Reactive sintering of B4C-TaB2 ceramics via carbide boronizing: Reaction process, microstructure and mechanical properties

doi:10.1016/j.jmst.2019.04.029

Abstract

Abstract:

Carbide boronizing is a promising approach to obtain fine grained boron carbide based ceramics with improved mechanical properties. In this work, reaction process, microstructural characteristics and mechanical properties of B_xC-TaB₂ (x?=?3.7, 4.9, 7.1) ceramics were comprehensively investigated via this method. Dense B_xC-TaB₂ ceramics with refined microstructure were obtained from submicro tantalum carbide and boron powder mixtures at 1800?°C/50?MPa/5?min by spark plasma sintering. The stoichiometry of boron carbide was determined from lattice parameters and Raman shift. It was found that uniformly distributed TaB₂ grains in the B_xC matrix is favor of the densification process and restricting grain growth. Besides, planar defects with high density were observed from the as-formed B_7.1C grains and transient stress was considered to contribute to the densification involved with plastic deformation. Microstructural observations indicate the dissolution of oxygen in the TaB₂ lattice and most of the B_7.1C/TaB₂ phase boundaries were clean. Owing to the highly faulted structure and finer grain size, as-obtained B_xC-TaB₂ ceramics exhibit high Vickers hardness (33.3-34.4?GPa at 9.8?N) and relatively high flexural strength ranging from 440 to 502?MPa.

Key words: Boron carbide, Reaction sintering, Densification, Microstructure, Mechanical properties

Junfeng Gu, Ji Zou, Peiyan Ma, Hao Wang, Jinyong Zhang, Weimin Wang, Zhengyi Fu. Reactive sintering of B₄C-TaB₂ ceramics via carbide boronizing: Reaction process, microstructure and mechanical properties[J]. J. Mater. Sci. Technol., 2019, 35(12): 2840-2850.

Figures/Tables 15

Table 1 Characteristics of boron carbide-tantalum diboride ceramics sintered at 1800℃.

	TaB₂		B₄C		Bulk density (g/cm³)	Relative density (%)	Average grain size of TaB₂ (μm)	Lattice parameter (Å)
	wt%	vol%	wt%	vol%	Bulk density (g/cm³)	Relative density (%)	Average grain size of TaB₂ (μm)	aBxC	cBxC	aTaB2	cTaB2
T-6B	78.57	42.29	21..43	57.71	6.757	99.64	0.66?±?0.12	5.593	12.053	3.070	3.300
T-8B	72.49	34.25	27.51	65.75	5.933	99.66	0.64?±?0.15	5.609	12.112	3.075	3.308
T-10B	67.29	28.78	32.71	71.22	5.378	99.80	0.61?±?0.11	5.629	12.170	3.072	3.308

Fig. 1. (a) Relative density of the BxC-TaB2 ceramics sintered at different temperatures. (b) The average grain size of TaB2 at different samples.

Fig. 2. (a) XRD patterns of the samples sintered at 1800?°C. (b) The enlarged area at 34-40° indicates the peak shift of BxC with an increase of the boron content.

Fig. 3. Raman spectra collected on different samples acquired using a laser with a wavenumber of 514.5?nm.

Fig. 4. Backscattered electron (BSE) images of the polished surface for (a) T-6B-18, (b) T-8B-18 and (c) T-10B-18. TaB2 and B4C are shown in white and black contrast, respectively. For comparison, BSE images of T-10B sintered at (d) 1700?°C and (e) 1900?°C are also presented. (f) A higher magnification BSE image of T-10B-18. The EDS analysis reveals the nano-sized precipitate is composed of Ta, B and C.

Fig. 5. (a) TEM images of T-10B-18, revealing lots of striations in B4C (white contrast). (b) The HRTEM image indicates the parallel striations have an angle about 32.5° to the (021) plane of boron carbide. Phase/grain boundaries in (c) and (d) show the clean interface of TaB2/B7.1C and B7.1C/B7.1C. (e)-(i) A HADDF image and element maps of Ta, B, C and O, showing the evidence of oxygen in the TaB2 grains. (j)-(k) A HADDF image and corresponding element maps of Ta & O, showing the presence of surface oxides around the ultra-fine TaB2 grain.

Table 2 Mechanical properties of boron carbide-transition metal diboride ceramics sintered at 1800℃.

	Composition	E (GPa)	G (GPa)	Hardness (GPa)	Flexural strength (MPa)	Fracture toughness (MPa∙m^1/2)
This work	B_3.7C-TaB₂ 1800	513	214	33.3?±?1.4	502?±?45	3.44?±?0.31
This work	B_4.9C-TaB₂ 1800	495	204	33.9?±?1.6	440?±?39	3.60?±?0.26
This work	B_7.1C-TaB₂ 1800	492	202	34.4?±?1.2	471?±?35	3.72?±?0.37
Ref. [47]	B₄C-TaB₂ 2350 (Eutectic)	424?±?17	/	26	430?±?25	4.5
Ref. [20]	B₄C-ZrB₂ 1800	462.58?±?1.30	195.89?±?0.55	33.39?±?2.23	/	3.08?±?0.46

Fig. 6. Typical FESEM images of (a) the surface of T-6B fractured after the three-point flexural strength test, (b) a typical indentation crack propagated on T-10B.

Fig. 7. The evolution of phase assemblage at different temperatures for T-10B.

Fig. 8. Raman spectra of T-10B acquired using a laser with a wavenumber of 633?nm, the change of the intensity for D and G peaks of carbon with increasing temperature is apparent.

Fig. 9. Heating power and displacements of punches during SPS for T-6B-18 and T-10B-18.

Fig. 10. TEM images of T-10B-14. (a) The overall view shows the presence of abundant carbon nano-sphere. (b)-(c) HRTEM images of the carbon nano-sphere, an interlayer distance about 0.34?nm was measured which is close to the (002) interplanar distance of graphite. (d) A TEM image shows the aggregation of B4C particles and their lattice fringes (e).

Fig. 11. TEM images of T-10B-14. (a) A typical image of a large TaB2 grain. The insets clearly reveal the core-shell structure. (b) A typical image of a small TaB2 grain. The insets also clearly indicate the core-shell structure. A HRTEM image (c) with corresponding EDS mappings (d)-(g) and a partially enlarged TEM image (h) indicate the core-shell structure and elemental distribution.

Fig. 12. Schematic for the reaction and densification process of T-10B.

Fig. 13. TEM images showing the defects in T-10B-18. (a) & (b) For small TaB2 grains, striations directly stride over them without changing the orientation. (c) HRTEM image of the point in (b) indicates the presence of an amorphous layer. (d) & (e) Striations prefer stopping at larger grains and are nearly perpendicular to phase boundaries.

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Reactive sintering of B₄C-TaB₂ ceramics via carbide boronizing: Reaction process, microstructure and mechanical properties

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