能的下降，并提高耐热性能。
上述陶瓷材料，希望是至少由下列物质中的一种组成的：HfC、NbC、SiC、TaC、Ta2C、TiC、WC、ZrC、HfB2、NbB2、TaB2、TiB2、ZrB2、BN、TaN、TiN、ZrN、HfO2以及ThO2。
在别的实施样态中，上述陶瓷材料最好在上述陶瓷层内部具有呈梯度分布的体积率，以使之从上述中间层的接合面开始，沿朝向外表面一侧的厚度方向增加。
此外，在另一侧面，本发明的热障涂层构件，其结构为：具有由高温合金形成的金属基材，该金属基材以至少一种Ni、Co及Fe为主要成份；在该金属基材上，通过由MCrAlY合金(M至少为Ni、Co及Fe中的一种)形成的中间层，形成了以稳定化氧化锆为主要成份的陶瓷层，其特征是：上述陶瓷层具有在厚度方向具有呈梯度分布的气孔率。
此时，上述陶瓷层所希望的气孔率是呈梯度分布的，并且使之从上述中间层的接合面一侧开始，沿朝向外表面一侧的厚度方向增加。
上述的热障涂层构件，可采用以下的制作方法加工。
即本发明的热障涂层构件的制作方法是：采用以至少一种Ni、Co及Fe为主要成份的高温合金加工金属基材，在该金属基材上，采用MCrAlY合金(M至少为Ni、Co及Fe中的一种)形成中间层，然后在该中间层上涂覆以稳定化氧化锆为主要成份的陶瓷层，其特征是：作为上述陶瓷层的原料，使用上述稳定化氧化锆原料粉末和熔点比氧化锆更高的陶瓷材料。
陶瓷层原料理想的制作方法如下：
1)：上述陶瓷层所使用的原料，为在上述稳定化氧化锆原料粉末上用高温热源使上述陶瓷材料熔融所得到的原料。
2)：上述陶瓷层所使用的原料，为采用机械合金化(MA)方法使上述稳定化氧化锆粉末和上述陶瓷材料相互混合所得到的原料。
3)：上述陶瓷层所使用的原料，为在上述稳定化氧化锆原料粉末上用化学气相沉积法涂覆上述陶瓷材料所得到的原料。
4)：使用上述稳定化氧化锆原料粉末形成上述陶瓷层，再用化学气相沉积法使上述陶瓷材料的供给气体扩散到该陶瓷层内，从而使上述陶瓷材料复合化。
作为上述陶瓷材料，希望采用至少由下列物质中的一种组成的材料：HfC、NbC、SiC、TaC、Ta2C、TiC、WC、ZrC、HfB2、NbB2、TiB2、TaB2、ZrB2、BN、TaN、TiN、ZrN、HfO2以及ThO2。
图1为说明本发明的热障涂层构件之概念的剖面示意图。
图2为工序示意图，表示本发明的热障涂层构件的制作方法。
图3为剖面示意图，说明陶瓷材料体积率的变化情况。
图4为剖面示意图，说明陶瓷层气孔率的变化情况。
图5为工序示意图，表示采用MA法时的制作方法。
图6为工序示意图，表示采用化学气相沉积法调整原料时的制作方法。
图7为剖面示意图，说明采用陶瓷材料的供给气体时的制作方法。
图8为剖面示意图，说明以前的热障涂层构件之概念。
下面参照图面说明本发明的热障涂层构件及其制作方法的实施形态。
图1所示的热障涂层构件可适用于高温零件，如燃气轮机的转子叶片、定子叶片、燃烧器等。它具有以下部分：以Ni、Co或Fe为主要成份的高温合金金属基材1；由涂覆在该基材1上的MCrAlY(M至少为Ni、Co及Fe中的一种)合金形成的中间层2；在该中间层2上以稳定化氧化锆为主要成份的陶瓷层3。在该陶瓷层3的内部，复合有熔点比上述氧化锆更高的陶瓷材料4。
当以图2为基础说明该热障涂层构件的制作方法时，则其制作方法如下：首先，在金属基材上用规定的涂覆方法形成中间层；其次，在该中间层上施以陶瓷涂层。如图2所示，在进行陶瓷涂层的涂覆时，在工序S1，采用大气等离子喷涂等方法，在稳定化氧化锆的原料粉末上，用高温热源(等离子体)使熔点比氧化锆更高的陶瓷材料熔融，以此为原料在工序S2使陶瓷材料复合成为一体。
