CN117004925A - Diamond aluminum nitride based composite material and preparation method thereof - Google Patents
Diamond aluminum nitride based composite material and preparation method thereof Download PDFInfo
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- CN117004925A CN117004925A CN202310986131.0A CN202310986131A CN117004925A CN 117004925 A CN117004925 A CN 117004925A CN 202310986131 A CN202310986131 A CN 202310986131A CN 117004925 A CN117004925 A CN 117004925A
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- 229910003460 diamond Inorganic materials 0.000 title claims abstract description 151
- 239000010432 diamond Substances 0.000 title claims abstract description 151
- PMHQVHHXPFUNSP-UHFFFAOYSA-M copper(1+);methylsulfanylmethane;bromide Chemical compound Br[Cu].CSC PMHQVHHXPFUNSP-UHFFFAOYSA-M 0.000 title claims abstract description 145
- 239000002131 composite material Substances 0.000 title claims abstract description 67
- 238000002360 preparation method Methods 0.000 title claims abstract description 7
- 238000000034 method Methods 0.000 claims abstract description 191
- 239000000843 powder Substances 0.000 claims abstract description 141
- 238000007747 plating Methods 0.000 claims abstract description 119
- 238000000231 atomic layer deposition Methods 0.000 claims abstract description 23
- 238000004519 manufacturing process Methods 0.000 claims abstract description 16
- 238000005229 chemical vapour deposition Methods 0.000 claims abstract description 13
- 239000002994 raw material Substances 0.000 claims abstract description 10
- 239000000654 additive Substances 0.000 claims abstract description 9
- 230000000996 additive effect Effects 0.000 claims abstract description 9
- 230000008878 coupling Effects 0.000 claims abstract description 3
- 238000010168 coupling process Methods 0.000 claims abstract description 3
- 238000005859 coupling reaction Methods 0.000 claims abstract description 3
- 230000001939 inductive effect Effects 0.000 claims abstract description 3
- 230000008569 process Effects 0.000 claims description 103
- XKRFYHLGVUSROY-UHFFFAOYSA-N Argon Chemical compound [Ar] XKRFYHLGVUSROY-UHFFFAOYSA-N 0.000 claims description 62
- 239000007789 gas Substances 0.000 claims description 62
- 239000012495 reaction gas Substances 0.000 claims description 53
- QGZKDVFQNNGYKY-UHFFFAOYSA-N Ammonia Chemical compound N QGZKDVFQNNGYKY-UHFFFAOYSA-N 0.000 claims description 52
- 239000001257 hydrogen Substances 0.000 claims description 33
- 229910052739 hydrogen Inorganic materials 0.000 claims description 33
- 229910052786 argon Inorganic materials 0.000 claims description 31
- 239000000463 material Substances 0.000 claims description 29
- 239000001301 oxygen Substances 0.000 claims description 28
- 229910052760 oxygen Inorganic materials 0.000 claims description 28
- QVGXLLKOCUKJST-UHFFFAOYSA-N atomic oxygen Chemical compound [O] QVGXLLKOCUKJST-UHFFFAOYSA-N 0.000 claims description 26
- 230000005284 excitation Effects 0.000 claims description 26
- JLTRXTDYQLMHGR-UHFFFAOYSA-N trimethylaluminium Chemical compound C[Al](C)C JLTRXTDYQLMHGR-UHFFFAOYSA-N 0.000 claims description 26
- 239000002243 precursor Substances 0.000 claims description 25
- 239000002245 particle Substances 0.000 claims description 24
- 229910021529 ammonia Inorganic materials 0.000 claims description 23
- UFHFLCQGNIYNRP-UHFFFAOYSA-N Hydrogen Chemical compound [H][H] UFHFLCQGNIYNRP-UHFFFAOYSA-N 0.000 claims description 20
- 238000009616 inductively coupled plasma Methods 0.000 claims description 20
- 238000000623 plasma-assisted chemical vapour deposition Methods 0.000 claims description 17
- 238000002844 melting Methods 0.000 claims description 13
- 230000008018 melting Effects 0.000 claims description 13
- 230000003746 surface roughness Effects 0.000 claims description 13
- 238000005245 sintering Methods 0.000 claims description 12
- 238000001513 hot isostatic pressing Methods 0.000 claims description 11
- IJGRMHOSHXDMSA-UHFFFAOYSA-N Atomic nitrogen Chemical compound N#N IJGRMHOSHXDMSA-UHFFFAOYSA-N 0.000 claims description 10
- 150000002431 hydrogen Chemical class 0.000 claims description 10
- QJGQUHMNIGDVPM-UHFFFAOYSA-N nitrogen group Chemical group [N] QJGQUHMNIGDVPM-UHFFFAOYSA-N 0.000 claims description 9
- 238000004050 hot filament vapor deposition Methods 0.000 claims description 8
- 238000002156 mixing Methods 0.000 claims description 7
- 229910052757 nitrogen Inorganic materials 0.000 claims description 5
- 238000009694 cold isostatic pressing Methods 0.000 claims description 4
- 239000010410 layer Substances 0.000 description 146
- 239000000758 substrate Substances 0.000 description 33
- 150000002500 ions Chemical class 0.000 description 10
- 239000011248 coating agent Substances 0.000 description 8
- 238000000576 coating method Methods 0.000 description 8
- 238000005516 engineering process Methods 0.000 description 7
- PIGFYZPCRLYGLF-UHFFFAOYSA-N Aluminum nitride Chemical compound [Al]#N PIGFYZPCRLYGLF-UHFFFAOYSA-N 0.000 description 6
- 230000009286 beneficial effect Effects 0.000 description 6
- 239000000919 ceramic Substances 0.000 description 5
- 239000011247 coating layer Substances 0.000 description 5
- -1 hydrogen ions Chemical class 0.000 description 5
- 230000001965 increasing effect Effects 0.000 description 5
- 229910052751 metal Inorganic materials 0.000 description 5
- 239000002184 metal Substances 0.000 description 5
- 239000011812 mixed powder Substances 0.000 description 5
- 229910017083 AlN Inorganic materials 0.000 description 4
- RYGMFSIKBFXOCR-UHFFFAOYSA-N Copper Chemical compound [Cu] RYGMFSIKBFXOCR-UHFFFAOYSA-N 0.000 description 4
- 230000000052 comparative effect Effects 0.000 description 4
- 229910052802 copper Inorganic materials 0.000 description 4
- 239000010949 copper Substances 0.000 description 4
- 230000017525 heat dissipation Effects 0.000 description 4
- 238000001755 magnetron sputter deposition Methods 0.000 description 4
- 239000011159 matrix material Substances 0.000 description 4
- 238000004806 packaging method and process Methods 0.000 description 4
- 239000000376 reactant Substances 0.000 description 4
- 238000011161 development Methods 0.000 description 3
- 238000010438 heat treatment Methods 0.000 description 3
- 238000009413 insulation Methods 0.000 description 3
- 229920005989 resin Polymers 0.000 description 3
- 239000011347 resin Substances 0.000 description 3
- 238000003892 spreading Methods 0.000 description 3
- 230000007480 spreading Effects 0.000 description 3
- 239000000853 adhesive Substances 0.000 description 2
- 230000001070 adhesive effect Effects 0.000 description 2
- 229910052782 aluminium Inorganic materials 0.000 description 2
- XAGFODPZIPBFFR-UHFFFAOYSA-N aluminium Chemical compound [Al] XAGFODPZIPBFFR-UHFFFAOYSA-N 0.000 description 2
- 230000015556 catabolic process Effects 0.000 description 2
- 238000005253 cladding Methods 0.000 description 2
- 230000007547 defect Effects 0.000 description 2
- 230000000694 effects Effects 0.000 description 2
- 238000004100 electronic packaging Methods 0.000 description 2
- 238000005538 encapsulation Methods 0.000 description 2
