传统的封接玻璃由于含有重金属元素铅,对环境和人类健康有着极大的损害,目前已经被世界各国限制使用或者禁止使用,因此,低熔点封接玻璃的无铅化将会是今后的主要发展方向。本文以低熔点封接玻璃的无铅化为出发点,归纳总结低熔点封接玻璃的主要性能。首先介绍了包括磷酸盐玻璃,钒酸盐、硼酸盐、铋酸盐玻璃在内的低熔点封接玻璃的组成、结构特点、性能以及研究现状。其次,提出了封接玻璃的封接低温化和无铅化的发展方向。最后,针对低熔点封接玻璃研究中存在的不足,对玻璃粉添加颗粒进行复合改性、加强玻璃理论研究、研发制备新工艺,是今后研究应该着力的突破点。
Traditional sealing glasses, which contain heavy metal Pb, posing threat to humans and environment, have been restricted or forbidden by most countries. Therefore, lead-free of low-melting sealing glasses will be the main future development direction. This article based on lead-free of low-melting sealing glasses, the main properties of low-melting sealing glasses were summarized. First, the composition, structural characteristics, performance and research status of several main low-melting sealing glasses, such as phosphate glass, borate glass, vanadate glass and bismuthate glass were introduced. Second, the low temperature and lead-free development directions were put forward. At last, regarding the shortcomings in the research of low-melting sealing glasses, it was pointed out that the future focused breaking points for research are composite doping modification, theoretical research on glass and new technology development of glass preparation.
参考文献
| [1] | HE F, CHENG J S, DENG D W, et al. Structure of Bi2O3-ZnO-B2O3 system low-melting sealing glass[J]. Journal of Central South University of Technology, 2010, 17(2) :257-262. |
| [2] | MA Y R. Sealing glasses-the application of low-melting glasses in electronic devices[J]. Glass and Enamel, 1993, 21(6) :50-57. 马英仁. 封接玻璃(九)-低熔玻璃在电子元器件的应用[J]. 玻璃与搪瓷, 1993, 21(6) :50-57. |
| [3] | CHEN P, LI S C, QIAO W J, et al. Structure and crystallization of ZnO-B2O3-P2O5 glasses[J]. Glass Physics and Chemistry, 2011, 37(1) :29-33. |
| [4] | LI C J, HUANG Y R, CUI Z, et al. Recent development of environment-friendly low-melting glasses[J]. Glass, 2008, 34(6) :17-23. 李长久, 黄幼榕, 崔竹, 等. 环境友好型无铅低温封接玻璃最新进展[J]. 玻璃, 2008, 34(6) :17-23. |
| [5] | MORENA R. Phosphate glasses as alternatives to Pb-based sealing frits[J]. Journal of Non-crystalline Solids, 2000, 263:382-387. |
| [6] | WOOD E P, NIMMO K L. In search of new lead-free electronic solders[J]. Journal of Electronic Materials, 1994, 23(8) :709-713. |
| [7] | ZHANG L, HE C, GUO Y, et al. Development of SnAg-based lead free solders in electronics packaging[J]. Microelectronics Reliability, 2012, 52(3) :559-578. |
| [8] | LI Y, MOON K, WONG C P. Electronics without lead[J]. Science, 2005, 308(5727) :1419-1420. |
| [9] | WU C M L, YU D Q, LAW C M T, et al. Properties of lead-free solder alloys with rare earth element additions[J]. Materials Science and Engineering:R, 2004, 44(1) :1-44. |
| [10] | ZHANG Y A, LIU H, YUAN J. Technique of glass solders to metal Seal[J]. Foshan Cermics, 2004, 14(1) :34-36. 张永爱,刘浩,袁坚. 玻璃焊料与金属封接技术[J]. 佛山陶瓷, 2004, 14(1) :34-36. |
