CN102709258A - Diamond-silicon composite material - Google Patents
Diamond-silicon composite material Download PDFInfo
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- CN102709258A CN102709258A CN2012101922746A CN201210192274A CN102709258A CN 102709258 A CN102709258 A CN 102709258A CN 2012101922746 A CN2012101922746 A CN 2012101922746A CN 201210192274 A CN201210192274 A CN 201210192274A CN 102709258 A CN102709258 A CN 102709258A
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Abstract
The invention relates to a diamond-silicon composite material. The diamond-silicon composite material is prepared by the following steps: 1) selecting diamond and silicon powder as initial materials and adding aluminum powder and aluminum nitride which serve as sintering accelerators; 2) mixing the components completely and uniformly; 3) selecting a graphite die of phi 20mm, placing the mixture into the graphite container and placing into a discharging plasma sintering furnace; 4) vacuumizing the discharging plasma sintering furnace and quickly sintering when the vacuum degree reaches below 12 to 15 Pa; 5) maintaining the sintering temperature for 4 to 5 minutes after reaching the sintering temperature and sintering under the vacuum or inert gas environment, wherein in the sintering process, the pressure is 35 to 39 MPa and the heating speed is 80 to 120 DEG C per minute and the sintering temperature is set to be 1,280 to 1,320 DEG C; and 6) performing furnace cooling on the products after the sintering is finished and releasing the pressure at the temperature of between 900 and 950 DEG C. The diamond-silicon composite material has simple equipment and process and low synthesis temperature, improves the density of the products and reduces the microcrack of the products to the maximum degree, and has high comprehensive performance of the products.
Description
Technical field
The present invention relates to a kind of electronic package material, relate in particular to a kind of preparation method of the diamond-silicon composite that makes through flash sintering method.
Background technology
Development of modern science and technology improves the requirement of material day by day.In the Electronic Packaging field, along with the complexity and the intensive of components and parts in electronic device and the electronic installation improves day by day, the exploitation excellent performance, the electronic devices and components enclosed chip that can satisfy various requirement has become the task of top priority.
The Electronic Packaging substrate material is a kind of base electronic component, is used to carry electronic devices and components and phase interconnection line thereof, and the matrix with good electrical insulating properties.Therefore enclosed chip must keep good coupling with components and parts placed on it aspect electrical properties, physical property, chemical property.Usually, enclosed chip should possess following character: (1) heat conductivility is good.Thermal conductivity is one of main performance index of Electronic Packaging substrate material.To influence the life-span of electronic equipment and operation conditions in addition if enclosed chip can not in time dispel the heat, temperature distributing disproportionation is even also can to cause electronic device noise to increase greatly; (2) coefficient of linear expansion coupling (main and Si and GaAs).If the two thermal coefficient of expansion differs bigger, the rapid thermal cycles during electronic device work is prone to introduce thermal stress and causes losing efficacy; (3) high frequency characteristics is good, promptly low dielectric constant and low dielectric loss.Because on high-speed transfer wiring lines circuit, be directly proportional with substrate material dielectric constant square root signal delay time.For satisfying requirement, require the enclosed chip material dielectric constant low as high-speed transfer speed device.In addition, the Electronic Packaging substrate also should have the mechanical performance height, electrical insulation capability is good, chemical property is stable (Corrosion of Metallic Materials is used in electroplating processes liquid, wiring), be easy to characteristics such as processing.Certainly, in practical application and large-scale industrial production, price factor also is a very important aspect.
The kind of Electronic Packaging substrate material is a lot, and common used material comprises: pottery, metal and metal-base composites, diamond etc.Some material has been obtained comparatively ripe application on Electronic Packaging.But with regard to above-mentioned various performance requirements, most materials all can not satisfy above-mentioned all requirements.
Ceramic material is a kind of substrate material commonly used in the Electronic Packaging; Its major advantage is: high insulation property and excellent high frequency characteristics; Have the linear expansivity close with components and parts, very high chemical stability and thermal conductivity (λ) preferably, in addition; Ceramic material also has good comprehensive performances, is widely used in hybrid integrated circuit (HIC) and multicore sheet module (MCM) ceramic packaging and often is multi-layered ceramic substrate (MLC).This technology starts from the casting technique patent of JL Park in 1961 invention, and the founder of ceramic packaging is considered to Bernard Schwartz, because of research department's exploitation of his leader and have the encapsulation technology patents of many relevant MLC.From the sixties so far, lamination multi-layered ceramic substrate and encapsulating material and technology are studied and released in developed countries such as U.S.A, day in succession, ceramic substrate has been one of several kinds of high-performance ceramicss of extensive use in the world today.At present, the high heat-conducting ceramic substrate material that has been used for actual production and Application and Development mainly comprises Al2O3, AlN, SiC and BeO etc.