- 230000002708 enhancing effect Effects 0.000 description 2
- 230000009477 glass transition Effects 0.000 description 2
- 239000004519 grease Substances 0.000 description 2
- 230000001788 irregular Effects 0.000 description 2
- 239000000203 mixture Substances 0.000 description 2
- 238000005457 optimization Methods 0.000 description 2
- 239000011148 porous material Substances 0.000 description 2
- 238000004321 preservation Methods 0.000 description 2
- 238000012546 transfer Methods 0.000 description 2
- 239000004593 Epoxy Substances 0.000 description 1
- 238000006243 chemical reaction Methods 0.000 description 1
- 239000013078 crystal Substances 0.000 description 1
- XLJMAIOERFSOGZ-UHFFFAOYSA-M cyanate Chemical compound [O-]C#N XLJMAIOERFSOGZ-UHFFFAOYSA-M 0.000 description 1
- 238000013461 design Methods 0.000 description 1
- 239000003822 epoxy resin Substances 0.000 description 1
- 238000005530 etching Methods 0.000 description 1
- 230000008642 heat stress Effects 0.000 description 1
- 230000002706 hydrostatic effect Effects 0.000 description 1
- 239000011156 metal matrix composite Substances 0.000 description 1
- 238000012986 modification Methods 0.000 description 1
- 230000004048 modification Effects 0.000 description 1
- 229920000647 polyepoxide Polymers 0.000 description 1
- 229920000642 polymer Polymers 0.000 description 1
- 229920013636 polyphenyl ether polymer Polymers 0.000 description 1
- 238000012545 processing Methods 0.000 description 1
- 230000009467 reduction Effects 0.000 description 1
- 238000007788 roughening Methods 0.000 description 1
- 239000004065 semiconductor Substances 0.000 description 1
- 238000004544 sputter deposition Methods 0.000 description 1
- 238000010025 steaming Methods 0.000 description 1
- 238000006467 substitution reaction Methods 0.000 description 1
- 239000013077 target material Substances 0.000 description 1
- 229920001187 thermosetting polymer Polymers 0.000 description 1
- 238000009827 uniform distribution Methods 0.000 description 1
Classifications
-
- C—CHEMISTRY; METALLURGY
- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/44—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the method of coating
- C23C16/455—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the method of coating characterised by the method used for introducing gases into reaction chamber or for modifying gas flows in reaction chamber
- C23C16/45523—Pulsed gas flow or change of composition over time
- C23C16/45525—Atomic layer deposition [ALD]
-
- B—PERFORMING OPERATIONS; TRANSPORTING
- B22—CASTING; POWDER METALLURGY
- B22F—WORKING METALLIC POWDER; MANUFACTURE OF ARTICLES FROM METALLIC POWDER; MAKING METALLIC POWDER; APPARATUS OR DEVICES SPECIALLY ADAPTED FOR METALLIC POWDER
- B22F10/00—Additive manufacturing of workpieces or articles from metallic powder
- B22F10/20—Direct sintering or melting
- B22F10/28—Powder bed fusion, e.g. selective laser melting [SLM] or electron beam melting [EBM]
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C26/00—Alloys containing diamond or cubic or wurtzitic boron nitride, fullerenes or carbon nanotubes
-
- C—CHEMISTRY; METALLURGY
- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/22—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the deposition of inorganic material, other than metallic material
- C23C16/26—Deposition of carbon only
- C23C16/27—Diamond only
- C23C16/271—Diamond only using hot filaments
-
- C—CHEMISTRY; METALLURGY
- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/22—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the deposition of inorganic material, other than metallic material
- C23C16/30—Deposition of compounds, mixtures or solid solutions, e.g. borides, carbides, nitrides
- C23C16/34—Nitrides
-
- C—CHEMISTRY; METALLURGY
- C23—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; CHEMICAL SURFACE TREATMENT; DIFFUSION TREATMENT OF METALLIC MATERIAL; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL; INHIBITING CORROSION OF METALLIC MATERIAL OR INCRUSTATION IN GENERAL
- C23C—COATING METALLIC MATERIAL; COATING MATERIAL WITH METALLIC MATERIAL; SURFACE TREATMENT OF METALLIC MATERIAL BY DIFFUSION INTO THE SURFACE, BY CHEMICAL CONVERSION OR SUBSTITUTION; COATING BY VACUUM EVAPORATION, BY SPUTTERING, BY ION IMPLANTATION OR BY CHEMICAL VAPOUR DEPOSITION, IN GENERAL
- C23C16/00—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes
- C23C16/44—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the method of coating
- C23C16/50—Chemical coating by decomposition of gaseous compounds, without leaving reaction products of surface material in the coating, i.e. chemical vapour deposition [CVD] processes characterised by the method of coating using electric discharges
-
- C—CHEMISTRY; METALLURGY
- C22—METALLURGY; FERROUS OR NON-FERROUS ALLOYS; TREATMENT OF ALLOYS OR NON-FERROUS METALS
- C22C—ALLOYS
- C22C26/00—Alloys containing diamond or cubic or wurtzitic boron nitride, fullerenes or carbon nanotubes
- C22C2026/007—Alloys containing diamond or cubic or wurtzitic boron nitride, fullerenes or carbon nanotubes with additional metal compounds being nitrides
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- Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
- Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
- Y02P—CLIMATE CHANGE MITIGATION TECHNOLOGIES IN THE PRODUCTION OR PROCESSING OF GOODS
- Y02P10/00—Technologies related to metal processing
- Y02P10/25—Process efficiency
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- Chemical & Material Sciences (AREA)
- Engineering & Computer Science (AREA)
- Materials Engineering (AREA)
- Mechanical Engineering (AREA)
- Metallurgy (AREA)
- Organic Chemistry (AREA)
- Chemical Kinetics & Catalysis (AREA)
- General Chemical & Material Sciences (AREA)
- Inorganic Chemistry (AREA)
- Physics & Mathematics (AREA)
- Plasma & Fusion (AREA)
- Manufacturing & Machinery (AREA)
- Chemical Vapour Deposition (AREA)
Abstract
The invention relates to a diamond aluminum nitride-based composite material and a preparation method thereof. The method comprises the following steps: treating the diamond powder by an inductive coupling plasma method or an anode layer ion source irradiation mode to obtain roughened diamond powder; preparing a first plating layer on the surface of the roughened diamond powder by a plasma enhanced atomic layer deposition method, and then preparing a second plating layer on the basis of the first plating layer by a chemical vapor deposition method to obtain plated diamond powder; the first plating layer and the second plating layer are both aluminum nitride plating layers; the diamond aluminum nitride based composite material is manufactured by taking plating diamond powder and aluminum nitride powder as raw materials through additive manufacturing. The diamond aluminum nitride-based composite material prepared by the invention has high thermal conductivity, high density and high insulativity.
Description
Technical Field
The invention relates to the technical field of additive manufacturing and composite materials, in particular to a diamond aluminum nitride-based composite material and a preparation method thereof.
