Journal Home > Volume 12 , Issue 1

Ti3SiC2/Al2O3 composites have attracted attention due to their excellent mechanical and electromagnetic properties, but the high temperatures (≥ 1400 ℃) required for the densification of aluminum oxide (Al2O3) leads to the decomposition of Ti3SiC2. To address this issue, Ti3(SixAl1−x)C2/Al2O3 (x represents the Si content) composites were synthesized for the first time via hot-pressing (HP) sintering and current-assisted sintering (CAS) of mixed Ti3AlC2 and silicon monoxide (SiO) powders at 1300 and 1200 ℃, respectively. Both approaches produced composites with x values greater than 0.9, indicating that the compositions of the prepared composites were similar to those of Ti3SiC2/Al2O3 composites. The synthetic mechanism involved substitution and continuous interdiffusion of Al and Si atoms. The composite prepared by CAS at 1200 ℃ was compacted, whereas the composite prepared by HP had a low density. The low-temperature densification mechanism is attributed to the combined effects of amorphous SiO, liquid Al, and the high heating rates for CAS. The flexural strength and hardness of the composite prepared by CAS were also comparable to those of compacted Ti3SiC2/Al2O3 composites.


menu
Abstract
Full text
Outline
Electronic supplementary material
About this article

Formation mechanisms of Ti3(Si,Al)C2/Al2O3 composites from Ti3AlC2 and SiO via low-temperature sintering

Show Author's information Zhenyu ZHANGa,Jun JIbYingying CHENbDeli MAaSique CHENbHailing YANGaGuopu SHIbZhi WANGbMengyong SUNcFei CHENdShifeng HUANGaQinggang LIa,( )
Shandong Provincial Key Laboratory of Preparation and Measurement of Building Materials, University of Jinan, Jinan 250022, China
School of Materials Science and Engineering, University of Jinan, Jinan 250022, China
52 Institute of China North Industries Group, Yantai 264003, China
State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology, Wuhan 430070, China

† Zhenyu Zhang and Qinggang Li contributed equally to this work.

Abstract

Ti3SiC2/Al2O3 composites have attracted attention due to their excellent mechanical and electromagnetic properties, but the high temperatures (≥ 1400 ℃) required for the densification of aluminum oxide (Al2O3) leads to the decomposition of Ti3SiC2. To address this issue, Ti3(SixAl1−x)C2/Al2O3 (x represents the Si content) composites were synthesized for the first time via hot-pressing (HP) sintering and current-assisted sintering (CAS) of mixed Ti3AlC2 and silicon monoxide (SiO) powders at 1300 and 1200 ℃, respectively. Both approaches produced composites with x values greater than 0.9, indicating that the compositions of the prepared composites were similar to those of Ti3SiC2/Al2O3 composites. The synthetic mechanism involved substitution and continuous interdiffusion of Al and Si atoms. The composite prepared by CAS at 1200 ℃ was compacted, whereas the composite prepared by HP had a low density. The low-temperature densification mechanism is attributed to the combined effects of amorphous SiO, liquid Al, and the high heating rates for CAS. The flexural strength and hardness of the composite prepared by CAS were also comparable to those of compacted Ti3SiC2/Al2O3 composites.

Keywords: aluminum oxide (Al2O3), current-assisted sintering (CAS), silicon monoxide (SiO), Ti3(Si,Al)C2

References(51)

