CN103756325B - A kind of low loading high thermal conductivity graphene/silicone grease composite and preparation method thereof - Google Patents
A kind of low loading high thermal conductivity graphene/silicone grease composite and preparation method thereof Download PDFInfo
- Publication number
- CN103756325B CN103756325B CN201410021248.6A CN201410021248A CN103756325B CN 103756325 B CN103756325 B CN 103756325B CN 201410021248 A CN201410021248 A CN 201410021248A CN 103756325 B CN103756325 B CN 103756325B
- Authority
- CN
- China
- Prior art keywords
- heat
- preparation
- silicone grease
- redox graphene
- graphene sheet
- Prior art date
- Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
- Active
Links
Landscapes
- Cooling Or The Like Of Semiconductors Or Solid State Devices (AREA)
- Lubricants (AREA)
- Carbon And Carbon Compounds (AREA)
Abstract
The invention discloses a kind of low loading high thermal conductivity graphene/silicone grease composite and preparation method thereof, this kind of heat-conducting silicone grease is made by functionalization redox graphene sheet filling silicon oil；The preparation method of described composite comprises the following steps: preparation functionalization redox graphene sheet is as heat filling；Modified heat filling and dimethicone matrix are sufficiently mixed in double; two roller mills so that functionalization redox graphene sheet can be evenly dispersed in silicone oil matrix；Heat-conducting silicone grease provided by the invention, can be effectively prevented from the contact gap between high power electronic components and parts heater and heat abstractor, reduces interface contact heat resistance, forms efficient heat dissipation channel, and accelerated heat is transmitted；The package cooling of high power electronic components and parts is had very big benefit by this, then improves reliability and the service life thereof of electronic component products, and preparation technology is simple simultaneously。
Description
Technical field
The present invention relates to the low loading high thermal conductivity graphene/silicone grease composite of one and preparation method thereof for the heat radiation of high power electronic component package。
Background technology
Heat-conducting silicone grease, also referred to as heat-conducting cream, is a kind of high heat conduction organosilicon material, can keep cream smectic state when using at-50 DEG C～300 DEG C temperature for a long time。Heat radiation with in heat conduction application, even two planes that surface is very bright and clean, space all can be had when contacting with each other to exist, and the air in space is hot non-conductor, heat that heater distributes can be hindered to the conduction of heat abstractor。Heat-conducting silicone grease is used to fill the contact interface between high power electronic components and parts heater (LED chip, computer CPU, large power supply etc.) and cooling base (radiating fin, metal shell etc.), help to eliminate the air gap of contact, increase heat passage, play the performances such as heat conduction instrumentality and moistureproof, dust-proof, shockproof, anticorrosion, radiation hardness are aging, be splendid thermal interfacial material。
At present, heat-conducting silicone grease is the white carbon, the Al that are prepared by vapor phase method mostly2O3, the filler such as SiC, BN forms with methyl-silicone oil or dimethicone mechanical mixture。Heat conductivity of heat conduction silicate prepared by the method is relatively low, generally only has 0.6～0.9W/ (m K), and properties of product are relatively poor。On the other hand, owing to the heat conductivity of metal-oxide is relatively low so that in the silicone grease of preparation, the loading of filler relatively big (100～1000 parts), this have impact on the mobility of silicone grease, actual radiating effect when finally have impact on it for encapsulating。Additionally, metal-oxide is poor with the compatibility of silicone oil so that heat-conducting silicone grease produces between matrix and filler bigger thermal resistance, finally affects the heat conductivity of heat-conducting silicone grease。