The metal-base composites that is used for enclosed chip is mainly Cu base and Al based composites.The Cu based composites adopts materials such as C fiber, B fiber etc., SiC particle to do the enhancing body, and the fibre-reinforced low bulk that obtains, high heat conduction Cu based composites have better comprehensive performance.For example the superficial expansivity of P130 graphite fibre Reinforced Cu-Base Composites is 6.5 * 10-6/K, and is keeping can also adding among the high thermal Cu W, Mo and low-expansion alloy powder such as (like the FeNi alloys).When making W/Cu or Mo/Cu composite material, Cu is penetrated among the W, Mo agglomerate of porous, to keep the continuity of each phase.The coefficient of linear expansion of this material can be adjusted according to the variation of constituent element relative amount, yet the copper basis material exists that wetability is low, thermal coefficient of expansion and density is all than problems such as height.Aluminum matrix composite not only has characteristics such as specific strength, specific stiffness height; And good heat conductivity, coefficient of linear expansion is adjustable, density is lower; Selection as the Electronic Packaging components and parts; Enhancing body commonly used comprises C, B, carbide (like SiC, TiC), nitride (like Si3N4) and oxide (like Al2O3, SiO2), and matrix alloy then can be pure Al or alloy.Because the coefficient of linear expansion of aluminium alloy itself is bigger, for making semi-conducting materials such as its coefficient of linear expansion and Si, Ge, GaAs close, usually has to adopt the enhancing body of high-volume fractional compound with it, addition even up to 70%.
Natural diamond has as semiconductor packages the most excellent necessary character, like high thermal conductivity (2000 W/mK, 25 ℃), low-k (5.5), high resistivity (1016 Ω cm) and disruptive field intensity (1000 kV/ mm).From the 60's of this century; Microelectronics circle begins to utilize the effort of diamond as the semiconductor packages substrate; And with diamond as heat sink material, be used on microwave avalanche diode, Ge IMPATT and the laser, successfully improved their power output.But the restriction of diamond synthesis fancy price and size under natural diamond or the HTHP makes this technology can't large-scale promotion.Comparatively ideal is to be equipped with composite material with diamond particles as strengthening system; The HIGH-PURITY SILICON material has lower density, high heat-conducting property and lower thermal coefficient of expansion; Silicon and diamond wetability are good; Generate carborundum at silicon and diamond interface place in the sintering process, reduced interface resistance.Therefore, the diamond/carbon silicon composite becomes one of focus of electronic package material research at present.
Because diamond easy graphitization when high temperature; Prior art for preparing diamond-silicon carbide composite material by adopting be infiltration method, specifically be with diamond and silica flour layering assembling, and be pressurized to very high force value; At high temperature carry out sintering again; This method is high to production environment, production equipment and operation technological requirement, and the finished product rate is low, and manufacturing cost is very high.
Summary of the invention
The object of the present invention is to provide a kind of diamond-silicon composite, this method prepared composite material interface contact is firm, and preparation technology is simple, and density and thermal property are significantly increased.
To achieve these goals, the technology side of the present invention's employing is: a kind of diamond-silicon composite is characterized in that the weight ratio of its each component is: C:Si:Al:N is 19.6～30.4:27.2～33.3:1.02～3.5:0.17 ~ 0.4; And this material makes through following steps:
1) selecting granularity is the diamond of 18～23 μ m, and granularity is 40～45 μ m, purity at 99. 99% silica flour as original material, and adds aluminium powder and aluminium nitride as sintering aids; The ratio of weight and number of diamond, silica flour, aluminium powder, aluminium nitride is 19.6～30.4:27.2～33.3:0.85～2.7:0.5 ~ 1.3;
2) said components is fully mixed after;
3) select the graphite jig of φ 20 mm, with pack into crystal vessel and put into the discharge plasma sintering stove of said mixture;
4) at the discharge plasma sintering stove evacuation, when vacuum degree reaches the Fast Sintering of beginning below 12 ~ 15Pa;
5) institute's plus-pressure is 35～39MPa in the sintering process, and programming rate is 80 ~ 120 ℃/minute, and sintering temperature is set at 1280～1320 ℃, reach after the sintering temperature to keep 4-5 minute, and under vacuum or inert gas environment sintering;
6) sintering finishes the back product is carried out laying down with the stove cooling and 900-950 ℃ the time pressure.
