Formation mechanisms of Ti<sub>2</sub>AlC and Ti<sub>3</sub>AlC during solid-state sintering between multilayer graphene and TiAl alloy composite

Wu Ming-Yu; Mi Guang-Bao; Li Pei-Jie; Huang Xu

doi:10.7498/aps.71.20220845

Abstract

Ti₂AlC and Ti₃AlC formed by the reaction between C and TiAl alloy can improve the plasticity and strength of TiAl alloy respectively. Generally, the peritectic reaction of L + TiC→Ti₂AlC (Ti₃AlC) occurs in the process of liquid-phase sintering, but different formation mechanisms of Ti₂AlC and Ti₃AlC may exist in the solid-state sintering. In this work, multilayer graphene is employed to fabricate the reaction interface with TiAl alloy under 1100–1350 ℃, which is the common solid-state sintering temperature of TiAl alloy. According to the microstructure characterization and analysis, Ti₂AlC and Ti₃AlC are verified to contain no TiC. The interface energy values of TiC/TiAl, Ti₂AlC/TiAl and Ti₃AlC/TiAl are calculated to be about 1.2, 0.87 and 0.39 J·m², respectively, indicating that Ti₂AlC and Ti₃AlC can be formed directly without TiC mesophase. Besides, only Ti₂AlC is observed to be formed at 1150–1250 ℃, while the interface products at 1250–1350 ℃ change into Ti₃AlC with a small amount of Ti₂AlC. The mechanism that the sintering temperature affects the formation tendency of Ti₂AlC and Ti₃AlC can be ascribed to the content of α phase. The TiAl alloy matrix is composed of γ and a few α phases at 1150–1250℃, but almost completely transforms into α phase at 1250–1350 ℃, and the increase in the α content can promote the formation of Ti₃AlC. The above results demonstrate the possibility of regulating the relative content of Ti₂AlC and Ti₃AlC through controlling the sintering temperature, which provides a promising method to improve the plasticity and strength of TiAl alloy.

Keywords:

Authors and contacts

1.
National Center of Novel Materials for International Research, Tsinghua University, Beijing 100084, China
2.
Aviation Key Laboratory of Science and Technology on Advanced Titanium Alloys, AECC Beijing Institute of Aeronautical Materials, Beijing 100095, China
3.
Beijing Engineering Research Center of Graphene and Application, Beijing 100094, China

Corresponding author: Mi Guang-Bao, guangbao.mi@biam.ac.cn

Funds: Project supported by the National Natural Science Foundation of China (Grant No. U2141222) and the Innovation Fund of AECC, China (Grant No. CXPT-2018-36).

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References

[1]	Appel F, Clemens H, Fischer F D 2016 Prog. Mater. Sci 81 55 Google Scholar
[2]	Ouyang P X, Mi G B, Cao J X, Huang X, He L J, Li P J 2018 Mater. Today Comm 16 364 Google Scholar
[3]	Yamaguchi M, Inui H, Ito K 2000 Acta Mater 48 307 Google Scholar
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[7]	Fang H, Chen R, Liu Y, Tan Y Guo J 2019 Intermetallics 115 106630 Google Scholar
[8]	Gouma P I, Mills M J, Kim Y W 1998 Phil. Mag Lett 78 59 Google Scholar
[9]	Wu H, Fan G H, Cui X P, Geng L, Yuan F, Pang J C, Wei L S, Huang M 2013 Mater. Sci. Eng. A 585 439 Google Scholar
[10]	Wu M Y, Mi G B, Li P J, Huang X, Cao C X 2020 J. Aeron. Mater 40 45
[11]	Nieto A, Bisht A, Lahiri D, Zhang C, Agarwal A 2016 Int. Mater. Rev 62 241
[12]	Wu M Y, Mi G B, Li P J, Huang X, Cao C X 2022 Mater. Lett 310 131515 Google Scholar
[13]	Guo B S, Ni S, Yi J H, Shen R J, Tang Z H, Du Y, Song M 2017 Mater. Sci. Eng. A 698 282 Google Scholar
[14]	Song Y, Chen Y, Liu W W, Li W L, Wang Y G, Zhao D, Liu X B 2016 Mater. Des 109 256 Google Scholar
[15]	Chen Y L, Yan M, Sun Y M, Mei B C, Zuo J Q 2009 Ceram. Int 35 1807 Google Scholar
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[20]	Pietzka M A, Schuster J C 1994 J. Phase Equilib 15 392 Google Scholar
[21]	Chen Y, Chu M Y, Wang L J, Bao X H, Lin Y, Shen J Y 2011 Phys. Status Solidi A 208 1879 Google Scholar
[22]	胡庚祥蔡珣戎咏华 2013 材料科学基础 (上海: 上海交通大学出版社) 第130页 Hu G X, Cai X, Rong Y H 2013 Fundamentals of Materials Science (Shanghai: Shanghai Jiao Tong University Press) p130 (in Chinese)
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图 1 MLG及TiAl合金粉体形貌　(a) MLG与TiAl粉体混合后的SEM形貌; (b) MLG的初始TEM形貌