Nano-carbon material is the heat filling with multinomial excellent combination properties such as high heat conduction, high chemical stability, low thermal coefficient of expansion, low-density, bigger serfaces。In numerous nano-carbon materials, Graphene has the features such as high heat conduction, corrosion-resistant, deformability is excellent, and is widely used in the preparation of conductivity thermal interfacial material。Wherein, Graphene is Stability Analysis of Structures thermodynamically, and has prominent heat conductivility, up to 3 times of diamond。At normal temperatures, the thermal conductivity of Graphene is 5000W/ (m K), is more than ten times of Cu thermal conductivity, and heat conductivility exceedes all known materials。Since 2004 find and 2010 obtain Nobel Prize, Graphene causes the research interest of numerous researcher, and therefore it be also widely used in the preparation of Heat Conduction Material。
For these reasons, this invention adopts vacuum and low temperature dilatometry to prepare redox graphene, and utilizes silane coupler that it is carried out functional modification, modified filler is filled dimethicone under low loading and prepares Novel heat-conducting silicone grease。The loading of filler is greatly reduced, has improved the heat conductivility of heat-conducting silicone grease further。
Summary of the invention
It is an object of the invention to provide a kind of low loading high thermal conductivity graphene/silicone grease composite for the heat radiation of high power electronic component package and preparation method thereof。
The technical solution adopted in the present invention is:
The low loading high thermal conductivity graphene/silicone grease composite of one provided by the invention, this kind of heat-conducting silicone grease is made by functionalization redox graphene sheet filling silicon oil；Its mass fraction consists of: dimethicone 100 parts, functionalization redox graphene sheet 0.1～1.5 part, silane coupler 0.01～0.05 part。
Described dimethicone is viscosity when 25 DEG C in temperature is 100～1000cps。
Described dimethicone is that viscosity when 25 DEG C is preferably 500 ± 25cps in temperature。Viscosity is too big, the poor processability of heat-conducting silicone grease。
Described silane coupler is selected from gamma-aminopropyl-triethoxy-silane (KH-550)。Heat filling is different from the interfacial property of silicone oil matrix, its poor compatibility, and the present invention, by adding silane coupler to heat filling modifying surface, strengthens the compatibility of itself and silicone oil, improves dispersibility。
The preparation method that the present invention also provides for a kind of described low loading high thermal conductivity graphene/silicone grease composite, comprises the following steps:
(1) preparation of redox graphene sheet: 5g natural flake graphite is added in 115ml concentrated sulphuric acid, is stirring evenly and then adding into 15gKMnO4, stirring at low speed 2.5 hours in the cryogenic thermostat water-bath of 3～5 DEG C, in the water bath with thermostatic control of 30～35 DEG C, then continue stirring 2 hours, afterwards water bath with thermostatic control temperature is increased to 80 DEG C and continues stirring；Within the scope of 60～70 DEG C, when color sample is brownish red, at the uniform velocity dropping 250ml deionized water, now color sample becomes shiny red, then at the uniform velocity drips 50mlH2O2Till color sample becomes golden yellow completely；Finally the product of acquisition being carried out sucking filtration, clean to neutral with deionized water, then sonic oscillation 30 minutes, at 45 DEG C after dry 72 hours, it is thus achieved that graphene oxide sample；The graphene oxide sample grind into powder that will obtain, heating in vacuum 10 minutes under 200 DEG C of conditions, redox graphene sheet can be obtained；
(2) alcoholic solution of the silane coupler 95wt% of 0.01～0.05 mass fraction is dissolved the solution being configured to 25wt%, continuously stirred, until completely dissolved, add the redox graphene of 0.1～1.5 mass fraction, it is placed in 65 DEG C of water-baths, ultrasonic agitation 4 hours；Treat that solvent evaporates, be placed in evaporating dish, put into drying baker, at 80 DEG C, dry 12h, after dry after 2 hours at 120 DEG C, it is thus achieved that functionalization redox graphene sheet is stand-by；
