机械合金化制备Sn-1.0Ag-0.5Cu高硼中间合金的组织演变
|
摘要
制订了合适的机械合金化方案,利用行星式高能球磨机,制备了一种Sn-1.0Ag-0.5Cu高硼新型中间合金,并以此作为配比微量硼掺杂的Sn-1.0Ag-0.5Cu低银无铅钎料合金的原料。发现随球磨时间的增加,样品颗粒尺寸先增大后减小,与机械合金化"破碎—冷焊—破碎"循环过程相符。结合物相分析与计算,锡的晶格畸变程度不断增加,球磨72 h后达到最大值0.1375%,表明硼在合金基体中的过饱和固溶度逐渐增大。同时晶粒显著细化至纳米晶,并在48 h达到临界值(57.9 nm)。结合电子显微观察与能谱(EDS)分析,合金基体中硼含量呈不断上升的趋势,且分布形态逐渐变得细小而弥散。可见在机械合金化过程中,样品的合金化程度随球磨时间的增加而变高。此外,合金粉体的显微硬度与其球磨过程中晶粒的大小呈负相关关系。以此中间合金制备的钎料合金组织得到了显著细化。
For proportioning the trace-boron doped Sn-1.0 Ag-0.5 Cu low-silver lead-free solder, a novel high-boron doped Sn-1.0 Ag-0.5 Cu master alloys were prepared by mechanical alloying using the planetary high energy ball mill with the suitable scheme. The results showed with the increase of milling time, the particle size increased first and then decreased, which was consistent with the cycle process of mechanical alloying(crushing—welding—crushing). Combined with the phase analysis and calculation, the lattice distortion of tin increased continuously, peaking at 72 h(0.1375%), indicating the supersaturated solid solubility increased. Meanwhile, the grain refined to nanocrystalline and reached critical value at 48 h(57.9 nm). Through electron microscopy and energy dispersive spectroscope(EDS) analysis, the samples′ alloying degree became higher as the milling time increased. Furthermore, the solidus of alloying powder gradually decreased, and microhardness values were negatively correlated with the grain size. The microstructure of the solder alloys prepared by this master alloys was remarkably refined.
For proportioning the trace-boron doped Sn-1.0 Ag-0.5 Cu low-silver lead-free solder, a novel high-boron doped Sn-1.0 Ag-0.5 Cu master alloys were prepared by mechanical alloying using the planetary high energy ball mill with the suitable scheme. The results showed with the increase of milling time, the particle size increased first and then decreased, which was consistent with the cycle process of mechanical alloying(crushing—welding—crushing). Combined with the phase analysis and calculation, the lattice distortion of tin increased continuously, peaking at 72 h(0.1375%), indicating the supersaturated solid solubility increased. Meanwhile, the grain refined to nanocrystalline and reached critical value at 48 h(57.9 nm). Through electron microscopy and energy dispersive spectroscope(EDS) analysis, the samples′ alloying degree became higher as the milling time increased. Furthermore, the solidus of alloying powder gradually decreased, and microhardness values were negatively correlated with the grain size. The microstructure of the solder alloys prepared by this master alloys was remarkably refined.
引文
[1] Zhang F W,Liu J,Yang F B,Hu Q,He H J,Xu J.Developing tendency and current situation of Sn-Ag-Cu lead-free solder [J].Chinese Journal of Rare Metals,2005,29(5):619.(张富文,刘静,杨福宝,胡强,贺会军,徐俊.Sn-Ag-Cu无铅焊料的发展现状与展望 [J].稀有金属,2005,29(5):619.)
[2] Qu J F,Xu J,Hu Q,Zhang F W,Zhang S M.Modification of Sn-1.0Ag-0.5Cu solder using nickel and boron [J].Rare Metals,2015,34(11):783.
[3] Choi H,Lee T K,Kim Y,Kwon H,Tseng C F,Duh J G,Choe H.Improved strength of boron-doped Sn-1.0 Ag-0.5 Cu solder joints under aging conditions [J].Intermetallics,2012,20(1),155.
[4] Ye L,Lai Z H,Liu J,Th?lén A.Microstructure investigation of Sn-3.5Ag-0.5Cu-0.5B lead-free solders [J].Soldering & Surface Mount Technology,2001,13(13):16.
[5] Wang R D,Zhang S M,Hu Q,Zhang F W.Effect of boron on microstructure and properties of Sn-1.0Ag-0.5Cu low-silver lead-free solder [J].Materials Science Forum,2017,898:908.
[6] Wu Z F,Liu C,Zhou F.Research progress on the thermodynamics of binary immiscible alloy systems by mechanical alloying [J].Powder Metallurgy Industry,2016,26(2):58.(吴志方,刘超,周帆.二元互不溶体系合金机械合金化的热力学研究进展 [J].粉末冶金工业,2016,26(2):58.)
[7] Wang E D,Liu J L,Liu Z Y.The research progression on the kinetics of extension [J].Powder Metallurgy Technology,2002,20(2):109.(王尔德,刘京雷,刘祖岩.机械合金化诱导固溶度扩展机制研究进展 [J].粉末冶金技术,2002,20(2):109.)