Background
For power electronics packaging applications, polymeric circuit boards are generally only used in the low power small appliance industries. In order to adapt to the characteristic of larger power loss of the power electronic device, epoxy resin is often modified to obtain epoxy substrates with different emphasis functions so as to meet the related requirements of high heat dissipation and stress reduction of the power electronic device package. For example, the cyanate resin has the advantages of low dielectric constant and dielectric loss factor, high glass transition temperature, low thermal expansion coefficient and the like, and can be used for high-frequency packaging substrates; the bismaleimide-triazine resin has better pressure resistance and steaming resistance, and can be used for chip packaging; the thermosetting polyphenyl ether resin has lower dielectric constant and dielectric loss factor, higher glass transition temperature and lower thermal expansion coefficient, excellent comprehensive dielectric property and good thermodynamic property, and is suitable for the field of high-frequency packaging.
Compared with a polymer insulating substrate, the metal and the composite material substrate thereof have higher heat conductivity and are mostly used in the field with higher requirements on heat dissipation performance; compared with a thick film ceramic substrate, the metal matrix composite substrate has better mechanical property and unique advantages.
With the rapid development of electronic information technology, it is difficult for traditional electronic packaging heat dissipation materials to ensure the operation safety and reliability of high-power devices such as large-scale integrated circuits, semiconductor lasers and the like. In order to improve the thermal management capability of the electronic packaging heat dissipation material, a high-efficiency thermal management material can be generally searched, and the diamond particle reinforced copper-based composite material has the characteristics of high thermal conductivity and matching with the thermal expansion coefficient of electronic components and parts, so that the diamond particle reinforced copper-based composite material has been widely paid attention in recent years. However, the diamond particle reinforced copper-based composite material has the problem of poor insulating property, and limits the application of the diamond particle reinforced copper-based composite material in the field with requirements on the insulating property.
In summary, it is highly desirable to provide a diamond aluminum nitride based composite material and a method for preparing the same.
Disclosure of Invention
In order to solve one or more technical problems in the prior art, the invention provides a diamond aluminum nitride-based composite material and a preparation method thereof. The diamond aluminum nitride-based composite material prepared by the invention has high thermal conductivity, high density and high insulativity.
The present invention provides in a first aspect a method of preparing a diamond aluminium nitride based composite material, the method comprising the steps of:
(1) Treating the diamond powder by an inductive coupling plasma method or an anode layer ion source irradiation mode to obtain roughened diamond powder;
(2) Preparing a first plating layer on the surface of the roughened diamond powder by a plasma enhanced atomic layer deposition method, and then preparing a second plating layer on the basis of the first plating layer by a chemical vapor deposition method to obtain plated diamond powder; the first plating layer and the second plating layer are both aluminum nitride plating layers;
(3) The diamond aluminum nitride based composite material is manufactured by taking plating diamond powder and aluminum nitride powder as raw materials through additive manufacturing.
Preferably, the diamond powder has a particle size of 20 to 400 μm; the surface roughness of the roughened diamond powder is 5-100 nm; the thickness of the first plating layer is 10-200 nm, preferably 40-60 nm; and/or the thickness of the second plating layer is not less than 10 μm.
Preferably, the process conditions of the inductively coupled plasma method are as follows: the power of the excitation source is 50-20000W; the process gas is a mixed gas of argon and hydrogen or a mixed gas of argon and oxygen, preferably, the partial pressure of hydrogen is 10-90% in the mixed gas of argon and hydrogen, and the partial pressure of oxygen is 10-90% in the mixed gas of argon and oxygen; the process air pressure is 0.1-10 Pa; and/or the process temperature is 25-200 ℃.
Preferably, the process conditions of the anode layer ion source irradiation mode are as follows: the power of the excitation source is 500-30000W; the process gas is a mixed gas of argon and hydrogen or a mixed gas of argon and oxygen, preferably, the partial pressure of hydrogen is 10-90% in the mixed gas of argon and hydrogen, and the partial pressure of oxygen is 10-90% in the mixed gas of argon and oxygen; the process air pressure is 0.1-10 Pa; and/or the process temperature is 25-200 ℃.
Preferably, the process conditions for preparing the first plating layer by the plasma enhanced atomic layer deposition method are: the precursor material is trimethylaluminum; the power of the excitation source is 50-20000W; the reaction gas is ammonia gas; the process air pressure is 0.5-20 Pa; and/or the process temperature is 30-300 ℃.
Preferably, the first plating layer comprises a first aluminum nitride layer, a second aluminum nitride layer and a third aluminum nitride layer in this order, the first aluminum nitride layer being closer to the surface of the roughened diamond powder than the second aluminum nitride layer; when preparing the first aluminum nitride layer, the volume flow ratio of the precursor material to the reaction gas is 1: (1.5-1.8); when preparing the second aluminum nitride layer, the volume flow ratio of the precursor material to the reaction gas is 1: (1.1-1.3); when preparing the third aluminum nitride layer, the volume flow ratio of the precursor material to the reaction gas is 1: (0.8-1).
Preferably, the process conditions for preparing the second plating layer by the chemical vapor deposition method are as follows: the reaction gas contains trimethylaluminum and ammonia, and preferably, the volume percentage of the ammonia in the reaction gas is 20-80%; the process air pressure is 0.5-20 Pa; and/or the process temperature is 200-500 ℃.
Preferably, the chemical vapor deposition method is a plasma enhanced chemical vapor deposition method or a hot wire chemical vapor deposition method; preferably, the process conditions for preparing the second plating layer by the plasma enhanced chemical vapor deposition method are as follows: the power of the excitation source is 50-20000W; the reaction gas contains trimethylaluminum and nitrogen-containing gas, preferably, the volume percentage of the nitrogen-containing gas in the reaction gas is 20-80%, and preferably, the nitrogen-containing gas is ammonia and/or nitrogen; the process air pressure is 0.5-20 Pa; and/or the process temperature is 30-300 ℃; preferably, the process conditions for preparing the second plating layer by the hot filament chemical vapor deposition method are as follows: the reaction gas contains trimethylaluminum and ammonia, and preferably, the volume percentage of the ammonia in the reaction gas is 20-80%; the process air pressure is 0.5-20 Pa; and/or the process temperature is 200-500 ℃.
Preferably, in step (3), the volume ratio of the plated diamond powder to the aluminum nitride powder is 1: (0.1-3); in the step (3), the aluminum nitride powder is aluminum nitride powder with the particle size of 1-5 mu m and/or aluminum nitride powder with the particle size of 20-40 mu m; and/or the step (3) is as follows: the diamond-coated aluminum nitride-based composite material is prepared by taking coated diamond powder and aluminum nitride powder as raw materials and sequentially carrying out a mixing step, a zone-selecting laser melting step, a sintering step and a hot isostatic pressing step; preferably, a cold isostatic pressing step is further included between the selective laser melting step and the sintering step.
The present invention provides in a second aspect a diamond aluminium nitride based composite material produced by the method of the invention described in the first aspect.
Compared with the prior art, the invention has at least the following beneficial effects:
(1) The diamond aluminum nitride based composite material prepared by the invention integrates the advantages of a metal substrate and a ceramic substrate, the invention adopts aluminum nitride (AlN) and diamond enhanced aluminum nitride composite material to form a multi-layer structure through the combination and matching of the thermal property and the interface of an aluminum nitride coating layer and diamond particles, the AlN coating layer can play the functions of effective insulation, protection and the like, and the diamond aluminum nitride based composite material in the invention has the advantages of mechanical property and high thermal conductivity, overcomes the defects of the ceramic substrate and the metal substrate, greatly improves the comprehensive performance, simultaneously adopts a proper coating technology and an interface connection optimization technology, greatly reduces the cost and can provide important technical support for the development of electronic device encapsulation.
