Abstract
Graphite/aluminum nitride (AlN) multiphase ceramics are pressureless sintered under 1850 °C using Dy2O3 and CaF2 as sintering additives. The effects of added graphite on microstructure, thermal conductivity, and electrochemical impedance spectroscopy of AlN ceramics were investigated. It was found that with 1wt% graphite addition the thermal conductivity of AlN in the through-plane to can achieve 210 W/(m K), which 25% higher than that of AlN without graphite. The graphite addition eliminates the oxygen impurity in AlN by a carbon reduction reaction in form of nanosized Dy2O3 particles. From electrochemical impedance spectroscopy manifested that the activation energy (Ea,g) of samples in grains is increased from 0.784 to 1.112 eV, suggesting that the concentrations of defects and impurities of Graphite/AlN multiphase ceramics are lower than those of monophase AlN ceramics.
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References
X. Jing, Y. Li, J. Zhu, L. Chang, S. Maganti, N. Naik, B. Xu, V. Murugadoss, M. Huang, Z. Guo, Improving thermal conductivity of polyethylene/polypropylene by styrene-ethylene-propylene-styrene wrapping hexagonal boron nitride at the phase interface. Adv. Compos. Hybrid Mater. (2022). https://doi.org/10.1007/s42114-022-00438-x
X. Hu, H. Wu, X. Lu, S. Liu, J. Qu, Improving thermal conductivity of ethylene propylene diene monomer/paraffin/expanded graphite shape-stabilized phase change materials with great thermal management potential via green steam explosion. Adv. Compos. Hybrid Mater. 4, 478–491 (2021). https://doi.org/10.1007/s42114-021-00300-6
D. Pan, J. Dong, G. Yang, F. Su, B. Chang, C. Liu, Y. Zhu, Z. Guo, Ice template method assists in obtaining carbonized cellulose/boron nitride aerogel with 3D spatial network structure to enhance the thermal conductivity and flame retardancy of epoxy-based composites. Adv. Compos. Hybrid Mater (2021). https://doi.org/10.1007/s42114-021-00362-6
J. Yu, Y. Zhang, Q. Guo, H. Hou, Y. Ma, Y, Zhao, Effect of pressure on anisotropy in elasticity, sound velocity, and thermal conductivity of vanadium borides. Adv. Compos. Hybrid Mater. (2022). https://doi.org/10.1007/s42114-021-00403-0
S. Baskut, A. Cinar, S. Turan, Directional properties and microstructures of spark plasma sintered aluminum nitride containing graphene platelets. J. Eur. Ceram. Soc. 37, 3759–3772 (2017). https://doi.org/10.1016/j.jeurceramsoc.2017.03.032
Q. Li, Z. Wang, C. Wu, X. Cheng, Microstructure and mechanical properties of aluminum nitride co-doped with cerium oxide via hot-pressing sintering. J. Alloy Compd. 640, 275–279 (2015). https://doi.org/10.1016/j.jallcom.2015.03.235
Y. Xiong, H. Wang, Z. Fu, Transient liquid-phase sintering of AlN ceramics with CaF2 additive. J. Eur. Ceram. Soc. 33, 2199–2205 (2013). https://doi.org/10.1016/j.jeurceramsoc.2013.03.024
C. Wang, C.Q. Peng, R.C. Wang, K. Yu, C. Li, Typical properties and preparation technologies of AlN packaging material. Chin. J. Nonferrous. Met. 7, 1729–1738 (2007)
