CN103145112A - BN-Si2N2O composite ceramic and preparation method thereof - Google Patents
BN-Si2N2O composite ceramic and preparation method thereof Download PDFInfo
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Abstract
The invention discloses a BN-Si2N2O composite ceramic and a preparation method thereof, relates to a boron nitride based ceramic material and a preparation method thereof, and aims to solve the problems that an existing method for preparing the boron nitride based composite material is high in preparation cost, low in efficiency and difficult in preparation of large-size boron nitride based ceramic components. The BN-Si2N2O composite ceramic is prepared from amorphous nano silicon dioxide, silicon nitride powder and hexagonal boron nitride powder. The preparation method comprises the following steps of: one, weighing; two, preparing slurry through ball milling; three, drying to prepare powder; four, prepressing and forming; five, performing isostatic cool pressing treatment; and six, performing sintering treatment to obtain the BN-Si2N2O composite ceramic. The preparation method has the advantages that the preparation cost is reduced, the efficiency is improved, and the difficulty for preparing the large-size boron nitride based ceramic components is reduced. The preparation method is mainly used for preparing the BN-Si2N2O composite ceramic.
Description
Technical field
The present invention relates to a kind of boron nitride-base ceramic material and preparation method thereof.
Background technology
Along with making rapid progress of science and technology, the maneuverability of the flight velocity of space vehicle is largely increased, and this has just proposed more harsh requirement to choosing of antenna windows or radome material.The High Mach number aircraft requires electromagnetic wave transparent material to have high heat resistance, good thermal shock resistance and stable dielectric properties, but the performance of existing ceramic wave-transmitting material obviously can't satisfy service requirements; Although the existing boron nitride-base matrix material of hot-press method preparation that adopts satisfies the requirement of High Mach number aircraft, but existing adopt hot-press method to prepare the boron nitride-base matrix material to have that preparation cost is high and efficient is low, and adopting hot-press method to prepare in boron nitride-base matrix material preparation process, hot pressing die to be had relatively high expectations (requires the volume of hot pressing die greater than the volume of product, otherwise can't prepare), therefore be difficult to prepare the problem of large size boron nitride-base ceramic member.
Summary of the invention
The objective of the invention is to solve the problem that existing boron nitride-base composite manufacture method exists that preparation cost is high, efficient is low and is difficult to prepare large size boron nitride-base ceramic member, a kind of BN-Si is provided
2N
2O composite ceramics and preparation method thereof.
A kind of BN-Si
2N
2O composite ceramics by volume per-cent is made by 15%～40% amorphous nano silicon-dioxide, 5%～30% alpha-silicon nitride powders and 30%～80% hexagonal boron nitride powder; And the volume ratio of wherein said alpha-silicon nitride powders and amorphous nano silicon oxide is less than 1.
A kind of BN-Si
2N
2The preparation method of O composite ceramics, specifically carry out in accordance with the following steps:
One, weighing: at first by volume per-cent measures 15%～40% amorphous nano silicon-dioxide, 5%～30% alpha-silicon nitride powders and 30%～80% hexagonal boron nitride powder, and the volume ratio of described alpha-silicon nitride powders and amorphous nano silicon oxide is less than 1;
Two, ball milling slurrying material: by volume per-cent measures 15%～40% amorphous silicon di-oxide, 5%～30% alpha-silicon nitride powders and 30%～80% hexagonal boron nitride powder is placed in container with step 1, then take dehydrated alcohol as medium, take zirconia ball as abrading-ball, in ratio of grinding media to material (10～20): 1 time ball milling 20h～24h namely obtains slurry; The mass ratio of the dehydrated alcohol described in step 2 and hexagonal boron nitride powder is (1.5～2.5): 1;
Three, dry powder process: the slurry that at first step 2 is obtained is dried, and grinds after oven dry again, excessively namely gets mixed powder after 200 mesh sieves;
Four, pre-molding: the mixed powder that at first step 3 is obtained is packed in mould, is then to carry out pre-molding under 10MPa～20MPa at pressure, namely obtains base substrate;
Five, isostatic cool pressing is processed: the base substrate that step 4 obtains is put into cold isostatic press, is pressurize 60s～120s under 150MPa～250MPa at pressure, namely obtains crude product to be sintered;
Six, sintering processes: temperature be 1700 ℃～1900 ℃ and nitrogen pressure be under the nitrogen protection of 1 standard atmospheric pressure to the crude product sintering 30min～90min to be sintered of step 5 preparation, then cool to room temperature with the furnace, namely obtain BN-Si
2N
2The O composite ceramics.
