Please wait a minute...
金属学报  2017, Vol. 53 Issue (12): 1645-1650    DOI: 10.11900/0412.1961.2017.00026
  本期目录 | 过刊浏览 |
溅射Al对Si3N4润湿性的改善与钎焊
刘葛亮1, 马冰洋1, 尚海龙1,2, 陈凡1, 李荣斌2, 李戈扬1()
1 上海交通大学金属基复合材料国家重点实验室 上海 200240
2 上海电机学院 上海 201306
Wettability Improvement and Brazing of Si3N4by Sputtered Al
Geliang LIU1, Bingyang MA1, Hailong SHANG1,2, Fan CHEN1, Rongbin LI2, Geyang LI1()
1 State Key Laboratory of Metal Matrix Composites, Shanghai Jiao Tong University, Shanghai 200240, China
2 Shanghai Dianji University, Shanghai 201306, China
全文: PDF(5227 KB)   HTML
摘要: 

采用溅射Al和Al-Ni薄膜作为钎料的方法,研究了溅射Al对Si3N4的润湿作用,实现了铝基薄膜钎料对Si3N4陶瓷的直接钎焊。结果表明,Al直接溅射在Si3N4表面所获得的各钎焊接头钎缝致密饱满,与陶瓷形成无反应过渡层的良好冶金结合,纯Al钎焊接头的剪切强度为106 MPa,Al-1.0%Ni亚共晶钎焊接头的强度提高到148 MPa,Al-3.0%Ni接头的强度因钎缝形成共晶组织而略有降低,为132 MPa,这些接头的剪切断裂均产生于钎缝之中。采用首先溅射Ni薄膜作为底层的Al-1.0%Ni薄膜钎料进行了对比,这种钎料得到的钎焊接头断裂产生于钎缝与陶瓷的界面,强度也仅为81 MPa。这表明,高能量溅射Al粒子直接撞击对Si3N4具有“润湿”作用,使得Al和Al-Ni合金薄膜熔化后即可实现对Si3N4的钎焊。

关键词 Si3N4陶瓷润湿溅射薄膜钎焊    
Abstract

In the present technology, the brazing of Si3N4 needs a reactive transition layers to resolve the non-wetting problem of usual metal fillers. Aluminum could wet Si3N4 without reaction but the brazing is very difficult due to wetting temperature above 1000 ℃. In this work, the wetting effect of sputtered Al films on Si3N4 and its physics essence were revealed. Based on this, the brazing of Si3N4 ceramic with Al or Al-Ni film fillers was realized near their melting temperature. The results showed that the seams of brazing joints with direct sputtered Al on Si3N4 film were well-stacked and less defects, and well metallurgically bonded to ceramic without reactive transition layers. The shear strength of pure Al/Si3N4 joint reached 106 MPa. The strength increased to 148 MPa with adding 1.0%Ni into film filler due hypoeutectic structure in the seam. With further increasing Ni content to 3.0%, the eutectic structure of the seam slightly decreased the strength of joint to 132 MPa. These joints above all fractured in joint seams. Moreover, the Al-1.0%Ni film filler first sputtered Ni layer was compared. Its brazing joint fractured at the interface between seam and ceramic and the shear strength decreased to only 81 MPa. This comparsion revealed the "wetting" effect of the bombardment of energetic sputtered Al particles. This effect still existed after filler melting and the direct brazing of Si3N4 ceramic without reactive transition layers was realized.

Key wordsSi3N4 ceramic    wetting    sputtered film    brazing
收稿日期: 2017-01-20     
ZTFLH:  TG454  
基金资助:国家自然科学基金项目Nos.51401120和51671125,上海自然科学基金项目No.16ZR1412800
作者简介:

作者简介 刘葛亮,男,1991年生,硕士生

引用本文:

刘葛亮, 马冰洋, 尚海龙, 陈凡, 李荣斌, 李戈扬. 溅射Al对Si3N4润湿性的改善与钎焊[J]. 金属学报, 2017, 53(12): 1645-1650.
Geliang LIU, Bingyang MA, Hailong SHANG, Fan CHEN, Rongbin LI, Geyang LI. Wettability Improvement and Brazing of Si3N4by Sputtered Al. Acta Metall Sin, 2017, 53(12): 1645-1650.

