High Thermal Conductivity of Diamond/Al Composites via High Pressure and High Temperature Sintering
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摘要: 以纯铝为基体，使用体积分数为50%的200 μm镀钛金刚石为填充材料，利用高温高压粉末冶金法在压力3 GPa、温度700 ℃条件下烧结10 min得到热导率为529 W/（m·K）的高导热金刚石/铝复合材料。通过光学显微镜和X射线衍射对镀钛金刚石的形貌和物性进行表征，并利用激光导热仪、扫描电镜和热膨胀仪对制备的金刚石/铝复合材料进行性能测试。研究发现，使用放电等离子体烧结制备的镀钛金刚石镀层成分主要是单质钛，并伴有少量碳化钛生成。通过对比在相同制备条件下没有经过镀覆处理的金刚石发现，使用镀钛金刚石能够有效提高金刚石/铝复合材料的热导率。同时，高温高压法能够制备全密度的金刚石/铝复合材料，有效提高铝基体与金刚石的界面结合，减少界面空隙，进而有效提高复合材料的热导率。相比真空热压、放电等离子体烧结、气压熔渗等常规方式，高温高压粉末冶金制备方式具有样品制备周期短（数分钟）的特点。此项研究有助于拓宽高导热复合材料的制备方式，同时能够扩大国内六面顶压机的产品种类，为其他金属基体导热复合材料的制备提供技术支持。Abstract: Diamond/aluminum composites with a high thermal conductivity of 529 W/（m·K） were prepared using pure aluminum as the matrix and 50 vol.% Ti-coated 200 μm diamond as the filling material within10 min by high temperature (700 ℃) and high pressure (3 GPa) powder metallurgy method. The morphology and properties of Ti-coated diamond were characterized by optical microscope and X-ray diffraction. The properties of the prepared diamond/aluminum composite were tested by laser thermal diffusion instrument, scanning electron microscope and thermal expansion instrument. It is found that the Ti-coating diamond prepared by spark plasma sintering is mainly composed of titanium and a small amount of titanium carbide. Compared with raw diamond under the same preparation conditions, the Ti-coated diamond could effectively improve the thermal conductivity of diamond/aluminum composites. Meanwhile, the high temperature and high pressure method can be used to prepare the full density of diamond/aluminum composites, which can effectively improve the interface bonding between aluminum matrix and diamond particles, reduce the interface spaces and effectively improve the thermal conductivity of composites. Compared with the conventional methods such as vacuum hot pressing, spark plasma sintering and gas pressure infiltration, the sample preparation period of high temperature and high pressure powder metallurgy is short (several minutes). This research is helpful to expand the preparation method of high thermal conductivity composites, expand the product types of domestic six-sided top press, and provide technical support for the preparation of other metal matrix thermal conductive composites.
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Key words:
- high temperature and high pressure /
- powder metallurgy method /
- composites /
- diamond /
- Ti-coated
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图 1 金刚石（a）、铝粉（b）和钛粉（c）的外观形貌
Figure 1. Morphology of diamond particles (a)，aluminum powders (b) and titanium powders (c)
图 2 金刚石颗粒放电等离子体烧结30 min前（a）、后（b）对比
Figure 2. Optical image comparison before (a) and after (b) diamond particles treatment for 30 min by SPS
图 3 金刚石/铝复合材料实验组装示意图：（a）高压组装块实物，（b）高压组装块示意图，（c）高压设备腔体示意图
Figure 3. Sample assembly for diamond/Al composites under high pressure conditions: (a) high pressure cell for composites fabrication, (b) assembly schematic diagram, (c) schematic diagram of high pressure apparatus
图 5 金刚石颗粒形貌：（a）原材料金刚石，（b）镀钛金刚石，（c）镀钛金刚石扫描电镜图像，（d）镀钛金刚石表面局部放大图像
Figure 5. Morphology of diamond particles: (a) raw diamond，(b) Ti-coated diamond，(c) SEM of Ti-coated diamond，(d) the surface of Ti-coated diamond
图 6 金刚石/铝复合材料断裂面扫描电镜图像：未镀钛金刚石（a）～（b），镀钛金刚石（c）～（d）
Figure 6. SEM images of fracture surfaces of the diamond/Al composites with diamond of un-coated （a），（b）and Ti-coated （c），（d）
图 7 镀钛金刚石/铝复合材料界面扫描电镜结果和元素分布：（a）界面结合部位，（b）铝，（c）金刚石，（d）钛
Figure 7. SEM images of the interface between diamond particles and Al matrix in the diamond/Al composites with Ti-coated on diamond particles：(a) interface area, (b) Al, (c) diamond, (d) Ti
图 8 金刚石/铝复合材料的热学性能：（a）热扩散系数，（b）热导率
Figure 8. Thermal properties of the diamond/Al composites: (a) thermal diffusion coefficient，(b) thermal conductivity
图 9 未镀钛和镀钛制备的金刚石/铝复合材料的变温伸长率（a）和热膨胀系数（b）
