Novelty phase synthesis mechanism and morphology in resin-bonded Al-Al₂O₃-TiO₂ composites at high temperatures under flowing N₂

Abstract

An Al-AlN core-shell structure is beneficial to the performance of Al-Al₂O₃ composites. In this paper, the phase evolution and microstructure of Al-Al₂O₃-TiO₂ composites at high temperatures in flowing N₂ were investigated after the Al-AlN core-shell structure was created at 853 K for 8 h. The results show that TiO₂ can convert Al into Al₃Ti (~1685 K), which reduces the content of metal Al and rearranges the structure of the composite. Under N₂ conditions, Al₃Ti is further transformed into a novelty non-oxide phase, TiCN. The transformation process can be expressed as follows: Al₃Ti reacts with C and other carbides (Al₄C₃ and Al₄O₄C) to form TiC _x (x < 1). As the firing temperature increases, Al₃Ti transforms into a liquid phase and produces Ti(g) and TiO(g). Finally, Ti(g) and TiO(g) are nitrided and solid-dissolved into the TiC _x crystals to form a TiCN solid solution.

Keywords

aluminum / titanium oxide / alloys / titanium carbonitride

References

[1] Ewais EMM. Carbon based refractories. J. Ceram. Soc. Jpn., 2004, 112, 517.

[2] Zhu TB, Li YW, Sang SB, Xie ZP. Improved thermal shock resistance of magnesia-graphite refractories by the addition of MgO-C pellets. Mater. Des., 2017, 124, 16.

[3] Yang W, Wang XH, Zhang LF, Shan QL, Liu XF. Cleanliness of low carbon aluminum-killed steels during secondary refining processes. Steel Res. Int., 2013, 84, 473.

[4] Ma CH, Li Y, Yan MW, Sun Y, Sun JL. Investigation on a postmortem resin-bonded Al-Si-Al₂O₃, sliding gate with functional gradient feature. Ceram. Int., 2018, 44, 6384.

[5] Atzenhofer C, Gschiel S, Harmuth H. Phase formation in Al₂O₃-C refractories with Al addition. J. Eur. Ceram. Soc., 2016, 37, 1805.

[6] Jiang P, Sun JL, Xue WD, Chen JH, Kumar RV, Li Y. New synthetic route to Al₄O₄C reinforced Al-Al₂O₃ composite materials. Solid State Sci., 2015, 46, 33.

[7] Yan MW, Li Y, Li HY, Sun JL. Theoretical analysis and synthesis of Al₄O₄C and Al₂CO phase in the resin bonded Al-Al₂O₃ refractory in N₂-flowing. Ceram. Int., 2017, 44, 1493.

[8] Zhang S, Yamaguchi A. Hydration resistances and reactions with CO of Al₄O₄C and Al₂OC formed in carbon-containing refractories with Al. J. Ceram. Soc. Jpn., 1996, 104, 393.

[9] Qiu CA, Metselaar R. Thermodynamic evaluation of the Al₂O₃-Al₄C₃ system and stability of Al-oxycarbides. Z. Metallkd., 1995, 86, 198

[10] Amma EL, Jeffrey GA. Structure of aluminum oxycarbide Al₂OC: a short-range wurtzite super-structure. J. Chem. Phys., 1961, 34, 252.

[11] Lihrmann JM, Tirlocq J, Descamps P, Cambier F. Thermodynamics of the Al-C-O system and properties of SiC-AlN-Al₂OC composites. J. Eur. Ceram. Soc., 1999, 19, 2781.

[12] Lihrmann JM. Thermodynamics of the Al₂O₃-Al₄C₃ system: I. Thermochemical functions of Al oxide, carbide and oxycarbides between 298 and 2100 K. J. Eur. Ceram. Soc., 2008, 28, 633.

[13] Lihrmann JM. Thermodynamics of the Al₂O₃-Al₄C₃ system: II. Free energies of mixing, solid solubilities and activities. J. Eur. Ceram. Soc., 2008, 28, 643.

[14] Lihrmanm JM. Thermodynamics of the Al₂O₃-Al₄C₃ system: III. Equilibrium vapour pressures and activation energies for volatilization. J. Eur. Ceram. Soc., 2008, 28, 649.

[15] Lihrmann JM, Zambetakis T, Daire M. High-temperature behavior of the aluminum oxycarbide Al₂OC in the system Al₂O₃-Al₄C₃ and with additions of aluminum nitride. J. Am. Ceram. Soc., 1989, 72, 1704.

[16] Kuo SY, Virkar AV. Phase equilibria and phase transformation in the aluminum nitride-aluminum oxycarbide pseudobinary system. J. Am. Ceram. Soc., 1989, 72, 540.

