大气等离子喷涂Y3Al5O12/Al2O3陶瓷涂层的CMAS腐蚀抗力

doi:10.15541/jim20240001

无机材料学报 ›› 2024, Vol. 39 ›› Issue (6): 671-680.DOI: 10.15541/jim20240001 CSTR: 32189.14.10.15541/jim20240001

所属专题：【结构材料】热障与环境障涂层(202409)

大气等离子喷涂Y₃Al₅O₁₂/Al₂O₃陶瓷涂层的CMAS腐蚀抗力

李捷¹^,²(), 罗志新¹, 崔阳¹, 张广珩¹^,², 孙鲁超¹(), 王京阳¹()

1.中国科学院金属研究所, 沈阳 110016
2.中国科学技术大学材料科学与工程学院, 沈阳 110016

收稿日期:2024-01-02 修回日期:2024-02-29 出版日期:2024-06-20 网络出版日期:2024-03-05
通讯作者: 孙鲁超, 研究员. E-mail: lcsun@imr.ac.cn;
王京阳，研究员. E-mail: jywang@imr.ac.cn
作者简介:李捷(1999-), 女, 博士研究生. E-mail: jli20s@imr.ac.cn
基金资助:
国家自然科学基金(52130204);国家自然科学基金(U21A2063);国家重点研发计划(2021YFB3702300);辽宁省‘兴辽英才计划’项目(XLYC2002018);辽宁省‘兴辽英才计划’项目(XLYC2203090);中国科学院国际伙伴计划(172GJHZ2022094FN)

CMAS Corrosion Resistance of Y₃Al₅O₁₂/Al₂O₃ Ceramic Coating Deposited by Atmospheric Plasma Spraying

LI Jie¹^,²(), LUO Zhixin¹, CUI Yang¹, ZHANG Guangheng¹^,², SUN Luchao¹(), WANG Jingyang¹()

1. Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China
2. School of Materials Science and Engineering, University of Science and Technology of China, Shenyang 110016, China

Received:2024-01-02 Revised:2024-02-29 Published:2024-06-20 Online:2024-03-05
Contact: SUN Luchao, professor. E-mail: lcsun@imr.ac.cn;
WANG Jingyang, professor. E-mail: jywang@imr.ac.cn
About author:LI Jie (1999-), female, PhD candidate. E-mail: jli20s@imr.ac.cn
Supported by:
National Natural Science Foundation of China(52130204);National Natural Science Foundation of China(U21A2063);National Key R&D Program of China(2021YFB3702300);Liaoning Revitalization Talents Program(XLYC2002018);Liaoning Revitalization Talents Program(XLYC2203090);International Partnership Program of the Chinese Academy of Sciences(172GJHZ2022094FN)

摘要/Abstract

摘要：

探索能够有效抵抗1300 ℃及以上温度钙镁铝硅酸盐(Calcium-Magnesium-Aluminum-Silicate, CMAS)腐蚀的新材料是近年来先进航空发动机用环境障涂层研究的重点任务。本工作围绕具有超强CMAS腐蚀抗力的YAG(Y₃Al₅O₁₂)/Al₂O₃体系, 采用大气等离子喷涂(Atmospheric Plasma Spraying, APS)技术制备了具有共晶成分的YAG/Al₂O₃涂层。通过在1100、1300和1500 ℃对制备态涂层进行热处理, 获得了具有不同微观结构的YAG/Al₂O₃涂层。利用不同表征手段研究了YAG/Al₂O₃涂层抵抗1300 ℃ CMAS腐蚀的性能及微观结构对涂层腐蚀抗性的影响。研究结果发现, 经不同温度热处理的YAG/Al₂O₃涂层与CMAS的反应产物均为石榴石结构固溶体、CaAl₂Si₂O₈和Ca₂MgSi₂O₇。腐蚀机制研究发现, 1100 ℃热处理YAG/Al₂O₃涂层与CMAS反应界面的近连续分布石榴石固溶体层可有效阻隔CMAS腐蚀元素的扩散; 1500 ℃热处理YAG/Al₂O₃涂层晶粒尺寸的增加及晶界数量的减少可降低涂层材料在CMAS中的溶解速率, 二者均可通过影响腐蚀过程中的离子传输速率而影响各生成物的竞争析出, 进而提升涂层的CMAS腐蚀抗力。本工作为YAG/Al₂O₃涂层热处理工艺优化提供了借鉴, 并为通过微观结构优化调控YAG/Al₂O₃涂层的CMAS腐蚀抗力提供了新思路。

关键词: YAG(Y₃Al₅O₁₂)/Al₂O₃, 大气等离子喷涂, 环境障涂层, CMAS腐蚀抗力, 晶界腐蚀, 热处理温度

Abstract:

The investigation of novel materials exhibiting exceptional resistance to calcium-magnesium-aluminum- silicate (CMAS) corrosion at temperatures of 1300 ℃ and above has emerged as a pivotal objective in the advancement of environmental barrier coatings for aircraft engines in recent years. In this study, atmospheric plasma spraying (APS) technology was employed to fabricate YAG(Y₃Al₅O₁₂)/Al₂O₃ coatings with eutectic composition, which was acknowledged as a promising material possessing outstanding CMAS corrosion resistance, thereby rendering it suitable for application in environmental barrier coatings. The as-deposited coatings were annealed at 1100, 1300, and 1500 ℃ to obtain different microstructures, and the corrosion resistance as well as mechanism of YAG/Al₂O₃ coatings against CMAS were investigated by comparing the corrosion results after exposure to CMAS at 1300 ℃. The reaction products between YAG/Al₂O₃ coatings and CMAS were found to be garnet-structure solid solution, CaAl₂Si₂O₈, and Ca₂MgSi₂O₇. The nearly continuous distribution of the garnet-structure solid solution layer at the reaction interface between YAG/Al₂O₃ coating annealed at 1100 ℃ and CMAS effectively impedes the diffusion of CMAS corrosion elements. For YAG/Al₂O₃coating annealed at 1500 ℃, the increase in grain size and decrease in grain boundaries reduce the dissolution rate of the coating. Both of the above can affect the competitive precipitation of various products by influencing the ion transport rate in the corrosion process, and then improve the CMAS corrosion resistance of the coating. Moreover, heat-treatment temperature can tailor grain size, which influences both dissolution-precipitation rate and competitive precipitation of reaction products during CMAS corrosion. These findings provide guidance for selecting appropriate heat-treatment temperature and offer a novel approach to optimize CMAS corrosion resistance of YAG/Al₂O₃ coatings through microstructure optimization.

Key words: YAG(Y₃Al₅O₁₂)/Al₂O₃, atmospheric plasma spraying, environmental barrier coating, CMAS corrosion resistance, grain boundary corrosion, heat-treatment temperature

中图分类号:

TQ174

李捷, 罗志新, 崔阳, 张广珩, 孙鲁超, 王京阳. 大气等离子喷涂Y₃Al₅O₁₂/Al₂O₃陶瓷涂层的CMAS腐蚀抗力[J]. 无机材料学报, 2024, 39(6): 671-680.

LI Jie, LUO Zhixin, CUI Yang, ZHANG Guangheng, SUN Luchao, WANG Jingyang. CMAS Corrosion Resistance of Y₃Al₅O₁₂/Al₂O₃ Ceramic Coating Deposited by Atmospheric Plasma Spraying[J]. Journal of Inorganic Materials, 2024, 39(6): 671-680.

图/表 15

表1 YAG/Al2O3涂层的大气等离子喷涂参数

Table 1 Atmospheric plasma spraying parameters for YAG/Al2O3 coating

Current/A	Ar flow rate/slpm	H₂ flow rate/slpm	Rotation velocity/%	Distance/mm
650	40	12	30	110

图1 经1300 ℃ CMAS腐蚀(a) 1、(b) 4和(c) 25 h后YAG/Al2O3涂层表面的XRD图谱

Fig. 1 XRD patterns of the surfaces of YAG/Al2O3 coatings after CMAS corrosion at 1300 ℃ for (a) 1, (b) 4, and (c) 25 h Colorful patterns are available on website

图2 YAG/Al2O3涂层经CMAS腐蚀试验后的表面形貌

Fig. 2 Surface morphologies of YAG/Al2O3 coatings after CMAS corrosion Coatings annealed at 1100, 1300, and 1500 ℃ after CMAS corrosion for (a-c) 1, (d-f) 4, and (g-i) 25 h

图3 1100 ℃热处理YAG/Al2O3涂层经CMAS腐蚀1 h后的TEM分析

Fig. 3 TEM analyses of YAG/Al2O3 coating annealed at 1100 ℃ after CMAS corrosion for 1 h (a) Selected area for TEM sample preparation via FIB; (b) Bright-field TEM image from the region indicated by black dashed box in (a); (c) SAED pattern of area marked with black circle in (b)

表2 1100 ℃热处理YAG/Al2O3涂层经CMAS腐蚀1 h后的表面SEM-EDS分析结果(%, 原子分数)

Table 2 SEM-EDS analytical results of the phases on the surface of YAG/Al2O3 coating annealed at 1100 ℃ after CMAS corrosion for 1 h (%, in atom)

Region	O	Mg	Al	Si	Ca	Y	Phase
A	50.41±1.59	—	17.47±0.70	22.27±0.71	10.16±0.45	—	CaAl₂Si₂O₈
B	54.10±3.25	—	16.47±0.78	19.42±0.95	10.00±1.84	—	CaAl₂Si₂O₈
C	58.95±0.44	5.60±0.29	3.79±0.49	16.57±0.32	15.09±0.20	—	Ca₂MgSi₂O₇
D	39.07±1.11	3.70±0.34	17.29±0.53	17.48±0.52	12.41±0.50	10.06±0.62	YAG
E	49.54±1.04	3.23±0.40	4.73±0.18	23.34±0.41	13.81±1.60	5.34±0.71	CMAS