| [11] | MA Y R. Sealing glasses-low melting glass[J]. Glass and Enamel, 1993, 21(4) :50-54. 马英仁. 封接玻璃(七)-低熔玻璃[J]. 玻璃与搪瓷, 1993, 21(4) :50-54. |
| [12] | CAI C P. Study on low melting point microcrystalline sealing glass[J]. Journal of Applied Optics, 1995, 16(5) :33-39. 蔡春平. 低熔点微晶封接玻璃的研究[J]. 应用光学, 1995, 16(5) :33-39. |
| [13] | HE F, TAN G J, CHENG J S. Research present status and trend in Development of low-melting sealing glasses[J]. The World of Building Materials, 2009, 30(1) :1-5. 何峰, 谭刚健, 程金树. 低熔点封接玻璃研究现状与发展趋势[J]. 建材世界, 2009, 30(1) :1-5. |
| [14] | BROW R K. Review:the structure of simple phosphate glasses[J]. Journal of Non-crystalline Solids, 2000, 263:1-28. |
| [15] | SHIH P Y, YUNG S W, CHEN C Y, et al. The effect of SnO and PbCl2 on properties of stannous chlorophosphate glasses[J]. Materials Chemistry and Physics. 1997, 50(1) :63-69. |
| [16] | 葉志贤. 无铅低熔点SnO-MgO-P2O5玻璃[D]. 台北:大同大学材料工程研究所, 2004. |
| [17] | SHIH P Y. Preparation of lead-free phosphate glasses with low Tg and excellent chemical durability[J]. Journal of Materials Science Letters, 2001, 19(20) :1811-1813. |
| [18] | LISITSYNA E A. Production and structure of the glasses 0.4Zn(PO3)2(0.6-x) Al(PO3)3[J]. Journal of Glass Physics and Chemistry, 1998, 14(4) :333-336. |
| [19] | TAKEBE H, BABA Y, KUWABARA. Dissolution behavior of ZnO-P2O5 system glass in water[J]. Journal of Non-crystalline Solids, 2006, 352:3088-3094. |
| [20] | SHYU J J, YEH C H. Formation and properties of SnO-MgO-P2O5 glasses[J]. Journal of Materials Science, 2007, 42(13) :4772-4777. |
| [21] | SHYU J J, LIN W Y. Sintering,crystallization,and properties of a low-viscosity SnO-MgO-P2O5 glass filled with (Co0.5Mg0.5)2P2O7 ceramic:influence of filler particle size[J]. Journal of the Ceramic Society of Japan, 2012, 20(1404) :324-329. |
| [22] | HONG J H, ZHAO D S, GAO J F, et al. Lead-free low-melting point sealing glass in SnO-CaO-P2O5 system[J]. Journal of Non-crystalline Solids, 2010, 356(28-30) :1400-1403. |
| [23] | SUN L Y, LU C H, NI Y R, et al. Research and development of leadless low-melting glasses[J]. Materials Review, 2008, 27(Suppl3) :331-334. 孙丽燕, 陆春华, 倪亚茹, 等. 无铅低熔玻璃的研究及进展[J]. 材料导报, 2007, 21(增刊3) :331-334. |
| [24] | MA Z F, LI Q J, ZHAO Y Z, et al. The study of partial heat properties about SnO-ZnO-P2O5 glasses[J]. Glass and Enamel, 2005, 33(5) :5-9. 马占峰, 李启甲, 赵彦钊, 等. SnO-ZnO-P2O5玻璃部分热性质的研究[J]. 玻璃与搪瓷, 2005, 33(5) :5-9. |
| [25] | LI C L, TIAN Y L,SUN S B. Influence of R2O3 on properties of lead-free SnO-ZnO-P2O5 glasses[J]. Glass and Enamel, 2007, 25(1) :12-14. 李春丽, 田英良, 孙诗兵. R2O3对SnO-ZnO-P2O5无铅玻璃[J]. 玻璃与搪瓷, 2007, 25(1) :12-14. |
| [26] | KOUDELK L, MOSNER P. Borophosphate glasses of the ZnO-B2O3-P2O5 system[J]. Materials Letters, 2000, 42(3) :194-199. |
| [27] | CHEN P, LI C L, QIAO W J, et al. Structure and crystallization of ZnO-B2O3-P2O5 glasses[J]. Glass Physics and Chemistry, 2011, 37(1) :29-33. |