Advantage of the present invention: one, the present invention utilizes hexagonal boron nitride as body material, adds silicon-dioxide or silicon sol as sintering aid, adds Si
3N
4As third phase, by cold isostatic compaction, pressureless sintering preparation technology obtains the good electromagnetic wave transparent materials of over-all properties such as a kind of mechanical property and dielectric properties, all can the reach a high temperature service requirements of electromagnetic wave transparent material of its mechanical property and dielectric wave penetrate capability; Two, in the boron nitride-base wave-penetrating composite material of the present invention's preparation, take hexagonal boron nitride as body material, silicon-dioxide or silicon sol are sintering aid, Si
3N
4Be distributed between blapharoplast as wild phase, play the effect of reinforcement, and generate Si as reaction in－situ in the process of sintering
2N
2The forming core core of O; After sintering, the main phase of material is hexagonal boron nitride, Si
2N
2O and a small amount of silicon-dioxide; The Si that reaction generates
2N
2O has excellent hot strength and resistance to oxidation stability, has lower thermal expansivity and good thermal shock resistance, also has simultaneously excellent dielectric properties, is very important structural ceramic material and functional materials; So BN-Si of the present invention's preparation
2N
2Si in the O composite ceramics
2N
2O plays and improves material at high temperature intensity and thermal shock resistance, and improves the effect of high-temperature dielectric wave penetrate capability; So BN-Si of the present invention's preparation
2N
2The O composite ceramics can satisfy the requirement of High Mach number aircraft; Three, utilization of the present invention cold pressing premolding, through etc. static pressure process after the high temperature pressure-free sintering prepare BN-Si by reaction in－situ
2N
2The O composite ceramics.In the premolding process of colding pressing low-cost graphite or steel mould and etc. the employing of rubber package set in the static pressure process, avoided in hot pressing member process to the demand of heat-resistant high-strength graphite jig and high temperature hot pressing apparatus expensive and to problems such as processing requirement complexity, thereby be conducive to improve yield rate and production efficiency, reduce preparation cost.
Description of drawings
Fig. 1 is the XRD figure spectrum, and in Fig. 1, A represents to test the BN-Si of a preparation
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 1, B represents to test the BN-Si of two preparations
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 1, C represents to test the BN-Si of three preparations
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 1, D represents to test the BN-Si of four preparations
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 1, E represents to test the BN-Si of five preparations
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 1, ■ represents the diffraction peak of BN, in Fig. 1 ◆ expression Si
2N
2The diffraction peak of O, in Fig. 1, ▽ represents α-Si
3N
4Diffraction peak, in Fig. 1, ▼ represents β-Si
3N
4Diffraction peak;
Fig. 2 is the XRD figure spectrum, and in Fig. 2, A represents to test the BN-Si of six preparations
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 2, B represents to test the BN-Si of seven preparations
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 2, C represents to test the BN-Si of eight preparations
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 2, D represents to test the BN-Si of nine preparations
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 2, E represents to test the BN-Si of ten preparations
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 2, ■ represents the diffraction peak of BN, in Fig. 2 ◆ expression Si
2N
2The diffraction peak of O, in Fig. 2, ▽ represents α-Si
3N
4Diffraction peak.
Embodiment
Embodiment one: present embodiment is a kind of BN-Si
2N
2O composite ceramics by volume per-cent is made by 15%～40% amorphous nano silicon-dioxide, 5%～30% alpha-silicon nitride powders and 30%～80% hexagonal boron nitride powder; And the volume ratio of wherein said alpha-silicon nitride powders and amorphous nano silicon oxide is less than 1.
The volume fraction sum of the described amorphous nano silicon-dioxide of present embodiment, alpha-silicon nitride powders and hexagonal boron nitride powder is 100%.
The described BN-Si of present embodiment
2N
2Contain Si in the O composite ceramics
2N
2O, Si
2N
2O is at BN-Si
2N
2Play in the O composite ceramics and improve material at high temperature intensity and thermal shock resistance, and improve the effect of high-temperature dielectric wave penetrate capability; So described BN-Si of present embodiment
2N
2The O composite ceramics can satisfy the requirement of High Mach number aircraft;
Embodiment two: the difference of present embodiment and embodiment one is: described amorphous nano silicon-dioxide is amorphous nano SiO 2 powder or silicon sol; Wherein said amorphous nano SiO 2 powder median size is 0.9 μ m～3 μ m; Amorphous Si O in wherein said silicon sol
2The granular mass mark is 30%, and amorphous Si O in silicon sol
2The median size of particle is 9nm～13nm.Other are identical with embodiment one.