A. Christensen, S. Graham, Thermal effects in packaging high power light emitting diode arrays. Appl. Therm. Eng. 29, 364–371 (2009). https://doi.org/10.1016/j.applthermaleng.2008.03.019
G.A. Slack, Nonmetallic crystals with high thermal conductivity. J. Phys. Chem. Solids. 34, 321–335 (1973). https://doi.org/10.1016/0022-3697(73)90092-9
G.A. Slack, T.F. McNelly, Growth of high purity AlN crystals. J. Cryst. Growth. 34, 263–279 (1976). https://doi.org/10.1016/0022-0248(76)90139-1
G.A. Slack, R.A. Tanzilli, R.O. Pohl, J.W. Vandersande, The intrinsic thermal conductivity of AIN. J. Phys. Chem. Solids. 48, 641–647 (1987). https://doi.org/10.1016/0022-3697(87)90153-3
R.R. Lee, Development of high thermal conductivity aluminum nitride ceramic. J. Am. Ceram. Soc. 74, 2242–2249 (1991). https://doi.org/10.1111/j.1151-2916.1991.tb08291.x
T. Sakai, M. Iwata, Effect of oxygen on sintering of AlN. J. Mater. Sci. 12, 1659–1665 (1977). https://doi.org/10.1007/BF00542817
T. Sakai, Effect of the oxygen impurity on the sintering and the thermal conductivity of AlN polycrystal. J. Ceram. Soc. Jpn. 86, 174 (1978). https://doi.org/10.2109/jcersj1950.86.992_174
W.J. Tseng, C.J. Tsai, Microporous layer structure in oxidized aluminium nitride polycrystals. J. Mater. Process. Technol. 146, 289–293 (2004). https://doi.org/10.1016/j.jmatprotec.2003.11.008
B. Abeles, Lattice thermal conductivity of disordered semiconductor alloys at high temperatures. Phys. Rev. 131, 1906 (1963). https://doi.org/10.1103/PhysRev.131.1906
N. Seiji, S. Kouichi, M. Takahiro, A. Yamakawa, Diffraction method detection of local lattice distortion in AIN ceramics by convergent beam electron. J. Am. Ceram. Soc. 78, 830–832 (1995). https://doi.org/10.1111/j.1151-2916.1995.tb08258.x
D.L. Callahan, Comment on “Diffraction method detection of local lattice distortion in AIN ceramics by convergent beam electron.” J. Am. Ceram. Soc. 79, 1982–1983 (1996). https://doi.org/10.1111/j.1151-2916.1996.tb08025.x
L. Qiao, H. Zhou, K. Chen, R. Fu, Effects of Li2O on the low temperature sintering and thermal conductivity of AlN ceramics. J. Eur. Ceram. Soc. 23, 1517–1524 (2003)
Y. Ru, Q. Jie, L. Min, L. Guoqaing, Synthesis of yttrium aluminum garnet (YAG) powder by homogeneous precipitation combined with supercritical carbon dioxide or ethanol fluid drying. J. Eur. Ceram. Soc. 28, 2903–2914 (2008). https://doi.org/10.1016/j.jeurceramsoc.2008.05.005
G. Pezzotti, A. Nakahira, M. Tajika, Effect of extended annealing cycles on the thermal conductivity of AlN/Y2O3 ceramics. J. Eur. Ceram. Soc. 20, 1319–1325 (2000)
F.M. Xu, Z.J. Zhang, X.L. Shi, Y. Tan, J.M. Yang, Effects of adding yttrium nitrate on the mechanical properties of hot-pressed AlN ceramics. J. Alloy Compd. 509, 8688–8691 (2011). https://doi.org/10.1016/j.jallcom.2011.05.110
G. Lai, Y. Nagai, Effect of oxygen on sintering of aluminium nitride with Y2O3 sintering aid. J. Ceram. Soc. Jpn. 103, 6–10 (1995). https://doi.org/10.2109/jcersj.103.6
Y. Xiong, Z.Y. Fu, H. Wang, Y.C. Wang, Q.J. Zhang, Microstructure and IR transmittance of spark plasma sintering translucent AlN ceramics with CaF2 additive. Mater. Sci. Eng. B 123, 57–62 (2005). https://doi.org/10.2109/jcersj.103.6
