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The in situ nano Ta4HfC5 reinforced SiBCN-Ta4HfC5 composite ceramics were prepared by a combination of two-step mechanical alloying and reactive hot-pressing sintering. The microstructural evolution and mechanical properties of the resulting SiBCN-Ta4HfC5 were studied. After the first-step milling of 30 h, the raw materials of TaC and HfC underwent crushing, cold sintering, and short-range interdiffusion to finally obtain the high pure nano Ta4HfC5. A hybrid structure of amorphous SiBCN and nano Ta4HfC5 was obtained by adopting a second-step ball-milling. After reactive hot-pressing sintering, amorphous SiBCN has crystallized to 3C-SiC, 6H-SiC, and turbostratic BN(C) phases and Ta4HfC5 retained the form of the nanostructure. With the in situ generations of 2.5 wt% Ta4HfC5, Ta4HfC5 is preferentially distributed within the turbostratic BN(C); however, as Ta4HfC5 content further raised to 10 wt%, it mainly distributed in the grain-boundary of BN(C) and SiC. The introduction of Ta4HfC5 nanocrystals can effectively improve the flexural strength and fracture toughness of SiBCN ceramics, reaching to 344.1 MPa and 4.52 MPa·m1/2, respectively. This work has solved the problems of uneven distribution of ultra-high temperature phases in the ceramic matrix, which is beneficial to the real applications of SiBCN ceramics.


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Microstructural evolution and mechanical properties of in situ nano Ta4HfC5 reinforced SiBCN composite ceramics

Show Author's information Bingzhu WANGa,bDaxin LIa,b( )Zhihua YANGa,b,cDechang JIAa,b,c( )Jingyi GUANa,bHao PENGa,bDelong CAIa,bPeigang HEa,bXiaoming DUANa,bYu ZHOUa,bTao ZHANGdChenguang GAOd
Institute for Advanced Ceramics, School of Materials Science and Engineering, Harbin Institute of Technology, Harbin 150001, China
Key Laboratory of Advanced Structural-Functional Integration Materials & Green Manufacturing Technology, Harbin Institute of Technology, Harbin 150001, China
State Key Laboratory of Advanced Welding and Joining, Harbin Institute of Technology, Harbin 150001, China
Beijing Institute of Control Engineering, Beijing 100080, China

Abstract

The in situ nano Ta4HfC5 reinforced SiBCN-Ta4HfC5 composite ceramics were prepared by a combination of two-step mechanical alloying and reactive hot-pressing sintering. The microstructural evolution and mechanical properties of the resulting SiBCN-Ta4HfC5 were studied. After the first-step milling of 30 h, the raw materials of TaC and HfC underwent crushing, cold sintering, and short-range interdiffusion to finally obtain the high pure nano Ta4HfC5. A hybrid structure of amorphous SiBCN and nano Ta4HfC5 was obtained by adopting a second-step ball-milling. After reactive hot-pressing sintering, amorphous SiBCN has crystallized to 3C-SiC, 6H-SiC, and turbostratic BN(C) phases and Ta4HfC5 retained the form of the nanostructure. With the in situ generations of 2.5 wt% Ta4HfC5, Ta4HfC5 is preferentially distributed within the turbostratic BN(C); however, as Ta4HfC5 content further raised to 10 wt%, it mainly distributed in the grain-boundary of BN(C) and SiC. The introduction of Ta4HfC5 nanocrystals can effectively improve the flexural strength and fracture toughness of SiBCN ceramics, reaching to 344.1 MPa and 4.52 MPa·m1/2, respectively. This work has solved the problems of uneven distribution of ultra-high temperature phases in the ceramic matrix, which is beneficial to the real applications of SiBCN ceramics.

