Synergistic Mechanism of Gd3+ and Yb3+ on Crystallization Behavior of CMAS Corrosion Products

doi:10.15541/jim20250073

Abstract

Abstract:

As the operating temperature of aero-engine rises, degradation of thermal barrier coatings (TBCs) and environmental barrier coatings (EBCs) on hot-section components affected mainly by infiltration of calcium-magnesium-alumina-silicate (CaO-MgO-AlO_1.5-SiO₂, CMAS) has garnered increasing attention. Rare earth constituents play an essential role in forming corrosion products and subsequent melt penetration when conventional TBCs and EBCs are attacked by CMAS deposits. This study focused on preparation of a series of gadolinium-ytterbium oxides ((Gd_xYb_1-_x)₂O₃, x=0, 0.05, 0.10, 0.20, 0.30, 0.50 and 1.00), with particular emphasis on the roles of ytterbium and gadolinium. Their reaction with CMAS deposits was systematically investigated at 1300 ℃ to explore the synergistic mechanism associated with these two rare earth elements. The results indicate that gadolinium cations can efficiently induce the crystallization of products with apatite structure which have a low melt consumption. Conversely, ytterbium cations can induce the formation of products with garnet and silicocarnotite structure which have sluggish kinetics. Furthermore, partitioning of gadolinium and ytterbium ions within corrosion products, along with variation of residual CMAS melt composition, was further analyzed. It is proposed that these two rare earth ions exhibit a synergistic effect within a certain composition range (5%-20% (in mole) of gadolinium content). The optimized ratio of gadolinium and ytterbium within coatings is anticipated to promote apatite crystallization, prevent melt penetration, and modify the sluggish crystallization kinetics of garnet and silicocarnotite, thereby significantly improving the melt consumption. This investigation on synergistic effect of gadolinium and ytterbium cations provides a theoretical support for the anti-CMAS-corrosion composition modification of TBCs/EBCs.

Key words: gadolinium-ytterbium oxide, CMAS corrosion, reactive crystallization product, synergistic effect

CLC Number:

TQ174

ZHANG Guangheng, SHI Jinyu, SHEN Hongyu, ZHANG Jie, WANG Jingyang. Synergistic Mechanism of Gd³⁺ and Yb³⁺ on Crystallization Behavior of CMAS Corrosion Products[J]. Journal of Inorganic Materials, 2026, 41(1): 27-36.

Figures/Tables 13

References 36

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药品名称	纯度	厂家	产地
氧化钆(GdO_1.5)	99.99%	定南大华新材料资源有限公司	江西赣州
氧化镱(YbO_1.5)	99.99%	定南大华新材料资源有限公司	江西赣州
氧化钙(CaO)	分析纯AR	国药集团化学试剂有限公司	上海
氧化镁(MgO)	分析纯AR	国药集团化学试剂有限公司	上海
氧化铝(AlO_1.5)	分析纯AR	国药集团化学试剂有限公司	上海
氧化硅(SiO₂)	分析纯AR	国药集团化学试剂有限公司	上海

药品名称	纯度	厂家	产地
氧化钆(GdO_1.5)	99.99%	定南大华新材料资源有限公司	江西赣州
氧化镱(YbO_1.5)	99.99%	定南大华新材料资源有限公司	江西赣州
氧化钙(CaO)	分析纯AR	国药集团化学试剂有限公司	上海
氧化镁(MgO)	分析纯AR	国药集团化学试剂有限公司	上海
氧化铝(AlO_1.5)	分析纯AR	国药集团化学试剂有限公司	上海
氧化硅(SiO₂)	分析纯AR	国药集团化学试剂有限公司	上海