Embodiment three: present embodiment and one of embodiment one or two difference are: the median size of described alpha-silicon nitride powders is 1 μ m～1.5 μ m; The median size of described hexagonal boron nitride powder is 0.9 μ m～1.5 μ m.Other are identical with embodiment one or two.
Embodiment four: one of present embodiment and embodiment one to three difference is: described BN-Si
2N
2O composite ceramics by volume per-cent is made by 20%～30% amorphous nano silicon-dioxide, 10%～20% alpha-silicon nitride powders and 50%～70% hexagonal boron nitride powder.Other are identical with embodiment one to three.
The volume fraction sum of the described amorphous nano silicon-dioxide of present embodiment, alpha-silicon nitride powders and hexagonal boron nitride powder is 100%.
Embodiment five: present embodiment is a kind of BN-Si
2N
2The preparation method of O composite ceramics, specifically carry out in accordance with the following steps:
One, weighing: at first by volume per-cent measures 15%～40% amorphous nano silicon-dioxide, 5%～30% alpha-silicon nitride powders and 30%～80% hexagonal boron nitride powder, and the volume ratio of described alpha-silicon nitride powders and amorphous nano silicon oxide is less than 1;
Two, ball milling slurrying material: by volume per-cent measures 15%～40% amorphous silicon di-oxide, 5%～30% alpha-silicon nitride powders and 30%～80% hexagonal boron nitride powder is placed in container with step 1, then take dehydrated alcohol as medium, take zirconia ball as abrading-ball, in ratio of grinding media to material (10～20): 1 time ball milling 20h～24h namely obtains slurry; The mass ratio of the dehydrated alcohol described in step 2 and hexagonal boron nitride powder is (1.5～2.5): 1;
Three, dry powder process: the slurry that at first step 2 is obtained is dried, and grinds after oven dry again, excessively namely gets mixed powder after 200 mesh sieves;
Four, pre-molding: the mixed powder that at first step 3 is obtained is packed in mould, is then to carry out pre-molding under 10MPa～20MPa at pressure, namely obtains base substrate;
Five, isostatic cool pressing is processed: the base substrate that step 4 obtains is put into cold isostatic press, is pressurize 60s～120s under 150MPa～250MPa at pressure, namely obtains crude product to be sintered;
Six, sintering processes: temperature be 1700 ℃～1900 ℃ and nitrogen pressure be under the nitrogen protection of 1 standard atmospheric pressure to the crude product sintering 30min～90min to be sintered of step 5 preparation, then cool to room temperature with the furnace, namely obtain BN-Si
2N
2The O composite ceramics.
The volume fraction sum of amorphous nano silicon-dioxide, alpha-silicon nitride powders and the hexagonal boron nitride powder described in the present embodiment step 1 is 100%.
Present embodiment utilizes hexagonal boron nitride as body material, adds silicon-dioxide or silicon sol as sintering aid, adds Si
3N
4As third phase, by cold isostatic compaction, pressureless sintering preparation technology obtains the good electromagnetic wave transparent materials of over-all properties such as a kind of mechanical property and dielectric properties, all can the reach a high temperature service requirements of electromagnetic wave transparent material of its mechanical property and dielectric wave penetrate capability.
In the boron nitride-base wave-penetrating composite material of present embodiment preparation, take hexagonal boron nitride as body material, silicon-dioxide or silicon sol are sintering aid, Si
3N
4Be distributed between blapharoplast as wild phase, play the effect of reinforcement, and generate Si as reaction in－situ in the process of sintering
2N
2The forming core core of O; After sintering, the main phase of material is hexagonal boron nitride, Si
2N
2O and a small amount of silicon-dioxide; The Si that reaction generates
2N
2O has excellent hot strength and resistance to oxidation stability, has lower thermal expansivity and good thermal shock resistance, also has simultaneously excellent dielectric properties, is very important structural ceramic material and functional materials; So BN-Si of present embodiment preparation
2N
2Si in the O composite ceramics
2N
2O plays and improves material at high temperature intensity and thermal shock resistance, and improves the effect of high-temperature dielectric wave penetrate capability; So BN-Si of present embodiment preparation
2N
2The O composite ceramics can satisfy the requirement of High Mach number aircraft.
The present embodiment utilization cold pressing premolding, through etc. static pressure process after the high temperature pressure-free sintering prepare BN-Si by reaction in－situ
2N
2The O composite ceramics.In the premolding process of colding pressing low-cost graphite or steel mould and etc. the employing of rubber package set in the static pressure process, avoided in hot pressing member process to the demand of heat-resistant high-strength graphite jig and high temperature hot pressing apparatus expensive and to problems such as processing requirement complexity, thereby be conducive to improve yield rate and production efficiency, reduce preparation cost.