图4 YAG/Al2O3涂层经CMAS腐蚀试验后的截面形貌

Fig. 4 Cross-sectional morphologies of YAG/Al2O3 coatings after CMAS corrosion Coatings annealed at 1100, 1300, and 1500 ℃ after CMAS corrosion for (a-c) 1, (d-f) 4, and (g-i) 25 h

表3 1300 ℃热处理YAG/Al2O3涂层经CMAS腐蚀4 h后的截面SEM-EDS分析结果(%, 原子分数)

Table 3 SEM-EDS analytical results of phases in the cross-section of YAG/Al2O3 coating annealed at 1300 ℃ after CMAS corrosion for 4 h (%, in atom)

Region	O	Mg	Al	Si	Ca	Y	Phase
A	24.15±0.56	—	24.40±0.29	34.29±0.21	17.16±0.22	—	CaAl₂Si₂O₈
B	23.06±3.46	5.43±0.30	11.72±0.42	28.70±1.50	31.09±1.49	—	CMAS
C	18.45±2.17	3.63±0.42	8.98±0.70	35.71±1.30	20.57±0.38	12.67±0.82	YAG
D	26.70±2.79	2.13±0.61	29.42±0.78	14.12±1.62	10.47±0.54	17.18±0.81	YAG
E	31.18±1.51	1.40±0.17	10.56±0.53	31.3±0.53	21.09±0.73	4.47±0.14	CMAS

图5 1300 ℃热处理YAG/Al2O3涂层经CMAS腐蚀4 h后的TEM分析

Fig. 5 TEM analyses of YAG/Al2O3 coating annealed at 1300 ℃ after CMAS corrosion for 4 h (a-c) Bright-field TEM images from regions indicated by dashed box with numbers 1, 2 and 3 in Fig. 4(e), respectively; (d) SAED pattern of area in (a) marked with letter A; (e-i) SAED patterns of areas in (a) marked with letters C-G, respectively

图6 1100 ℃热处理YAG/Al2O3涂层经CMAS腐蚀1 h后截面的EDS面扫描结果

Fig. 6 EDS mappings of the cross-section of YAG/Al2O3 coating annealed at 1100 ℃ after CMAS corrosion for 1 h

图7 1500 ℃热处理YAG/Al2O3涂层经CMAS腐蚀1 h后截面的EDS面扫描结果

Fig. 7 EDS mappings of the cross-section of YAG/Al2O3 coating annealed at 1500 ℃ after CMAS corrosion for 1 h

图S1 1300 ℃热处理YAG/Al2O3涂层经CMAS腐蚀(a) 1, (b) 4和(c) 25 h后样品截面形貌的高倍照片

Fig. S1 High-magnification cross-section observations of YAG/Al2O3 coatings annealed at 1300 ℃ after CMAS corrosion for (a) 1, (b) 4, and (c) 25 h

图S2 1500 ℃热处理YAG/Al2O3涂层经CMAS腐蚀(a) 1, (b) 4和(c) 25 h后样品截面形貌的高倍照片

Fig. S2 High-magnification cross-section observations of YAG/Al2O3 coatings annealed at 1500 ℃ after CMAS corrosion for (a) 1, (b) 4, and (c) 25 h

图S3 (a)制备态YAG/Al2O3涂层和分别经(b)1100、(c)1300和(d)1500 ℃热处理的截面形貌

Fig. S3 Cross-section observations of (a) as-deposited YAG/Al2O3 coating and coatings annealed at (b) 1100, (c) 1300, and (d) 1500 ℃

图S4 不同温度热处理后涂层析出YAG石榴石固溶体相的“等效”厚度统计

Fig. S4 Equivalent thickness statistics of precipitation YAG garnet-structure solid solution of coatings annealed at different temperatures

表S1 图5(c)中区域E、F和G的TEM-EDS结果(%, 原子分数)

Table S1 TEM-EDS results of the regions marked with letters E, F, and G in Fig. 5(c)(%, in atom)

Region	O	Mg	Al	Si	Ca	Y	Phase
E	43.12±4.00	6.84±0.22	3.49±0.30	21.96±1.32	24.59±2.26		Ca₂MgSi₂O₇
F	50.79±0.93	5.61±0.19	6.51±0.27	17.50±0.82	11.34±0.49	8.25±0.42	YAG
G	59.33±2.03	0.54±0.14	4.95±0.26	19.53±0.73	13.38±0.89	2.27±0.14	CMAS

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大气等离子喷涂Y₃Al₅O₁₂/Al₂O₃陶瓷涂层的CMAS腐蚀抗力

CMAS Corrosion Resistance of Y₃Al₅O₁₂/Al₂O₃ Ceramic Coating Deposited by Atmospheric Plasma Spraying

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