Al-Ti合金钎焊SiC陶瓷接头界面微观结构与力学性能

doi:10.15541/jim20210652

摘要/Abstract

摘要：

SiC陶瓷具有优异的综合性能, 通过钎焊获得高强度接头是其获得广泛应用的重要前提。研究采用Al-(10, 20, 30, 40)Ti(Ti的名义原子含量10%、20%、30%、40%)系列合金, 在1550 ℃条件下, 对SiC陶瓷进行钎焊30 min。当中间层厚度为~50 μm时, SiC钎焊接头的平均剪切强度处于100~260 MPa范围内。当采用Al-20Ti合金作为钎料时, 随着中间层厚度从~100 μm减小至25 μm, 钎焊接头的平均强度逐渐提高, 且最大强度~315 MPa。同时, 钎焊中间层中(Al)相逐渐减少直至消失, 只留下Al₄C₃、TiC和(Al,Si)₃Ti相。SiC/Al-20Ti/SiC钎焊接头的断裂主要发生在靠近中间层/陶瓷界面位置的陶瓷基体内。

关键词: SiC, 钎焊, 界面, 微结构, 力学性能

Abstract:

SiC ceramic has excellent overall properties, and joining it to other materials with high joint strength is an important issue in the actual applications. Brazing of SiC ceramic to itself was performed using the as-fabricated Al-(10, 20, 30, 40)Ti alloys with nominal Ti concentrations of 10%, 20%, 30%, and 40% at 1550 ℃ × 30 min. The average joint shear strength fluctuates in the range of ~100‒260 MPa with the interlayer thickness of ~50 μm. Moreover, the average strength SiC/Al-20Ti/SiC joint is increased markedly with the interlayer thickness decreasing from ~100 to 25 μm, reaching the maximum of ~315 MPa. Meanwhile, the (Al) phase in the interlayers is reduced gradually till disappear with the thinnest brazing interlayer, leaving the Al₄C₃, TiC and (Al,Si)₃Ti phases in the interlayer. The joint fractures of SiC/Al-20Ti/SiC joint mainly occur in the SiC ceramic substrate near the interlayer/ceramic interface.

Key words: SiC, brazing, interfaces, microstructures, mechanical property

中图分类号:

TG456

徐谱昊, 张相召, 刘桂武, 张明芬, 桂新易, 乔冠军. Al-Ti合金钎焊SiC陶瓷接头界面微观结构与力学性能[J]. 无机材料学报, 2022, 37(6): 683-690.

XU Puhao, ZHANG Xiangzhao, LIU Guiwu, ZHANG Mingfen, GUI Xinyi, QIAO Guanjun. Microstructure and Mechanical Properties of SiC Joint Brazed by Al-Ti Alloys as Filler Metal[J]. Journal of Inorganic Materials, 2022, 37(6): 683-690.

图/表 14

Fig. S1 Schematic of the shear test fixture

Fig. 1 BSE images of four nominal Al-Ti alloys (a) Al-10Ti; (b) Al-20Ti; (c) Al-30Ti; (d) Al-40Ti. The black dots are the diamond particles introduced during the polishing

Fig. 2 XRD patterns of the Al-Ti alloys

Fig. S2 Typical BSE images of Al-(10, 20, 30, 40)Ti alloys and the corresponding elemental mapping

Fig. S3 Typical BSE image of Al-40Ti alloy and the corresponding elemental compositions of the selected area

Fig. 3 Cross-sectional BSE images of SiC/SiC joints brazed using the four nominal Al-Ti alloys (a-h) and corresponding EDS elemental mapping (i) (a, b) Al-10Ti; (c, d) Al-20Ti; (e, f) Al-30Ti; (g, h) Al-40Ti

Table 1 EDS results of partial phases in joint interlayers (atom percent)

Data from	Elemental composition /%				Possible phases
Data from	Ti	Al	C	Si	Possible phases
Fig. 3(b)	0.87	98.04	‒	1.09	(Al)
	55.33	‒	45.67	‒	TiC
	25.85	62.83	‒	11.32	(Al,Si)₃Ti
Fig. 3(d)	‒	98.91	‒	1.09	(Al)
	53.98	0.06	45.11	0.84	TiC
	26.27	59.23	2.47	12.03	(Al,Si)₃Ti
Fig. 3(f)	48.61	1.85	31.39	18.15	Ti₃Si(Al)C₂
Fig. 3(h)	50.29	1.26	30.42	18.03	Ti₃Si(Al)C₂

Fig. S4 Cross-sectional BSE image of the SiC/Al-30Ti/SiC joint brazed at 1550 ℃ × 30 min and the corresponding elemental mappings

Fig. 4 Cross-sectional BSE images of SiC/Al-20Ti/SiC joints brazed with interlayers of different thickness (a) ~25 μm; (b) 50 μm; (c) 70 μm; (d) 100 μm

Fig. 5 Interfacial (a) TEM and (b?f) HRTEM images of SiC/Al-20Ti/SiC joint sample with interlayer thickness of ~25 μm and the corresponding (g?i) SAED patterns