[8] Yang F,Yan G,Zhang P X,Wang Q Y,Xiong X M,Li S Q,Feng J Q,Li C S,Feng Y.Research progress of MgB2 superconducting materials prepared by high-energy ball milling [J].Rare Metal Materials and Engineering,2017,46(5):1452.(杨芳,闫果,张平祥,王庆阳,熊晓梅,李少强,冯建情,李成山,冯勇.高能球磨法制备MgB2超导材料的研究进展 [J].稀有金属材料与工程,2017,46(5):1452.)
[9] Chen Z H,Chen D.Mechanical Alloying and Solid-Liquid Reaction Ball Milling [M].Beijing:Chemical Industry Press,2006.34.(陈振华,陈鼎.机械合金化与固液反应球磨 [M].北京:化学工业出版社,2006.34.)
[10] Shuai G W,Guo Z H,Huang H Z,Lu B P.Research progress in supersaturated solid solution prepared by mechanical alloying [J].Materials Review,2008,22(z2):201.(帅歌旺,郭正华,黄惠珍,卢百平.机械合金化制备过饱和固溶体的研究进展 [J].材料导报,2008,22(z2):201.)
[11] Yao Z H.Research on Properties and Microstructure of 12Cr-ODS Fe-Based Superalloy Fabricated by Mechanical Alloying [D].Wuhan:Huazhong University of Science & Technology,2011.32.(姚振华.12Cr-ODS铁基高温合金的机械合金化制备及其组织性能研究 [D].武汉:华中科技大学,2011.32.)
[12] Li S S,Li J L,Li W,Xiong Y C.Synthesis of nanocrystalline 7050 aluminium alloy powder by cryomilling [J].Rare Metal Materials and Engineering,2012,41(S2):761.(厉沙沙,李炯利,李伟,熊艳才.低温球磨制备纳米晶7050合金粉体 [J].稀有金属材料与工程,2012,41(S2):761.)
[13] Wu Z F,Zhou F.Research development of nanocrystalline supersaturated solid solution in immiscible system by mechanical alloying [J].Materials Review,2014,28(13):78.(吴志方,周帆.二元互不溶体系中纳米晶过饱和固溶体机械合金化的研究进展 [J].材料导报,2014,28(13):78.)
[14] Xiao S W,Xiao X,Zeng Z G.Research progress in behavior and mechanism of mechano-chemical phase transformation of ceramic material under ball milling [J].Materials Review,2008,22(1):37.(肖松文,肖骁,曾子高.球磨作用下陶瓷粉体材料的机械化学相变行为机制研究进展 [J].材料导报,2008,22(1):37.)
[15] Wang H,Hu L X,Chen X J,Wang E D.Preparation of nanocrystalline magnesium alloy powders by high-energy ball milling [J].Powder Metallurgy Technology,2008,26(6):403.(王珩,胡连喜,陈先觉,王尔德.高能球磨制备纳米晶镁合金粉末的研究 [J].粉末冶金技术,2008,26(6):403.)
[16] Lu Y,Jin W X,Li W S,Wang Y Q,Li Z.Influence of ball milling technique on morphology of Cu-14Al-X powders [J].Hot Working Technology,2008,(6):30.(路阳,金硪馨,李文生,王亚青,李振.球磨工艺参数对Cu-14Al-X粉末形貌的影响 [J].热加工工艺,2008,(6):30.)
[17] Li L F,Qiu T,Yang J,Feng Y B,Zhang Z Z.Preparation and characterization of nanocrystalline (Ag-Cu28)-25Sn alloy powder [J].Rare Metal Materials and Engineering,2010,39(5):902.(李良锋,丘泰,杨建,冯永宝,张振忠.纳米晶(Ag-Cu28)-25Sn合金粉末的制备及表征 [J].稀有金属材料与工程,2010,39(5):902.)
[18] Ling Z C,Yan C X,Shi Q N,Feng Z X,Qu Y D,Li T,Yang Y X.Effect of ball-milling time on microstructure and mechanical properties of graphene/copper composite materials [J].Rare Metal Materials and Engineering,2017,46(1):207.(凌自成,闫翠霞,史庆南,冯中学,曲永冬,李涛,杨应湘.球磨时间对石墨烯/铜复合材料组织和性能的影响 [J].稀有金属材料与工程,2017,46(1):207.)
[2] Qu J F,Xu J,Hu Q,Zhang F W,Zhang S M.Modification of Sn-1.0Ag-0.5Cu solder using nickel and boron [J].Rare Metals,2015,34(11):783.
[3] Choi H,Lee T K,Kim Y,Kwon H,Tseng C F,Duh J G,Choe H.Improved strength of boron-doped Sn-1.0 Ag-0.5 Cu solder joints under aging conditions [J].Intermetallics,2012,20(1),155.
[4] Ye L,Lai Z H,Liu J,Th?lén A.Microstructure investigation of Sn-3.5Ag-0.5Cu-0.5B lead-free solders [J].Soldering & Surface Mount Technology,2001,13(13):16.