T.B. Jackson, A.V. Virkar, K.L. More, R.B.D. Jr., R.A. Cutler, High‐thermal‐conductivity aluminum nitride ceramics: the effect of thermodynamic, kinetic, and microstructural factors, J. Am. Ceram. Soc. 80, 1421–1435 (1997). https://doi.org/10.1111/j.1151-2916.1997.tb03000.x
Z. Fang, Y. Liu, Y. Wu, H. Zhou, Microstructure and dielectric dispersion of low-temperature sintered AlN microstructure and dielectric dispersion of low-temperature sintered AlN. J. Mater. Sci. Lett. 19, 95–97 (2000). https://doi.org/10.1023/A:1006626825671
S. Kume, M. Yasuoka, S.K. Lee, A. Kan, H. Ogawa, K. Watari, Dielectric and thermal properties of AlN ceramics. J. Eur. Ceram. Soc. 27, 2967–2971 (2007). https://doi.org/10.1016/j.jeurceramsoc.2006.11.023
P.H. Klein, W.J. Croft, Thermal conductivity, diffusivity, and expansion of Y2O3, Y3Al5O12, and LaF3 in the range 77–300 K. J. Appl. Phys. 38, 1603–1607 (1967). https://doi.org/10.1063/1.1709730
Y. Kurokawa, K. Utsumi, H. Takamizawa, Development and microstructural characterization of high-thermal-conductivity aluminum nitride ceramics. J. Am. Ceram. Soc. 71, 588–594 (1988). https://doi.org/10.1111/j.1151-2916.1988.tb05924.x
S.N. Ivanov, P.A. Popov, G.V. Egorov, A.A. Sidorov, B.I. Kornev, L.M. Zhukova, V.P. Ryabov, Thermophysical properties of aluminum nitride ceramic. Phys. Solid State. 39, 81–83 (1997). https://doi.org/10.1134/1.1129837
H. Buhr, G. Müller, Microstructure and thermal conductivity of AlN(Y2O3) ceramics sintered in different atmospheres. J. Eur. Ceram. Soc. 12, 271–277 (1993). https://doi.org/10.1016/0955-2219(93)90102-W
M. Bickermann, B.M. Epelbaum, A. Winnacker, Characterization of bulk AlN with low oxygen content. J. Cryst. Growth. 269, 432–442 (2004). https://doi.org/10.1016/j.jcrysgro.2004.05.071
K. Watari, T. Tsugoshi, H. Nakano, K. Urabe, S. Cao, K. Mori, K. Ishizaki, Microstructure and thermal conductivity of AlN ceramic with eliminated Grain boundary phase. Key. Eng. Mater. 247, 361–364 (2003). https://doi.org/10.4028/www.scientific.net/kem.247.361
K. Watari, A. Tsuzuki, Y. Torii, Effect of rare-earth oxide addition on the thermal conductivity of sintered aluminium nitride. J. Mater. Sci. Lett. 11, 1508–1510 (1992). https://doi.org/10.1007/bf00729274
K. Watari, H. Nakano, K. Urabe, K. Ishizaki, S. Cao, K. Mori, Thermal conductivity of AlN ceramic with a very low amount of grain boundary phase at 4 to 1000 K. J. Mater. Res. 17, 2940–2944 (2002). https://doi.org/10.1557/JMR.2002.0426
H.S. Kim, J.M. Chae, Y.S. Oh, H.T. Kim, K.B. Shim, S.M. Lee, Effects of carbothermal reduction on the thermal and electrical conductivities of aluminum nitride ceramics. Ceram. Int. 36, 2039–2045 (2010). https://doi.org/10.1016/j.ceramint.2010.04.001
H. Jiang, X.H. Wang, W. Lei, G.F. Fan, W.Z. Lu, Effects of two-step sintering on thermal and mechanical properties of aluminum nitride ceramics by impedance spectroscopy analysis. J. Eur. Ceram. Soc. 39, 249–254 (2019). https://doi.org/10.1016/j.jeurceramsoc.2018.09.026