链接本文:

https://www.ams.org.cn/CN/10.11900/0412.1961.2017.00026      或      https://www.ams.org.cn/CN/Y2017/V53/I12/1645

Sample No. Structure of film filler Atomic fraction of Ni Shear strength / MPa
1 Si3N4 /Al(7 μm) - 106
2 Si3N4/Al(7 μm)/Ni(50 nm) 1.0% 148
3 Si3N4/Al(7 μm)/Ni(150 nm) 3.0% 132
表1  铝基薄膜钎料的结构、成分及Si3N4钎焊接头的剪切强度
图1  不同成分钎料接头焊缝的SEM像
图2  各钎料钎焊接头剪切断口的OM像
图3  结构为Si3N4/Ni(50 nm)/Al(7 μm)的Al-1.0%Ni薄膜钎料(样品No.2b)所获接头剪切断口的OM像
图4  2种薄膜熔化后的OM三维形貌像
[1] Cui W, Yan J C, Dai Y, et al.Building a nano-crystalline α-alumina layer at a liquid metal/sapphire interface by ultrasound[J]. Ultrason. Sonochem., 2015, 22: 108
[2] Ali M, Knowles K M, Mallinson P M, et al.Microstructural evolution and characterisation of interfacial phases in Al2O3/Ag-Cu-Ti/Al2O3 braze joints[J]. Acta Mater., 2015, 96: 143
[3] Yadav D P, Kaul R, Ganesh P, et al.Study on vacuum brazing of high purity alumina for application in proton synchrotron[J]. Mater. Des., 2014, 64: 415
[4] Laik A, Mishra P, Bhanumurthy K, et al.Microstructural evolution during reactive brazing of alumina to Inconel 600 using Ag-based alloy[J]. Acta Mater., 2013, 61: 126
[5] Xia H Y, Wu A P, Fan Y L, et al.Effects of ion implantation on the brazing properties of high purity alumina[J]. Surf. Coat. Technol., 2012, 206: 2098
[6] Ghosh S, Chakraborty R, Dandapat N, et al.Characterization of alumina-alumina/graphite/monel superalloy brazed joints[J]. Ceram. Int., 2012, 38: 663
[7] Ksiazek M, Sobczak N, Mikulowski B, et al.Wetting and bonding strength in Al/Al2O3 system[J]. Mater. Sci. Eng., 2002, A324: 162
[8] Prin G R, Baffie T, Jeymond M, et al.Contact angles and spreading kinetics of Al and Al-Cu alloys on sintered AlN[J]. Mater. Sci. Eng., 2001, A298: 34
[9] Sobczak N, Stobierski L, Radziwill W, et al.Wettability and interfacial reactions in Al/TiO2 [J]. Surf. Interface Anal., 2004, 36: 1067
[10] Ljungberg L, Warren R.Wetting of silicon nitride with selected metals and alloys [A]. Proceedings of the International Forum on Structural Ceramics Joining: Ceramic Engineering and Science Proceedings[C]. American: The American Ceramic Society, Inc., 2008, 10: 1655
[11] Naka M, Kubo M.Brazing of Si3N4 to metals with Al-Si filler metals (physics, process, instruments & measurement)[J]. Trans. JWRI, 1990, 19: 181
[12] Chen F, Shi K C, Sun S Y, et al.Direct brazing of Al/Al2O3 without wettability of molten metal[J]. J. Inorg. Mater., 2016, 31: 602(陈凡, 石恺成, 孙士阳等. 不基于熔态润湿的Al/Al2O3直接钎焊[J]. 无机材料学报, 2016, 31: 602)
[13] Zhao B W, Shang H L, Chen F, et al."Wetting" and brazing of AlN by sputtered Al[J]. Acta Phys. Sin., 2016, 65: 086801(赵博文, 尚海龙, 陈凡等. 溅射Al对AlN的“润湿”与钎焊[J]. 物理学报, 2016, 65: 086801)
[14] Mouradoff L, Tristant P, Desmaison J, et al.Interaction between liquid aluminium and non-oxide ceramics (AlN, Si3N4, SiC)[J]. Key Eng. Mater., 1995, 113: 177
[15] Eustathopoulos N, Nicholas M G, Drevet B.Wettability at High Temperatures[M]. New York: Pergamon, 1999: 294