| [28] | LI S S, CHEN P. Properties and structure of the ZnO-B2O3-P2O5 low melting point glass[J]. Electronic Components and Materials, 2007, 26(6) :34-36. 李胜春, 陈培. ZnO-B2O3-P2O5低熔点玻璃的性能和结构[J]. 电子元件与材料, 2007, 26(6) :34-36. |
| [29] | CHEN P. Effect of doped oxides on the properties and structure of the phosphate low-melting glasses[J]. Bulletin of the Chinese Ceramic Society, 2008, 27(6) :1134-1139. 陈培. 氧化物掺杂对磷酸盐低熔点玻璃结构与封接性能的影响[J]. 硅酸盐通报, 2008, 27(6) :1134-1139. |
| [30] | 成茵. 新硼酸盐功能玻璃结构及析晶动力学研究[D]. 长沙:湖南大学, 2004. |
| [31] | JANAKIRAMA-RAO B V. Structure and mechanism of conduction of semiconductor glasses[J]. Journal of American Ceramic Society,1965, 48(6) :311-319. |
| [32] | LI C J, HUANG Y R, YU L, et al. The new development on low temperature lead-free sealing glass of vanadium system[J]. China Building Materials Science and Technology, 2007, (3) :30-33. 李长久, 黄幼榕, 俞琳, 等. 钒酸盐系统无铅低温封接玻璃最新进展[J]. 建筑玻璃与工业玻璃, 2007,(3) :30-33. |
| [33] | BAI J W. Composition and developments in low-melting seal glasses[J]. Materials Review, 2002, 16(12) :43-46. 白进伟. 低熔封接玻璃组成及发展[J]. 材料导报, 2002, 16(12) :43-46. |
| [34] | GARBARCZYK J E, JOZWIAK P, WASIUCIONEK M, et al. Enhancement of electrical conductivity in lithium vanadate glasses by nanocrystallization[J]. Solid State Ionics, 2005, 175(1-4) :691-694. |
| [35] | GARBARCZYK J E, WASIUCIONEK M, JOZWIAK P et al. Studies of Li2O-V2O5-P2O5 glasses by DSC, EPR and impedance spectroscopy[J]. Solid State Ionics, 2002, 154-155:367-373. |
| [36] | 上海玻搪所封接小组. 低温封接玻璃及应用[J]. 玻璃与搪瓷, 1973,(1) :25-34. |
| [37] | HUA Y J, XU S Q, ZHAO S L. Characteristics of a V2O5-B2O3-ZnO-TeO2-Li2O low-melting sealing glass[J]. Acta Photonica Sinica,2008, 37(1) :160-163. 华有杰, 徐时清,赵士龙, 等. V2O5-B2O3-ZnO-TeO2-Li2O系低熔点封接玻璃性能研究[J]. 光子学报,2008, 37(1) :160-163. |
| [38] | 吴春娥, 秦国斌.一种无铅低熔玻璃粉及其制造[P].中国专利:200310103592, 2005-05-18. |
| [39] | 齐济. 钒氧化物及其复合玻璃的制备与性质研究[D]. 大连:大连理工大学, 2008. |
| [40] | ZHAO H S, LI Y Q, ZHOU W C. Preparation and properties of MoO3-V2O5-P2O5-Fe2O3 glasses[J]. Journal of Inorganic Materials, 2005, 20(3) :563-569. 赵宏生, 李艳青, 周万城, 等. MoO3-V2O5-P2O5-Fe2O3玻璃的制备及性能研究[J]. 无机材料学报, 2005, 20(3) :563-569. |
| [41] | FRANCIS G L, MORENA R. Non-lead sealing glasses[P]. US Patent:5281560, 1994-01-25. |
| [42] | TOSHIO Y. Lead-free silicate-phosphate glass and sealing materials containing the same[P]. US Patent:20020019303, 2002-02-14. |
| [43] | PENG Y B, DAY D E. High thermal expansion phosphate glasses[J]. Glass Technology, 1991, 32(6) :200-205. |
| [44] | SHARMA B I, ROBI P S, SRINIVASAN A. Microhardness of ternary vanadium pentoxide glasses[J]. Materials Letters, 2003, 57(22) :3504-3507. |
| [45] | 樊先平, 洪樟连, 翁文剑. 无机非金属材料科学基础[M]. 杭州:浙江大学出版社, 2004. |
| [46] | BOURHIS E L. Glass Mechanics and Technology[M]. Weinheim:Wiley-v ch Verlag GmbH & Co. KGaA, 2008. |
| [47] | KIM D N, LEE J, HUH J S, et al. Thermal and electrical properties of BaO-B2O3-ZnO glasses[J]. Journal of Non-crystalline solids, 2002, 306(1) :70-75. |
