Effects of Ceramic Precursor Ratio on Antioxidation Properties of Pitch-based Carbon Materials Doped with Si-Zr-B

doi:10.15541/jim20150647

Abstract

Abstract:

The Si-Zr-B doped coal-tar pitch was synthesized by co-pyrolysis of xylene soluble pitch, silicon carbide precursor, zirconium boride precursor, and zirconium carbide precursor. The pitch-based carbon materials doped with Si-Zr-B were prepared through co-carbonization, cold moulding and followed by high temperature heat treatment from the obtained Si-Zr-B doped coal-tar pitch. The phase composition and microstructure of the carbon materials were characterized by XRD, SEM and EDS. The oxidation behavior of specimens was tested at 1500℃ in static air. The results show that weight loss of the doped carbon materials is increased firstly and then decreased with the decrease of content of silicon carbide precursor in Si-Zr-B doped coal-tar pitch. The doped carbon materials obtained from Si-Zr-B doped coal-tar pitch, with a mass ratio of the polycarbosilane, zirconium carbide precursor and zirconium boride precursor at 1:2:1, shows an excellent oxidant resistance. After oxidation in air at 1500℃ for 4 h, its weight loss and oxidation depth is 27.5wt% and 0.7 mm, respectively. A dense SiO₂-ZrO₂-B₂O₃ glassy oxide layer which formed during oxidation in air can effectively reduce the rate of oxygen diffusion and thus improve the oxidation resistance of the carbon materials derived from the doped coal-tar pitch.

Key words: Si-Zr-B, doping, pitch-based carbon material, antioxidation properties

CLC Number:

TB332

ZHANG Xu, DONG Zhi-Jun, YUAN Guan-Ming, CONG Ye, LI Xuan-Ke. Effects of Ceramic Precursor Ratio on Antioxidation Properties of Pitch-based Carbon Materials Doped with Si-Zr-B[J]. Journal of Inorganic Materials, 2016, 31(12): 1311-1319.

Figures/Tables 11

Table 1 Element contents of Si-Zr-B doped pitch-based carbon materials

Sample	C/wt%	Si/wt%	Zr/wt%	B/wt%
SZB0	100	0	0	0
SZB411	66.3	25.2	7.6	0.9
SZB211	66.9	19.8	11.9	1.4
SZB121	63.5	9.9	23.9	2.7
SZB141	57.8	6.3	30.4	3.5

Fig. 1 XRD patterns of the doped coal-pitch based carbon materials after heat-treatment at different temperatures

Fig. 2 XRD patterns of pitch-based carbon materials doped with Si-Zr-B

Fig. 3 Elemental analysis results of the specimen SZB211 after heat-treatment at 1600℃^(a) SEM image of SZB211; (b) Boron, (c) Carbon; (d) Sillion; (e) Zirconium

Fig. 4 Typical SEM images of pitch-based carbon materials doped with Si-Zr-B after heat-treatment at 1600℃^(a) SZB0; (b,c) SZB411; (d) SZB211; (e,f) SZB121; (g,h) SZB141

Fig. 5 Optical pictures of pitch-based carbon materials doped with Si-Zr-B after oxidation at 1500℃ for 4 h in air

Fig. 6 Optical pictures of the transverse section of pitch- based carbon materials doped with Si-Zr-B after oxidation at 1500℃ for 4 h in air

Fig. 7 Oxidation weight loss curves of pitch-based carbon materials doped with Si-Zr-B after oxidation at 1500℃ in air

Fig. 8 XRD patterns of pitch-based carbon materials doped with Si-Zr-B after oxidation at 1500℃ for 4 h in air

Fig. 9 Typical SEM images of pitch-based carbon materials doped with Si-Zr-B after oxidation at 1500℃ in air for 4 h^(a) SZB411; (b) SZB211; (c) SZB121; (d) SZB14

Fig. 10 Cross section linear EDS analysis of pitch-based carbon materials doped with Si-Zr-B after oxidation at 1500℃ for 4 h in air^(a) SZB411; (b) SZB211; (c) SZB121; (d) SZB141

References 13

[1]	XIAO CHUN, WANG RUI, WANG LING-LING,et al.Research on rheology performance of doped pitch precursor . Carbon Techniques, 2011, 30(4): 18-21.
[2]	FU QIAN-GANG, LI HE-JUN, SHEN XUE-TAO,et al. Domestic research process of matrix modification for carbon/carbon composites . Materials China, 2011, 30(11): 6-12.
[3]	MI QUN, CAO LI-YUN, HUANG JIAN-FENG,et al. Research progress in matrix oxidation-resistance modification of carbon/ carbon composites . Ordnance Material Scinence and Engineering, 2010, 33(2): 98-102.
	XIE JING, LI KE-ZHI, HUANG JIAN-FENG,et al. Preparation and properties of C/C-ZrC-SiC-ZrB2 composites via polymer infiltration and pyrolysis . Journal of Inorganic Materials, 2013, 28(6): 605-610.
[4]	EICHNER T, BRAUN M, HÜTTINGER K J. Element-substituted polyaromatic mesophases: I. Boron-substitution with the pyridine- borane complex.Carbon, 1996, 34(11): 1367-1381.
[5]	CZOSNEK C, JANIK J F, OLEJNICZAK Z.Silicon carbide modified carbon materials. Formation of nanocrystalline SiC from thermochemical processes in the system coal tar pitch/poly (carbosilane).Journal of Cluster Science, 2002, 13(4): 487-502.
[6]	DONG ZHI-JUN, ZUO XIAO-HUA, ZHANG XU,et al. On the preparation and oxidation behavior of B-Si doped pitch based on carbon materials . China Ceramics, 2015, 51(2): 12-16.
[7]	ZUO X H, DONG Z J, LI W,et al. Oxidation behavior of carbon- silicon and carbon-boron-silicon alloys derived from solvent- soluble silicon and boron-silicon-doped coal-tar pitches . Materiali in Technologije/Materials and technology, 2014, 48(1): 59-66.
[8]	ZHANG WEI-GANG.Self-healing oxidation resistance of C/C composite covering a broader temperatures range.Materials China, 2011, 30(11): 25-31.
[9]	WU HAI-TANG, WEI XI, YU SHOU-QUAN,et al. Ablation performances of muti-phased C/C-ZrC-SiC ultra-high temperature composites . Journal of Inorganic Materials, 2011, 26(8): 852-856.
[10]	ZHUANG LEI, FU QIAN-GANG, LI HE-JUN,et al. Oxidation behavior and ablation resistance of C/C-ZrC-SiC composites prepared by polymer infiltration and pyrolysis . Materials China, 2015, 34(6): 425-431.
[11]	KARAMIAN E, MONSHI A, BATAILLE A,et al. Formation of nano SiC whiskers in bauxite-carbon composite materials and their consequences on strength and density. Journal of the European Ceramic Society, 2011, 31(11): 2677-2685.
[12]	QIAN YANG-BAO, ZHANG WEI-GANG.Phase-transformation behavior of plasma-sprayed ZrSiO4 coating materials.Journal of the Chinese ceramic society, 2008, 36(8): 1103-1108.
[13]	HE JIANG-YI.High temperature oxidation resistance of ZrB2 and its composites.Aerospace Materials & Technology, 2015, 45(3): 1-6.

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