[5] Wang R D,Zhang S M,Hu Q,Zhang F W.Effect of boron on microstructure and properties of Sn-1.0Ag-0.5Cu low-silver lead-free solder [J].Materials Science Forum,2017,898:908.
[6] Wu Z F,Liu C,Zhou F.Research progress on the thermodynamics of binary immiscible alloy systems by mechanical alloying [J].Powder Metallurgy Industry,2016,26(2):58.(吴志方,刘超,周帆.二元互不溶体系合金机械合金化的热力学研究进展 [J].粉末冶金工业,2016,26(2):58.)
[7] Wang E D,Liu J L,Liu Z Y.The research progression on the kinetics of extension [J].Powder Metallurgy Technology,2002,20(2):109.(王尔德,刘京雷,刘祖岩.机械合金化诱导固溶度扩展机制研究进展 [J].粉末冶金技术,2002,20(2):109.)
[8] Yang F,Yan G,Zhang P X,Wang Q Y,Xiong X M,Li S Q,Feng J Q,Li C S,Feng Y.Research progress of MgB2 superconducting materials prepared by high-energy ball milling [J].Rare Metal Materials and Engineering,2017,46(5):1452.(杨芳,闫果,张平祥,王庆阳,熊晓梅,李少强,冯建情,李成山,冯勇.高能球磨法制备MgB2超导材料的研究进展 [J].稀有金属材料与工程,2017,46(5):1452.)
[9] Chen Z H,Chen D.Mechanical Alloying and Solid-Liquid Reaction Ball Milling [M].Beijing:Chemical Industry Press,2006.34.(陈振华,陈鼎.机械合金化与固液反应球磨 [M].北京:化学工业出版社,2006.34.)
[10] Shuai G W,Guo Z H,Huang H Z,Lu B P.Research progress in supersaturated solid solution prepared by mechanical alloying [J].Materials Review,2008,22(z2):201.(帅歌旺,郭正华,黄惠珍,卢百平.机械合金化制备过饱和固溶体的研究进展 [J].材料导报,2008,22(z2):201.)
[11] Yao Z H.Research on Properties and Microstructure of 12Cr-ODS Fe-Based Superalloy Fabricated by Mechanical Alloying [D].Wuhan:Huazhong University of Science & Technology,2011.32.(姚振华.12Cr-ODS铁基高温合金的机械合金化制备及其组织性能研究 [D].武汉:华中科技大学,2011.32.)
[12] Li S S,Li J L,Li W,Xiong Y C.Synthesis of nanocrystalline 7050 aluminium alloy powder by cryomilling [J].Rare Metal Materials and Engineering,2012,41(S2):761.(厉沙沙,李炯利,李伟,熊艳才.低温球磨制备纳米晶7050合金粉体 [J].稀有金属材料与工程,2012,41(S2):761.)
[13] Wu Z F,Zhou F.Research development of nanocrystalline supersaturated solid solution in immiscible system by mechanical alloying [J].Materials Review,2014,28(13):78.(吴志方,周帆.二元互不溶体系中纳米晶过饱和固溶体机械合金化的研究进展 [J].材料导报,2014,28(13):78.)
[14] Xiao S W,Xiao X,Zeng Z G.Research progress in behavior and mechanism of mechano-chemical phase transformation of ceramic material under ball milling [J].Materials Review,2008,22(1):37.(肖松文,肖骁,曾子高.球磨作用下陶瓷粉体材料的机械化学相变行为机制研究进展 [J].材料导报,2008,22(1):37.)
[15] Wang H,Hu L X,Chen X J,Wang E D.Preparation of nanocrystalline magnesium alloy powders by high-energy ball milling [J].Powder Metallurgy Technology,2008,26(6):403.(王珩,胡连喜,陈先觉,王尔德.高能球磨制备纳米晶镁合金粉末的研究 [J].粉末冶金技术,2008,26(6):403.)
[16] Lu Y,Jin W X,Li W S,Wang Y Q,Li Z.Influence of ball milling technique on morphology of Cu-14Al-X powders [J].Hot Working Technology,2008,(6):30.(路阳,金硪馨,李文生,王亚青,李振.球磨工艺参数对Cu-14Al-X粉末形貌的影响 [J].热加工工艺,2008,(6):30.)
[17] Li L F,Qiu T,Yang J,Feng Y B,Zhang Z Z.Preparation and characterization of nanocrystalline (Ag-Cu28)-25Sn alloy powder [J].Rare Metal Materials and Engineering,2010,39(5):902.(李良锋,丘泰,杨建,冯永宝,张振忠.纳米晶(Ag-Cu28)-25Sn合金粉末的制备及表征 [J].稀有金属材料与工程,2010,39(5):902.)
[18] Ling Z C,Yan C X,Shi Q N,Feng Z X,Qu Y D,Li T,Yang Y X.Effect of ball-milling time on microstructure and mechanical properties of graphene/copper composite materials [J].Rare Metal Materials and Engineering,2017,46(1):207.(凌自成,闫翠霞,史庆南,冯中学,曲永冬,李涛,杨应湘.球磨时间对石墨烯/铜复合材料组织和性能的影响 [J].稀有金属材料与工程,2017,46(1):207.)