[1]
Ji J, Zhang L, Yu JM, et al. Interface properties of Ti3SiC2/Al2O3 ceramics: Combined experiments and first-principles calculations. Ceram Int 2021, 47: 6409–6417.
[2]
Wang XY, Shi GP, Li QG, et al. Effect of Ge on microstructure and mechanical properties of Ti3SiC2/Al2O3 composites. Ceram Int 2021, 47: 2280–2287.
[3]
Wang XY, Qi FF, Wang Z, et al. Dependence of Al doping on the in-situ reactive preparation and mechanical properties of Ti3SiC2/Al2O3 composites. ES Mater Manuf 2022, 15: 85–95.
[4]
Qi FF, Shi GP, Xu K, et al. Microstructure and mechanical properties of hot pressed Ti3SiC2/Al2O3. Ceram Int 2019, 45: 11099–11104.
[5]
Wang HJ, Jin ZH, Miyamoto Y. Effect of Al2O3 on mechanical properties of Ti3SiC2/Al2O3 composite. Ceram Int 2002, 28: 931–934.
[6]
Wang HJ, Jin ZH, Miyamoto Y. Ti3SiC2/Al2O3 composites prepared by SPS. Ceram Int 2003, 29: 539–542.
[7]
Zhou AG, Liu Y, Li SB, et al. From structural ceramics to 2D materials with multi-applications: A review on the development from MAX phases to MXenes. J Adv Ceram 2021, 10: 1194–1242.
[8]
Shi SL, Zhang LZ, Li JS. High frequency electromagnetic interference shielding behaviors of Ti3SiC2/Al2O3 composites. J Appl Phys 2008, 103: 124103.
[9]
Zhao D, Xia SQ, Wang YG, et al. High-performance microwave absorption properties of Ti3SiC2/Al2O3 coatings prepared by plasma spraying. Appl Phys A 2020, 126: 69.
[10]
Liu Y, Luo F, Su JB, et al. Mechanical, dielectric, and microwave-absorption properties of alumina ceramic containing dispersed Ti3SiC2. J Electron Mater 2015, 44: 867–873.
[11]
Fu XL, Hu YB, Peng G, et al. Effect of reinforcement content on the density, mechanical and tribological properties of Ti3SiC2/Al2O3 hybrid reinforced copper-matrix pantograph slide. Sci Eng Compos Mater 2017, 24: 807–815.
[12]
Luo YM, Pan W, Li SQ, et al. Fabrication of Al2O3–Ti3SiC2 composites and mechanical properties evaluation. Mater Lett 2003, 57: 2509–2514.
[13]
Palmquist JP, Li S, Persson POÅ, et al. Mn+1AXn phases in the Ti–Si–C system studied by thin-film synthesis and ab initio calculations. Phys Rev B 2004, 70: 165401.
[14]
Yeh CL, Li RF, Shen YG. Formation of Ti3SiC2–Al2O3 in situ composites by SHS involving thermite reactions. J Alloys Compd 2009, 478: 699–704.
[15]
Turki F, Abderrazak H, Schoenstein F, et al. Physico-chemical and mechanical properties of Ti3SiC2-based materials elaborated from SiC/Ti by reactive spark plasma sintering. J Adv Ceram 2019, 8: 47–61.
[16]
Wakelkamp WJJ, van Loo FJJ, Metselaar R. Phase relations in the Ti–Si–C system. J Eur Ceram Soc 1991, 8: 135–139.
[17]
Radhakrishnan R, Williams JJ, Akinc M. Synthesis and high-temperature stability of Ti3SiC2. J Alloys Compd 1999, 285: 85–88.
[18]
Low IM, Oo Z, Prince KE. Effect of vacuum annealing on the phase stability of Ti3SiC2. J Am Ceram Soc 2007, 90: 2610–2614.
[19]
Emmerlich J, Music D, Eklund P, et al. Thermal stability of Ti3SiC2 thin films. Acta Mater 2007, 55: 1479–1488.
[20]
Zeng JL, Ren SF, Lu JJ. Phase evolution of Ti3SiC2 annealing in vacuum at elevated temperatures. Int J Appl Ceram Technol 2013, 10: 527–539.
[21]
Kwon ST, Kim DY, Kang TK, et al. Effect of sintering temperature on the densification of Al2O3. J Am Ceram Soc 1987, 70: C-69–C-70.
[22]
Wang SW, Chen LD, Hirai T. Densification of Al2O3 powder using spark plasma sintering. J Mater Res 2000, 15: 982–987.
[23]
Lorenz M, Travitzky N, Rambo CR. Effect of processing parameters on in situ screen printing-assisted synthesis and electrical properties of Ti3SiC2-based structures. J Adv Ceram 2021, 10: 129–138.
[24]
Xu JK, Lang JF, An D, et al. A novel alternating current-assisted sintering method for rapid densification of Al2O3 ceramics with ultrahigh flexural strength. Ceram Int 2020, 46: 5484–5488.
[25]
Zhang ZR, Yin XH, Qian YH, et al. Determination of interdiffusion coefficients of Si and Al in Ti3SiC2–Ti3AlC2 diffusion couple at 1373–1673 K. J Am Ceram Soc 2020, 103: 670–680.
[26]
Ji J, Zhang L, Zhang ZY, et al. First-principle study and experiment on temperature-dependent substitution process of Si in Ti3(Si,Al)C2 solid solution. ES Mater Manuf 2021, 13: 82–88.
[27]
Wang S, Cheng J, Zhu SY, et al. A novel route to prepare a Ti3SnC2/Al2O3 composite. Scripta Mater 2017, 131: 80–83.
[28]
Duan XJ, Fang Z, Yang T, et al. Maximizing the mechanical performance of Ti3AlC2-based MAX phases with aid of machine learning. J Adv Ceram 2022, 11: 1307–1318.
[29]
Toropov NA, Barzakovskii VP. Stable and metastable phase relations in the system magnesium oxide–alumina–silica. In: High-temperature Chemistry of Silicates and Other Oxide Systems. Toropov NA, Barzakovskii VP, Eds. New York: Springer New York, 1966: 25–43.