| [48] | LU A X, LIN N. Formation rule and relationship between the composition and properties of B2O3-BaO-ZnO glass[J]. Bulletin of the Chinese Ceramic Society, 2005, 24(1) :44-47. 卢安贤, 林娜. B2O3-BaO-ZnO系统玻璃的形成规律及组成与性能之间的关系研究[J]. 硅酸盐通报, 2005, 24(1) :44-47. |
| [49] | GAO D N,LIU X N,GUO H W. Crystallization process of ZnO-B2O3-BaO system lead-free sealing glass[J]. Glass, 2006, 32(6) :10-13. 高档妮, 刘新年, 郭宏伟. ZnO-B2O3-BaO系无铅封接玻璃析晶行为的研究[J]. 玻璃, 2006, 32(6) :10-13. |
| [50] | DING M Y, LU C H, CUI Q Q, et al. Fabrication and characterization of B2O3-Al2O3-Na2O glass system for transparent dielectric layer[J]. Ceramics International, 2014, 40(1) :233-239. |
| [51] | DOWEIDAR H, MOUSTAFA Y M, ABD E M. Properties of Na2O-Al2O3-B2O3 glasses[J]. Materials Science and Engineering:A, 2001, 301(2) :207-212. |
| [52] | CHEN F, YIN H R, WU L H, et al. The preparation of low-melting point glass of Na2O-Al2O3-B2O3 system[J]. Journal of Shaanxi University of Science and Technology, 2006, 23(4) :33-36. 陈福, 殷海荣, 武丽华, 等. Na2O-Al2O3-B2O3系统低熔点玻璃的研究[J]. 陕西科技大学学报:自然科学版, 2006, 23(4) :33-36. |
| [53] | CHEN F, AN B J, ZENG X W, et al. Study on thermal properties of low melting point glass of Na2O-Al2O3-B2O3[J]. Ceramics, 2007(3) :16-18. 陈福, 安百江, 曾雄伟, 等. Na2O-Al2O3-B2O3系统低熔点玻璃的热学性质研究[J]. 陶瓷, 2007, (3) :16-18. |
| [54] | KLIMAS D A, FRAZEE B R. Lead-free glass frit compositions[P]. US Patent:4970178, 1989-08-14. |
| [55] | MERIGAUD B. Zinc-containing lead and cadmium-free glass frits method of their production and their use[P]. US Patent:5342810, 1994-08-30. |
| [56] | NAUMANN K, WINKLER T, WOELFEL U, et al. Lead-free bismuth-containing silicate glasses and uses thereof[P]. US Patent:6403507, 2002-06-11. |
| [57] | RODEK E, KIEFER W, SIEBERS F. Lead-and cadmium-free glass composition for glazing, enameling and decorating glass[P]. US Patent:5633090, 1997-05-27. |
| [58] | 田英良, 孙诗兵. 新编玻璃工艺学[M]. 北京:中国轻工业出版社, 2009. |
| [59] | 赵彦钊, 殷海荣. 玻璃工艺学[M]. 北京:化学工业出版社,2006. |
| [60] | SHAABAN E R, SHAPAAN M, SADDEEK Y B. Structural and thermal stability criteria of Bi2O3-B2O3 glasses[J]. Journal of Physics:Condensed Matter, 2008, 20(15) :155108. |
| [61] | BECKER P. Thermal and optical properties of glasses of the system Bi2O3-B2O3[J]. Crystal Research and Technology, 2003, 38(1) :74-82. |
| [62] | CHENG Y, XIAO H N, GUO W M. Influences of La3+ and Er3+ on structure and properties of Bi2O3-B2O3 glass[J]. Ceramics International, 2008, 34(5) :1335-1339. |
| [63] | SINGH S P, KARMKAR B. Synthesis and characterization of low softening point high Bi2O3 glasses in the K2O-B2O3-Bi2O3 system[J]. Materials Characterization, 2011, 62(6) :626-634. |
| [64] | QIAO W, CHEN P. Study on the properties of Bi2O3-B2O3-BaO lead-free glass using in the electronic pastes[J]. Glass Physics and Chemistry, 2010, 36(3) :304-308. |