[17] Motzfeldt K. Comment on “Thermodynamics of the Al-C-O ternary system”. J. Electrochem. Soc., 2007, 154, S1.

[18] Cheng K, Yu C, Ding J, Deng CJ, Zhu HX, Xue ZL. Synthesis and characterization of AlN whiskers by nitridation of Al₄O₄C. J. Alloys Compd., 2017, 719, 308.

[19] Cheng K, Deng CJ, Ding J, Yu C, Zhu HX. Synthesis of Al₂O₃ nanowires by heat-treating Al₄O₄C in a carbon-containing environment. Ceram. Int., 2017, 44, 4996.

[20] Li YB, Bando Y, Golberg D. Single-crystalline α-Al₂O₃ nanotubes converted from Al₄O₄C nanowires. Adv. Mater., 2005, 17, 1401.

[21] Zhu HG, Jiang YL, Yao YQ, Song JZ, Li JL, Xie ZH. Reaction pathways, activation energies and mechanical properties of hybrid composites synthesized in-situ from Al-TiO₂-C powder mixtures. Mater. Chem. Phys., 2012, 137, 532.

[22] Xia TD, Liu TZ, Zhao WJ, Ma BY, Wang TM. Self-propagating high-temperature synthesis of Al₂O₃-TiC-Al composites by aluminothermic reactions. J. Mater. Sci., 2001, 36, 5581.

[23] Ahmed YMZ, Zaki ZI, Besisa DHA, Amin AMM, Bordia RK. Effect of zirconia and iron on the mechanical properties of Al₂O₃/TiC composites processed using combined self-propagating synthesis and direct consolidation technique. Mater. Sci. Eng. A, 2017, 696, 182.

[24] Hajalilou A, Hashim M, Nahavandi M, Ismail I. Mechanochemical carboaluminothermic reduction of rutile to produce TiC-Al₂O₃, nanocomposite. Adv. Powder Technol., 2014, 25, 423.

[25] Yamanoglu R, Gulsoy N, Olevsky EA, Gulsoy HO. Production of porous Ti₅Al_2.5Fe alloy via pressureless spark plasma sintering. J. Alloys Compd., 2016, 680, 654.

[26] Rajabi A, Ghazali MJ, Daud AR. Chemical composition, microstructure and sintering temperature modifications on mechanical properties of TiC-based cermet-A review. Mater. Des., 2015, 67, 95.

[27] Yan MW, Li Y, Wang JJ, Li HY, Sun Y, Ma CH. Phase evolution mechanism of non-oxide bonded Al-Al₂O₃-MgO-ZrO₂ composites at 1873K in flowing nitrogen. J. Am. Ceram. Soc., 2017, 101, 2162.

[28] Kattner UR, Lin JC, Chang YA. Thermodynamic assessment and calculation of the Ti-Al system. Metall. Trans. A, 1992, 23, 2081.

[29] Mirjalili M, Soltanieh M, Matsuura K, Ohno M. On the kinetics of TiAl₃ intermetallic layer formation in the titanium and aluminum diffusion couple. Intermetallics., 2013, 32, 297.

[30] Sujata M, Bhargava S, Sangal S. On the formation of TiAl₃ during reaction between solid Ti and liquid Al. J. Mater. Sci. Lett., 1997, 16, 1175

[31] Mehrizi MZ, Beygi R, Eisaabadi G. Synthesis of Al/TiC-Al₂O₃ nanocomposite by mechanical alloying and subsequent heat treatment. Ceram. Int., 2016, 42, 8895.

[32] Chase MW Jr. NIST-JANAF Thermochemical Tables, 1998, 4th, Washington DC, American Chemical Society and the American Institute of Physics for the National Institute of Standards and Technology

[33] Qin YF, Zheng GF, Zhu LY, He JN, Zhang FY, Dong YC, Yin FC. Structure and wear characteristics of TiCN nanocomposite coatings fabricated by reactive plasma spraying. Surf. Coat. Technol., 2018, 342, 137.

[34] Kostov A, Friedrich B, Zivkovic D. Predicting thermodynamic properties in Ti-Al binary system by FactSage. Comput. Mater. Sci., 2006, 37, 355.

[35] Ashley NJ, Grimes RW, McClellan KJ. Accommodation of non-stoichiometry in TiN_1-x, and ZrN_1-x. J. Mater. Sci., 2007, 42, 1884.

[36] Dridi Z, Bouhafs B, Ruterana P, Aourag H. First-principles calculations of vacancy effects on structural and electronic properties of TiC_x and TiN_x. J. Phys. Condens. Matter, 2002, 14, 10237.