Figure 9. Relative elongations （a）and CTEs （b）of diamond/Al composites reinforced with uncoated and Ti-coated diamond particles
表 1 金刚石/铝复合材料的密度和致密度
Table 1. Density and relative density of diamond/Al composites
Diamond type Density of composites/(g·cm−3) Relative density of composites/% Raw 3.06 98.40 Ti-coated 3.11 100.00 
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[1] MOORE A L, SHI L. Emerging challenges and materials for thermal management of electronics [J]. Materials Today, 2014, 17(4): 163–174. doi: 10.1016/j.mattod.2014.04.003 [2] ZWEBEN C. Advances in composite materials for thermal management in electronic packaging [J]. JOM, 1998, 50(6): 47–51. doi: 10.1007/s11837-998-0128-6 [3] JOHNSON W B, SONUPARLAK B. Diamond/Al metal matrix composites formed by the pressureless metal infiltration process [J]. Journal of Materials Research, 1993, 8(5): 1169–1173. doi: 10.1557/JMR.1993.1169 [4] YANG W L, PENG K, ZHOU L P, et al. Finite element simulation and experimental investigation on thermal conductivity of diamond/aluminium composites with imperfect interface [J]. Computational Materials Science, 2014, 83: 375–380. doi: 10.1016/j.commatsci.2013.11.059 [5] ABYZOV A M, KIDALOV S V, SHAKHOV F M. High thermal conductivity composite of diamond particles with tungsten coating in a copper matrix for heat sink application [J]. Applied Thermal Engineering, 2012, 48: 72–80. doi: 10.1016/j.applthermaleng.2012.04.063 [6] HE J S, WANG X T, ZHANG Y, et al. Thermal conductivity of Cu–Zr/diamond composites produced by high temperature-high pressure method [J]. Composites Part B: Engineering, 2015, 68: 22–26. doi: 10.1016/j.compositesb.2014.08.023 [7] MA S D, ZHAO N Q, SHI C S, et al. Mo2C coating on diamond: different effects on thermal conductivity of diamond/Al and diamond/Cu composites [J]. Applied Surface Science, 2017, 402: 372–383. doi: 10.1016/j.apsusc.2017.01.078 [8] TAN Z Q, LI Z Q, FAN G L, et al. Fabrication of diamond/aluminum composites by vacuum hot pressing: process optimization and thermal properties [J]. Composites Part B: Engineering, 2013, 47: 173–180. doi: 10.1016/j.compositesb.2012.11.014 [9] MIZUUCHI K, INOUE K, AGARI Y, et al. Bimodal and monomodal diamond particle effect on the thermal properties of diamond-particle-dispersed Al-matrix composite fabricated by SPS [J]. Microelectronics Reliability, 2014, 54(11): 2463–2470. doi: 10.1016/j.microrel.2014.04.006 [10] CHE Z F, WANG Q X, WANG L H, et al. Interfacial structure evolution of Ti-coated diamond particle reinforced Al matrix composite produced by gas pressure infiltration [J]. Composites Part B: Engineering, 2017, 113: 285–290. doi: 10.1016/j.compositesb.2017.01.047 [11] ZHANG Y, LI W J, ZHAO L L, et al. Optimisation of high thermal conductivity Al/diamond composites produced by gas pressure infiltration by controlling infiltration temperature and pressure [J]. Journal of Materials Science, 2015, 50(2): 688–696. doi: 10.1007/s10853-014-8628-y [12] FANG C, SHEN W X, ZHANG Y W, et al. Si doping effects on the growth of large single-crystal diamond in a Ni-based metal catalyst system under high pressure and high temperature [J]. Crystal Growth & Design, 2019, 19(7): 3955–3961. doi: 10.1021/acs.cgd.9b00355 [13] ZHANG Z F, JIA X P, LIU X B, et al. Synthesis and characterization of a single diamond crystal with a high nitrogen concentration [J]. Chinese Physics B, 2012, 21(3): 038103. doi: 10.1088/1674-1056/21/3/038103 [14] FANG C, ZHANG Y W, SHEN W X, et al. Synthesis and characterization of HPHT large single-crystal diamonds under the simultaneous influence of oxygen and hydrogen [J]. CrystEngComm, 2017, 19(38): 5727–5734. doi: 10.1039/C7CE01349C [15] CHANG R, ZANG J B, WANG Y H, et al. Study of Ti-coated diamond grits prepared by spark plasma coating [J]. Diamond and Related Materials, 2017, 77: 72–78. doi: 10.1016/j.diamond.2017.06.004 [16] EKIMOVE A, SUETIN N V, POPOVICH A F, et al. Thermal conductivity of diamond composites sintered under high pressures [J]. Diamond and Related