稀土氧化物对SPS烧结AlN陶瓷电性能的影响

doi:10.15541/jim20140428

无机材料学报 ›› 2015, Vol. 30 ›› Issue (3): 267-271.DOI: 10.15541/jim20140428

稀土氧化物对SPS烧结AlN陶瓷电性能的影响

黄林芸¹, 李晨辉¹, 柯文明¹, 史玉升¹, 贺智勇², 张启富²

(1. 华中科技大学材料成形与模具技术国家重点实验室, 武汉430074; 2. 中国钢研科技集团有限公司, 北京100081)

收稿日期:2014-08-25 修回日期:2014-10-12 出版日期:2015-03-20 网络出版日期:2015-03-06
作者简介:黄林芸(1991–), 女, 硕士研究生. E-mail: huanglinyun.2009@163.com
基金资助:
国家重大科技专项基金(2013ZX02104001) National Key Scientitic and Technological Project (2013ZX02104001)

Effect of Rare Earth Oxides on Electrical Properties of Spark
Plasma Sintered AlN Ceramics

HUANG Lin-Yun¹, LI Chen-Hui¹, KE Wen-Ming¹, SHI Yu-Sheng¹, HE Zhi-Yong², ZHANG Qi-Fu²

(1. Huazhong University of Science and Technology, State Key Laboratory of Material Processing and Die & Mould Technology, Wuhan 430074, China; 2. China Iron & Steel Research Institute Group, Beijing 100081, China)

Received:2014-08-25 Revised:2014-10-12 Published:2015-03-20 Online:2015-03-06
About author:HUANG Lin-Yun. E-mail: huanglinyun.2009@163.com

摘要/Abstract

摘要：

以AlN粉末为原料, 添加稀土氧化物(Sm₂O₃、Y₂O₃), 在氮气气氛下, 采用SPS烧结方法制备AlN陶瓷, 研究稀土氧化物的掺杂对AlN烧结试样相组成、微观结构和电性能的影响。实验表明: Sm₂O₃、Y₂O₃与Al₂O₃反应生成的液相稀土金属铝酸盐会提高AlN陶瓷致密度, 且在晶界处形成导电通路降低了AlN陶瓷电阻率。随着Sm₂O₃掺杂量的增加, 晶界相逐渐由Sm₄Al₂O₉过渡到SmAlO₃, 且Sm₄Al₂O₉对电阻率贡献最大。其中, 3wt% Sm₂O₃掺杂AlN陶瓷电阻率最低, 为

, 相对密度为99.33%。Y₂O₃掺杂量的增加会使晶界处钇铝酸盐由富铝酸盐向富钇酸盐转变, 三者电阻率相差较小, Y₂O₃含量高于3wt%的AlN陶瓷电阻率维持在

左右, 其中4wt%Y₂O₃掺杂AlN相对密度最高为99.08%。

关键词: 氮化铝, 氧化钐, 氧化钇, 放电等离子烧结, 电性能

Abstract:

AlN ceramics doped with rare earth oxide (Sm₂O₃, Y₂O₃) were prepared by Spark Plasma Sintering (SPS) in nitrogen atmosphere using AlN powder as raw materials. The effect of rare earth oxide on the phase composition, microstructure and electrical resistivity of AlN ceramics were investigated. The results showed that those sintering additives promoted densification through liquid-phase sintering. AlN ceramics with electrical resistivity values of 1×10¹⁰-1×10¹²Ω•cm were obtained by precipitating rare earth aluminates as a conducting pathway at the grain boundaries. With the increasing of Sm₂O₃ doping, the phase of samarium aluminate gradually changed from Sm₄Al₂O₉ to SmAlO₃ which had a higher resistivity than Sm₄Al₂O₉. 3wt% Sm₂O₃ doped AlN ceramics had the minimum resistivity of 1.32×10¹⁰Ω•cm with the relative density of 99.33%. The yttrium aluminate phase gradually changed from Y₃Al₅O₁₂ to Y₄Al₂O₉ with the increase of Y₂O₃-doping. The electrical resistivity of different yttrium aluminates were about 1×10⁸Ω•cm. Y₂O₃- doped AlN sample with over 3wt% Y₂O₃ had an electrical resistivity about 1×10¹⁰Ω•cm. 4wt% Y₂O₃ doped AlN ceramic had the electrical resistivity of 1.60×10¹⁰Ω•cm with the maximum relative density of 99.08%.

Key words: AlN, Sm2O3, Y2O3, SPS, electrical properties

中图分类号:

TN304

黄林芸, 李晨辉, 柯文明, 史玉升, 贺智勇, 张启富. 稀土氧化物对SPS烧结AlN陶瓷电性能的影响[J]. 无机材料学报, 2015, 30(3): 267-271.