Fig. S5 Interfacial TEM image of SiC/Al-20Ti/SiC joint sample and the corresponding elemental mappings

Fig. 6 Variations of joint shear strength with (a) Ti concentration of Al-Ti alloys and (b) interlayer thickness of Al-20Ti alloy

Fig. 7 Typical fracture surface morphologies of SiC/SiC joints brazed using different nominal Al-Ti alloys (a, b) Al-10Ti; (c, d) Al-20Ti; (e, f) Al-30Ti ; (g, h) Al-40Ti

Fig. 8 XRD patterns of fracture surfaces of SiC/SiC joints brazed using various nominal Al-Ti alloys

参考文献 37

[1]	LIU G W, ZHANG X Z, YANG J, et al. Recent advances in joining of SiC-based materials (monolithic SiC and SiC_f/SiC composites): joining processes, joint strength, and interfacial behavior. Journal of Advanced Ceramics, 2019, 8(1): 19-38. DOI URL
[2]	ZHAO S, YANG Z C, ZHOU X G. Fracture behavior of SiC/SiC composites with different interfaces. Journal of Inorganic Materials, 2016, 31(1): 58-62. DOI URL
[3]	FERNIE J, DREW R, KNOWLES K. Joining of engineering ceramics. International Materials Reviews, 2009, 54: 283-331. DOI URL
[4]	YOON D H, REIMANIS I E. A review on the joining of SiC for high-temperature applications. Journal of the Korean Ceramic Society, 2020, 57(5): 246-270. DOI URL
[5]	VALENZA F, GAMBARO S, MUOLO M L, et al. Wetting of SiC by Al-Ti alloys and joining by in-situ formation of interfacial Ti₃Si(Al)C₂. Journal of the European Ceramic Society, 2018, 38(11): 3727-3734. DOI URL
[6]	LIU Y, HUANG Z R, LIU X J. Joining of sintered silicon carbide using ternary Ag-Cu-Ti active brazing alloy. Ceramics International, 2009, 35(8): 3479-3484. DOI URL
[7]	XIONG H P, WEI M, XIE Y H, et al. Control of interfacial reactions and strength of the SiC/SiC joints brazed with newly- developed Co-based brazing alloy. Journal of Materials Research, 2007, 22(10): 2727-2736. DOI URL
[8]	KOLTSOV A, HODAJ F, EUSTATHOPOULOS N. Brazing of AlN to SiC by Pr silicides: physicochemichal aspects. Materials Science and Engineering: A, 2008, 495(1/2): 259-264. DOI URL
[9]	RICCARDI B, NANNETTI C A, WOLTERSDORF J, et al. Joining of SiC based ceramics and composites with Si-16Ti and Si-18Cr eutectic alloys. International Journal of Materials & Product Technology, 2004, 20(5): 440-451.
[10]	ZHAO S T, ZHAGN X Z, LIU G W, et al. Surface metallization of SiC ceramic by Mo-Ni-Si coatings for improving its wettability by molten Ag. Rare Metal Materials and Engineering, 2018, 47(3): 759-765. DOI URL
[11]	LIU G W, MUOLO M L, VALENZA F, et al. Survey on wetting of SiC by molten metals. Ceramics International, 2010, 36(4): 1177-1188. DOI URL
[12]	ZHAO H T, HUANG J H, ZHANG H, et al. Vacuum brazing of Si/SiC ceramic and low expansion titanium alloy by using Cu-Ti fillers. Rare Metal Materials and Engineering, 2007, 36(12): 2184-2188.
[13]	LI J K, LIU L, LIU X. Joining of SiC ceramic by 22Ti-78Si high- temperature rutectic brazing alloy. Journal of Inorganic Materials, 2011, 26(12): 1314-1318. DOI URL
[14]	FU W, SONG X G, TIAN R C, et al. Wettability and joining of SiC by Sn-Ti: Microstructure and mechanical properties. Journal of Materials Science and Technology, 2020, 40: 15-23. DOI URL
[15]	XU P H, GUI X Y, ZHANG X Z, et al. Wetting and interfacial behavior of Al-Ti/4H-SiC system: A combined study of experiment and DFT simulation. Ceramics International, 2021, 47: 69-77.
[16]	HAO Z T, WANG D P, YANG Z W, et al. Microstructural evolution and mechanical properties of FeNi₄₂alloy and SiC ceramic joint vacuum brazed with Ag-based filler metals. Ceramics International, 2020, 46(8): 12795-12805. DOI URL
[17]	PRAKASH P, MOHANDAS T, RAJU P D. Microstructural characterization of SiC ceramic and SiC-metal active metal brazed joints. Scripta Materialia, 2005, 52(11): 1169-1173. DOI URL
[18]	TIAN W B, SUN Z M, ZHANG P, et al. Brazing of silicon carbide ceramics with Ni-Si-Ti powder mixtures. Journal of the Australian Ceramic Society, 2017, 53(2): 511-516. DOI URL