Discharge plasma sintering (Spark Plasma Sintering; SPS) be a kind of novel Fast Sintering technology that development in recent years is got up; It melts plasma activation, hot pressing is one; Have that programming rate is fast, sintering time is short, cooling rapidly, impressed pressure and characteristics such as sintering atmosphere is controlled, energy-conserving and environment-protective; But discharging plasma sintering equipment is similar to hot-pressed sintering furnace, and different is to add the controllable pulse electric current to a pressure-bearing conductive die, through galvanic size control programming rate of regulating impulse and sintering temperature.Also do not see at present the report that discharge plasma sintering technique is used to prepare diamond-silicon composite.
The present invention specifically applies to the preparation of diamond-silicon composite with discharge plasma sintering, makes the silicon substrate particle under the silicon fusing point, in-situ chemical reaction take place in sintering process and diamond particles, generates the interface silicon carbide layer.And the present invention is through a large amount of tests, selected best set of dispense than and technological parameter, can effectively stop the diamond graphitization in utmost point chien shih sample densification in short-term.In addition; Through adding aluminium powder and aluminium nitride as auxiliary agent, reduced the fusing point of silicon, improved sintered density thereby reduced sintering temperature; Because aluminium all dissolves and is liquid under the hot conditions; Diffusion coefficient is bigger, and aluminium all is diffused into silicon and at the interface adamantine, and aluminium nitride stops the diamond graphitization simultaneously.
Beneficial effect of the present invention is; Equipment and technology are simple, synthesis temperature is low, and prepared composite material density reaches more than 99%, and thermal conductivity is 480-510W/mK; Thereby farthest improve the product density, reduce the product micro-crack, The comprehensive performance is good.
Embodiment
Below set forth technical scheme of the present invention through specific embodiment; Wherein, The discharge plasma sintering stove (SPS) that Fast Sintering adopted among the present invention is the Dr Sinter that SUMITOMO CHEMICAL stone carbon mining industry Co., Ltd. produces, SPS-1050 discharge plasma sintering stove.
Embodiment 1:
1) selecting granularity is the diamond of 19 μ m, and granularity is 40 μ m, purity at 99. 99% silica flour as original material, and adds aluminium powder and aluminium nitride as sintering aids; The ratio of weight and number of diamond, silica flour, aluminium powder, aluminium nitride is 19.6:33.3:2.7:0.5;
2) said components is fully mixed after;
3) select the graphite jig of φ 20 mm, with pack into crystal vessel and put into the discharge plasma sintering stove of said mixture;
4),, vacuum degree begins Fast Sintering below the 12Pa when reaching at the discharge plasma sintering stove evacuation;
5) institute's plus-pressure is 35MPa in the sintering process, and programming rate is 120 ℃/minute, and sintering temperature is set at 1280 ℃, reach after the sintering temperature to keep 4 minutes, and under vacuum or inert gas environment sintering;
6) sintering finishes the back product is carried out laying down with the stove cooling and 950 ℃ the time pressure.
Through test, the density of the product that obtains is more than 99.2%, and thermal conductivity is 492W/mK.
Embodiment 2:
1) selecting granularity is the diamond of 23 μ m, and granularity is 45 μ m, purity at 99. 99% silica flour as original material, and adds aluminium powder and aluminium nitride as sintering aids; The ratio of weight and number of diamond, silica flour, aluminium powder, aluminium nitride is 30.4:27.2:0.85:1.3;
2) said components is fully mixed after;
3) select the graphite jig of φ 20 mm, with pack into crystal vessel and put into the discharge plasma sintering stove of said mixture;
4),, vacuum degree begins Fast Sintering below the 15Pa when reaching at the discharge plasma sintering stove evacuation;
5) institute's plus-pressure is 35MPa in the sintering process, and programming rate is 80 ℃/minute, and sintering temperature is set at 1320 ℃, reach after the sintering temperature to keep 5 minutes, and under vacuum or inert gas environment sintering;
6) sintering finishes the back product is carried out laying down with the stove cooling and 900 ℃ the time pressure.
Through test, its density is more than 99.3%, and thermal conductivity is 505W/mK.