(3) by 100 mass fractions, at 25 DEG C, viscosity is that the dimethicone of 100～1000cps is placed in double; two roller mill, after silicone oil bag roller, add 0.1～1.5 mass fraction functionalization redox graphene sheet, at 25 DEG C, open refining 30min, be sufficiently mixed, finally collect mixture, ageing 24h, the low loading high thermal conductivity graphene/silicone grease composite of final acquisition。
Described in step (1), the vacuum of vacuum heating conditions is-0.2～-0.6mPa,
The vacuum of described vacuum heating conditions is preferably-0.6mPa。
Beneficial effects of the present invention:
The low loading high thermal conductivity graphene of one prepared by the present invention/silicone grease composite selects Novel Carbon Nanomaterials Graphene as heat filling, under low loading (0.1～1.5wt%) condition, and by silane coupler, filling surface has been modifiied, improve the compatibility and the filler dispersibility in silicone oil of heat filling and matrix silicone oil, improve the heat conductivility of heat-conducting silicone grease, heat conductivity is up to 2.7W/ (m K), reduce interface contact heat resistance, thermal resistance value is only 0.68K/W, defines effective heat dissipation channel。The present invention has very big benefit for the package cooling of high power electronic components and parts, can improve reliability and the service life of electronic devices and components, and preparation technology of the present invention is simple, with low cost, reproducible, it is highly suitable for the package cooling material of high power electronic components and parts。
Accompanying drawing explanation
Accompanying drawing 1 is the structural representation of applicable object of the present invention (for high-power LED lamp)。
Wherein: 1.LED lamp lens, 2.LED chip module, 3.LED chip substrate, 4. heat dissipation interface material, 5.LED heat abstractor, 6. radiating fin。
Detailed description of the invention
For the present invention is better described, it is simple to understand technical scheme, the typical but non-limiting enforcement of the present invention is as follows:
The concrete technology step of the present invention is:
(1) preparation of redox graphene sheet: 5g natural flake graphite is added in 115ml concentrated sulphuric acid, is stirring evenly and then adding into 15gKMnO4, stirring at low speed 2.5 hours in the cryogenic thermostat water-bath of 3～5 DEG C, in the water bath with thermostatic control of 30～35 DEG C, then continue stirring 2 hours, afterwards water bath with thermostatic control temperature is increased to 80 DEG C and continues stirring；Within the scope of 60～70 DEG C, when color sample is brownish red, at the uniform velocity dropping 250ml deionized water, now color sample becomes shiny red, then at the uniform velocity drips 50mlH2O2Till color sample becomes golden yellow completely；Finally the product of acquisition being carried out sucking filtration, clean to neutral with deionized water, then sonic oscillation 30 minutes, at 45 DEG C after dry 72 hours, it is thus achieved that graphene oxide sample；The graphene oxide sample grind into powder that will obtain, heating in vacuum 10 minutes under 200 DEG C of conditions, redox graphene sheet can be obtained；
(2) alcoholic solution of the silane coupler 95wt% of 0.01～0.05 mass fraction is dissolved the solution being configured to 25wt%, continuously stirred, until completely dissolved, add the redox graphene of 0.1～1.5 mass fraction, it is placed in 65 DEG C of water-baths, ultrasonic agitation 4 hours。Treat that solvent evaporates, be placed in evaporating dish, put into drying baker, at 80 DEG C, dry 12h, after dry after 2 hours at 120 DEG C, it is thus achieved that functionalization redox graphene sheet is stand-by。
(3) by 100 mass fractions, at 25 DEG C, viscosity is that the dimethicone of 500 ± 25cps is placed in double; two roller mill, after silicone oil bag roller, add 0.1～1.5 mass fraction functionalization redox graphene sheet, at 25 DEG C, open refining 30min, be sufficiently mixed, finally collect mixture, ageing 24h, the final heat-conducting silicone grease composite obtaining functionalization redox graphene sheet filling silicon oil。