[19]	SUDMEYER I, HETTESHEIMER T, ROHDE M. On the shear strength of laser brazed SiC-steel joints: effects of braze metal fillers and surface patterning. Ceramics International, 2010, 36(3): 1083-1090. DOI URL
[20]	CHEN Z B, HU S P, SONG X G, et al. Brazing of SiC ceramics pretreated by chromium coating using inactive AgCu filler metal. International Journal of Applied Ceramic Technology, 2020, 17(6): 2591-2597. DOI URL
[21]	LIU Y, ZHU Y Z, YANG Y, et al. Microstructure of reaction layer and its effect on the joining strength of SiC/SiC joints brazed using Ag-Cu-In-Ti alloy. Journal of Advanced Ceramics, 2014, 3(1): 71-75. DOI URL
[22]	MOSZNER F, MATA-OSORO G, CHIODI M, et al. Mechanical behavior of SiC joints brazed using an active Ag-Cu-In-Ti braze at elevated temperatures. International Journal of Applied Ceramic Technology, 2017, 14(4): 703-711. DOI URL
[23]	HE H M, LU C Y, HE H M, et al. Characterization of SiC ceramic joints brazed using Au-Ni-Pd-Ti high-temperature filler alloy. Materials, 2019, 12(6): 931. DOI URL
[24]	QIN Q, ZHANG J, LU CJ, et al. Microstructure and mechanical properties of the SiC/Zr₄ joints brazed with TiZrNiCu filler for nuclear application. Progress in Natural Science-Materials International, 2018, 28(3): 124-131.
[25]	XIONG H P, WEI M, XIE Y H, et al. Brazing of SiC to a wrought nickel-based superalloy using CoFeNi(Si, B)CrTi filler metal. Materials Letters, 2007, 61(25): 4662-4665. DOI URL
[26]	SONG X G, CHEN Z B, HU S P, et al. Wetting behavior and brazing of titanium-coated SiC ceramics using Sn_0.3Ag_0.7Cu filler. Journal of the American Ceramic Society, 2019, 103(2): 912-920. DOI URL
[27]	CHEN Z B, BIAN H, NIU C N, et al. Titanium-deposition assisted brazing of SiC ceramics using inactive AgCu filler. Materials Characterization, 2018, 142: 219-222. DOI URL
[28]	DAI X Y, CAO J, CHEN Z, et al. Brazing SiC ceramic using novel B4C reinforced Ag-Cu-Ti composite filler. Ceramics International, 2016, 42(5): 6319-6328. DOI URL
[29]	LIU Y, QI Q, ZHU Y, et al. Microstructure and joining strength evaluation of SiC/SiC joints brazed with SiC_p/Ag-Cu-Ti hybrid tapes. Journal of Adhesion Science and Technology, 2015, 29(15): 1563-1571. DOI URL
[30]	LI Z, WEI R W, WEN Q, et al. Microstructure and mechanical properties of SiC ceramic joints vacuum brazed with in-situ formed SiC particulate reinforced Si-24Ti alloy. Vacuum, 2019, 173: 109160. DOI URL
[31]	ZHONG Z H, HOU G X, ZHU Z X, et al. Microstructure and mechanical strength of SiC joints brazed with Cr₃C₂ particulate reinforced Ag-Cu-Ti brazing alloy. Ceramics International, 2018, 44(10): 11862-11868. DOI URL
[32]	SONG Y Y, LIU D, HU S P, et al. Graphene nanoplatelets reinforced AgCuTi composite filler for brazing SiC ceramic. Journal of the European Ceramic Society, 2019, 39(4): 696-704. DOI URL
[33]	ZHOU X B, LI Y B, LI Y F, et al. Residual thermal stress of SiC/Ti₃SiC₂/SiC joints calculation and relaxed by post-annealing. International Journal of Applied Ceramic Technology, 2018, 15: 1157-1165. DOI URL
[34]	ZHOU X B, HAN Y H, SHEN X F, et al. Fast joining SiC ceramics with Ti₃SiC₂ tape film by electric field-assisted sintering technology. Journal of Nuclear Materials, 2015, 466: 322-327. DOI URL
[35]	YANG D X, ZHOU Y, YAN X H, et al. Highly conductive wear resistant Cu/Ti₃SiC₂(TiC/SiC) co-continuous composites via vacuum infiltration process. Journal of Advanced Ceramics, 2020, 9(1): 83-93. DOI URL
[36]	ZHANG X Z, LIU G W, TAO J N, et al. Brazing of WC-8Co cemented carbide to steel using Cu-Ni-Al alloys as filler metal: microstructures and joint mechanical behavior. Journal of Materials Science and Technology, 2018, 34(7): 1180-1188. DOI URL
[37]	ZHOU X B, JING L, KWON Y D, et al. Fabrication of SiC_w/Ti₃SiC₂ composites with improved thermal conductivity and mechanical properties using spark plasma sintering. Journal of Advanced Ceramics, 2020, 9(4): 462-470. DOI URL