Embodiment six: the difference of present embodiment and embodiment five is: the amorphous nano silicon-dioxide described in step 1 is amorphous nano SiO 2 powder or silicon sol; Wherein said amorphous nano SiO 2 powder median size is 0.9 μ m～3 μ m; In wherein said silicon sol, amorphous Si 02 granular mass mark is 30%, and amorphous Si O in silicon sol
2The median size of particle is 9nm～13nm.Other are identical with embodiment five.
Embodiment seven: present embodiment and one of embodiment five or six difference are: the median size of alpha-silicon nitride powders described in step 1 is 1 μ m～1.5 μ m; The median size of hexagonal boron nitride powder described in step 1 is 0.9 μ m～1.5 μ m.Other are identical with embodiment five or six.
Embodiment eight: one of present embodiment and embodiment five to seven difference is: in step 1 at first by volume per-cent measure 20%～30% amorphous nano silicon-dioxide, 10%～20% alpha-silicon nitride powders and 50%～70% hexagonal boron nitride powder.Other are identical with embodiment five to seven.
The volume fraction sum of the described amorphous nano silicon-dioxide of present embodiment, alpha-silicon nitride powders and hexagonal boron nitride powder is 100%.
Embodiment nine: one of present embodiment and embodiment five to eight difference is: the base substrate that in step 5, step 4 is obtained is put into cold isostatic press, is pressurize 90～120s under 200MPa～250MPa at pressure, namely obtains crude product to be sintered.Other are identical with embodiment five to eight.
Embodiment ten: one of present embodiment and embodiment five to nine difference is: be that 1750 ℃～1850 ℃ and nitrogen pressure are to the crude product sintering 45min～75min to be sintered of step 5 preparation under the nitrogen protection of 1 standard atmospheric pressure in temperature in step 6; then cool to room temperature with the furnace, namely obtain BN-Si
2N
2The O composite ceramics.Other are identical with embodiment five to nine.
Adopt following verification experimental verification effect of the present invention:
Test one: a kind of BN-Si
2N
2The preparation method of O composite ceramics, specifically carry out in accordance with the following steps:
One, weighing: at first by volume per-cent measures 30% amorphous nano silicon-dioxide, 5% alpha-silicon nitride powders and 65% hexagonal boron nitride powder;
Two, ball milling slurrying material: by volume per-cent measures 30% amorphous nano silicon-dioxide, 5% alpha-silicon nitride powders and 65% hexagonal boron nitride powder is placed in container with step 1, then take dehydrated alcohol as medium, take zirconia ball as abrading-ball, ball milling 24h under ratio of grinding media to material 15:1 namely obtains slurry; The mass ratio of the dehydrated alcohol described in step 2 and hexagonal boron nitride powder is 2:1;
Three, dry powder process: the slurry that at first step 2 is obtained is dried, and grinds after oven dry again, excessively namely gets mixed powder after 200 mesh sieves;
Four, pre-molding: the mixed powder that at first step 3 is obtained is packed in mould, is then to carry out pre-molding under 20MPa at pressure, namely obtains base substrate;
Five, isostatic cool pressing is processed: the base substrate that step 4 obtains is put into cold isostatic press, is pressurize 90s under 200MPa at pressure, namely obtains crude product to be sintered;
Six, sintering processes: temperature be 1800 ℃ and nitrogen pressure be under the nitrogen protection of 1 standard atmospheric pressure to the crude product sintering 60min to be sintered of step 5 preparation, then cool to room temperature with the furnace, namely obtain BN-Si
2N
2The O composite ceramics.
Amorphous nano silicon-dioxide described in this testing sequence one is the amorphous nano SiO 2 powder; Wherein said amorphous nano SiO 2 powder median size is 0.9 μ m～3 μ m.
The median size of alpha-silicon nitride powders described in this testing sequence one is 1 μ m～1.5 μ m.
The median size of hexagonal boron nitride powder described in this testing sequence one is 0.9 μ m～1.5 μ m.
The BN-Si of this test preparation
2N
2The flexural strength of O composite ceramics (being labeled as the BS5 pottery) adopts the three-point bending method to test, fracture toughness property adopts monolateral breach beam three-point bending method test, and dielectric properties adopt the high-q cavity method to carry out the dielectric complex permittivity test under 18GHz～40GHz frequency; The flexural strength that records, fracture toughness property and dielectric properties data see Table 1.