(4) for high-power LED lamp, the actually used situation of heat-conducting silicone grease prepared by the test present invention。In conjunction with accompanying drawing 1, above-mentioned heat-conducting silicone grease is applied in the gap location between LED chip substrate 3 and heat abstractor 5 uniformly。
(5) by measuring the real time temperature of LED chip substrate 3 and heat abstractor 5, calculate temperature difference between the two and assess the heat-conducting silicone grease of preparation heat-transfer capability on high power electronic component package is dispelled the heat and thermal resistance。
The technological parameter that embodiment 1～5 heat-conducting silicone grease is pressed in mass fraction composition and preparation process is as shown in table 1。
Table 1 heat-conducting silicone grease composition and preparation technology parameter
| Embodiment 1 | Embodiment 2 | Embodiment 3 | Embodiment 4 | Embodiment 5 | |
| Dimethicone | 100 | 100 | 100 | 100 | 100 |
| Functionalization redox graphene sheet | 0.1 | 0.3 | 0.5 | 1.0 | 1.5 |
| Silane coupling agent KH550 | 0.01 | 0.01 | 0.02 | 0.03 | 0.05 |
| Incorporation time (minute) | 30 | 30 | 30 | 30 | 30 |
| Mixing temperature (DEG C) | 25 | 25 | 25 | 25 | 25 |
Formula described in embodiment 1～5, under process conditions as above, prepares paste heat-conducting silicone grease described in embodiment 1～5。And embodiment 1～5 heat-conducting silicone grease is carried out performance test, result is as shown in table 2。
Table 2 heat-conducting silicone grease performance test
By Hotdisk thermal constant analyser, heat conductivity of heat conduction silicate is measured, by high-power LED lamp actual measurement, practice effect is described。Final result shows, heat-conducting silicone grease prepared by functionalization redox graphene sheet filling dimethicone can have higher thermal conductivity and good heat-conductive characteristic, is highly suitable for the heat radiation of high power electronic component package。
Claims (4)
1. the preparation method of one kind low loading high thermal conductivity graphene/silicone grease composite, it is characterised in that: this kind of heat-conducting silicone grease is made by functionalization redox graphene sheet filling silicon oil；Its mass fraction consists of: dimethicone 100 parts, functionalization redox graphene sheet 0.1 ~ 1.5 part, silane coupler 0.01 ~ 0.05 part；Described dimethicone is viscosity when 25 DEG C in temperature is 100 ~ 1000cps；Described silane coupler is gamma-aminopropyl-triethoxy-silane；
The preparation method of described low loading high thermal conductivity graphene/silicone grease composite comprises the following steps:
(1) preparation of redox graphene sheet: 5g natural flake graphite is added in 115ml concentrated sulphuric acid, is stirring evenly and then adding into 15gKMnO4, stirring at low speed 2.5 hours in the cryogenic thermostat water-bath of 3 ~ 5 DEG C, in the water bath with thermostatic control of 30 ~ 35 DEG C, then continue stirring 2 hours, afterwards water bath with thermostatic control temperature is increased to 80 DEG C and continues stirring；Within the scope of 60 ~ 70 DEG C, when color sample is brownish red, at the uniform velocity dropping 250ml deionized water, now color sample becomes shiny red, then at the uniform velocity drips 50mlH2O2Till color sample becomes golden yellow completely；Finally the product of acquisition being carried out sucking filtration, clean to neutral with deionized water, then sonic oscillation 30 minutes, at 45 DEG C after dry 72 hours, it is thus achieved that graphene oxide sample；The graphene oxide sample grind into powder that will obtain, heating in vacuum 10 minutes under 200 DEG C of conditions, redox graphene sheet can be obtained；
(2) alcoholic solution of the silane coupler 95wt% of 0.01 ~ 0.05 mass fraction is dissolved the solution being configured to 25wt%, continuously stirred, until completely dissolved, add the redox graphene of 0.1 ~ 1.5 mass fraction, it is placed in 65 DEG C of water-baths, ultrasonic agitation 4 hours；Treat that solvent evaporates, be placed in evaporating dish, put into drying baker, at 80 DEG C, dry 12h, after dry after 2 hours at 120 DEG C, it is thus achieved that functionalization redox graphene sheet is stand-by；