HUANG Lin-Yun, LI Chen-Hui, KE Wen-Ming, SHI Yu-Sheng, HE Zhi-Yong, ZHANG Qi-Fu. Effect of Rare Earth Oxides on Electrical Properties of Spark
Plasma Sintered AlN Ceramics[J]. Journal of Inorganic Materials, 2015, 30(3): 267-271.

图/表 8

图1 不同Sm2O3含量的AlN陶瓷XRD图谱

Fig. 1 XRD patterns of AlN ceramics containing different Sm2O3 mass fractions

图2 添加不同含量Sm2O3的AlN陶瓷断口SEM照片和能谱图

Fig. 2 SEM images and EDS analyses of AlN with different Sm2O3 contents (a) 2wt%; (b) 3wt%; (c) 4wt%; (d) 5wt %; (e) 6wt%; (f) 10wt%

图3 Sm2O3掺量对AlN陶瓷电阻率和相对密度的影响

Fig. 3 Electrical resistivity and relative density of AlN ceramics containing different Sm2O3 mass fractions

图4 不同钐铝比烧结产物的XRD图谱

Fig. 4 XRD patterns of sintering bodies with different mole ratios of Sm2O3 to Al2O3 a-Sm: Al=1: 1; b-Sm: Al=2: 1

图5 不同Y2O3含量的AlN陶瓷XRD图谱

Fig. 5 XRD patterns of AlN ceramics containing different Y2O3 mass fractions

图6 添加Y2O3的AlN陶瓷断口SEM照片和能谱图

Fig. 6 SEM images and EDS analyses of AlN with different Y2O3 contents (a) 1wt%; (b) 3wt%; (c) 5wt%; (d) 7wt%; (e) 10wt%; (f) 10wt%

图7 Y2O3掺杂量对AlN陶瓷电阻率和相对密度的影响

Fig. 7 Electrical resistivity and relative density of AlN ceramics containing different Y2O3 mass fractions

图8 不同钇铝比烧结产物的XRD图谱

Fig. 8 XRD patterns of sintering bodies with different moles ratio of Y2O3 to Al2O3 a-Y: Al=1: 1; b-Y: Al=3: 5; c-Y: Al=2: 1

参考文献 11

[1]	YAN DONG-MING, GAO XIAO-JU, LIU GUO-XI, et al.Research progress of alumina nitride ceramics with high thermal conductivity. Bulletin of the Chinese Ceramic Society, 2011, 30(3): 602-607.
[2]	OMORI MAMORU.Sintering, consolidation, reaction and crystal growth by the spark plasma system(SPS).Mater. Sci. Eng. A, 2000, 287(2): 183-188.
[3]	WATARI K, HWANG H J, TORIYAMA M, et al.Effective sintering aids for low temperature sintering of AlN ceramics. J. Mater. Res., 1999, 14(4): 1409-1417.
[4]	DU XUE-LI, QIN MING-LI, FENG PEI-ZHONG, et al.Effects of Y2O3 on the SPS sintering nanometer AlN powers.Rare Metal Materials and Engineering, 2007, 36(3): 79-81.
[5]	HE XIU-LAN, YE FENG, ZHANG HAI-JIAO, et al.Study of rare-earth oxide sintering additive systems for spark plasma sintering AlN ceramics.Mater. Sci. Eng. A, 2010, 527(20): 5268-5272.
[6]	ZHANG ZHI-JUN, XU FU-MIN, TAN YI.Research progress in thermal conductivity and sintering additives of AlN packaging material.Materials Review, 2009, 23(9): 56-62.
[7]	HE XIU-LAN, YE FENG, ZHANG HAI-JIAO, et al.Effect of Sm2O3 content on microstructure and thermal conductivity of spark plasma sintered AlN ceramics.J. Alloys Compd., 2009, 482(1/2): 345-348.
[8]	KHOR K A, YU L G, MURAKOSHI Y.Spark plasma sintering of Sm2O3-doped aluminum nitride.J. Eur. Ceram. Soc., 2005, 25(7): 1057-1065.
[9]	LI M J, ZHANG M, SHEN Q, et al.Microstructure and properties of spark plasma sintered AlN ceramics. J. Mater. Sci., 2006, 41(23): 7934-7938.
[10]	ZHU JIANG, LI CHEN-HUI, LIU KAI, et al.Electrical properties of TiN/AlN composite ceramic.Semiconductor Technology, 2014, 39(3): 204-209.
[11]	KUSUNOSE T, SEKINO T, NIIHARA K.Production of a grain boundary phase as conducting pathway in insulating AlN ceramics.Acta Mater., 2007, 55(18): 6170-6175.