Table 1
| Material | Flexural strength/MPa | Specific inductivity (21GHz) | Loss tangent (21GHz) |
| The BS5 pottery | 24.2±1.1 | 2.93 | 0.0048 |
Test two: the difference of this test and embodiment one is: in step 1 at first by volume per-cent measure 30% amorphous nano silicon-dioxide, 10% alpha-silicon nitride powders and 60% hexagonal boron nitride powder.Other are identical with test one.
The BN-Si of this test preparation
2N
2The flexural strength of O composite ceramics (being labeled as the BS10 pottery) adopts the three-point bending method to test, fracture toughness property adopts monolateral breach beam three-point bending method test, and dielectric properties adopt the high-q cavity method to carry out the dielectric complex permittivity test under 18GHz～40GHz frequency; The flexural strength that records, fracture toughness property and dielectric properties data see Table 2.
Table 2
| Material | Flexural strength/MPa | Specific inductivity (21GHz) | Loss tangent (21GHz) |
| The BS10 pottery | 26.9±2.5 | 3.01 | 0.0044 |
Test three: the difference of this test and embodiment one is: in step 1 at first by volume per-cent measure 30% amorphous nano silicon-dioxide, 15% alpha-silicon nitride powders and 55% hexagonal boron nitride powder.Other are identical with test one.
The BN-Si of this test preparation
2N
2The flexural strength of O composite ceramics (being labeled as the BS15 pottery) adopts the three-point bending method to test, fracture toughness property adopts monolateral breach beam three-point bending method test, and dielectric properties adopt the high-q cavity method to carry out the dielectric complex permittivity test under 18GHz～40GHz frequency; The flexural strength that records, fracture toughness property and dielectric properties data see Table 3.
Table 3
| Material | Flexural strength/MPa | Specific inductivity (21GHz) | Loss tangent (21GHz) |
| The BS15 pottery | 52.5±3.3 | 3.11 | 0.0048 |
Test four: the difference of this test and embodiment one is: in step 1 at first by volume per-cent measure 30% amorphous nano silicon-dioxide, 20% alpha-silicon nitride powders and 50% hexagonal boron nitride powder.Other are identical with test one.
The BN-Si of this test preparation
2N
2The flexural strength of O composite ceramics (being labeled as the BS20 pottery) adopts the three-point bending method to test, fracture toughness property adopts monolateral breach beam three-point bending method test, and dielectric properties adopt the high-q cavity method to carry out the dielectric complex permittivity test under 18GHz～40GHz frequency; The flexural strength that records, fracture toughness property and dielectric properties data see Table 4.
Table 4
| Material | Flexural strength/MPa | Specific inductivity (21GHz) | Loss tangent (21GHz) |
| The BS20 pottery | 36.8±1.8 | 3.31 | 0.0051 |
Test five: the difference of this test and embodiment one is: in step 1 at first by volume per-cent measure 30% amorphous nano silicon-dioxide, 30% alpha-silicon nitride powders and 40% hexagonal boron nitride powder.Other are identical with test one.
The BN-Si of this test preparation
2N
2The flexural strength of O composite ceramics (being labeled as the BS30 pottery) adopts the three-point bending method to test, fracture toughness property adopts monolateral breach beam three-point bending method test, and dielectric properties adopt the high-q cavity method to carry out the dielectric complex permittivity test under 18GHz～40GHz frequency; The flexural strength that records, fracture toughness property and dielectric properties data see Table 5.
Table 5
| Material | Flexural strength/MPa | Specific inductivity (21GHz) | Loss tangent (21GHz) |
| The BS30 pottery | 35.9±3.6 | 3.16 | 0.0053 |
Adopt X-ray diffractometer to detect test one to the BN-Si of test five preparations
2N
2O composite ceramics, detected result as shown in Figure 1, Fig. 1 is XRD figure spectrum, in Fig. 1, A represents to test the BN-Si of a preparation
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 1, B represents to test the BN-Si of two preparations
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 1, C represents to test the BN-Si of three preparations
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 1, D represents to test the BN-Si of four preparations
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 1, E represents to test the BN-Si of five preparations
2N
2The XRD figure spectrum of O composite ceramics is in Fig. 1
■The diffraction peak of expression BN is in Fig. 1 ◆ expression Si
2N
2The diffraction peak of O, in Fig. 1, ▽ represents α-Si
3N
4Diffraction peak, in Fig. 1, ▼ represents β-Si
3N
4Diffraction peak; As can be seen from Figure 1, when amorphous silicon di-oxide is introduced with powder type, along with Si
3N
4Introducing, in matrix material, Si is arranged after the high temperature pressure-free sintering
2N
2The generation of O.