Keywords: mechanical properties, Ta4HfC5, SiBCN, microstructure evolution

References(35)

[1]
R Riedel, A Kienzle, W Dressler, et al. A silicoboron carbonitride ceramic stable to 2,000 ℃. Nature 1996, 382: 796-798.
[2]
R Riedle, LM Ruswisch, LA Rishi Raj. Amorphous silicoboron carbonitride ceramic with very high viscosity at temperatures above 1500 ℃. J Am Ceram Soc 1998, 81: 3341-3344.
[3]
NV Ravi Kumar, S Prinz, Y Cai, et al. Crystallization and creep behavior of Si-B-C-N ceramics. Acta Mater 2005, 53: 4567-4578.
[4]
GB Thiyagarajan, R Devasia. Simple and low-cost synthetic route for SiBCN ceramic powder from a boron-modified cyclotrisilazane. J Am Ceram Soc 2019, 102: 476-489.
[5]
CK Song, XF Liu, F Ye, et al. Mechanical and dielectric properties of SiCf/BN/SiBCN composites via different synthesis technologies. J Eur Ceram Soc 2019, 39: 4417-4423.
[6]
DC Jia, B Liang, ZH Yang, et al. Metastable Si-B-C-N ceramics and their matrix composites developed by inorganic route based on mechanical alloying: Fabrication, microstructures, properties and their relevant basic scientific issues. Prog Mater Sci 2018, 98: 1-67.
[7]
DX Li, Q Li, JK Yuan, et al. Effects of high pressure on the low-temperature sintering of dense amorphous SiBCN monoliths. J Eur Ceram Soc 2018, 38: 3777-3786.
[8]
PF Zhang, DC Jia, ZH Yang, et al. Progress of a novel non-oxide Si-B-C-N ceramic and its matrix composites. J Adv Ceram 2012, 1: 157-178.
[9]
JY Wang, XM Duan, ZH Yang, et al. Ablation mechanism and properties of SiCf/SiBCN ceramic composites under an oxyacetylene torch environment. Corros Sci 2014, 82: 101-107.
[10]
DX Li, ZH Yang, DC Jia, et al. Ablation behavior of graphene reinforced SiBCN ceramics in an oxyacetylene combustion flame. Corros Sci 2015, 100: 85-100.
[11]
N Liao, DC Jia, ZH Yang, et al. Enhanced mechanical properties, thermal shock resistance and ablation resistance of Si2BC3N ceramics with nano ZrB2 addition. J Eur Ceram Soc 2019, 39: 846-859.
[12]
B Feng, Y Zhang, BY Li, et al. Medium-temperature sintering efficiency of ZrB2 ceramics using polymer- derived SiBCN as a sintering aid. J Am Ceram Soc 2018, 102: 855-866.
[13]
SH Wang, YC Zhang, Y Sun, et al. Synthesis and characteristic of SiBCN/HfN ceramics with high temperature oxidation resistance. J Alloys Compd 2016, 685: 828-835.
[14]
M Sun, RY Fu, J Chen, et al. Fabrication and microstructures of functional gradient SiBCN-Nb composite by hot pressing. Mater Charact 2016, 114: 115-121.
[15]
B Feng, Y Zhang, BY Li, et al. Medium-temperature sintering efficiency of ZrB2 ceramics using polymer-derived SiBCN as a sintering aid. J Am Ceram Soc 2018, 102: 855-866.
[16]
SH Wang, YC Zhang, Y Sun, et al. Synthesis and characteristic of SiBCN/HfN ceramics with high temperature oxidation resistance. J Alloys Compd 2016, 685: 828-835.
[17]
B Liang, ZH Yang, DC Jia, et al. Densification, microstructural evolution and mechanical properties of Si-B-C-N monoliths with LaB6 addition. J Alloys Compd 2017, 696: 1090-1095.
[18]
B Liang, ZH Yang, Y Miao, et al. Si-B-C-N monoliths with LaB6-induced well-developed BN(C) flakes. Mater Lett 2017, 187: 36-39.
[19]
B Liang, ZH Yang, Y Miao, et al. Microstructural evolution, mechanical and thermal properties of LaB6 embedded in Si-B-C-N prepared by spark plasma sintering. Ceram Int 2017, 43: 4814-4820.
[20]
Y Miao, ZH Yang, B Liang, et al. A novel in situ synthesis of SiBCN-Zr composites prepared by a sol-gel process and spark plasma sintering. Dalton Trans 2016, 45: 12739-12744.