System	Phase	Chemical composition/% (in mole)
System	Phase	CaO	MgO	AlO_1.5	SiO₂	GdO_1.5	YbO_1.5
Yb : CMAS = 1 : 10	Apatite	15.5 ± 0.4	—	—	37.2 ± 0.2	—	47.3 ± 0.2
	Melt	31.7 ± 0.2	8.7 ± 0.3	12.2 ± 0.5	42.0 ± 0.5	—	5.5 ± 0.4
Yb : CMAS = 1 : 5	Apatite	15.9 ± 0.7	—	—	38.0 ± 0.6	—	46.1 ± 0.8
	Garnet	15.4 ± 0.7	15.5 ± 1.4	16.4 ± 1.7	30.4 ± 2.0	—	22.4 ± 2.3
	Silicocarnotite	35.1 ± 0.1	—	—	39.4 ± 0.2	—	25.5 ± 0.2
	Melt	43.6 ± 0.2	2.6 ± 0.2	3.9 ± 0.1	46.0 ± 0.3	—	3.9 ± 0.2
Gd_0.05Yb_0.95: CMAS = 1 : 10	Apatite	15.6 ± 0.2	—	—	39.4 ± 0.8	2.7 ± 0.2	42.2 ± 0.4
	Garnet	24.8 ± 1.6	13.1 ± 1.2	12.4 ± 1.2	37.3 ± 0.6	0.5 ± 0.1	11.9 ± 1.5
	Gehlenite	41.1 ± 0.5	13.9 ± 0.2	7.3 ± 0.3	37.7 ± 0.5	—	—
	Melt	28.4 ± 0.6	5.1 ± 1.0	15.5 ± 0.2	45.6 ± 1.1	0.2 ± 0.1	5.2 ± 0.6
Gd_0.05Yb_0.95: CMAS = 1 : 5	Apatite	13.9 ± 0.3	—	—	38.9 ± 0.5	3.1 ± 0.5	44.1 ± 0.3
	Garnet	19.2 ± 1.4	14.1 ± 0.5	13.8 ± 1.3	33.0 ± 0.8	0.5 ± 0.1	19.3 ± 1.2
	Silicocarnotite	36.4 ± 0.2	—	—	37.7 ± 0.2	1.3 ± 0.2	24.5 ± 0.4
	Melt	44.1 ± 1.6	2.3 ± 0.4	4.1 ± 1.6	46.2 ± 0.5	0.2 ± 0.1	3.2 ± 0.5
Gd_0.10Yb_0.90 : CMAS = 1 : 10	Apatite	15.3 ± 0.2	—	—	40.5 ± 0.1	5.4 ± 0.2	38.9 ± 0.4
	Garnet	22.4 ± 0.6	14.7 ± 0.6	10.5 ± 0.6	37.2 ± 0.6	0.9 ± 0.1	14.2 ± 0.9
	Gehlenite	42.2 ± 0.2	13.2 ± 0.3	8.4 ± 0.1	36.1 ± 0.5	—	—
	Melt	27.9 ± 1.4	5.2 ± 0.2	16.9 ± 1.3	44.6 ± 0.5	0.3 ± 0.1	5.1 ± 0.5
Gd_0.10Yb_0.90 : CMAS = 1 : 5	Apatite	16.8 ± 0.6	—	—	40.5 ± 0.9	5.2 ± 0.1	37.4 ± 0.4
	Garnet	17.0 ± 1.5	14.1 ± 0.1	15.5 ± 1.2	31.0 ± 0.4	1.0 ± 0.2	21.3 ± 0.9
	Silicocarnotite	35.9 ± 0.2	—	—	38.3 ± 0.2	2.5 ± 0.2	23.3 ± 0.2
	Melt	35.9 ± 0.9	2.2 ± 0.4	13.6 ± 0.5	45.5 ± 0.3	0.5 ± 0.1	2.3 ± 0.2