R. Roy, D. Das, P.K. Rout, A review of advanced mullite ceramics. Eng. Sci. (2021). https://doi.org/10.30919/es8d582
H. Yang, Q. Li, Z. Wang, H. Wu, Y. Wu, X. Cheng, Effect of different sintering additives on the microstructure, phase compositions and mechanical properties of Si3N4/SiC. Ceram. ES Mater. Manuf. 15, 65–71 (2021)
H. Wu, Y. Zhong, Y. Tang et al., Precise regulation of weakly negative permittivity in CaCu3Ti4O12 metacomposites by synergistic effects of carbon nanotubes and grapheme. Adv. Compos. Hybrid. Mater. (2021). https://doi.org/10.1007/s42114-021-00378-y
Z. Sun, X. Huang, A. Xia, Z. Yan, L. Qian, Tunable bandwidth of negative permittivity from graphene-silicon carbide ceramics. Eng. Sci. 16, 19–25 (2021). https://doi.org/10.30919/es8d564
H. Yang, Q. Li, Z. Wang, H. Wu, Y. Wu, P. Hou, X. Cheng, Effect of graphene on microstructure and mechanical properties of Si3N4/SiC ceramics. ES. Mater. Manuf. 12, 29–34 (2021). https://doi.org/10.30919/esmm5f418
T. Wang, J. Xie, S. Dai, M. Ding, Y. Wang, Y. Shi, D. Zhou, Y. Shi, Influence of Dy2O3–CaF2 addition on preparation, microstructure and properties of AlN ceramics. J. Chin. Ceram. Soc. 46, 760–765 (2018). https://doi.org/10.14062/j.issn.0454-5648.2018.06.02
K. Chang, W. Feng, L.Q. Chen, Effect of second-phase particle morphology on grain growth kinetics. Acta. Mater. 57, 5229–5236 (2009). https://doi.org/10.1016/j.actamat.2009.07.025
K. Wang, C. Wang, Aluminum-vacancy-related dielectric relaxations in AlN ceramics. J. Am. Ceram. Soc. 101, 2009–2016 (2018). https://doi.org/10.1111/jace.15370
S. Wang, X. Lu, A. Negi, J. He, K. Kim, H. Shao, P. Jiang, J. Liu, Q. Hao, Revisiting the Reduction of Thermal Conductivity in Nano-to Micro-Grained Bismuth Telluride: The Importance of Grain-Boundary Thermal Resistance, Eng. Sci.17, 45–55 (2021)
Y. Zhao, F. Liu, K. Zhu, S. Maganti, Z. Zhao, P. Bai, Three-dimensional printing of the copper sulfate hybrid composites for supercapacitor electrodes with ultra-high areal and volumetric capacitances. Adv. Compos. Hybrid Mater. (2022). https://doi.org/10.1007/s42114-022-00430-5
S. Gao, X. Zhao, Q. Fu et al., Highly transmitted silver nanowires-SWCNTs conductive flexible film by nested density structure and aluminum-doped zinc oxide capping layer for flexible amorphous silicon solar cells. J. Mater. Sci. Technol. 126, 152–160 (2022). https://doi.org/10.1016/j.jmst.2022.03.01
Acknowledgments
The authors acknowledge the Loughborough Materials Characterization Centre (LMCC) for providing the characterization facilities. This work was supported by the Shanghai Municipal Natural Science Foundation, China (Granted No.19ZR1418500).
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Wang, T., Xie, J., Zhang, L. et al. The effect of graphite addition on thermal conductivity, microstructure, and electrochemical impedance spectroscopy of AlN ceramics. Journal of Materials Research 37, 2749–2760 (2022). https://doi.org/10.1557/s43578-022-00633-y
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DOI: https://doi.org/10.1557/s43578-022-00633-y