[16] Li J G.Wetting of ceramic materials by liquid silicon, aluminium and metallic melts containing titanium and other reactive elements: A review[J]. Ceram. Int., 1994, 20: 391
[17] Nicholas M G, Mortimer D A, Jones L M, et al.Some observations on the wetting and bonding of nitride ceramics[J]. J. Mater. Sci., 1990, 25: 2679
[18] Naka M, Kubo M, Okamoto I.Joining of silicon nitride with Al-Cu alloys[J]. J. Mater. Sci., 1987, 22: 4417
[19] Naka M, Kubo M, Okamoto I.Wettability of silicon nitride by aluminium, copper and silver[J]. J. Mater. Sci. Lett., 1987, 6: 965
[20] Mouradoff L, Lachau-Durand A, Desmaison J, et al.Study of the interaction between liquid aluminum and silicon nitride[J]. J. Eur. Ceram. Soc., 1994, 13: 323
[21] Zhang Q, ?a??n T, van Duin A, et al. Adhesion and nonwetting-wetting transition in the Al/α-Al2O3 interface[J]. Phys. Rev., 2004, 69B: 045423
[22] Zheng W T.Thin Film Materials and Thin Film Technology [M]. Beijing: Chemical Industry Press, 2004: 72(郑伟涛. 薄膜材料与薄膜技术 [M]. 北京: 化学工业出版社, 2004: 72)
[23] Fujii H, Nakae H, Okada K.Interfacial reaction wetting in the boron nitride/molten aluminum system[J]. Acta Metall. Mater., 1993, 41: 2963
[24] Li G C, Ning X S, Chen K X, et al.Interaction of Si3N4 ceramics and liquid aluminum at interface without oxidation[J]. Rare Met. Mater. Eng., 2009, 38(S2): 186(李国才, 宁晓山, 陈克新等. 界面无氧化膜条件下氮化硅陶瓷和铝溶液的反应[J]. 稀有金属材料与工程, 2009, 38(S2): 186)
[25] Ning X S, Okamoto T, Miyamoto Y, et al.Reaction chemistry at joined interfaces between silicon nitride and aluminium[J]. J. Mater. Sci., 1991, 26: 4142
[1] 赵旭,孙元,侯星宇,张洪宇,周亦胄,丁雨田. 取向偏差对镍基单晶高温合金钎焊接头组织与力学性能的影响[J]. 金属学报, 2020, 56(2): 171-181.
[2] 邱丰, 佟昊天, 沈平, 丛晓霜, 王轶, 姜启川. 综述:SiC/Al界面反应与界面结构演变规律及机制[J]. 金属学报, 2019, 55(1): 87-100.
[3] 姚彦桃, 陈礼清, 王文广. 原位反应浸渗法制备(B4C+Ti)混杂增强Mg及AZ91D复合材料及其阻尼性能[J]. 金属学报, 2019, 55(1): 141-148.
[4] 李淑波, 杜文博, 王旭东, 刘轲, 王朝辉. Zr对Mg-Gd-Er合金晶粒细化机理的影响[J]. 金属学报, 2018, 54(6): 911-917.
[5] 张笑一, 尚海龙, 马冰洋, 李荣斌, 李戈扬. 镀膜Al箔钎料对AlN陶瓷的钎焊[J]. 金属学报, 2018, 54(4): 575-580.
[6] 孙磊,陈明和,张亮,杨帆. Sn-Ag-Cu钎料焊接显微组织演化和性能研究[J]. 金属学报, 2017, 53(5): 615-621.
[7] 刘积厚,赵洪运,李卓霖,宋晓国,董红杰,赵一璇,冯吉才. Cu/Sn/Cu超声-TLP接头的显微组织与力学性能[J]. 金属学报, 2017, 53(2): 227-232.
[8] 孙元,刘纪德,侯星宇,王广磊,杨金侠,金涛,周亦胄. DD5单晶高温合金大间隙钎焊的组织演变与界面形成机制*[J]. 金属学报, 2016, 52(7): 875-882.
[9] 付伟,宋晓国,龙隆,柴鉴航,冯吉才,王国栋. 石墨/紫铜间接钎焊接头的界面组织及力学性能*[J]. 金属学报, 2016, 52(6): 734-740.
[10] 陈晓燕,金喆,白雪峰,周亦胄,金涛,孙晓峰. C对一种镍基高温合金与陶瓷型壳界面反应及润湿性的影响*[J]. 金属学报, 2015, 51(7): 853-858.
[11] 羊浩, 黄继华, 陈树海, 赵兴科, 王奇, 李德华. Zn-Al钎料成分对Cu/Zn-Al/Al钎焊接头界面结构及性能的影响[J]. 金属学报, 2015, 51(3): 364-370.
[12] 陈晓燕, 周亦胄, 张朝威, 金涛, 孙晓峰. Hf对一种高温合金与陶瓷材料润湿性及界面反应的影响*[J]. 金属学报, 2014, 50(8): 1019-1024.
[13] 马国峰,贺春林, 李正坤,张波,李宏,张海峰,胡壮麒. Ti或Al添加对Zr50Cu50非晶合金W润湿行为和界面特性的影响[J]. 金属学报, 2013, 29(4): 495-500.
[14] 孙元,刘纪德,刘忠明,杨金侠,李金国,金涛,孙晓峰. 钴基钎料钎焊DD5单晶高温合金的接头微观组织演变与力学性能研究[J]. 金属学报, 2013, 49(12): 1581-1589.
[15] 张青科,裴夤崟,龙伟民. 奥氏体不锈钢钎焊界面裂纹形成机制研究[J]. 金属学报, 2013, 49(10): 1177-1184.