CN117383937A - 一种高熵稀土钽酸盐陶瓷涂层材料及制备方法 - Google Patents
一种高熵稀土钽酸盐陶瓷涂层材料及制备方法 Download PDFInfo
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- 239000000463 material Substances 0.000 title claims abstract description 54
- 229910052761 rare earth metal Inorganic materials 0.000 title claims abstract description 37
- 150000002910 rare earth metals Chemical class 0.000 title claims abstract description 36
- 238000005524 ceramic coating Methods 0.000 title claims abstract description 35
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- VQCBHWLJZDBHOS-UHFFFAOYSA-N erbium(iii) oxide Chemical compound O=[Er]O[Er]=O VQCBHWLJZDBHOS-UHFFFAOYSA-N 0.000 claims description 8
- PLDDOISOJJCEMH-UHFFFAOYSA-N neodymium(3+);oxygen(2-) Chemical compound [O-2].[O-2].[O-2].[Nd+3].[Nd+3] PLDDOISOJJCEMH-UHFFFAOYSA-N 0.000 claims description 8
- LFQSCWFLJHTTHZ-UHFFFAOYSA-N Ethanol Chemical compound CCO LFQSCWFLJHTTHZ-UHFFFAOYSA-N 0.000 claims description 6
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- 229910001936 tantalum oxide Inorganic materials 0.000 claims description 5
- 229910003440 dysprosium oxide Inorganic materials 0.000 claims description 4
- NLQFUUYNQFMIJW-UHFFFAOYSA-N dysprosium(iii) oxide Chemical compound O=[Dy]O[Dy]=O NLQFUUYNQFMIJW-UHFFFAOYSA-N 0.000 claims description 4
- JYTUFVYWTIKZGR-UHFFFAOYSA-N holmium oxide Inorganic materials [O][Ho]O[Ho][O] JYTUFVYWTIKZGR-UHFFFAOYSA-N 0.000 claims description 4
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- SIWVEOZUMHYXCS-UHFFFAOYSA-N oxo(oxoyttriooxy)yttrium Chemical compound O=[Y]O[Y]=O SIWVEOZUMHYXCS-UHFFFAOYSA-N 0.000 claims description 4