Gd_0.20Yb_0.80 : CMAS = 1 : 10	Apatite	14.0 ± 0.4	—	—	39.8 ± 0.8	11.9 ± 0.6	34.3 ± 1.2
	Gehlenite	41.1 ± 0.2	13.0 ± 0.2	8.3 ± 0.2	37.5 ± 0.6	—	—
	Melt	27.7 ± 0.5	5.5 ± 0.3	16.9 ± 0.5	44.5 ± 0.3	0.8 ± 0.1	4.6 ± 0.5
Gd_0.20Yb_0.80 : CMAS = 1 : 5	Apatite	15.4 ± 0.6	—	—	41.0 ± 0.7	11.2 ± 0.7	32.3 ± 0.9
	Garnet	18.4 ± 0.6	14.2 ± 0.3	13.7 ± 1.1	33.2 ± 1.6	2.3 ± 0.3	18.1 ± 1.4
	Silicocarnotite	36.7 ± 0.3	—	—	37.8 ± 0.3	4.6 ± 0.4	20.8 ± 0.7
	Melt	34.8 ± 0.8	3.1 ± 1.2	14.4 ± 1.4	44.6 ± 0.9	1.1 ± 0.1	1.9 ± 0.3
Gd_0.30Yb_0.70 : CMAS = 1 : 10	Apatite	17.0 ± 0.9	—	—	39.8 ± 0.5	15.2 ± 0.8	27.9 ± 1.0
	Gehlenite	39.8 ± 0.9	11.3 ± 0.3	11.3 ± 0.6	37.6 ± 0.7	—	—
	Melt	31.6 ± 0.5	9.4 ± 0.3	13.1 ± 0.3	41.6 ± 0.5	1.0 ± 0.1	3.4 ± 0.2
Gd_0.30Yb_0.70 : CMAS = 1 : 5	Apatite	15.7 ± 0.1	—	—	38.5 ± 0.4	15.2 ± 0.4	30.6 ± 0.8
	Garnet	22.8 ± 0.7	13.3 ± 0.5	13.5 ± 0.9	37.0 ± 0.6	2.9 ± 0.2	10.4 ± 0.4
	Melt	33.8 ± 0.2	2.1 ± 0.1	12.6 ± 0.5	47.8 ± 0.7	1.2 ± 0.1	2.5 ± 0.1
Gd_0.50Yb_0.50 : CMAS = 1 : 10	Apatite	18.4 ± 0.2	—	—	37.6 ± 1.3	27.3 ± 1.1	16.7 ± 0.8
	Gehlenite	40.3 ± 0.4	11.8 ± 0.1	9.5 ± 0.4	38.4 ± 0.1	—	—
	Melt	27.0 ± 0.2	5.3 ± 0.1	18.2 ± 0.1	45.1 ± 0.2	1.5 ± 0.2	2.8 ± 0.2
Gd_0.50Yb_0.50 : CMAS = 1 : 5	Apatite	15.1 ± 0.3	—	—	38.0 ± 0.6	25.1 ± 0.7	21.7 ± 0.9
	Melt	39.9 ± 0.6	11.3 ± 0.2	9.9 ± 0.2	34.3 ± 0.3	2.5 ± 0.6	2.1 ± 0.4
Gd : CMAS = 1 : 10	Apatite	20.7 ± 1.0	—	—	38.6 ± 0.1	40.7 ± 1.0	—
	Gehlenite	39.9 ± 0.9	13.7 ± 0.8	9.2 ± 0.4	37.2 ± 1.3	—	—
	Melt	25.7 ± 0.1	5.4 ± 0.5	20.6 ± 0.7	45.6 ± 0.7	2.7 ± 0.1	—
Gd : CMAS = 1 : 5	Apatite	19.9 ± 0.7	—	—	39.9 ± 0.8	40.2 ± 1.5	—
	Melt	39.7 ± 0.7	12.8 ± 0.4	9.9 ± 0.6	34.9 ± 0.7	2.7 ± 1.6	—