(2) The invention adopts ICP (inductively coupled plasma) or anode layer ion source to excite oxygen or hydrogen to form oxygen or hydrogen ions to treat the surface of diamond powder, thereby removing grease on the surface of the diamond powder and forming a surface microstructure with roughness (Ra) of 5-100 nm on the micro surface of the diamond powder, being beneficial to increasing the surface area, improving the surface area by more than 2 times, improving the contact area between the diamond powder and the first plating layer, enhancing the bonding and cladding property of the diamond powder and the first plating layer, reducing the peeling and falling phenomena of the surface, and improving the adhesive force and durability of the first plating layer; in addition, the surface microstructure with the roughness (Ra) of 5-100 nm is formed on the surface of the diamond powder, so that the heat conduction capability between the diamond powder and aluminum nitride can be enhanced, the heat transfer capability can be effectively improved, the heat conduction performance of the diamond aluminum nitride-based composite material can be improved, and the diamond aluminum nitride-based composite material is more suitable for the application field with high heat conduction requirements.
(3) The invention adopts the plasma enhanced atomic layer deposition method (PE-ALD process) to prepare a layer of aluminum nitride plating layer (first plating layer) on the surface of the roughened diamond powder, the plasma enhanced atomic layer deposition method adopted by the invention can be used for plating the film layer with good coverage on any irregular surface, the coverage is more than 99 percent, and the compactness is very good, so that the contact area between the diamond powder and the first plating layer is increased by more than 2 times, thereby improving the heat conduction channel of the composite plating layer, simultaneously the compact plating layer is beneficial to reducing pores, the purpose of improving the heat conduction effect can be achieved, and the heat conductivity can be improved by more than 30 percent.
Detailed Description
In order to make the objects, technical solutions and advantages of the present invention more apparent, the technical solutions of the present invention will be clearly and completely described below in connection with the embodiments of the present invention. It will be apparent that the described embodiments are some, but not all, embodiments of the invention. All other embodiments, which can be made by those skilled in the art based on the embodiments of the invention without making any inventive effort, are intended to be within the scope of the invention.
The present invention provides in a first aspect a method of preparing a diamond aluminium nitride based composite material, the method comprising the steps of:
(1) Treating the diamond powder by an Inductively Coupled Plasma (ICP) method or an anode layer ion source irradiation mode to obtain roughened diamond powder;
(2) Preparing a first plating layer (also called an inner plating layer) on the surface of the roughened diamond powder by a plasma enhanced atomic layer deposition method (PE-ALD method), and then preparing a second plating layer (also called an outer plating layer) on the basis of the first plating layer by a chemical vapor deposition method to obtain a plated diamond powder; the first plating layer and the second plating layer are both aluminum nitride plating layers; the method comprises the steps of sequentially plating a first plating layer and a second plating layer on the surface of roughened diamond powder;
(3) Preparing a diamond aluminum nitride-based composite material by taking plating diamond powder and aluminum nitride powder as raw materials through additive manufacturing; the invention does not limit the process conditions of additive manufacturing specifically, and is a conventional technology in the field; the diamond aluminum nitride-based composite material with various shapes can be prepared through additive manufacturing, for example, the diamond aluminum nitride-based composite material with complex shape can be prepared.
The diamond aluminum nitride based composite material prepared by the invention integrates the advantages of a metal substrate and a ceramic substrate, the invention adopts aluminum nitride (AlN) and diamond enhanced aluminum nitride composite material to form a multi-layer structure through the combination and matching of the thermal property and the interface of an aluminum nitride coating layer and diamond particles, the AlN coating layer can play the functions of effective insulation, protection and the like, and the diamond aluminum nitride based composite material in the invention has the advantages of mechanical property and high thermal conductivity, overcomes the defects of the ceramic substrate and the metal substrate, greatly improves the comprehensive performance, simultaneously adopts a proper coating technology and an interface connection optimization technology, greatly reduces the cost and can provide important technical support for the development of electronic device encapsulation.
The invention adopts ICP (inductively coupled plasma) or anode layer ion source to excite oxygen or hydrogen to form oxygen ions or hydrogen ions to treat the surface of the diamond powder (namely, pretreatment and surface texturing are carried out on the surface), thereby removing grease on the surface of the diamond powder and forming a surface microstructure with roughness (Ra) of 5-100 nm on the micro surface of the diamond powder, being beneficial to increasing the surface area, improving the contact area of the diamond powder and the first plating layer by more than 2 times, enhancing the bonding property and cladding property of the diamond powder and the first plating layer, reducing the peeling and falling phenomena of the surface, and improving the adhesive force and durability of the first plating layer; in addition, the surface microstructure with the roughness (Ra) of 5-100 nm is formed on the surface of the diamond powder, so that the heat conduction capability of the diamond powder and the aluminum nitride matrix is enhanced, the heat transfer capability of the diamond powder and the aluminum nitride matrix can be effectively improved, and the heat conduction performance of the diamond aluminum nitride matrix composite material is improved, so that the diamond aluminum nitride matrix composite material is more suitable for the application field with high heat conduction requirements.
The invention adopts the plasma enhanced atomic layer deposition method (PE-ALD process) to prepare a layer of aluminum nitride plating layer (first plating layer) on the surface of the roughened diamond powder, the plasma enhanced atomic layer deposition method adopted by the invention can be used for plating the film layer with good coverage on any irregular surface, the coverage is more than 99 percent, and the compactness is very good, so that the contact area between the diamond powder and the first plating layer is increased by more than 2 times, thereby improving the heat conduction channel of the composite plating layer, simultaneously the compact plating layer is beneficial to reducing pores, the purpose of improving the heat conduction effect can be achieved, and the heat conductivity can be improved by more than 30 percent.
According to some preferred embodiments, the diamond powder has a particle size of 20 to 400 μm; preferably, the diamond powder is a single crystal diamond powder; the surface roughness of the roughened diamond powder is 5-100 nm, preferably 80-100 nm; the thickness of the first plating layer is 10-200 nm, preferably 40-60 nm; and/or the thickness of the second plating layer is not less than 10 μm.
In the present invention, it is preferable that the surface roughness of the roughened diamond powder is 5 to 100nm, the present invention allows the roughened diamond powder to have a proper surface roughness to ensure that the diamond powder can exert optimal performance, by properly roughening the surface, the surface area of the diamond powder is effectively increased, more "anchor points" are provided, contact and bonding with the first plating layer are advantageously enhanced, adhesion and adhesion of the diamond powder are effectively improved, and the proper roughened surface also helps to achieve more uniform distribution by the PE-ALD method, holes or unevenness in the first plating layer is reduced, however, too small roughness may not effectively increase the surface area, and too large surface roughness may cause an increase in cost; in some more preferred embodiments, the roughened diamond powder has a surface roughness of 80 to 100nm.