Test six: this test with the difference of embodiment one is: the amorphous nano silicon-dioxide described in step 1 is silicon sol; In wherein said silicon sol, amorphous Si 0
2The granular mass mark is 30%, and amorphous Si 0 in silicon sol
2The median size of particle is 9nm～13nm.。Other are identical with test one.
The BN-Si of this test preparation
2N
2The flexural strength of O composite ceramics (being labeled as the BSR5 pottery) adopts the three-point bending method to test, fracture toughness property adopts monolateral breach beam three-point bending method test, and dielectric properties adopt the high-q cavity method to carry out the dielectric complex permittivity test under 18GHz～40GHz frequency; The flexural strength that records, fracture toughness property and dielectric properties data see Table 6.
Table 6
| Material | Flexural strength/MPa | Specific inductivity (21GHz) | Loss tangent (21GHz) |
| The BSR5 pottery | 14.5±2.0 | 2.90 | 0.0032 |
Test seven: the difference of this test and embodiment six is: in step 1 at first by volume per-cent measure 30% amorphous nano silicon-dioxide, 10% alpha-silicon nitride powders and 60% hexagonal boron nitride powder.Other are identical with test six.
The BN-Si of this test preparation
2N
2The flexural strength of O composite ceramics (being labeled as the BSR10 pottery) adopts the three-point bending method to test, fracture toughness property adopts monolateral breach beam three-point bending method test, and dielectric properties adopt the high-q cavity method to carry out the dielectric complex permittivity test under 18GHz～40GHz frequency; The flexural strength that records, fracture toughness property and dielectric properties data see Table 7.
Table 7
| Material | Flexural strength/MPa | Specific inductivity (21GHz) | Loss tangent (21GHz) |
| The BSR10 pottery | 23.2±5.2 | 2.90 | 0.0040 |
Test eight: the difference of this test and embodiment six is: in step 1 at first by volume per-cent measure 30% amorphous nano silicon-dioxide, 15% alpha-silicon nitride powders and 55% hexagonal boron nitride powder.Other are identical with test six.
The BN-Si of this test preparation
2N
2The flexural strength of O composite ceramics (being labeled as the BSR15 pottery) adopts the three-point bending method to test, fracture toughness property adopts monolateral breach beam three-point bending method test, and dielectric properties adopt the high-q cavity method to carry out the dielectric complex permittivity test under 18GHz～40GHz frequency; The flexural strength that records, fracture toughness property and dielectric properties data see Table 8.
Table 8
| Material | Flexural strength/MPa | Specific inductivity (21GHz) | Loss tangent (21GHz) |
| The BSR15 pottery | 21.1±2.3 | 3.33 | 0.0040 |
Test nine: the difference of this test and embodiment six is: in step 1 at first by volume per-cent measure 30% amorphous nano silicon-dioxide, 20% alpha-silicon nitride powders and 50% hexagonal boron nitride powder.Other are identical with test six.
The BN-Si of this test preparation
2N
2The flexural strength of O composite ceramics (being labeled as the BSR20 pottery) adopts the three-point bending method to test, fracture toughness property adopts monolateral breach beam three-point bending method test, and dielectric properties adopt the high-q cavity method to carry out the dielectric complex permittivity test under 18GHz～40GHz frequency; The flexural strength that records, fracture toughness property and dielectric properties data see Table 9.
Table 9
| Material | Flexural strength/MPa | Specific inductivity (21GHz) | Loss tangent (21GHz) |
| BSR20 | 25.9±1.9 | 3.24 | 0.0038 |
Test ten: the difference of this test and embodiment six is: in step 1 at first by volume per-cent measure 30% amorphous nano silicon-dioxide, 30% alpha-silicon nitride powders and 40% hexagonal boron nitride powder.Other are identical with test six.
The BN-Si of this test preparation
2N
2The flexural strength of O composite ceramics (being labeled as the BSR30 pottery) adopts the three-point bending method to test, fracture toughness property adopts monolateral breach beam three-point bending method test, and dielectric properties adopt the high-q cavity method to carry out the dielectric complex permittivity test under 18GHz～40GHz frequency; The flexural strength that records, fracture toughness property and dielectric properties data see Table 10.