Figure 1. Morphology of MLG and TiAl powders: (a) SEM morphology of MLG mixed with TiAl powders; (b) original morphology of MLG under TEM.

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图 2 1100 ℃烧结后由未反应的MLG与TiAl基体组成的界面组织

Figure 2. Interface structure composed of unreacted MLG and TiAl matrix sintered at 1100 ℃.

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图 3 1150 ℃烧结后MLG/TiAl的界面组织　(a) 部分反应的MLG及形成的Ti₂AlC; (b) Ti₂AlC的SAED图样

Figure 3. Interface structure of MLG/TiAl composite sintered at 1150 ℃: (a) Partly reacted MLG and formed Ti₂AlC; (b) SAED pattern of Ti₂AlC.

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图 4 1300 ℃烧结后MLG/TiAl的界面组织　(a) 部分反应的MLG及生成Ti₃AlC的TEM形貌; (b) Ti₃AlC的SAED图样

Figure 4. Interface structure of MLG/TiAl composite sintered at 1300 ℃: (a) TEM morphology of partly reacted MLG and formed Ti₃AlC; (b) SAED pattern of Ti₃AlC.

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图 5 Ti-Al-C 三元相图　(a) 1000 ℃等温截面图^[17]; (b) 1250 ℃部分等温截面图^[17]; (c) Ti-Al二元相图^[18]

Figure 5. Ternary diagram of Ti-Al-C: (a) Section at 1000 ℃^[17]; (b) partial section at 1250 ℃^[17]; (c) Ti-Al binary diagram^[18]

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图 6 晶体结构示意图　(a) TiAl; (b) Ti₃Al; (c) TiC; (d) Ti₃AlC; (e) Ti₂AlC

Figure 6. Schematic diagram of crystal structure: (a) TiAl; (b) Ti₃Al; (c) TiC; (d) Ti₃AlC; (e) Ti₂AlC.

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图 7 晶面原子排列示意图　(a) TiAl(111); (b) Ti₃Al(0001); (c) Ti₃AlC(111); (d) Ti₂AlC(0001)

Figure 7. Schematic diagram of atoms arrayed in crystal plane: (a) TiAl(111); (b) Ti₃Al(0001); (c) Ti₃AlC(111); (d) Ti₂AlC(0001).

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图 8 C与TiAl合金的反应路径　(a) 液相烧结经由TiC发生包晶反应; (b) 1150—1250 ℃固相烧结界面反应形成Ti₂AlC; (c) 1250—1350 ℃固相烧结界面反应形成Ti₃AlC

Figure 8. Reaction paths of C and TiAl alloy: (a) peritectic reaction via TiC during liquid-phase sintering; (b) Ti₂AlC formed at 1150—1250 ℃ by solid-state sintering interface reaction; (c) Ti₃AlC formed at 1250—1350 ℃ by solid-state sintering interface reaction.

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表 1 Ti-Al-C主要化合物的摩尔生成自由能

Table 1. Molar free energy of formation of compounds formed by Ti-Al-C.

化合物	摩尔生成自由能 ${\varDelta _{\text{f} } }G_{\text{m} }$/(kJ·mol^–1)
TiAl₃	0.06522T – 289.37
TiAl	0.02224T – 91.078
Ti₃Al	0.01678T – 109.75
TiC	0.01522T – 189.07
Ti₂AlC	0.03045T – 387.13
Ti₃AlC	0.1208T – 583.45

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表 2 C与TiAl的摩尔反应自由能${\varDelta _{\text{r}}}G_{\text{m}}$(kJ·mol^–1)

Table 2. Molar free energy ${\varDelta _{\text{r}}}G_{\text{m}}$ of reaction between C and TiAl (kJ·mol^–1).