According to some preferred embodiments, the process conditions of the inductively coupled plasma method are:
excitation source power (ICP excitation source power supply power) is 50 to 20000W (for example, 50, 100, 500, 1000, 2000, 3000, 4000, 5000, 6000, 7000, 8000, 9000, 10000, 12000, 15000, 18000, or 20000W), preferably 2000 to 20000W; the process gas is a mixed gas of argon and hydrogen or a mixed gas of argon and oxygen, preferably, the partial pressure of hydrogen is 10 to 90% (e.g., 10%, 20%, 30%, 40%, 50%, 60%, 70%, 80% or 90%) in the mixed gas of argon and hydrogen, and the partial pressure of oxygen is 10 to 90% (e.g., 10%, 20%, 30%, 40%, 50%, 60%, 70%, 80% or 90%) in the mixed gas of argon and oxygen; the process gas pressure is 0.1 to 10Pa (e.g., 0.1, 0.5, 1, 2, 3, 4, 5, 6, 7, 8, 9, or 10 Pa), preferably 1 to 10Pa; and/or the process temperature is 25-200deg.C (e.g., 25deg.C, 40deg.C, 60deg.C, 80deg.C, 100deg.C, 120deg.C, 150deg.C, 180deg.C or 200deg.C). In the invention, the higher the excitation source power (namely radio frequency power) and the higher the oxygen or hydrogen partial pressure, the faster the etching speed can lead to the higher surface roughness in the same inductively coupled plasma processing time.
According to some preferred embodiments, the irradiation of the anode layer ion source is to excite oxygen or hydrogen to form oxygen ions or hydrogen ions, and the surface of the diamond powder is treated to obtain roughened diamond powder, and the process conditions of the irradiation mode of the anode layer ion source are as follows: the excitation source power (anode layer ion source excitation power supply power) is 500 to 30000W (e.g., 500, 1000, 2000, 3000, 4000, 5000, 6000, 7000, 8000, 9000, 10000, 12000, 15000, 18000, 20000, 22000, 25000, 28000, or 30000W); the process gas is a mixed gas of argon and hydrogen or a mixed gas of argon and oxygen, preferably, the partial pressure of hydrogen is 10 to 90% (e.g., 10%, 20%, 30%, 40%, 50%, 60%, 70%, 80% or 90%) in the mixed gas of argon and hydrogen, and the partial pressure of oxygen is 10 to 90% (e.g., 10%, 20%, 30%, 40%, 50%, 60%, 70%, 80% or 90%) in the mixed gas of argon and oxygen; the process gas pressure is 0.1 to 10Pa (e.g., 0.1, 0.5, 1, 2, 3, 4, 5, 6, 7, 8, 9, or 10 Pa), preferably 1 to 10Pa; and/or the process temperature is 25-200deg.C (e.g., 25deg.C, 40deg.C, 60deg.C, 80deg.C, 100deg.C, 120deg.C, 150deg.C, 180deg.C or 200deg.C).
The invention does not limit the treatment time by the inductively coupled plasma method or the anode layer ion source irradiation method, and can lead the diamond powder to reach the preset surface roughness.
According to some preferred embodiments, the process conditions for preparing the first plating layer by a plasma enhanced atomic layer deposition method are: the precursor material is trimethylaluminum; the excitation source power (radio frequency power) is 50 to 20000W (e.g., 50, 100, 500, 1000, 2000, 3000, 4000, 5000, 6000, 7000, 8000, 9000, 10000, 12000, 15000, 18000, or 20000W), preferably 2000 to 20000W; the reaction gas is ammonia gas; the process gas pressure is 0.5 to 20Pa (e.g., 0.1, 0.5, 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, or 20 Pa), preferably 1 to 20Pa; and/or the process temperature is 30-300 ℃ (e.g. 30 ℃, 40 ℃, 50 ℃, 60 ℃, 70 ℃, 80 ℃, 90 ℃, 100 ℃, 120 ℃, 150 ℃, 180 ℃, 200 ℃, 220 ℃, 250 ℃, 280 ℃ or 300 ℃).
When the first plating layer is prepared by the plasma enhanced atomic layer deposition method, in each cycle, the precursor material is firstly introduced, then the reaction gas is introduced, and the flow ratio of the precursor material to the reaction gas is not particularly limited, so that the method is a conventional technology in the field; in some preferred embodiments, the flow ratio of precursor material to reactant gas is 100: (80 to 180), specifically, for example, the flow rate of the precursor material is 100sccm, and the flow rate of the reaction gas is 80 to 180sccm.
The invention does not limit the time for carrying out the plasma enhanced atomic layer deposition specifically, and can reach the preset thickness of the first plating layer.
According to some preferred embodiments, the first plating layer comprises a first aluminum nitride layer, a second aluminum nitride layer, and a third aluminum nitride layer in this order, the first aluminum nitride layer being closer to the surface of the roughened diamond powder than the second aluminum nitride layer; when preparing the first aluminum nitride layer, the volume flow ratio of the precursor material to the reaction gas is 1: (1.5-1.8) (e.g., 1:1.5, 1:1.6, 1:1.7, or 1:1.8), in some preferred embodiments, the trimethylaluminum flow is, for example, 100sccm, and the reactant gas flow may be, for example, 150-180 sccm; when preparing the second aluminum nitride layer, the volume flow ratio of the precursor material to the reaction gas is 1: (1.1-1.3) (e.g., 1:1.1, 1:1.2, or 1:1.3), in some preferred embodiments, the trimethylaluminum flow is, for example, 100sccm, and the reactant gas flow may be, for example, 110-130 sccm; when preparing the third aluminum nitride layer, the volume flow ratio of the precursor material to the reaction gas is 1: (0.8-1) (e.g., 1:0.8, 1:0.9, or 1:1), in some preferred embodiments, the trimethylaluminum flow is, for example, 100sccm, and the reactant gas flow may be, for example, 80-100 sccm.
In the present invention, it is preferable that the first plating layer is composed of the first aluminum nitride layer, the second aluminum nitride layer and the third aluminum nitride layer, that is, it is preferable that the first plating layer is designed in a gradient manner, that the nitrogen content on the side close to the diamond powder is higher, and the aluminum content on the side far from the diamond powder is higher, and the gradient design can better realize strong bonding of diamond and aluminum nitride and low interface thermal resistance on the whole, and can improve the heat conduction performance of the diamond aluminum nitride based composite material at high temperature.
According to some preferred embodiments, the process conditions for preparing the second plating layer by chemical vapor deposition methods are: the reaction gas contains trimethylaluminum and ammonia, preferably, the reaction gas contains ammonia in an amount of 20 to 80% by volume (e.g., 20%, 30%, 40%, 50%, 60%, 70% or 80%); the process gas pressure is 0.5 to 20Pa (e.g., 0.1, 0.5, 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, or 20 Pa), preferably 1 to 20Pa; and/or the process temperature is 200-500 ℃ (e.g. 200 ℃, 250 ℃, 300 ℃, 350 ℃, 400 ℃, 450 ℃ or 500 ℃).
According to some preferred embodiments, the chemical vapor deposition method is a plasma enhanced chemical vapor deposition method (PECVD) or a hot filament chemical vapor deposition method (hot filament CVD); preferably, the process conditions for preparing the second plating layer by the plasma enhanced chemical vapor deposition method are as follows: the excitation source power is 50 to 20000W (e.g., 50, 100, 500, 1000, 2000, 3000, 4000, 5000, 6000, 7000, 8000, 9000, 10000, 12000, 15000, 18000, or 20000W), preferably 2000 to 20000W; the reaction gas contains trimethylaluminum and a nitrogen-containing gas, preferably, the volume percentage of the nitrogen-containing gas in the reaction gas is 20-80% (for example, 20%, 30%, 40%, 50%, 60%, 70% or 80%), preferably, the nitrogen-containing gas is ammonia and/or nitrogen; the process gas pressure is 0.5 to 20Pa (e.g., 0.1, 0.5, 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, or 20 Pa), preferably 1 to 20Pa; and/or a process temperature of 30-300 ℃ (e.g., 30 ℃, 40 ℃, 50 ℃, 60 ℃, 70 ℃, 80 ℃, 90 ℃, 100 ℃, 120 ℃, 150 ℃, 180 ℃, 200 ℃, 220 ℃, 250 ℃, 280 ℃ or 300 ℃); preferably, the process conditions for preparing the second plating layer by the hot filament chemical vapor deposition method are as follows: the reaction gas contains trimethylaluminum and ammonia, preferably, the reaction gas contains ammonia in an amount of 20 to 80% by volume (e.g., 20%, 30%, 40%, 50%, 60%, 70% or 80%); the process gas pressure is 0.5 to 20Pa (e.g., 0.1, 0.5, 1, 2, 3, 4, 5, 6, 7, 8, 9, 10, 11, 12, 13, 14, 15, 16, 17, 18, 19, or 20 Pa), preferably 1 to 20Pa; and/or the process temperature is 200-500 ℃ (e.g. 200 ℃, 250 ℃, 300 ℃, 350 ℃, 400 ℃, 450 ℃ or 500 ℃).