DOI
[30]
Zhu HG, Dong K, Huang JW, et al. Reaction mechanism and mechanical properties of an aluminum-based composite fabricated in-situ from Al–SiO2 system. Mater Chem Phys 2014, 145: 334–341.
[31]
Zhou YC, Chen JX, Wang JY. Strengthening of Ti3AlC2 by incorporation of Si to form Ti3Al1−xSixC2 solid solutions. Acta Mater 2006, 54: 1317–1322.
[32]
Gao HL, Benitez R, Son W, et al. Structural, physical and mechanical properties of Ti3(Al1−xSix)C2 solid solution with x = 0–1. Mater Sci Eng A 2016, 676: 197–208.
[33]
Wang XH, Zhou YC. Microstructure and properties of Ti3AlC2 prepared by the solid–liquid reaction synthesis and simultaneous in-situ hot pressing process. Acta Mater 2002, 50: 3143–3151.
[34]
Gong YM, Tian WB, Zhang PG, et al. Slip casting and pressureless sintering of Ti3AlC2. J Adv Ceram 2019, 8: 367–376.
[35]
Sun W, Dcosta DJ, Lin F, et al. Freeform fabrication of Ti3SiC2 powder-based structures: Part I—Integrated fabrication process. J Mater Process Technol 2002, 127: 343–351.
[36]
Piconi C. Alumina. In: Comprehensive Biomaterials. Ducheyne P, Healy KE, Hutmacher DW, et al., Eds. Amsterdam, the Netherlands: Elsevier Amsterdam, 2011: 73–94.
DOI
[37]
Wang CW, Ping WW, Bai Q, et al. A general method to synthesize and sinter bulk ceramics in seconds. Science 2020, 368: 521–526.
[38]
Tuan WH, Chen RZ, Wang TC, et al. Mechanical properties of Al2O3/ZrO2 composites. J Eur Ceram Soc 2002, 22: 2827–2833.
[39]
Gandhi AS, Jayaram V, Chokshi AH. Low temperature densification behaviour of metastable phases in ZrO2–Al2O3 powders produced by spray pyrolysis. Mater Sci Eng A 2001, 304–306: 785–789.
[40]
Fang Y, Liu XH, Feng YX, et al. Microstructure and mechanical properties of Ti3(Al,Ga)C2/Al2O3 composites prepared by in situ reactive hot pressing. J Adv Ceram 2020, 9: 782–790.
[41]
Zhang HB, Zhou YC, Bao YW, et al. Improving the oxidation resistance of Ti3SiC2 by forming a Ti3Si0.9Al0.1C2 solid solution. Acta Mater 2004, 52: 3631–3637.
[42]
Zou Y, Sun ZM, Tada SJ, et al. Effect of Al addition on low-temperature synthesis of Ti3SiC2 powder. J Alloys Compd 2008, 461: 579–584.
[43]
Atazadeh N, Heydari MS, Baharvandi HR, et al. Reviewing the effects of different additives on the synthesis of the Ti3SiC2 MAX phase by mechanical alloying technique. Int J Refract Met H 2016, 61: 67–78.
[44]
El-Raghy T, Zavaliangos A, Barsoum MW, et al. Damage mechanisms around hardness indentations in Ti3SiC2. J Am Ceram Soc 2005, 80: 513–516.
[45]
Guenette MC, Tucker MD, Ionescu M, et al. Carbon diffusion in alumina from carbon and Ti2AlC thin films. J Appl Phys 2011, 109: 083503.
[46]
Garay JE. Current-activated, pressure-assisted densification of materials. Annu Rev Mater Res 2010, 40: 445–468.
[47]
Yang SL, Sun ZM, Yang QQ, et al. Effect of Al addition on the synthesis of Ti3SiC2 bulk material by pulse discharge sintering process. J Eur Ceram Soc 2007, 27: 4807–4812.
[48]
Liang BY, Jin SZ, Wang MZ. Low-temperature fabrication of high purity Ti3SiC2. J Alloys Compd 2008, 460: 440–443.
[49]
Yang SL, Sun ZM, Hashimoto H, et al. Ti3SiC2 powder synthesis from Ti/Si/TiC powder mixtures. J Alloys Compd 2003, 358: 168–172.
[50]
Murray JL, McAlister AJ. The Al–Si (aluminum–silicon) system. Bull Alloy Phase Diagr 1984, 5: 74–84.
[51]
Wang H, Han H, Yin G, et al. First-principles study of vacancies in Ti3SiC2 and Ti3AlC2. Materials 2017, 10: 103.
File
JAC0669_ESM.pdf (537.1 KB)
Publication history
Copyright
Acknowledgements
Rights and permissions

Publication history

Received: 10 June 2022
Revised: 29 September 2022
Accepted: 30 September 2022
Published: 23 December 2022
Issue date: January 2023

Copyright

© The Author(s) 2022.

Acknowledgements

Authors appreciate the financial support by the Shandong Province Key Research and Development Plan (Grant No. 2020JMRH0401), the National Natural Science Foundation of China (Grant No. 51872118), the Key Research and Development Program of Shandong Province (Grant No. 2019RKB01018), and the Shandong Provincial Natural Science Foundation (Grant Nos. ZR2018PEM008 and ZR2019MEM055). This study was supported by the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing, Wuhan University of Technology and was financially supported by the National Natural Science Foundation of China (Grant No. 51632003), the Taishan Scholars Program, and the Case-by-Case Project for Top Outstanding Talents of Jinan.

Rights and permissions

Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made.

The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder.

To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.

Return