摩尔反应自由能	温度/℃
摩尔反应自由能	1150	1250
$ \Delta {G_1} $	–3.72	–3.69
$ \Delta {G_2} $	–5.52	–5.50
$ \Delta {G_3} $	–6.88	–6.68

DownLoad: CSV

表 3 Ti-Al-C化合物晶体结构数据

Table 3. Crystal structure data of Ti-Al-C compounds.

序号	晶体	空间群	晶格常数
a	TiAl	${ { {{Pm} }\bar 3 m} }$	a = b = 4.0051 Å, c = 4.0707 Å
b	Ti₃Al	${{P63/mmc} }$	a = b = 5.764 Å, c = 4.664 Å
c	TiC	${ { {{Fm} }\bar 3 m} }$	a = b = c = 4.328 Å
d	Ti₃AlC	${ { {{Pm} }\bar 3 m} }$	a = b = c = 4.156 Å
e	Ti₂AlC	${{P63/mmc} }$	a = b = 3.063 Å, c = 13.668 Å

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表 4 TiAl, Ti₃Al, TiC, Ti₂AlC, Ti₃AlC的基本物理参数^[24-30]

Table 4. Basic physical parameters of TiAl, Ti₃Al, TiC, Ti₂AlC and Ti₃AlC^[24-30].

相	TiAl	Ti₃Al	TiC	Ti₂AlC	Ti₃AlC
弹性模量 G/GPa	70	56	182	115	83
泊松比 ν	0.23	0.28	0.228	0.164	0.25
线膨胀系数 α/10^–6	12—14.5	12—14.5	7.74	9.62	10.1

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表 5 TiAl/TiC, TiAl/Ti₂AlC, α/Ti₂AlC, TiAl/Ti₃AlC和α/Ti₃AlC的界面能

Table 5. Interfacial energy of TiAl/TiC, TiAl/Ti₂AlC, α/Ti₂AlC, TiAl/Ti₃AlC and α/Ti₃AlC.

温度/ ℃	$ {\sigma _{{\text{γ /TiC}}}} $/ (J·m²)	$ {\sigma _{{\text{γ /H}}}} $/ (J·m²)	$ {\sigma _{{\text{α /H}}}} $/ (J·m²)	$ {\sigma _{{\text{γ /P}}}} $/ (J·m²)	$ {\sigma _{^{{\text{α /P}}}}} $/ (J·m²)
1150	1.243	0.879	0.831	0.396	0.308
1200	1.230	0.872	0.827	0.390	0.303
1250	1.223	0.868	0.821	0.385	0.288
1300	1.220	0.866	0.819	0.384	0.288
1350	1.217	0.864	0.819	0.383	0.287

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表 6 MLG与TiAl合金反应生成单C原子层的TiC, Ti₂AlC, Ti₃AlC的总能量变化

Table 6. Total energy change of the interface reaction between MLG and TiAl with the formation of TiC, Ti₂AlC, Ti₃AlC per C atom layer.

界面反应产物	反应式	1150 ℃总能量变化$ \Delta E $/$ {\text{J}} $	1250 ℃总能量变化$ \Delta E $/$ {\text{J}} $
TiC	(1)	–2.477S	–2.467S
Ti₂AlC	(2)	–4.641S	–4.632S
Ti₃AlC	(3)	–6.572S	–6.392S