The invention plates a layer of second coating on the surface of the first coating by a Chemical Vapor Deposition (CVD), which is characterized by fast growth speed, and can prepare an aluminum nitride film layer (second coating) with the thickness of more than 10 microns on the surface of the first coating, so that the aluminum nitride film layer can be well combined with the subsequent process, and the plasma enhanced chemical vapor deposition method is more preferable to plate a layer of second coating on the surface of the first coating, thereby being more beneficial to improving the bonding force with the subsequent process.
The present invention is not described in detail in relation to Inductively Coupled Plasma (ICP) methods, anode layer ion source irradiation or plasma enhanced atomic layer methods, chemical vapor deposition methods, plasma enhanced chemical vapor deposition methods, and hot filament chemical vapor deposition methods, and is well known to those skilled in the art.
According to some preferred embodiments, the second coating layer in the coated diamond powder is 20 to 70% by mass.
According to some preferred embodiments, in step (3), the volume ratio of the plated diamond powder and the aluminum nitride powder is 1: (0.1-3) (e.g., 1:0.1, 1:0.5, 1:0.8, 1:1, 1:1.5, 1:2, 1:2.5, or 1:3); and/or the aluminum nitride powder is aluminum nitride powder with the particle size of 1-5 mu m and/or aluminum nitride powder with the particle size of 20-40 mu m.
According to some preferred embodiments, step (3) is: the diamond-coated aluminum nitride-based composite material is prepared by taking coated diamond powder and aluminum nitride powder as raw materials and sequentially carrying out a mixing step, a zone-selecting laser melting step, a sintering step and a hot isostatic pressing step; preferably, a cold isostatic pressing step is further included between the selective laser melting step and the sintering step; that is, it is preferable that the step (3) is: the diamond aluminum nitride based composite material is prepared by taking coated diamond powder and aluminum nitride powder as raw materials and sequentially carrying out a mixing step, a selective laser melting step, a cold isostatic pressing step, a sintering step and a hot isostatic pressing step.
According to some specific embodiments, the mixing step is: the volume ratio of the diamond plating powder to the aluminum nitride powder is 1: (0.1-3); the aluminum nitride powder is aluminum nitride powder with the particle size of 1-5 mu m and/or aluminum nitride powder with the particle size of 20-40 mu m; the selective laser melting step comprises the following steps: in the selective laser melting equipment, the oxygen content is controlled to be lower than 0.1 percent, the substrate is preheated to 20-200 ℃, under the conditions that the laser power is 30-500W, the scanning speed is 1-1500 mm/s, the spot diameter is 0.05-1 mm, the substrate temperature is 20-200 ℃ and the single powder spreading thickness of the substrate is 0.1-0.4 mm, the mixed powder is utilized for laser forming, finally, the heating is stopped, and after the substrate is cooled, the formed composite material is taken off from the substrate; preferably, the substrate is an aluminum nitride substrate; the sintering step is to place the formed composite material in a vacuum furnace, vacuumize the material until the pressure is less than 1Pa, and keep the temperature for 0.5 to 3 hours under the condition that the sintering temperature is 850 to 1100 ℃ to obtain the sintered composite material; the hot isostatic pressing step is as follows: and (3) under the conditions that the hot isostatic pressing temperature is 850-1050 ℃ and the hot isostatic pressing pressure is 50-200 MPa, the temperature and pressure of the sintered composite material are maintained for 0.5-4 h, and the diamond aluminum nitride based composite material is obtained.
According to some specific embodiments, the molded composite material is placed in a sheath, vacuumized until the pressure is less than 10Pa, the composite material after the sheath is placed in a cold isostatic press, the sheath is removed after the pressure is maintained for 2-20 min under the condition that the hydrostatic pressure is 50-400 MPa, and then the densified composite material is subjected to a subsequent sintering step.
The present invention provides in a second aspect a diamond aluminium nitride based composite material produced by the method of the invention described in the first aspect.
The invention is further illustrated below with reference to examples. These examples are merely illustrative of preferred embodiments of the present invention and the scope of the present invention should not be construed as being limited to these examples only.
Example 1
The preparation method of the diamond aluminum nitride-based composite material comprises the following steps:
(1) treating diamond powder (average particle diameter of 200 μm) by an inductively coupled plasma method to obtain roughened diamond powder; the process conditions of the inductively coupled plasma method are as follows: the excitation source power is 10000W; the process gas is a mixed gas of argon and hydrogen, the partial pressure of the hydrogen in the mixed gas is 50%, the process air pressure is 5Pa, and the process temperature is 100 ℃; the surface roughness of the obtained roughened diamond powder was 80nm.
(2) Preparing a first plating layer (aluminum nitride plating layer) on the surface of the roughened diamond powder by a plasma enhanced atomic layer deposition method, and then preparing a second plating layer (aluminum nitride plating layer) on the basis of the first plating layer by a plasma enhanced chemical vapor deposition method to obtain plated diamond powder; the thickness of the first plating layer is 60nm, and the thickness of the second plating layer is 15 mu m; the process conditions for preparing the first plating layer by the plasma enhanced atomic layer deposition method are as follows: the precursor material is trimethylaluminum; excitation source power is 12000W; the reaction gas is ammonia gas; the process air pressure is 6Pa, the process temperature is 180 ℃, and the volume flow ratio of the precursor material to the reaction gas is 1:1.2; the process conditions for preparing the second plating layer by a plasma enhanced chemical vapor deposition method are as follows: the excitation source power is 10000W; the reaction gas comprises trimethylaluminum and ammonia, wherein the volume percentage of the ammonia in the reaction gas is 65%, and the volume percentage of the trimethylaluminum in the reaction gas is 35%; the process air pressure is 6Pa; the process temperature was 180 ℃.
