La, Y掺杂对非晶晶化法制备ZrO2-mullite纳米复相陶瓷的影响

doi:10.15541/jim20150142

摘要/Abstract

摘要：

借助DSC、XRD、SEM和TEM等技术探讨了La₂O₃、Y₂O₃掺杂对非晶晶化法制备ZrO₂-mullite纳米复相陶瓷的影响。结果表明, 当Y₂O₃和La₂O₃的掺杂量分别小于4wt%和1.8wt%时, 能有效降低Si-Al-Zr-O系非晶的熔制温度, 抑制冷却过程中的失透现象, 有利于非晶形成且不影响主晶相的析出。单一Y₂O₃掺杂时, Y主要固溶于氧化锆中, 稳定t-ZrO₂, 且抑制堇青石析出, 对晶粒大小影响不大; 而Y₂O₃和La₂O₃混合掺杂时, Y和La主要存在于玻璃相中, 强化晶界, 且La能明显促进ZrO₂、mullite晶粒长大。Y₂O₃和La₂O₃的合适添加量分别为1.0wt%~ 2.0wt%和0.6wt%~ 1.2wt%。

关键词: 掺杂, 非晶晶化, 结构变化

Abstract:

Effects of Y₂O₃ and La₂O₃ doping on ZrO₂-mullite nano-composite ceramics, prepared by in-situ controlled crystallizing from the Si-Al-Zr-O amorphous bulk, were revealed by means of DSC, XRD, SEM and TEM technologies. The results indicate that the addition of Y₂O₃ and La₂O₃ (Y₂O₃ <1.8wt% and La₂O₃ <4wt%) can effectively reduce the melting temperatures of Si-Al-Zr-O based amorphous, limit the devitrification phenomenon and is beneficial for the formation of amorphous during cooling process, without changing the main crystalline phase precipitation. For Y₂O₃ single doping, Y is mainly dissolved in the zirconium oxide, stabilizes t-ZrO₂, and inhibits precipitation of the cordierite, and exerts little effect on the grain size. For both Y₂O₃ and La₂O₃ mixed doping, Y and La mainly locate in the glass phase, strengthen the grain boundary, of which La promotes the grain growth of ZrO₂ and mullite. The appropriate doping amount of Y₂O₃ and La₂O₃ should be in the range of 1.0wt%-2.0wt% and 0.6wt%-1.2wt%, respectively.

Key words: doping, amorphous, microstructure changes

中图分类号:

TQ171

谭小平, 秦利平, 梁叔全 . La, Y掺杂对非晶晶化法制备ZrO₂-mullite纳米复相陶瓷的影响[J]. 无机材料学报, 2016, 31(1): 47-52.

TAN Xiao-Ping, QI Li-Ping, LIANG Shu-Quan. Effect of La, Y Additions on ZrO₂-mullite Nano-composite Ceramics by In-situ Controlled Crystallizing from Si-Al-Zr-O Amorphous Bulk[J]. Journal of Inorganic Materials, 2016, 31(1): 47-52.

图/表 10

表1 配方组成(wt%)

Table 1 Composition of the samples in the study(wt%)

No.	SiO₂	Al₂O₃	ZrO₂	Y₂O₃	La₂O₃	MgO+CaO
Z3	35	40	20	0	0	5
ZY1	35	40	20	0.5	0	5
ZY2	35	40	20	1.0	0	5
ZY3	35	40	20	2.0	0	5
ZY4	35	40	20	4.0	0	5
ZYL0(ZY2)	35	40	20	1.0	0	5
ZYL1	35	40	20	1.0	0.6	5
ZYL2	35	40	20	1.0	1.2	5
ZYL3	35	40	20	1.0	1.8	5

图1 掺杂和未掺杂试样的DSC曲线

Fig. 1 DSC curves of the samples with and without dopants

表2 La2O3, Y2O3掺杂试样DSC曲线放热峰值温度

Table.2 Top temperatures on the DSC curves of samples with the additives of La2O3 and Y2O3

No.	T_p1/℃	T_p2 /℃
Z3	1007	1174
ZY1	1004	1172
ZY2	1007	1174
ZY3	1009	1170
ZY4	1015	1167
ZYL1	1008	1172
ZYL2	1006	1170
ZYL3	1004	1168

图 2 添加不同量Y2O3试样的XRD图谱

Fig. 2 XRD patterns of the samples with different Y2O3 contents (a) 0; (b) 0.5; (c) 1.0; (d) 4.0

图3 掺杂Y2O3的ZY2样品的TEM照片(a)及区域1和区域2的EDS分析结果( b)

Fig. 3 TEM image of the ZY2 sample (a) and EDS patterns of area 1 and area 2 (b) in (a)

图4 添加不同量La2O3试样的XRD图谱

Fig.4 XRD patterns of the samples with different La2O3 contents (a) 0; (b) 0.6; (c) 1.2

图5 掺杂试样ZYL1的TEM照片(a)及试样的区域1和区域2相的EDS分析结果( b)

Fig. 5 TEM image of the ZYL1 sample (a) and EDS patterns of area 1 and area 2 (b) in (a)

图6 试样的SEM照片

Fig. 6 SEM images of the samples without doping (a), with 1.0wt% Y2O3 (b) and with 1.0wt%Y2O3+0.6wt%La2O3 (c) doping

图7 ZY系试样断裂韧性(a)和抗弯强度(b)随Y2O3含量的变化关系

Fig. 7 Fracture toughness (a) and flexural strengths (b) of ZY samples as a function of the content of Y2O3

图8 ZYL系试样断裂韧性(a)和抗弯强度(b)随La2O3含量的变化关系

Fig. 8 Fracture toughness (a) and flexural strengths (b) of ZY samples as a function of the content of La2O3

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La, Y掺杂对非晶晶化法制备ZrO₂-mullite纳米复相陶瓷的影响

Effect of La, Y Additions on ZrO₂-mullite Nano-composite Ceramics by In-situ Controlled Crystallizing from Si-Al-Zr-O Amorphous Bulk

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