Table 10
| Material | Flexural strength/MPa | Specific inductivity (21GHz) | Loss tangent (21GHz) |
| BSR30 | 33.2±1.2 | 3.19 | 0.0052 |
Adopt X-ray diffractometer to detect test six to the BN-Si of test ten preparations
2N
2O composite ceramics, detected result as shown in Figure 2, Fig. 2 is XRD figure spectrum, in Fig. 2, A represents to test the BN-Si of six preparations
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 2, B represents to test the BN-Si of seven preparations
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 2, C represents to test the BN-Si of eight preparations
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 2, D represents to test the BN-Si of nine preparations
2N
2The XRD figure spectrum of O composite ceramics, in Fig. 2, E represents to test the BN-Si of ten preparations
2N
2The XRD figure spectrum of O composite ceramics is in Fig. 2
■The diffraction peak of expression BN is in Fig. 2 ◆ expression Si
2N
2The diffraction peak of O, in Fig. 2, ▽ represents α-Si
3N
4Diffraction peak; As can be seen from Figure 2, when amorphous silicon di-oxide is introduced with the silicon sol form, along with Si
3N
4Introducing, in matrix material, Si is arranged after the high temperature pressure-free sintering
2N
2The generation of O.
Claims (10)
1. BN-Si
2N
2The O composite ceramics is characterized in that BN-Si
2N
2O composite ceramics by volume per-cent is made by 15%～40% amorphous nano silicon-dioxide, 5%～30% alpha-silicon nitride powders and 30%～80% hexagonal boron nitride powder; And the volume ratio of wherein said alpha-silicon nitride powders and amorphous nano silicon oxide is less than 1.
2. a kind of BN-Si according to claim 1
2N
2The O composite ceramics is characterized in that described amorphous nano silicon-dioxide is amorphous nano SiO 2 powder or silicon sol; Wherein said amorphous nano SiO 2 powder median size is 0.9 μ m～3 μ m; Amorphous Si O in wherein said silicon sol
2The granular mass mark is 30%, and amorphous Si 0 in silicon sol
2The median size of particle is 9nm～13nm.
3. a kind of BN-Si according to claim 1
2N
2O composite ceramics, the median size that it is characterized in that described described alpha-silicon nitride powders are 1 μ m～1.5 μ m; The median size of described hexagonal boron nitride powder is 0.9 μ m～1.5 μ m.
4. according to claim 1,2 or 3 described a kind of BN-Si
2N
2The O composite ceramics is characterized in that described BN-Si
2N
2O composite ceramics by volume per-cent is made by 20%～30% amorphous nano silicon-dioxide, 10%～20% alpha-silicon nitride powders and 50%～70% hexagonal boron nitride powder.
5. a kind of BN-Si as claimed in claim 1
2N
2The preparation method of O composite ceramics is characterized in that BN-Si
2N
2The preparation method of O composite ceramics carries out in accordance with the following steps:
One, weighing: at first by volume per-cent measures 15%～40% amorphous nano silicon-dioxide, 5%～30% alpha-silicon nitride powders and 30%～80% hexagonal boron nitride powder, and the volume ratio of described alpha-silicon nitride powders and amorphous nano silicon oxide is less than 1;
Two, ball milling slurrying material: by volume per-cent measures 15%～40% amorphous silicon di-oxide, 5%～30% alpha-silicon nitride powders and 30%～80% hexagonal boron nitride powder is placed in container with step 1, then take dehydrated alcohol as medium, take zirconia ball as abrading-ball, in ratio of grinding media to material (10～20): 1 time ball milling 20h～24h namely obtains slurry; The mass ratio of the dehydrated alcohol described in step 2 and hexagonal boron nitride powder is (1.5～2.5): 1;
Three, dry powder process: the slurry that at first step 2 is obtained is dried, and grinds after oven dry again, excessively namely gets mixed powder after 200 mesh sieves;
Four, pre-molding: the mixed powder that at first step 3 is obtained is packed in mould, is then to carry out pre-molding under 10MPa～20MPa at pressure, namely obtains base substrate;
Five, isostatic cool pressing is processed: the base substrate that step 4 obtains is put into cold isostatic press, is pressurize 60s～120s under 150MPa～250MPa at pressure, namely obtains crude product to be sintered;
Six, sintering processes: temperature be 1700 ℃～1900 ℃ and nitrogen pressure be under the nitrogen protection of 1 standard atmospheric pressure to the crude product sintering 30min～90min to be sintered of step 5 preparation, then cool to room temperature with the furnace, namely obtain BN-Si
2N
2The O composite ceramics.
6. a kind of BN-Si according to claim 5
2N
2The preparation method of O composite ceramics is characterized in that the amorphous nano silicon-dioxide described in step 1 is amorphous nano SiO 2 powder or silicon sol; Wherein said amorphous nano SiO 2 powder median size is 0.9 μ m～3 μ m; In wherein said silicon sol, amorphous Si 02 granular mass mark is 30%, and amorphous Si 0 in silicon sol
2The median size of particle is 9nm～13nm.