因此，根据本实施形态，通过熔点比氧化锆更高的陶瓷材料，可有效地抑制陶瓷层中反应烧结的进行，并抑制由裂纹引起的隔热性能下降，结果，可提供耐热性大幅度提高的热障涂层构件。
另外，作为该热障涂层构件的变形例，也可以采用如图3或图4所示的构件。
图3所示的热障涂层构件是一种复合体，其中陶瓷材料4的体积率在陶瓷层3的内部呈梯度分布，并且在越靠近表面的地方，体积率越大。陶瓷层3由于越靠近表面，温度变得越高，所以通过改变陶瓷材料的体积率使之与陶瓷层3的温度梯度相一致，便可抑制陶瓷层3中反应烧结的进行，同时可使收缩率保持恒定，这种收缩现象是与陶瓷层3内部的烧结相伴而生的。因此，通过有效抑制陶瓷层3内部起因于不同收缩率的开裂的发生，便可抑制由开裂引起的隔热性能的下降。结果可使热障涂层构件的耐热性更进一步提高。
图4所示的热障涂层构件，它的陶瓷层3是这样设计的，即该陶瓷层3的气孔率呈梯度分布，并且在越靠近表面的地方，陶瓷层3内的气孔3a变得越大。即使在这种情况下，借助于陶瓷层3内的气孔3a，也可抑制陶瓷层中反应烧结的进行。另外，由于使陶瓷层3内的气孔率呈梯度分布，因而能够保持恒定的收缩率，这种收缩现象是与陶瓷层3内部的烧结相伴而生的。结果，可产生与上述情况大致相同的效果，而且还具有这样的优点，即它未必需要熔点比氧化锆更高的陶瓷材料。
另外，作为热障涂层构件制作方法的变形例，也可以采取如图5～图7所示的陶瓷涂覆方法。
图5说明了采用机械合金化(MA)方法调整原料时的制作方法。该方法可以制作陶瓷层，在工序S3，采用MA法使稳定化氧化锆原料粉末与熔点更高于氧化锆的陶瓷材料相互混合，在工序S4，它以此为原料使陶瓷材料与其复合成为一体。此时，由于陶瓷材料可均匀分散在整个陶瓷层中，因而在整体上可均匀、稳定地抑制陶瓷层中反应烧结的进行，结果可更有成效地抑制由开裂引起的隔热性能的下降。
图6说明了采用化学气相沉积(CVD)法调整原料时的制作方法。该方法可以制作陶瓷层，在工序S5，采用化学气相沉积法在稳定化氧化锆原料粉末上涂覆熔点比氧化锆更高的陶瓷材料，在工序S6，以此为原料使陶瓷材料与其复合成为一体。即使在这种情况下，也能使陶瓷材料均匀分散在整个陶瓷层中，因而可产生与上述情况大致相同的效果。
图7说明了采用化学气相沉积法使供给气体扩散到陶瓷层内时的制作方法。该制作方法可制作陶瓷层3，首先，在覆盖金属基材1的中间层2之表面上，涂覆形成以稳定化氧化锆为主要成份的陶瓷层3，然后用化学气相沉积法，使陶瓷材料4的供给气体4a在陶瓷层3内进行渗镀。藉此使陶瓷材料4与其复合成为一体。即使在这种情况下，也能使陶瓷材料均匀分散在整个陶瓷层中，因而可产生与上述情况大致相同的效果，而且还具有这样的优点，它即使在陶瓷层业已涂覆完毕的构件上也能实施。
其次，为验证所得到的上述热障涂层构件的特性，制作各种试样进行了试验，其结果如表1所示。
试  样No. 金属基材 中间层             陶    瓷    层 高温氧化试验结  果(μm)
种类 种类 制作条件 主要成份 复合化陶瓷材料 气孔率(％)
种类 体积率(％)
实施例1 HS-188 NiCoCrAlY APS ZrO2 SiC 5 13 3.1
实施例2 HS-188 NiCoCrAlY APS ZrO2 SiC 2→5→8 13 2.9
实施例3 HS-188 NiCoCrAlY APS ZrO2 无 无 10→16→20 3.2
实施例4 HS-188 NiCoCrAlY MA→APS ZrO2 SiC 5 13 2.4