[1]	汪波, 余健, 李存成, 聂晓蕾, 朱婉婷, 魏平, 赵文俞, 张清杰. Gd/Bi_0.5Sb_1.5Te₃热电磁梯度复合材料的服役稳定性[J]. 无机材料学报, 2023, 38(6): 663-670.
[2]	林俊良, 王占杰. 铁电超晶格的研究进展[J]. 无机材料学报, 2023, 38(6): 606-618.
[3]	贺丹琪, 魏明旭, 刘蕤之, 汤志鑫, 翟鹏程, 赵文俞. 一步法制备重费米子YbAl₃热电材料及其性能提升[J]. 无机材料学报, 2023, 38(5): 577-582.
[4]	林思琪, 李艾燃, 付晨光, 李荣斌, 金敏. Zintl相Mg₃X₂(X=Sb, Bi)基晶体生长及热电性能研究进展[J]. 无机材料学报, 2023, 38(3): 270-279.
[5]	陈雷, 胡海龙. 柔性PDMS基介电复合材料的电场及击穿损伤形貌演变规律研究[J]. 无机材料学报, 2023, 38(2): 155-162.
[6]	韦婷婷, 徐华蕊, 朱归胜, 龙神峰, 张秀云, 赵昀云, 江旭鹏, 宋金杰, 郭宁杰, 龚祎鹏. BaTiO₃陶瓷的低温冷烧结制备及性能研究[J]. 无机材料学报, 2022, 37(8): 903-910.
[7]	程成, 李建波, 田震, 王鹏将, 康慧君, 王同敏. In₂O₃/InNbO₄复合材料的热电性能研究[J]. 无机材料学报, 2022, 37(7): 724-730.
[8]	姚晓刚, 彭海益, 顾忠元, 何飞, 赵相毓, 林慧兴. 聚苯醚/钙镧钛微波复合基板[J]. 无机材料学报, 2022, 37(5): 493-498.
[9]	叶芬, 江向平, 陈云婧, 黄枭坤, 曾仁芬, 陈超, 聂鑫, 成昊. (0.96NaNbO₃-0.04CaZrO₃)-xFe₂O₃反铁电陶瓷的介电及储能性能研究[J]. 无机材料学报, 2022, 37(5): 499-506.
[10]	孙扬善, 杨治华, 蔡德龙, 张正义, 柳琪, 房树清, 冯良, 石丽芬, 王友乐, 贾德昌. 粉末烧结法制备α-堇青石基玻璃陶瓷的析晶动力学和性能[J]. 无机材料学报, 2022, 37(12): 1351-1357.
[11]	刘鼎伟, 曾江涛, 郑嘹赢, 满振勇, 阮学政, 时雪, 李国荣. BiAlO₃掺杂PZT陶瓷的高压电性能和低电场应变滞后[J]. 无机材料学报, 2022, 37(12): 1365-1370.
[12]	刘丹, 赵亚欣, 郭锐, 刘艳涛, 张志东, 张增星, 薛晨阳. 退火条件对磁控溅射MgO-Ag₃Sb-Sb₂O₄柔性薄膜热电性能的影响[J]. 无机材料学报, 2022, 37(12): 1302-1310.
[13]	任培安, 汪聪, 訾鹏, 陶奇睿, 苏贤礼, 唐新峰. Te与In共掺杂对Cu₂SnSe₃热电性能的影响[J]. 无机材料学报, 2022, 37(10): 1079-1086.
[14]	逯旭, 侯绩翀, 张强, 樊建锋, 陈少平, 王晓敏. Mg含量对Mg₃₍₁₊_z₎Sb₂化合物热电传输性能的影响[J]. 无机材料学报, 2021, 36(8): 835-840.
[15]	张维维, 陆晨, 应国兵, 张建峰, 江莞. AlN表面处理及级配填充对覆铜板绝缘层性能的影响规律与机制研究[J]. 无机材料学报, 2021, 36(8): 847-855.

稀土氧化物对SPS烧结AlN陶瓷电性能的影响

Effect of Rare Earth Oxides on Electrical Properties of Spark
Plasma Sintered AlN Ceramics

RichHTML

PDF (PC)

可视化

被引次数

摘要/Abstract

引用本文

使用本文

图/表 8

参考文献 11

相关文章 15

编辑推荐

Metrics

本文评价

稀土氧化物对SPS烧结AlN陶瓷电性能的影响

Effect of Rare Earth Oxides on Electrical Properties of SparkPlasma Sintered AlN Ceramics

RichHTML

PDF (PC)

可视化

被引次数

摘要/Abstract

引用本文

使用本文

图/表 8

参考文献 11

相关文章 15

编辑推荐

Metrics

本文评价

Effect of Rare Earth Oxides on Electrical Properties of Spark
Plasma Sintered AlN Ceramics