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Abstract
本发明涉及一种高熵稀土钽酸盐陶瓷涂层材料及制备方法，属于高熵陶瓷材料技术领域。所述涂层材料的物相组成为(Nd0.2Dy0.2Ho0.2Y0.2Er0.2)TaO4。所述制备方法通过将原料粉体湿法球磨混合均匀，形成浆料，干燥后得到的粉体升温至1450℃～1550℃恒温煅烧8h～10h，制得所述涂层材料。所述涂层材料通过将五种稀土氧化物与Ta2O5固溶，形成具有单斜晶体结构的单相化合物，由于高熵化的晶格畸变效应显著改善了稀土钽酸盐的热导率，因此所述涂层材料具有优异热物理性能，具有1.41W·m‑1·K‑1的低热导率，10.5×10‑6K‑1的热膨胀系数，并具有优异的热稳定性，可以作为TPC的候选材料，在关键高端装备热防护涂层领域具有广泛的应用场景；采用高温固相反应法制备所述涂层材料的工艺流程简洁，制备成本较低，易于推广。
Description
技术领域
本发明涉及一种高熵稀土钽酸盐陶瓷涂层材料及制备方法，具体地说，涉及一种具有低热导率、良好热稳定性和高结合强度的(Nd0.2Dy0.2Ho0.2Y0.2Er0.2)TaO4热防护陶瓷涂层材料及制备方法，属于高熵陶瓷材料技术领域。
背景技术
随着航空发动机、燃气轮机等高温设备向着高质量方向发展，其内部零件将面临更加严苛的高温环境。为了提高此类零部件的寿命，提高其使用性能，通常在零部件表面添加一层陶瓷涂层作为热防护涂层，以起到隔热，抗腐蚀的作用，保证其在相对较低的温度下工作。目前，常用的热防护材料是氧化钇稳定氧化锆(YSZ)。但是，YSZ在高温下会发生相变，造成涂层开裂、剥落等问题，导致它最高的服役温度为1200℃，限制了它的使用。因此，人们开始寻找能在更高温下服役，热防护性能更好的涂层材料。
稀土钽酸盐(RETaO4)由于其优异的热物理性能，引起了极大的关注。Levi教授的前期研究表明，YTaO4的使用温度可以达到1600℃，且在800℃下热导率为1.51W/m·K，是一种极具潜力的热防护涂层(TPC)材料。然而，先前的研究表明，YTaO4导热系数仍然不够低。这极大的限制了YTaO4作为TPC材料的应用。
与单元素陶瓷相比，高熵陶瓷(HECs)由于其独特的高熵效应，如低热导率、热膨胀系数可调等，并表现出良好的高温稳定性。因此，通过设计高熵陶瓷材料组件、微结构，特别是利用HEC中独特的晶格畸变效应来降低材料的导热系数，合成具有优良性能的HEC，为创造新的TPC材料提供了有效途径。
发明内容
为克服现有技术存在的缺陷，本发明的目的在于提供一种高熵稀土钽酸盐陶瓷涂层材料及其制备方法。
为实现本发明的目的，提供以下技术方案。
一种高熵稀土钽酸盐陶瓷涂层材料，所述陶瓷涂层材料的物相组成为(Nd0.2Dy0.2Ho0.2Y0.2Er0.2)TaO4。
一种本发明所述高熵稀土钽酸盐陶瓷涂层材料的制备方法，所述方法步骤如下：
(1)按照所述涂层材料的物相组成，采用化学计量比称取各个原料粉体，采用湿法球磨混合均匀，形成浆料；
步骤(1)中：
所述原料粉体为氧化钕、氧化镝、氧化钬、氧化钇、氧化铒和氧化钽的粉体。
优选所述原料粉体的粒径均为5μm～10μm。
优选所述原料粉体的纯度≥99.9％。
优选所述球磨的磨球与原料粉体的质量比为5:1。
优选所述球磨的球磨介质为无水乙醇。
优选所述球磨的球磨转速为250r/min～300r/min，球磨时间为8h～10h。
(2)将步骤(1)制得的浆料干燥去除球磨介质，得到粉体，将粉体升温至1450℃～1550℃恒温煅烧8h～10h，制备得到本发明所述的一种高熵稀土钽酸盐陶瓷涂层材料。
步骤(2)中：
优选先采用旋转蒸发进行干燥，然后烘干，具体方法如下：
将步骤(1)制得的浆料置于容器中在75℃～80℃旋转蒸发进行干燥，待容器中无明显液滴后，继续旋转蒸发5min～8min，保证旋转蒸发后的粉体中不含或含少量的球磨介质；然后将旋转蒸发后的原料在95℃～100℃继续干燥6h～10h。