System	Phase	Chemical composition/% (in mole)
System	Phase	CaO	MgO	AlO_1.5	SiO₂	GdO_1.5	YbO_1.5
Yb : CMAS = 1 : 10	Apatite	15.5 ± 0.4	—	—	37.2 ± 0.2	—	47.3 ± 0.2
	Melt	31.7 ± 0.2	8.7 ± 0.3	12.2 ± 0.5	42.0 ± 0.5	—	5.5 ± 0.4
Yb : CMAS = 1 : 5	Apatite	15.9 ± 0.7	—	—	38.0 ± 0.6	—	46.1 ± 0.8
	Garnet	15.4 ± 0.7	15.5 ± 1.4	16.4 ± 1.7	30.4 ± 2.0	—	22.4 ± 2.3
	Silicocarnotite	35.1 ± 0.1	—	—	39.4 ± 0.2	—	25.5 ± 0.2
	Melt	43.6 ± 0.2	2.6 ± 0.2	3.9 ± 0.1	46.0 ± 0.3	—	3.9 ± 0.2
Gd_0.05Yb_0.95: CMAS = 1 : 10	Apatite	15.6 ± 0.2	—	—	39.4 ± 0.8	2.7 ± 0.2	42.2 ± 0.4
	Garnet	24.8 ± 1.6	13.1 ± 1.2	12.4 ± 1.2	37.3 ± 0.6	0.5 ± 0.1	11.9 ± 1.5
	Gehlenite	41.1 ± 0.5	13.9 ± 0.2	7.3 ± 0.3	37.7 ± 0.5	—	—
	Melt	28.4 ± 0.6	5.1 ± 1.0	15.5 ± 0.2	45.6 ± 1.1	0.2 ± 0.1	5.2 ± 0.6
Gd_0.05Yb_0.95: CMAS = 1 : 5	Apatite	13.9 ± 0.3	—	—	38.9 ± 0.5	3.1 ± 0.5	44.1 ± 0.3
	Garnet	19.2 ± 1.4	14.1 ± 0.5	13.8 ± 1.3	33.0 ± 0.8	0.5 ± 0.1	19.3 ± 1.2
	Silicocarnotite	36.4 ± 0.2	—	—	37.7 ± 0.2	1.3 ± 0.2	24.5 ± 0.4
	Melt	44.1 ± 1.6	2.3 ± 0.4	4.1 ± 1.6	46.2 ± 0.5	0.2 ± 0.1	3.2 ± 0.5
Gd_0.10Yb_0.90 : CMAS = 1 : 10	Apatite	15.3 ± 0.2	—	—	40.5 ± 0.1	5.4 ± 0.2	38.9 ± 0.4
	Garnet	22.4 ± 0.6	14.7 ± 0.6	10.5 ± 0.6	37.2 ± 0.6	0.9 ± 0.1	14.2 ± 0.9
	Gehlenite	42.2 ± 0.2	13.2 ± 0.3	8.4 ± 0.1	36.1 ± 0.5	—	—
	Melt	27.9 ± 1.4	5.2 ± 0.2	16.9 ± 1.3	44.6 ± 0.5	0.3 ± 0.1	5.1 ± 0.5
Gd_0.10Yb_0.90 : CMAS = 1 : 5	Apatite	16.8 ± 0.6	—	—	40.5 ± 0.9	5.2 ± 0.1	37.4 ± 0.4
	Garnet	17.0 ± 1.5	14.1 ± 0.1	15.5 ± 1.2	31.0 ± 0.4	1.0 ± 0.2	21.3 ± 0.9
	Silicocarnotite	35.9 ± 0.2	—	—	38.3 ± 0.2	2.5 ± 0.2	23.3 ± 0.2
	Melt	35.9 ± 0.9	2.2 ± 0.4	13.6 ± 0.5	45.5 ± 0.3	0.5 ± 0.1	2.3 ± 0.2
Gd_0.20Yb_0.80 : CMAS = 1 : 10	Apatite	14.0 ± 0.4	—	—	39.8 ± 0.8	11.9 ± 0.6	34.3 ± 1.2
	Gehlenite	41.1 ± 0.2	13.0 ± 0.2	8.3 ± 0.2	37.5 ± 0.6	—	—
	Melt	27.7 ± 0.5	5.5 ± 0.3	16.9 ± 0.5	44.5 ± 0.3	0.8 ± 0.1	4.6 ± 0.5
Gd_0.20Yb_0.80 : CMAS = 1 : 5	Apatite	15.4 ± 0.6	—	—	41.0 ± 0.7	11.2 ± 0.7	32.3 ± 0.9
	Garnet	18.4 ± 0.6	14.2 ± 0.3	13.7 ± 1.1	33.2 ± 1.6	2.3 ± 0.3	18.1 ± 1.4