实施例5 HS-188 NiCoCrAlY CVD→APS ZrO2 SiC 5 13 2.3
实施例6 HS-188 NiCoCrAlY APS→CVD ZrO2 SiC 5 13 2.5
比较例1 HS-188 NiCoCrAlY APS ZrO2 无 无 13 3.8
(实施例1)
实施例1采用大气等离子喷涂方法(APS)制作热障涂层构件，该热障涂层构件使用HS-188(Co基高温合金)作为金属基材，使用NiCoCrAlY合金作为中间层。陶瓷层则以稳定化氧化锆为主要成份。并使SiC与之复合。该喷涂方法所设定的工艺条件为：喷涂距离100mm、喷涂速度450mm/Sec、粉末供给量30g/min、电流500A、电压68V。其结果正如表1所示，所得到的试样，其陶瓷层的气孔率为13％，陶瓷材料的体积率为5％。
(实施例2)
实施例2采用与实施例1大致相同的工艺条件制作含有陶瓷层的热障涂层构件，在该陶瓷层中，陶瓷材料的体积率呈梯度分布。其结果正如表1所示，所得到的试样，其陶瓷层的气孔率为13％，陶瓷材料的体积率沿着朝陶瓷层表面的方向、分阶段依次为2％、5％、8％。
(实施例3)
实施例3采用与实施例1大致相同的工艺条件制作热障涂层构件，它没有使用陶瓷材料，而是使陶瓷层的气孔率呈梯度分布。其结果正如表1所示，所得到的试样，其陶瓷层的气孔率沿着朝陶瓷层表面的方向、分阶段依次为10％、16％、20％。
(实施例4)
实施例4在采用上述MA法时的工艺条件下，制作了与实施例1相同的热障涂层构件。其结果正如表1所示，所得到的试样，其陶瓷层的气孔率为13％，陶瓷材料的体积率为5％。
(实施例5)
实施例5在采用上述化学气相沉积法调整原料时的工艺条件下，制作了与实施例1相同的热障涂层构件。其结果正如表1所示，所得到的试样，其陶瓷层的气孔率为13％，陶瓷材料的体积率为5％。
(实施例6)
实施例6在采用化学气相沉积法使供给气体向陶瓷层内扩散时的工艺条件下，制作了热障涂层构件。其结果正如表1所示，所得到的试样，其陶瓷层的气孔率为13％，陶瓷材料的体积率为5％。
(比较例1)
比较例1采用与实施例1相同的工艺条件，不使用陶瓷材料而制作了热障涂层构件。其结果正如表1所示，其陶瓷层的气孔率为13％。
上述各试样均在850℃进行2000小时的大气高温氧化试验。其中，热障涂层构件的中间层和陶瓷层之间生成的氧化膜一般是产生剥离的主要原因，所以，作为评价热障涂层构件性能的指标，对中间层和陶瓷层之间因高温氧化试验而生成的氧化膜的厚度进行了测定。
其结果正如表1所示，根据实施例1～3的情况可以确认：与比较例1相比，实施例1～3的氧化膜厚度明显要薄；通过陶瓷材料的复合以及使之呈梯度分布、或者仅使陶瓷材料呈梯度分布，便能提供耐热性比以前的例子更为优良的热障涂层构件。另外，根据实施例4～6可以确认：由于氧化膜厚度更加薄，通过采用MA法以及化学气相沉积法制作原料粉末，可提供耐热性更为优良的热障涂层构件。
另外，对于下列的其它情况，其结果也与上述结果大致相同，这些情况分别是：1)：金属基材采用HS-188以外的上述高温合金，2)：中间层采用除NiCoCrAlY合金以外的上述MCrAlY(M为Co、Fe或其合金以及与Ni形成的合金)合金，3)：复合在陶瓷层中的陶瓷材料采用除SiC以外的至少由下列物质中的一种材料或者该材料与SiC的混合物所形成，这些物质包括：HfC、NbC、TaC、Ta2C、TiC、WC、ZrC、HfB2、NbB2、TaB2、TiB2、ZrB2、BN、TaN、TiN、ZrN、HfO2及ThO2。