7. a kind of BN-Si according to claim 5
2N
2The preparation method of O composite ceramics, the median size that it is characterized in that alpha-silicon nitride powders described in step 1 are 1 μ m～1.5 μ m; The median size of hexagonal boron nitride powder described in step 1 is 0.9 μ m～1.5 μ m.
8. according to claim 5,6 or 7 described a kind of BN-Si
2N
2The preparation method of O composite ceramics is characterized in that in step 1 that at first by volume per-cent measures 20%～30% amorphous nano silicon-dioxide, 10%～20% alpha-silicon nitride powders and 50%～70% hexagonal boron nitride powder.
9. a kind of BN-Si according to claim 8
2N
2The preparation method of O composite ceramics is characterized in that the base substrate that in step 5, step 4 is obtained puts into cold isostatic press, is pressurize 90～120s under 200MPa～250MPa at pressure, namely obtains crude product to be sintered.
10. a kind of BN-Si according to claim 8
2N
2The preparation method of O composite ceramics; it is characterized in that in step 6 in temperature being that 1750 ℃～1850 ℃ and nitrogen pressure are to the crude product sintering 45min～75min to be sintered of step 5 preparation under the nitrogen protection of 1 standard atmospheric pressure; then cool to room temperature with the furnace, namely obtain BN-Si
2N
2The O composite ceramics.
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103964860A (en) * | 2014-05-05 | 2014-08-06 | 哈尔滨工业大学 | Boron nitride-based wave-transparent composite material prepared by nano silica sol as sintering aid and preparation method of composite material |
| CN105541340A (en) * | 2015-12-11 | 2016-05-04 | 天津城建大学 | Nitride ceramic-microcrystalline glass composite material and preparation method thereof |
| CN115180957A (en) * | 2022-07-11 | 2022-10-14 | 哈尔滨工业大学 | Preparation method of hexagonal boron nitride ceramic with excellent thermal wave transmission performance |
| CN116332654A (en) * | 2023-03-23 | 2023-06-27 | 西安理工大学 | BN/SiBN/Si with onion-like microstructure 3 N 4 /Si 2 N 2 O/Si 3 N 4 Preparation method of composite material |
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| CN1562885A (en) * | 2004-04-14 | 2005-01-12 | 哈尔滨工业大学 | Method preparing BN/SiO2 composite ceramics through dipping, and cracking precursor body |
| CN1569743A (en) * | 2004-04-23 | 2005-01-26 | 山东工业陶瓷研究设计院 | Silicon nitride - boron nitride- silicon dioxide ceramic wave-transparent material and preparation process thereof |
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| Publication number | Priority date | Publication date | Assignee | Title |
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| CN1562885A (en) * | 2004-04-14 | 2005-01-12 | 哈尔滨工业大学 | Method preparing BN/SiO2 composite ceramics through dipping, and cracking precursor body |
| CN1569743A (en) * | 2004-04-23 | 2005-01-26 | 山东工业陶瓷研究设计院 | Silicon nitride - boron nitride- silicon dioxide ceramic wave-transparent material and preparation process thereof |
Cited By (6)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN103964860A (en) * | 2014-05-05 | 2014-08-06 | 哈尔滨工业大学 | Boron nitride-based wave-transparent composite material prepared by nano silica sol as sintering aid and preparation method of composite material |
| CN105541340A (en) * | 2015-12-11 | 2016-05-04 | 天津城建大学 | Nitride ceramic-microcrystalline glass composite material and preparation method thereof |
| CN105541340B (en) * | 2015-12-11 | 2018-05-08 | 天津城建大学 | Nitride ceramics-glass ceramic composite and preparation method thereof |
| CN115180957A (en) * | 2022-07-11 | 2022-10-14 | 哈尔滨工业大学 | Preparation method of hexagonal boron nitride ceramic with excellent thermal wave transmission performance |
| CN116332654A (en) * | 2023-03-23 | 2023-06-27 | 西安理工大学 | BN/SiBN/Si with onion-like microstructure 3 N 4 /Si 2 N 2 O/Si 3 N 4 Preparation method of composite material |
| CN116332654B (en) * | 2023-03-23 | 2024-02-09 | 西安理工大学 | BN/SiBN/Si with onion-like microstructure 3 N 4 /Si 2 N 2 O/Si 3 N 4 Preparation method of composite material |
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