Embodiment 3:
1) selecting granularity is the diamond of 21 μ m, and granularity is 43 μ m, purity at 99. 99% silica flour as original material, and adds aluminium powder and aluminium nitride as sintering aids; The ratio of weight and number of diamond, silica flour, aluminium powder, aluminium nitride is 21.1:30.2:1.4:0.9;
2) said components is fully mixed after;
3) select the graphite jig of φ 20 mm, with pack into crystal vessel and put into the discharge plasma sintering stove of said mixture;
4),, vacuum degree begins Fast Sintering below the 12Pa when reaching at the discharge plasma sintering stove evacuation;
5) institute's plus-pressure is 38MPa in the sintering process, and programming rate is 100 ℃/minute, and sintering temperature is set at 1300 ℃, reach after the sintering temperature to keep 5 minutes, and under vacuum or inert gas environment sintering;
6) sintering finishes the back product is carried out laying down with the stove cooling and 940 ℃ the time pressure.
Through test, its density is more than 99.5%, and thermal conductivity is 502W/mK.
Claims (1)
1. a diamond-silicon composite is characterized in that, the weight ratio of its each atomic composition is: C:Si:Al:N is 19.6～30.4:27.2～33.3:1.02～3.5:0.17 ~ 0.4; And this material makes through following steps:
1) selecting granularity is the diamond of 18～23 μ m, and granularity is 40～45 μ m, purity at 99. 99% silica flour as original material, and adds aluminium powder and aluminium nitride as sintering aids; The ratio of weight and number of diamond, silica flour, aluminium powder, aluminium nitride is 19.6～30.4:27.2～33.3:0.85～2.7:0.5 ~ 1.3;
2) said components is fully mixed after;
3) select the graphite jig of φ 20 mm, with pack into crystal vessel and put into the discharge plasma sintering stove of said mixture;
4) at the discharge plasma sintering stove evacuation, when vacuum degree reaches the Fast Sintering of beginning below 12 ~ 15Pa;
5) institute's plus-pressure is 35～39MPa in the sintering process, and programming rate is 80 ~ 120 ℃/minute, and sintering temperature is set at 1280～1320 ℃, reach after the sintering temperature to keep 4-5 minute, and under vacuum or inert gas environment sintering;
6) sintering finishes the back product is carried out laying down pressure with the stove cooling and 900-950 ℃ the time, obtains product.
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| CN2012101922746A CN102709258A (en) | 2012-06-12 | 2012-06-12 | Diamond-silicon composite material |
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| CN2012101922746A CN102709258A (en) | 2012-06-12 | 2012-06-12 | Diamond-silicon composite material |
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Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106673653A (en) * | 2017-01-19 | 2017-05-17 | 北京科技大学 | Preparation method for diamond/silicon composite material |
| CN111111558A (en) * | 2020-01-08 | 2020-05-08 | 营口鑫成达新型建材股份有限公司 | Method for synthesizing diamond |
| CN111320476A (en) * | 2020-04-13 | 2020-06-23 | 北京科技大学广州新材料研究院 | Diamond-silicon carbide composite material, preparation method thereof and electronic equipment |
| CN111730054A (en) * | 2020-06-30 | 2020-10-02 | 湖南大学 | Low-temperature synthesis method and application of silicon carbide coated diamond composite powder |
Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102674840A (en) * | 2012-06-08 | 2012-09-19 | 李超 | Rapid sintering preparation method for diamond-silicon material |
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- 2012-06-12 CN CN2012101922746A patent/CN102709258A/en active Pending
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102674840A (en) * | 2012-06-08 | 2012-09-19 | 李超 | Rapid sintering preparation method for diamond-silicon material |
Cited By (4)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN106673653A (en) * | 2017-01-19 | 2017-05-17 | 北京科技大学 | Preparation method for diamond/silicon composite material |
| CN111111558A (en) * | 2020-01-08 | 2020-05-08 | 营口鑫成达新型建材股份有限公司 | Method for synthesizing diamond |
| CN111320476A (en) * | 2020-04-13 | 2020-06-23 | 北京科技大学广州新材料研究院 | Diamond-silicon carbide composite material, preparation method thereof and electronic equipment |
| CN111730054A (en) * | 2020-06-30 | 2020-10-02 | 湖南大学 | Low-temperature synthesis method and application of silicon carbide coated diamond composite powder |
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Application publication date: 20121003 |