正如上面所说明的那样，根据本发明，由于使熔点比氧化锆更高的陶瓷材料复合在以稳定化氧化锆为主要成份的陶瓷层内，因而难以发生陶瓷层保护膜的反应烧结，抑制了陶瓷层内裂纹的发生以及与裂纹相伴而生的隔热性能的下降，结果，大幅度提高了热障涂层构件的耐热性。特别是在陶瓷材料的体积率或陶瓷层内的气孔率呈梯度分布的情况下，这种效果可更加充分地发挥出来。

Claims (12)

1.一种热障涂层构件，它具有由高温合金形成的金属基材，这种高温合金以Ni、Co及Fe中的至少一种为主要成份，在该金属基材上，通过由MCrAlY合金—M为Ni、Co及Fe中的一种—形成的中间层，形成了以稳定化氧化锆为主要成份的陶瓷层；其特征在于：上述陶瓷层是由熔点比氧化锆更高的陶瓷材料复合而成的。
2.一种如权利要求1所记载的热障涂层构件，其特征在于：上述陶瓷材料至少由下列物质中的一种所组成：HfC、NbC、SiC、TaC、Ta2C、TiC、WC、ZrC、HfB2、NbB2、TaB2、TiB2、ZrB2、BN、TaN、TiN、ZrN、HfO2及ThO2。
3.一种如权利要求1或2所记载的热障涂层构件，其特征在于：上述陶瓷材料在上述陶瓷层的内部，具有呈梯度分布的体积率，使该体积率从上述中间层的接合面开始，沿朝向外表面的厚度方向增加。
4.一种热障涂层构件，包括由高温合金形成的金属基材，这种高温合金以Ni、Co及Fe中至少一种为主要成份，在该金属基材上，通过由MCrAlY合金—M至少为Ni、Co及Fe中的一种—形成的中间层，形成了以稳定化氧化锆为主要成份的陶瓷层；其特征在于：上述陶瓷层具有在厚度方向呈梯度分布的气孔率。
5.一种如权利要求4所记载的热障涂层构件，其特征在于：上述陶瓷层的气孔率呈梯度分布，使气孔率从上述中间层的接合面开始，沿朝向外表面的厚度方向增加。
6.一种热障涂层构件的制作方法，它采用以Ni、Co及Fe中的至少一种为主要成份的高温合金形成金属基材，在该金属基材上采用MCrAlY合金—M至少为Ni、Co及Fe中的一种-形成中间层，在该中间层上涂覆形成以稳定化氧化锆为主要成份的陶瓷层；其特征在于：作为上述陶瓷层的原料，使用上述稳定化氧化锆原料粉末和熔点比氧化锆更高的陶瓷材料。
7.一种如权利要求6所记载的热障涂层构件的制作方法，其特征在于：作为上述陶瓷层的原料，使用在上述稳定化氧化锆原料粉末上，用高温热源使上述陶瓷材料熔融所得到的原料。
8.一种如权利要求6所记载的热障涂层构件的制作方法，其特征在于：作为上述陶瓷层的原料，使用以机械合金化-MA-方法使上述稳定化氧化锆原料粉末和上述陶瓷材料相互混合所得到的原料。
9.一种如权利要求6所记载的热障涂层构件的制作方法，其特征在于：作为上述陶瓷层的原料，使用以化学气相沉积方法在上述稳定化氧化锆原料粉末上涂覆上述陶瓷材料所得到的原料。
10.一种如权利要求6所记载的热障涂层构件的制作方法，其特征在于：使用上述稳定化氧化锆原料粉末形成上述陶瓷层，再用化学气相沉积法使上述陶瓷材料的供给气体扩散到该陶瓷层内，藉此使上述陶瓷材料复合化。
11.一种如权利要求6至权利要求10中的任一项所记载的热障涂层构件的制作方法，其特征在于：作为上述陶瓷材料，采用至少由下列物质中的一种形成的材料：HfC、NbC、SiC、TaC、Ta2C、TiC、WC、ZrC、HfB2、NbB2、TaB2、TiB2、ZrB2、BN、TaN、TiN、ZrN、HfO2及ThO2。
12.一种燃气轮机零件，其特征在于：该零件使用权利要求1至权利要求5中的任一项所记载的热障涂层构件。
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