	Silicocarnotite	36.7 ± 0.3	—	—	37.8 ± 0.3	4.6 ± 0.4	20.8 ± 0.7
	Melt	34.8 ± 0.8	3.1 ± 1.2	14.4 ± 1.4	44.6 ± 0.9	1.1 ± 0.1	1.9 ± 0.3
Gd_0.30Yb_0.70 : CMAS = 1 : 10	Apatite	17.0 ± 0.9	—	—	39.8 ± 0.5	15.2 ± 0.8	27.9 ± 1.0
	Gehlenite	39.8 ± 0.9	11.3 ± 0.3	11.3 ± 0.6	37.6 ± 0.7	—	—
	Melt	31.6 ± 0.5	9.4 ± 0.3	13.1 ± 0.3	41.6 ± 0.5	1.0 ± 0.1	3.4 ± 0.2
Gd_0.30Yb_0.70 : CMAS = 1 : 5	Apatite	15.7 ± 0.1	—	—	38.5 ± 0.4	15.2 ± 0.4	30.6 ± 0.8
	Garnet	22.8 ± 0.7	13.3 ± 0.5	13.5 ± 0.9	37.0 ± 0.6	2.9 ± 0.2	10.4 ± 0.4
	Melt	33.8 ± 0.2	2.1 ± 0.1	12.6 ± 0.5	47.8 ± 0.7	1.2 ± 0.1	2.5 ± 0.1
Gd_0.50Yb_0.50 : CMAS = 1 : 10	Apatite	18.4 ± 0.2	—	—	37.6 ± 1.3	27.3 ± 1.1	16.7 ± 0.8
	Gehlenite	40.3 ± 0.4	11.8 ± 0.1	9.5 ± 0.4	38.4 ± 0.1	—	—
	Melt	27.0 ± 0.2	5.3 ± 0.1	18.2 ± 0.1	45.1 ± 0.2	1.5 ± 0.2	2.8 ± 0.2
Gd_0.50Yb_0.50 : CMAS = 1 : 5	Apatite	15.1 ± 0.3	—	—	38.0 ± 0.6	25.1 ± 0.7	21.7 ± 0.9
	Melt	39.9 ± 0.6	11.3 ± 0.2	9.9 ± 0.2	34.3 ± 0.3	2.5 ± 0.6	2.1 ± 0.4
Gd : CMAS = 1 : 10	Apatite	20.7 ± 1.0	—	—	38.6 ± 0.1	40.7 ± 1.0	—
	Gehlenite	39.9 ± 0.9	13.7 ± 0.8	9.2 ± 0.4	37.2 ± 1.3	—	—
	Melt	25.7 ± 0.1	5.4 ± 0.5	20.6 ± 0.7	45.6 ± 0.7	2.7 ± 0.1	—
Gd : CMAS = 1 : 5	Apatite	19.9 ± 0.7	—	—	39.9 ± 0.8	40.2 ± 1.5	—
	Melt	39.7 ± 0.7	12.8 ± 0.4	9.9 ± 0.6	34.9 ± 0.7	2.7 ± 1.6	—

System	Phase	Chemical composition/% (in mole)
System	Phase	CaO	MgO	AlO_1.5	SiO₂	GdO_1.5
1300 ℃, 1 h	Apatite	14.1 ± 0.5	—	—	36.5 ± 0.5	49.4 ± 1.0
1300 ℃, 20 h	Apatite	13.7 ± 0.7	—	—	35.9 ± 0.5	50.3 ± 0.9
1300 ℃, 50 h	Apatite	13.6 ± 0.1	—	—	35.4 ± 0.4	51.0 ± 0.4
1300 ℃,100 h	Apatite	14.1 ± 0.2	—	—	35.8 ± 0.6	50.0 ± 0.7

Synergistic Mechanism of Gd³⁺ and Yb³⁺ on Crystallization Behavior of CMAS Corrosion Products

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CMAS	Chemical composition/% (in mole)
CMAS	CaO	MgO	AlO_1.5	SiO₂
Theoretical value	33	9	13	45
Measured value	32.2±2.3	9.4±1.0	13.2±1.4	45.2±0.9

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