(3) The diamond aluminum nitride based composite material is prepared by taking plating diamond powder and aluminum nitride powder as raw materials through additive manufacturing: a: mechanically and uniformly mixing the plated diamond powder and the aluminum nitride powder to obtain mixed powder; the aluminum nitride powder is a mixture of aluminum nitride powder with the particle size of 20-40 mu m and aluminum nitride powder with the particle size of 1-5 mu m; the volume ratio of the plating diamond powder to the aluminum nitride powder with the grain diameter of 20-40 μm is 7:2; the volume ratio of the plating diamond powder to the aluminum nitride powder with the grain diameter of 1-5 mu m is 7:1; b: in a selective laser melting device, introducing high-purity argon to ensure that the oxygen content in a forming cavity is lower than 0.1%, preheating a substrate (aluminum nitride substrate) to 200 ℃, carrying out laser forming by using mixed powder according to a designed shape under the conditions that the laser power is 100W, the scanning speed is 1500mm/s, the spot diameter is 0.075mm, the substrate temperature is 200 ℃ and the single powder spreading thickness of the substrate is 0.22mm, and finally stopping heating, and taking the formed composite material off the substrate after the substrate is cooled; in the selective laser melting step, laser forming is specifically performed according to a designed shape: scanning the first layer for two periods, and then scanning each layer for one period, wherein the scanning directions between the layers are in an orthogonal relationship, and the overlapping rate of the scanning intervals is 50%, so that a block is obtained; c: placing the formed composite material into a vacuum furnace, vacuumizing until the pressure is less than 1Pa, and preserving heat for 3 hours under the condition that the sintering temperature is 1050 ℃ to obtain a sintered composite material; d: and (3) under the conditions that the hot isostatic pressing temperature is 1050 ℃ and the hot isostatic pressing pressure is 180MPa, the sintered composite material is subjected to heat preservation and pressure maintaining for 2 hours, and the diamond aluminum nitride-based composite material is obtained.
Example 2
Example 2 is substantially the same as example 1 except that:
(1) treating diamond powder (average particle diameter of 200 μm) by an inductively coupled plasma method to obtain roughened diamond powder; the process conditions of the inductively coupled plasma method are as follows: the excitation source power is 2000W; the process gas is a mixed gas of argon and hydrogen, the partial pressure of the hydrogen in the mixed gas is 20%, the process air pressure is 5Pa, and the process temperature is 100 ℃; the surface roughness of the obtained roughened diamond powder was 30nm.
Example 3
Example 3 is substantially the same as example 1 except that:
(1) treating diamond powder (average particle diameter of 200 μm) by an inductively coupled plasma method to obtain roughened diamond powder; the process conditions of the inductively coupled plasma method are as follows: the excitation source power is 15000W; the process gas is a mixed gas of argon and hydrogen, the partial pressure of the hydrogen in the mixed gas is 65%, the process air pressure is 5Pa, and the process temperature is 100 ℃; the surface roughness of the obtained roughened diamond powder was 100nm.
Example 4
Example 4 is substantially the same as example 1 except that:
(1) Treating diamond powder (average particle diameter of 200 μm) by an inductively coupled plasma method to obtain roughened diamond powder; the process conditions of the inductively coupled plasma method are as follows: the excitation source power is 20000W; the process gas is a mixed gas of argon and hydrogen, the partial pressure of the hydrogen in the mixed gas is 80%, the process air pressure is 5Pa, and the process temperature is 100 ℃; the surface roughness of the obtained roughened diamond powder was 130nm.
Example 5
Example 5 is substantially the same as example 1 except that:
(2) preparing a first plating layer on the surface of the roughened diamond powder by a plasma enhanced atomic layer deposition method, and then preparing a second plating layer (aluminum nitride plating layer) on the basis of the first plating layer by a plasma enhanced chemical vapor deposition method to obtain plated diamond powder; the first plating layer sequentially comprises a first aluminum nitride layer, a second aluminum nitride layer and a third aluminum nitride layer, the first aluminum nitride layer is closer to the surface of the roughened diamond powder than the second aluminum nitride layer, the thicknesses of the first aluminum nitride layer, the second aluminum nitride layer and the third aluminum nitride layer are 20nm, and the thickness of the second plating layer is 15 mu m; the first aluminum nitride layer, the second aluminum nitride layer and the third aluminum nitride layer are prepared by a plasma enhanced atomic layer deposition method, except that the volume flow ratio of precursor materials to reaction gases is different, and other process conditions are as follows: the precursor material is trimethylaluminum; excitation source power is 12000W; the reaction gas is ammonia gas; the process air pressure is 6Pa, the process temperature is 180 ℃, the volume flow ratio of the precursor material to the reaction gas is 1:1.5 when the first aluminum nitride layer is prepared, the volume flow ratio of the precursor material to the reaction gas is 1:1.2 when the second aluminum nitride layer is prepared, and the volume flow ratio of the precursor material to the reaction gas is 1:1 when the third aluminum nitride layer is prepared; the process conditions for preparing the second plating layer by a plasma enhanced chemical vapor deposition method are as follows: the excitation source power is 10000W; the reaction gas comprises trimethylaluminum and ammonia, wherein the volume percentage of the ammonia in the reaction gas is 65%, and the volume percentage of the trimethylaluminum in the reaction gas is 35%; the process air pressure is 6Pa; the process temperature was 180 ℃.
Comparative example 1
(1) Preparing a first plating layer (aluminum nitride plating layer) on the surface of diamond powder (average grain size of 200 mu m) by a plasma enhanced atomic layer deposition method, and then preparing a second plating layer (aluminum nitride plating layer) on the basis of the first plating layer by a plasma enhanced chemical vapor deposition method to obtain plated diamond powder; the thickness of the first plating layer is 60nm, and the thickness of the second plating layer is 15 mu m; the process conditions for preparing the first plating layer by the plasma enhanced atomic layer deposition method are as follows: the precursor material is trimethylaluminum; excitation source power is 12000W; the reaction gas is ammonia gas; the process air pressure is 6Pa, the process temperature is 180 ℃, and the volume flow ratio of the precursor material to the reaction gas is 1:1.2; the process conditions for preparing the second plating layer by a plasma enhanced chemical vapor deposition method are as follows: the excitation source power is 10000W; the reaction gas comprises trimethylaluminum and ammonia, wherein the volume percentage of the ammonia in the reaction gas is 65%, and the volume percentage of the trimethylaluminum in the reaction gas is 35%; the process air pressure is 6Pa; the process temperature was 180 ℃.
(2) The diamond aluminum nitride based composite material is prepared by taking plating diamond powder and aluminum nitride powder as raw materials through additive manufacturing: a: mechanically and uniformly mixing the plated diamond powder and the aluminum nitride powder to obtain mixed powder; the aluminum nitride powder is a mixture of aluminum nitride powder with the particle size of 20-40 mu m and aluminum nitride powder with the particle size of 1-5 mu m; the volume ratio of the plating diamond powder to the aluminum nitride powder with the grain diameter of 20-40 μm is 7:2; the volume ratio of the plating diamond powder to the aluminum nitride powder with the grain diameter of 1-5 mu m is 7:1; b: in a selective laser melting device, introducing high-purity argon to ensure that the oxygen content in a forming cavity is lower than 0.1%, preheating a substrate (aluminum nitride substrate) to 200 ℃, carrying out laser forming by using mixed powder according to a designed shape under the conditions that the laser power is 100W, the scanning speed is 1500mm/s, the spot diameter is 0.075mm, the substrate temperature is 200 ℃ and the single powder spreading thickness of the substrate is 0.22mm, and finally stopping heating, and taking the formed composite material off the substrate after the substrate is cooled; in the selective laser melting step, laser forming is specifically performed according to a designed shape: scanning the first layer for two periods, and then scanning each layer for one period, wherein the scanning directions between the layers are in an orthogonal relationship, and the overlapping rate of the scanning intervals is 50%, so that a block is obtained; c: placing the formed composite material into a vacuum furnace, vacuumizing until the pressure is less than 1Pa, and preserving heat for 3 hours under the condition that the sintering temperature is 1050 ℃ to obtain a sintered composite material; d: and (3) under the conditions that the hot isostatic pressing temperature is 1050 ℃ and the hot isostatic pressing pressure is 180MPa, the sintered composite material is subjected to heat preservation and pressure maintaining for 2 hours, and the diamond aluminum nitride-based composite material is obtained.