Materials, 2008, 17(4/5): 838–843. doi: 10.1016/j.diamond.2007.12.051 [17] KIDALOV S V, SHAKHOV F M, VUL A Y. Thermal conductivity of sintered nanodiamonds and microdiamonds [J]. Diamond and Related Materials, 2008, 17(4/5): 844–847. doi: 10.1016/j.diamond.2008.01.091 [18] EKIMOVE A, SUETINN V, POPOVICH A F, et al. Effect of microstructure and grain size on the thermal conductivity of high-pressure-sintered diamond composites [J]. Inorganic Materials, 2008, 44(3): 224–229. doi: 10.1134/S0020168508030035 [19] YOSHIDA K, MORIGAMI H. Thermal properties of diamond/copper composite material [J]. Microelectronics Reliability, 2004, 44(2): 303–308. doi: 10.1016/S0026-2714(03)00215-4 [20] HE J S, ZHANG H L, ZHANG Y, et al. Effect of boron addition on interface microstructure and thermal conductivity of Cu/diamond composites produced by high temperature-high pressure method [J]. Physica Status Solidi A, 2014, 211(3): 587–594. doi: 10.1002/pssa.201330237 [21] CHEN H, JIA C C, LI S J. Effect of sintering parameters on the microstructure and thermal conductivity of diamond/Cu composites prepared by high pressure and high temperature infiltration [J]. International Journal of Minerals, Metallurgy, and Materials, 2013, 20(2): 180–186. doi: 10.1007/s12613-013-0711-x [22] CHU K, JIA C C, LIANG X B, et al. Modeling the thermal conductivity of diamond reinforced aluminium matrix composites with inhomogeneous interfacial conductance [J]. Materials & Design, 2009, 30(10): 4311–4316. doi: 10.1016/j.matdes.2009.04.019 [23] LIANG X B, JIA C C, CHU K, et al. Thermal conductivity and microstructure of Al/diamond composites with Ti-coated diamond particles consolidated by spark plasma sintering [J]. Journal of Composite Materials, 2012, 46(9): 1127–1136. doi: 10.1177/0021998311413689 [24] YAMAMOTO Y, IMAI T, TANABE K, et al. The measurement of thermal properties of diamond [J]. Diamond and Related Materials, 1997, 6(8): 1057–1061. doi: 10.1016/S0925-9635(96)00772-8 [25] TWITCHEN D J, PICKLES C S J, COE S E, et al. Thermal conductivity measurements on CVD diamond [J]. Diamond and Related Materials, 2001, 10(3/4/5/6/7): 731–735. doi: 10.1016/S0925-9635(00)00515-X [26] STONER R J, MARIS H J. Kapitza conductance and heat flow between solids at temperatures from 50 to 300 K [J]. Physical Review B, 1993, 48(22): 16373–16387. doi: 10.1103/PhysRevB.48.16373 [27] 王平平. 金刚石/铝复合材料的界面结构与导热性能 [D]. 哈尔滨: 哈尔滨工业大学, 2017.WANG P P. Interface microstructure and thermal properties of diamond particles reinforced Al matrix composites [D]. Harbin: Harbin Institute of Technology, 2017. [28] 刘永正. 金刚石/铝复合材料影响因素研究 [J]. 超硬材料工程, 2009, 21(5): 15–17. doi: 10.3969/j.issn.1673-1433.2009.05.005LIU Y Z. Research on influencing factors of diamond-aluminium composites [J]. Superhard Material Engineering, 2009, 21(5): 15–17. doi: 10.3969/j.issn.1673-1433.2009.05.005 [29] 郭静, 孙久娜, 孙璐, 等. 铝-金刚石双相连续导热复合材料的制备 [J]. 粉末冶金工业, 2010, 20(3): 17–20. doi: 10.3969/j.issn.1006-6543.2010.03.004GUO J, SUN J N, SUN L, et al. Preparation of Al/diamond composite with consecutive phases [J]. Powder Metallurgy Industry, 2010, 20(3): 17–20. doi: 10.3969/j.issn.1006-6543.2010.03.004 [30] 刘永正, 崔岩. 超高导热金刚石/铝复合材料研究 [C]//第七届中国功能材料及其应用学术会议论文集. 长沙: 中国仪器仪表学会, 2010: 439–441. [31] ARAI S, UEDA M. Fabrication of high thermal conductivity Cu/diamond composites at ambient temperature and pressure [J]. AIP Advances, 2019, 9(8): 085309. doi: 10.1063/1.5111416 [32] 王新宇, 于家康, 朱晓敏. 镀TiC金刚石/铝复合材料的热膨胀性能 [J]. 特种铸造及有色合金, 2011, 31(11): 1046–1049. doi: 10.3870/tzzz.2011.11.019WANG X Y, YU J K, ZHU X M. Thermal expansion behevior of TiC-coated diamond/Al composites [J]. Special Casting & Nonferrous Alloys, 2011, 31(11): 1046–1049. doi: 10.3870/tzzz.2011.11.019 [33] 王一鸣. 金刚石/铝复合材料性能及其影响因素研究 [D]. 北京: 北方工业大学, 2019.WANG Y M. Research on properties and influencing factors of diamond/aluminum composites [D]. Beijing: North China University of Technology, 2019. -
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