[21]
Y Miao, ZH Yang, JC Rao, et al. Influence of Sol-gel derived ZrB2 additions on microstructure and mechanical properties of SiBCN composites. Ceram Int 2017, 43: 4372-4378.
[22]
Y Miao, ZH Yang, QS Zhu, et al. Thermal ablation behavior of SiBCN-Zr composites prepared by reactive spark plasma sintering. Ceram Int 2017, 43: 7978-7983.
[23]
C Agte, H Alterthum. Investigations of the High-Melting Carbide Systems Connected with Problem of the Carbon Melting. Z Techn Phys 1930, 11: 182.
[24]
RA Andrievskii, NS Strel'Nikova, NI Poltoratskii, et al. Melting point in systems ZrC-HfC, TaC-ZrC, TaC-HfC. Powder Metall Met Ceram 1967, 6: 65-67.
[25]
EP Simonenko, NA Ignatov, NP Simonenko, et al. Zirconium Carbide Ta4ZrC5 and Tantalum-Hafnium Carbide Ta4HfC5 via sol-gel Technology, Synth Prop Inorg Compd 2011, 56: 1763-1769.
[26]
Y Lu, YN Sun, TZ Zhang, et al. Polymer-derived Ta4HfC5 nanoscale ultrahigh-temperature ceramics: Synthesis, microstructure and properties. J Eur Ceram Soc 2019, 39: 205-211.
[27]
O Gaballa, BA Cook, AM Russell. Reduced-temperature processing and consolidation of ultra-refractory Ta4HfC5. Int J Refract Met Hard Mater 2013, 41: 293-299.
[28]
N Liao, DC Jia, ZH Yang, et al. Strengthening and toughening effects of MWCNTs on Si2BC3N ceramics sintered by SPS technique. Mater Sci Eng: A 2018, 710: 142-150.
[29]
N Liao, DC Jia, ZH Yang, et al. Mechanical properties and thermal shock resistance of Si2BC3N ceramics with ternary Al4SiC4 additive. Ceram Int 2018, 44: 9009-9017.
[30]
PM Kibasomba, S Dhlamini, M Maaza, et al. Strain and grain size of TiO2 nanoparticles from TEM, Raman spectroscopy and XRD: The revisiting of the Williamson-Hall plot method. Results Phys 2018, 9: 628-635.
[31]
HT Chen, B Tang, CW Zhong, et al. The dielectric constant and quality factor calculation of the microwave dielectric ceramic solid solutions. Ceram Int 2017, 43: 7383-7386.
[32]
QM Hang, ZB Xing, XH Zhu, et al. Dielectric properties and related ferroelectric domain configurations in multiferroic BiFeO3-BaTiO3 solid solutions. Ceram Int 2012, 38: S411-S414.
[33]
E Antolini. Li2O evaporation from LixCo1-xO solid solutions at 1200 ℃. Ceram Int 2001, 27: 675-679.
[34]
K Zaara, M Chemingui, V Optasanu, et al. Solid solution evolution during mechanical alloying in Cu-Nb-Al compounds. Int J Miner Metall Mater 2019, 26: 1129-1139.
[35]
DX Li, ZH Yang, DC Jia, et al. Structure evolution, amorphization and nucleation studies of carbon-lean to -rich SiBCN powder blends prepared by mechanical alloying. RSC Adv 2016, 6: 48255-48271.
Publication history
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Publication history

Received: 11 March 2020
Revised: 25 June 2020
Accepted: 16 July 2020
Published: 27 November 2020
Issue date: December 2020

Copyright

© The Author(s) 2020

Acknowledgements

We appreciate the financial support from the National Natural Science Foundation of China (52002092, 51621091, 51472059, 51225203, and 51272300), the National Key Research and Development Program (2017YFB0310400), the Postdoctoral Innovative Talents Support Program (BX20190095), and the China Postdoctoral Science Foundation (Grant Nos. LBH-Z19141 and 2019M660072). This work was also funded by Advanced Space Propulsion Laboratory of BICE and Beijing Engineering Research center of Efficient and Green Aerospace Propulsion Technology (No. LabASP-2019-08).

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