优选浆料干燥后进行研磨，过筛，得到过筛后的粉体，再升温煅烧。
优选将粉体以5℃/min～10℃/min的速率升温至1450℃～1550℃。
一种高熵稀土钽酸盐陶瓷涂层，所述涂层采用本发明所述的一种高熵稀土钽酸盐陶瓷涂层材料高温镍基合金基底上制备得到。
有益效果
(1)本发明提供了一种高熵稀土钽酸盐陶瓷涂层材料，所述涂层材料通过将Nd2O3、Dy2O3、Ho2O3、Y2O3和Er2O3五种稀土氧化物与Ta2O5固溶，形成具有单斜晶体结构的单相化合物，物相组成为(Nd0.2Dy0.2Ho0.2Y0.2Er0.2)TaO4，相对于常用的单组分YTaO4，由于高熵化的晶格畸变效应显著改善了稀土钽酸盐的热导率，因此所述涂层材料具有优异热物理性能，具有1.41W·m-1·K-1的低热导率，10.5×10-6K-1的热膨胀系数，并具有优异的热稳定性，可以作为TPC的候选材料，在关键高端装备热防护涂层领域具有广泛的应用场景。
(2)本发明提供了一种高熵稀土钽酸盐陶瓷涂层材料的制备方法，所述制备方法将五种稀土氧化物和氧化钽通过固相烧结的方式制得所述涂层材料。
(3)本发明提供了一种高熵稀土钽酸盐陶瓷涂层材料的制备方法，所述制备方法中，步骤(1)中通过湿法球磨使得原料粉末充分均匀混合，可以使高温合成的高熵稀土钽酸盐陶瓷涂层材料元素分布均匀，不会存在某一稀土元素团聚富集；
优选所述原料粉体的粒径均为5μm～10μm，粉体粒径均匀能有效提高合成效率，保证合成材料物相组成单一性；
优选所述球磨的磨球与原料粉体的质量比为5:1；所述球磨的球磨转速为250r/min～300r/min，球磨时间为8h～10h；保证原料充分混合均匀。
(4)本发明提供了一种高熵稀土钽酸盐陶瓷涂层材料的制备方法，所述制备方法中，所述制备方法中，步骤(2)中在1450℃～1550℃，恒温煅烧8h～10h；在此煅烧条件下，可以合成单一相的(Nd0.2Dy0.2Ho0.2Y0.2Er0.2)TaO4，超出此条件，产物将会有第二相杂质，无法保证(Nd0.2Dy0.2Ho0.2Y0.2Er0.2)TaO4单一相；
优选先干燥时对浆料二次烘干，能够充分的将无水乙醇蒸干。降低粉体的团聚，提高过筛效率
优选浆料干燥后进行研磨，过筛，得到过筛后的粉体，再升温煅烧，使得煅烧的粉体颗粒均匀，可以使所述涂层材料颗粒大小分布均匀，具有较好的颗粒形貌。
(6)本发明提供了一种高熵稀土钽酸盐陶瓷涂层，所述涂层采用本发明所述的一种高熵稀土钽酸盐陶瓷涂层材料，适于配合高温镍基合金基底使用；所述涂层具有低热导率，高热膨胀系数和优异的热稳定性，在关键高端装备热防护涂层领域具有广泛的应用场景。
附图说明
图1为实施例1中制备的粉体样品的XRD图。
图2为实施例1中制备的粉体样品的SEM图。
图3为实施例2中制备的粉体样品的XRD图。
图4为实施例1中制备的块体样品的热导率结果。
图5为实施例1中制备的块体样品的热膨胀系数图
具体实施方式
下面结合附图和具体实施例来详述本发明，但不作为对本发明专利的限定。本发明中所述实验材料如没有特别说明均可以从商业途径获取，所述实验方法如没有特别说明均为常规方法。
以下实施例中：
原料粉体氧化钕、氧化镝、氧化钬、氧化钇、氧化铒和氧化钽的粒径均为5μm～10μm，纯度均≥99.9％。
对制得的粉体样品和块体样品进行如下测试：
(1)X射线衍射(XRD)
厂家：荷兰PANalytical，仪器型号：帕纳科Empyrean。采用Cu靶进行测试，工作电压为45KV，电流40mA，每步扫描速度为10.2/s，步长为0.013。
(2)场发射扫描电子显微镜
厂家：卡尔蔡司，仪器型号：帕纳科EmpyreanZeiss/Auriga。将待测样磨抛至厚度小于0.5mm，表面抛光至镜面且没有明显，对待测表面进行喷金处理后进行表面形貌的测试。利用扫描电镜配备的能谱仪对待测样品进行成分分析。