| [65] | YU L A, DU J P, HAN M F, et al. Structure and sealing properties of Bi2O3-BaO-SiO2-RxOy glass[J]. Journal of University of Science and Technology Beijing, 2012, 33(12) :1529-1533. 于立安, 杜俊平, 韩敏芳, 等. Bi2O3-BaO-SiO2-RxOy玻璃的结构及其封接性能[J]. 北京科技大学学报, 2012, 33(12) :1529-1533. |
| [66] | HE F, TAN G J, CHENG J S, et al. Research on the characteristic of Bi2O3-ZnO-B2O3 system low-melting sealing glass[J]. Journal of Wuhan University of Technology, 2009, 31(11) :16-19. 何峰, 谭刚健, 程金树, 等. Bi2O3-ZnO-B2O3低熔点封接玻璃的性能研究[J]. 武汉理工大学学报, 2009, 31(11) :16-19. |
| [67] | HE F,WANG J,DENG D W, et al. Sintering behavior of Bi2O3-ZnO-B2O3 system low-melting sealing glass[J]. Journal of the Chinese Ceramic Society, 2009, 37(10) :1791-1795. 何峰, 王俊, 邓大伟, 等. Bi2O3-ZnO-B2O3低熔点封接玻璃的烧结特性[J]. 硅酸盐学报, 2009, 37(10) :1791-1795. |
| [68] | HE F, CHENG J S, DENG D W, et al. Structure of Bi2O3-ZnO-B2O3 system low-melting sealing glass[J]. Journal of Central South University of Technology, 2010, 17:257-262. |
| [69] | HE F, WANG J, DENG D W. Effect of Bi2O3 on structure and wetting studies of Bi2O3-ZnO-B2O3 glasses[J]. Journal of Alloys, 2011, 509(21) :6332-6336. |
| [70] | BALE S, RAHMANS, AWASTHI A M, et al. Role of Bi2O3 content on physical, optical and vibrational studies in Bi2O3-ZnO-B2O3 glasses[J]. Journal of Alloys and Compounds, 2008, 460(1) :699-703. |
| [71] | DONG F H, XIA X F, HE Y F, et al. Effect of Bi2O3 contents on electronic properties and structure of electronic glass[J]. Electronic Components and Materials, 2009, 27(8) :33-35. 董福惠, 夏秀峰, 贺雅飞, 等. Bi2O3含量对电子玻璃电性能及结构的影响[J]. 电子元件与材料, 2009, 27(8) :33-35. |
| [72] | LI Z,ZHU X, FENG S. Research on preparation and performance for lead-free glass used for glass-to-titanium and titanium alloy seals[J]. Titanium, 2013, 30(1) :35-37. 李赞, 朱训, 冯生. 钛及钛合金封接用无铅玻璃的制备及封接性能初探[J]. 钛工业进展, 2013, 30(1) :35-37. |
| [73] | HAN M F, DU J P. Properties of Bi2O3-BaO-SiO2-RxOy glass with MgO-Filler composite sealant[J]. Journal of the Chinese Ceramic Society, 2011, 39(7) :1102-1107. 韩敏芳, 杜俊平. Bi2O3-BaO-SiO2-RxOy 玻璃封接材料性能[J]. 硅酸盐学报, 2011, 39(7) :1102-1107. |
| [74] | HAN M F, DU J P, YU L A. Properties of Bi2O3-BaO-SiO2-RxOy glass with ZrO2-filler composite sealant[J]. Journal of Inorganic Mateials, 2010, 25(10) :1058-1064. 韩敏芳, 杜俊平, 于立安. 氧化锆复合Bi2O3-BaO-SiO2-RxOy 玻璃封接材料性能研究[J]. 无机材料学报, 2010, 25(10) :1058-1064. |
| [75] | YU L A, TONG J J, HAN M F. Sealing properties of SOFC stack sealed by mica and glass composite[J]. Journal of Materials Science and Engineering, 2012, 30(2) :172-175. 于立安, 童菁菁, 韩敏芳. 玻璃和云母复合封接SOFC电池堆性能[J].材料科学与工程学报, 2012, 30(2) :172-175. |
| [76] | GARBARCZYK J E, JOZWIAK P, WASIUCIONEK M, et al. Nanocrystallization as a method of improvement of electrical properties and thermal stability of V2O5-rich glasses[J]. Journal of Power Sources, 2007, 173(2) :743-747. |
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