Comparative example 2
Comparative example 2 is substantially the same as example 1 except that:
(2) preparing a first plating layer (aluminum nitride plating layer) on the surface of the roughened diamond powder by a magnetron sputtering method, and then preparing a second plating layer (aluminum nitride plating layer) on the basis of the first plating layer by a plasma enhanced chemical vapor deposition method to obtain plated diamond powder; the thickness of the first plating layer is 60nm, and the thickness of the second plating layer is 15 mu m; the process conditions for preparing the first plating layer by a magnetron sputtering method are as follows: an aluminum target material is adopted, the nitrogen flow is 60sccm, the argon flow is 120sccm, the working air pressure is 6Pa, the sputtering temperature is 60 ℃, and the magnetron sputtering power density (radio frequency magnetron sputtering power density) is 4W/cm 2 The method comprises the steps of carrying out a first treatment on the surface of the The process conditions for preparing the second plating layer by a plasma enhanced chemical vapor deposition method are as follows: the excitation source power is 10000W; the reaction gas comprises trimethylaluminum and ammonia, wherein the volume percentage of the ammonia in the reaction gas is 65%, and the volume percentage of the trimethylaluminum in the reaction gas is 35%; the process air pressure is 6Pa; the process temperature was 100 ℃.
The present invention measured the results of the density, room temperature thermal conductivity, 500 c thermal conductivity and breakdown voltage resistance of the diamond aluminum nitride based composite materials prepared in each example and each comparative example as shown in table 1.
TABLE 1
In table 1, the symbol "-" indicates that the performance index was not tested. As shown in the results of Table 1, the thermal conductivity of the diamond aluminum nitride-based composite material prepared in some preferred embodiments of the invention can reach 600-700W/(m.K), the density is not less than 99%, and the diamond aluminum nitride-based composite material has high insulation performance and breakdown voltage resistance as high as 14kV.
The invention is not described in detail in a manner known to those skilled in the art.
Finally, it should be noted that: the above embodiments are only for illustrating the technical solution of the present invention, and are not limiting; although the invention has been described in detail with reference to the foregoing embodiments, it will be understood by those of ordinary skill in the art that: the technical scheme described in the foregoing embodiments can be modified or some technical features thereof can be replaced by equivalents; such modifications and substitutions do not depart from the spirit and scope of the technical solutions of the embodiments of the present invention.
Claims (10)
1. A method for preparing a diamond aluminum nitride based composite material, which is characterized by comprising the following steps:
(1) Treating the diamond powder by an inductive coupling plasma method or an anode layer ion source irradiation mode to obtain roughened diamond powder;
(2) Preparing a first plating layer on the surface of the roughened diamond powder by a plasma enhanced atomic layer deposition method, and then preparing a second plating layer on the basis of the first plating layer by a chemical vapor deposition method to obtain plated diamond powder; the first plating layer and the second plating layer are both aluminum nitride plating layers;
(3) The diamond aluminum nitride based composite material is manufactured by taking plating diamond powder and aluminum nitride powder as raw materials through additive manufacturing.
2. The method of manufacturing according to claim 1, characterized in that:
the grain diameter of the diamond powder is 20-400 mu m;
the surface roughness of the roughened diamond powder is 5-100 nm;
the thickness of the first plating layer is 10-200 nm, preferably 40-60 nm; and/or
The thickness of the second plating layer is not less than 10 μm.
3. The method according to claim 1, wherein the inductively coupled plasma method comprises the following process conditions:
the power of the excitation source is 50-20000W;
the process gas is a mixed gas of argon and hydrogen or a mixed gas of argon and oxygen, preferably, the partial pressure of hydrogen is 10-90% in the mixed gas of argon and hydrogen, and the partial pressure of oxygen is 10-90% in the mixed gas of argon and oxygen;
The process air pressure is 0.1-10 Pa; and/or
The process temperature is 25-200 ℃.
4. The preparation method according to claim 1, wherein the process conditions of the anode layer ion source irradiation mode are as follows:
the power of the excitation source is 500-30000W;
the process gas is a mixed gas of argon and hydrogen or a mixed gas of argon and oxygen, preferably, the partial pressure of hydrogen is 10-90% in the mixed gas of argon and hydrogen, and the partial pressure of oxygen is 10-90% in the mixed gas of argon and oxygen;
the process air pressure is 0.1-10 Pa; and/or the process temperature is 25-200 ℃.
5. The method of manufacturing according to claim 1, characterized in that:
the process conditions for preparing the first plating layer by the plasma enhanced atomic layer deposition method are as follows:
the precursor material is trimethylaluminum;
the power of the excitation source is 50-20000W;
the reaction gas is ammonia gas;
the process air pressure is 0.5-20 Pa; and/or
The process temperature is 30-300 ℃.
6. The method of manufacturing according to claim 5, wherein:
the first plating layer comprises a first aluminum nitride layer, a second aluminum nitride layer and a third aluminum nitride layer in sequence, wherein the first aluminum nitride layer is closer to the surface of the roughened diamond powder than the second aluminum nitride layer;
When preparing the first aluminum nitride layer, the volume flow ratio of the precursor material to the reaction gas is 1: (1.5-1.8);
when preparing the second aluminum nitride layer, the volume flow ratio of the precursor material to the reaction gas is 1: (1.1-1.3);
when preparing the third aluminum nitride layer, the volume flow ratio of the precursor material to the reaction gas is 1: (0.8-1).
7. The method of manufacturing according to claim 1, characterized in that:
the process conditions for preparing the second plating layer by the chemical vapor deposition method are as follows:
the reaction gas contains trimethylaluminum and ammonia, and preferably, the volume percentage of the ammonia in the reaction gas is 20-80%;
the process air pressure is 0.5-20 Pa; and/or
The process temperature is 200-500 ℃.
8. The method of manufacturing according to claim 1, characterized in that:
the chemical vapor deposition method is a plasma enhanced chemical vapor deposition method or a hot wire chemical vapor deposition method;
preferably, the process conditions for preparing the second plating layer by the plasma enhanced chemical vapor deposition method are as follows:
the power of the excitation source is 50-20000W;
the reaction gas contains trimethylaluminum and a nitrogen-containing gas, preferably, the volume percentage of the nitrogen-containing gas in the reaction gas is 20-80%, and preferably, the nitrogen-containing gas is ammonia and/or nitrogen;
The process air pressure is 0.5-20 Pa; and/or
The process temperature is 30-300 ℃;
preferably, the process conditions for preparing the second plating layer by the hot filament chemical vapor deposition method are as follows:
the reaction gas contains trimethylaluminum and ammonia, and preferably, the volume percentage of the ammonia in the reaction gas is 20-80%;
the process air pressure is 0.5-20 Pa; and/or
The process temperature is 200-500 ℃.
9. The method of manufacturing according to claim 1, characterized in that:
in step (3), the volume ratio of the plated diamond powder to the aluminum nitride powder is 1: (0.1-3);
in the step (3), the aluminum nitride powder is aluminum nitride powder with the particle size of 1-5 mu m and/or aluminum nitride powder with the particle size of 20-40 mu m; and/or
The step (3) is as follows: the diamond-coated aluminum nitride-based composite material is prepared by taking coated diamond powder and aluminum nitride powder as raw materials and sequentially carrying out a mixing step, a zone-selecting laser melting step, a sintering step and a hot isostatic pressing step;
preferably, a cold isostatic pressing step is further included between the selective laser melting step and the sintering step.
10. A diamond aluminum nitride based composite material produced by the production method according to any one of claims 1 to 9.
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