(3)热导率
厂家：德国耐驰仪器公司，仪器型号：LFA-457。采用激光热导仪对制备的块体样品进行室温至1200℃之间的导热系数的测试。将块体样品制备成直径为12.7mm的圆片，将切好的圆片进行抛光处理至厚度小于3mm，表面抛光至光亮。
(4)热膨胀系数
采用高温热膨胀仪测量块体样品热膨胀速率，利用常规计算方法得到样品在不同温度间的热膨胀系数。
厂家：德国耐驰仪器公司，仪器型号：DIL402PC。将待测块体切割至3mm×3mm×30mm的块体，抛光至两端平行，放入仪器中进行室温至1200℃之间的热膨胀系数测试。
实施例1
(1)按照所述涂层材料的物相组成(Nd0.2Dy0.2Ho0.2Y0.2Er0.2)TaO4，采用化学计量比称取各个原料粉体：
将氧化钕、氧化镝、氧化钬、氧化钇、氧化铒及氧化钽按照摩尔比为1:1:1:1:1:5称取；
将称取好的原料放入球磨罐，并加入提前用酒精清洗并烘干的氧化锆磨球，保持所述磨球与原料粉体的质量比为5:1，球磨介质选择无水乙醇并添加至没过磨球和原料粉体；将球磨罐放入球磨机中设置转速为300r/min球磨10h混合均匀，形成浆料。
(2)将步骤(1)制得的浆料置入茄形瓶中，在80℃旋转蒸发进行干燥，待瓶中无明显液滴后，继续旋转蒸发5分钟，保证旋转蒸发后的粉体中不含或含少量的球磨介质；然后将旋转蒸发后的粉体放入烘箱中，在100℃继续烘干2h；将彻底干燥的粉体放入研钵充分研磨，并过300目筛，得到过筛后额粉体。
便于后续反应充分；
将过筛后的粉体装入氧化铝坩埚中，放入高温箱式烧结炉中，以5℃/min的速率升温至1450℃恒温煅烧10h，制备得到终产物粉体；随后随炉降温至室温，取出后利用研钵进行研磨至无明显颗粒，作为测试用粉体样品。
为了进行扫描电子显微镜观察、热导率以及热膨胀系数的测试，需将本实施例步骤(2)中过筛后的粉体制成用于测试的块体样品，具体方法如下：
将过筛后的粉体利用手动压片机进行初次压制，使用的模具为直径20mm的圆形磨具和5mm×5mm×50mm的条形模具，压力为8MPa，保压时间为1min；再利用冷等静压进行二次压制，压力为250MPa，保压时间为5min，得到坯体；
将坯体装入氧化铝坩埚中，放入无压箱式烧结炉中，以5℃/min的速率升温至1450℃恒温煅烧10h，制备得的用于测试的块体样品；随炉降温至室温。
对本实施例制得的粉体样品及块体样品进行测试如下：
(1)X射线衍射(XRD)
测试结果如图1所示，可以看出所述粉体样品为单一相高熵稀土钽酸盐。
(2)扫描电镜-能谱(SEM-EDS)
将粉体样品采用SEM-EDS观察其显微组织结构以及元素分布情况，结果如图2所示，所有元素分布均匀，没有明显的元素偏析。
综上所述，可知本实施例制备得到的终产物为本发明所述的一种高熵稀土钽酸盐陶瓷涂层材料(Nd0.2Dy0.2Ho0.2Y0.2Er0.2)TaO4。
(3)热导率
冷却后的块体样品的热导率测试结果如图4，可知热导率最低为1.43W/m·K，具有良好的隔热性能。
(4)热膨胀系数
冷却后的块体样品的热膨胀系数测试结果可知，热膨胀系数为10.3×10-6K-1。
实施例2
(1)同实施例1步骤(1)；
(2)以10℃/min的速率升温至1500℃恒温煅烧8h，其余同实施例1步骤(2)。
为了进行扫描电子显微镜观察、热导率以及热膨胀系数的测试，需将本实施例步骤(2)中过筛后的粉体制成用于测试的块体样品，具体方法如下：
将过筛后的粉体利用手动压片机进行初次压制，使用的模具为直径20mm的圆形磨具和5mm×5mm×50mm的条形模具，压力为8MPa，保压时间为1min；再利用冷等静压进行二次压制，压力为250MPa，保压时间为5min，得到坯体；
将坯体装入氧化铝坩埚中，放入无压箱式烧结炉中，以10℃/min的速率升温至1500℃恒温煅烧8h，制备得的用于测试的块体样品；随炉降温至室温。
对本实施例制得的粉体样品及块体样品进行测试如下：