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[1]	Appel F, Clemens H, Fischer F D 2016 Prog. Mater. Sci 81 55 Google Scholar
[2]	Ouyang P X, Mi G B, Cao J X, Huang X, He L J, Li P J 2018 Mater. Today Comm 16 364 Google Scholar
[3]	Yamaguchi M, Inui H, Ito K 2000 Acta Mater 48 307 Google Scholar
[4]	Gao B, Peng H, Liang Y, Lin J, Chen B 2021 Mater. Sci. Eng. A 881 141059
[5]	Kan W, Chen B, Peng H, Liang Y, Lin J 2020 Mater. Lett. 259 126856
[6]	Lapin J, Pelachova T, Bajana O 2019 J. Alloys Compd 797 754 Google Scholar
[7]	Fang H, Chen R, Liu Y, Tan Y Guo J 2019 Intermetallics 115 106630 Google Scholar
[8]	Gouma P I, Mills M J, Kim Y W 1998 Phil. Mag Lett 78 59 Google Scholar
[9]	Wu H, Fan G H, Cui X P, Geng L, Yuan F, Pang J C, Wei L S, Huang M 2013 Mater. Sci. Eng. A 585 439 Google Scholar
[10]	Wu M Y, Mi G B, Li P J, Huang X, Cao C X 2020 J. Aeron. Mater 40 45
[11]	Nieto A, Bisht A, Lahiri D, Zhang C, Agarwal A 2016 Int. Mater. Rev 62 241
[12]	Wu M Y, Mi G B, Li P J, Huang X, Cao C X 2022 Mater. Lett 310 131515 Google Scholar
[13]	Guo B S, Ni S, Yi J H, Shen R J, Tang Z H, Du Y, Song M 2017 Mater. Sci. Eng. A 698 282 Google Scholar
[14]	Song Y, Chen Y, Liu W W, Li W L, Wang Y G, Zhao D, Liu X B 2016 Mater. Des 109 256 Google Scholar
[15]	Chen Y L, Yan M, Sun Y M, Mei B C, Zuo J Q 2009 Ceram. Int 35 1807 Google Scholar
[16]	Song X J, Cui H Z, Hou N, Wei N, Han Y, Tian J, Song Q 2016 Ceram. Int 42 13586 Google Scholar
[17]	MSIT, Cornish L, Cacciamani G, Cupid D M, Keyzer J D https://materials.springer.com/msi/docs/sm_msi_r_10_014870_02/ [2021-5-6]
[18]	Kim Y W 1992 Acta Metall. Mater 40 1121 Google Scholar
[19]	王苹, 梅炳初, 洪小林, 朱教群, 周卫兵, 严明, 2007 武汉理工大学学报 29 5 Wang P, Mei B C, Hong X L, Zhu J Q, Zhou W B, Yan M 2007 J. Wuhan Univ. Technol. 29 5 (in Chinese)
[20]	Pietzka M A, Schuster J C 1994 J. Phase Equilib 15 392 Google Scholar
[21]	Chen Y, Chu M Y, Wang L J, Bao X H, Lin Y, Shen J Y 2011 Phys. Status Solidi A 208 1879 Google Scholar
[22]	胡庚祥蔡珣戎咏华 2013 材料科学基础 (上海: 上海交通大学出版社) 第130页 Hu G X, Cai X, Rong Y H 2013 Fundamentals of Materials Science (Shanghai: Shanghai Jiao Tong University Press) p130 (in Chinese)
[23]	Merwe J, Woltersdorf J, Jesser W A 1986 Mater. Sci. Eng 81 1 Google Scholar
[24]	刘文胜, 黄伯云, 周科朝, 唐建成 2000 材料导报 14 19 Liu W S, Huang B Y, Zhou K C, Tang J C 2000 Mater. Rep. 14 19 (in Chinese)
[25]	Zhang W J, Reddy B V, Deevi S C 2001 Scr. Mater 45 645 Google Scholar
[26]	Kumpfert J 2001 Adv. Eng. Mater 3 851 Google Scholar
[27]	Todorova T Z, Gaier M, Zwanziger J W, Plucknett K P 2019 J. Alloy. Compd 789 712 Google Scholar
[28]	Arusei G K, Chepkoech M, Amolo G O, Wambua N 2020 arXiv: 2011.07102 v1 [cond-mat. mtrl]
[29]	Zhang X W, Wang X H, Li F Z, Zhou Y C 2010 J. Am. Ceram. Soc 92 2698
[30]	Schuster J C, Nowotny H, Vaccaro C 1980 J. Solid State Chem 32 213 Google Scholar
[31]	Болецкая B М1979 Metal Sci. Heat Treatm. Metals 12 37(in Russian)
[32]	Vanloo F, Bastin G F 1989 Metall. Meter. Trans. A 20 403

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Formation mechanisms of Ti₂AlC and Ti₃AlC during solid-state sintering between multilayer graphene and TiAl alloy composite

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Corresponding author: Mi Guang-Bao, guangbao.mi@biam.ac.cn

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Formation mechanisms of Ti2AlC and Ti3AlC during solid-state sintering between multilayer graphene and TiAl alloy composite

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Corresponding author: Mi Guang-Bao, guangbao.mi@biam.ac.cn

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Formation mechanisms of Ti₂AlC and Ti₃AlC during solid-state sintering between multilayer graphene and TiAl alloy composite