(1)X射线衍射(XRD)
测试结果如图3所示，可以看出所述粉体样品为单一相高熵稀土钽酸盐。
(2)扫描电镜-能谱(SEM-EDS)
将粉体样品采用SEM-EDS观察其显微组织结构以及元素分布情况，结果显示，所有元素分布均匀，没有明显的元素偏析。
综上所述，可知本实施例制备得到的终产物为本发明所述的一种高熵稀土钽酸盐陶瓷涂层材料(Nd0.2Dy0.2Ho0.2Y0.2Er0.2)TaO4。
(3)热导率
冷却后的块体样品的热导率测试结果如，可知热导率最低为1.41W/m·K，具有良好的隔热性能。
(4)热膨胀系数
冷却后的块体样品的热膨胀系数测试结果可知，热膨胀系数为10.5×10-6K-1。
Claims (10)
1.一种高熵稀土钽酸盐陶瓷涂层材料，其特征在于：所述陶瓷涂层材料的物相组成为(Nd0.2Dy0.2Ho0.2Y0.2Er0.2)TaO4。
2.一种如权利要求1所述的高熵稀土钽酸盐陶瓷涂层材料的制备方法，其特征在于：所述方法步骤如下：
(1)按照所述涂层材料的物相组成，采用化学计量比称取各个原料粉体，采用湿法球磨混合均匀，形成浆料；所述原料粉体为氧化钕、氧化镝、氧化钬、氧化钇、氧化铒和氧化钽的粉体；
(2)将浆料干燥得到粉体，将粉体升温至1450℃～1550℃恒温煅烧8h～10h，制备得到一种高熵稀土钽酸盐陶瓷涂层材料。
3.根据权利要求2所述的一种高熵稀土钽酸盐陶瓷涂层材料的制备方法，其特征在于：步骤(1)中，所述原料粉体的粒径均为5μm～10μm，纯度均≥99.9％。
4.根据权利要求2或3所述的一种高熵稀土钽酸盐陶瓷涂层材料的制备方法，其特征在于：步骤(1)中，所述球磨的磨球与原料粉体的质量比为5:1；所述球磨的球磨介质为无水乙醇；所述球磨的球磨转速为250r/min～300r/min，球磨时间为8h～10h。
5.根据权利要求2所述的一种高熵稀土钽酸盐陶瓷涂层材料的制备方法，其特征在于：步骤(2)中，干燥方式具体为：将浆料置于容器中在75℃～80℃旋转蒸发进行干燥，待容器中无明显液滴后，继续旋转蒸发5min～8min；然后在95℃～100℃继续干燥6h～10h。
6.根据权利要求2所述的一种高熵稀土钽酸盐陶瓷涂层材料的制备方法，其特征在于：步骤(2)中，浆料干燥后进行研磨，过筛，得到过筛后的粉体，再升温煅烧。
7.根据权利要求2所述的一种高熵稀土钽酸盐陶瓷涂层材料的制备方法，其特征在于：步骤(2)中，煅烧的升温速率为5℃/min～10℃/min。
8.根据权利要求2所述的一种高熵稀土钽酸盐陶瓷涂层材料的制备方法，其特征在于：步骤(2)中，干燥方式具体为：将浆料置于容器中在75℃～80℃旋转蒸发进行干燥，待容器中无明显液滴后，继续旋转蒸发5min～8min；然后在95℃～100℃继续干燥6h～10h；
浆料干燥后进行研磨，过筛，得到过筛后的粉体，再升温煅烧；
煅烧的升温速率为5℃/min～10℃/min。
9.根据权利要求2所述的一种高熵稀土钽酸盐陶瓷涂层材料的制备方法，其特征在于：步骤(1)中所述原料粉体的粒径均为5μm～10μm，纯度均≥99.9％；
所述球磨的磨球与原料粉体的质量比为5:1；所述球磨的球磨介质为无水乙醇；所述球磨的球磨转速为250r/min～300r/min，球磨时间为8h～10h；
步骤(2)中，干燥方式具体为：将浆料置于容器中在75℃～80℃旋转蒸发进行干燥，待容器中无明显液滴后，继续旋转蒸发5min～8min；然后在95℃～100℃继续干燥6h～10h；
浆料干燥后进行研磨，过筛，得到过筛后的粉体，再升温煅烧；
煅烧的升温速率为5℃/min～10℃/min。
10.一种高熵稀土钽酸盐陶瓷涂层，其特征在于：所述涂层采用如权利要求1所述的一种高熵稀土钽酸盐陶瓷涂层材料高温镍基合金基底上制备得到。
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