(3) by 100 mass fractions, at 25 DEG C, viscosity is that the dimethicone of 100 ~ 1000cps is placed in double; two roller mill, after silicone oil bag roller, add 0.1 ~ 1.5 mass fraction functionalization redox graphene sheet, at 25 DEG C, open refining 30min, be sufficiently mixed, finally collect mixture, ageing 24h, the low loading high thermal conductivity graphene/silicone grease composite of final acquisition。
2. preparation method as claimed in claim 1, it is characterised in that: described dimethicone is viscosity when 25 DEG C in temperature is 500 ± 25cps。
3. preparation method as claimed in claim 1, it is characterised in that: described in step (1), the vacuum of vacuum heating conditions is-0.2 ~-0.6mPa。
4. preparation method as claimed in claim 3, it is characterised in that: the vacuum of described vacuum heating conditions is-0.6mPa。
Priority Applications (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201410021248.6A CN103756325B (en) | 2014-01-16 | 2014-01-16 | A kind of low loading high thermal conductivity graphene/silicone grease composite and preparation method thereof |
Applications Claiming Priority (1)
| Application Number | Priority Date | Filing Date | Title |
|---|---|---|---|
| CN201410021248.6A CN103756325B (en) | 2014-01-16 | 2014-01-16 | A kind of low loading high thermal conductivity graphene/silicone grease composite and preparation method thereof |
Publications (2)
| Publication Number | Publication Date |
|---|---|
| CN103756325A CN103756325A (en) | 2014-04-30 |
| CN103756325B true CN103756325B (en) | 2016-06-22 |
Family
ID=50523661
Family Applications (1)
| Application Number | Title | Priority Date | Filing Date |
|---|---|---|---|
| CN201410021248.6A Active CN103756325B (en) | 2014-01-16 | 2014-01-16 | A kind of low loading high thermal conductivity graphene/silicone grease composite and preparation method thereof |
Country Status (1)
| Country | Link |
|---|---|
| CN (1) | CN103756325B (en) |
Families Citing this family (21)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN104893296A (en) * | 2015-06-05 | 2015-09-09 | 哈尔滨工业大学 | Composite silicone grease with high thermal conductivity and preparation method thereof |
| CN105400201A (en) * | 2015-12-14 | 2016-03-16 | 湖南工业大学 | Spherical alumina/graphene composite heat-conducting silicone grease and preparation method thereof |
| CN105885418A (en) * | 2015-12-14 | 2016-08-24 | 湖南工业大学 | Aluminum nitride/graphene composite thermally conductive silicone grease and preparing method thereof |
| CN105400202A (en) * | 2015-12-14 | 2016-03-16 | 湖南工业大学 | Boron nitride/graphene composite heat-conducting silicone grease and preparation method thereof |
| CN105348807A (en) * | 2015-12-14 | 2016-02-24 | 湖南工业大学 | Silicon dioxide/graphene/graphite compound heat-conducting silicone grease and preparation method thereof |
| CN105351774B (en) * | 2015-12-21 | 2019-02-22 | 朱惠冲 | LED module and lamps and lanterns split structure |
| CN105733265B (en) * | 2016-03-25 | 2019-05-17 | 江南石墨烯研究院 | A kind of preparation method of heat-conducting silicone grease |
| CN107488349A (en) * | 2016-06-13 | 2017-12-19 | 沈阳芯光科技有限公司 | A kind of heat-conducting silicone grease being modified using graphene and aluminum oxide binary additive and preparation method thereof |
| CN106633887B (en) * | 2016-06-21 | 2020-03-27 | 深圳市大族元亨光电股份有限公司 | Graphene heat-conducting silicone grease for high-power LED and preparation method thereof |
| CN106832961B (en) * | 2017-02-28 | 2019-12-03 | 深圳市大族元亨光电股份有限公司 | The preparation method of graphene thermal conductive silicon rubber mat |
| CN107337881B (en) * | 2017-06-29 | 2020-05-08 | 华中科技大学鄂州工业技术研究院 | Fluororesin interface agent for LED packaging, preparation and use method |
| CN107275465B (en) * | 2017-06-29 | 2019-01-04 | 华中科技大学鄂州工业技术研究院 | LED encapsulation and preparation method thereof |
| CN107746576A (en) * | 2017-11-15 | 2018-03-02 | 郴州国盛新材科技有限公司 | A kind of silica/micro- swollen graphite/graphite composite heat-conducting silicone grease and preparation method thereof |
| CN108276615B (en) * | 2017-12-29 | 2020-05-19 | 华中科技大学 | High-thermal-conductivity layered graphene composite material and preparation method thereof |
| CN108165016A (en) * | 2018-01-19 | 2018-06-15 | 林荣铨 | A kind of preparation method of modified graphene heat-conducting silicone grease |
| CN108264771A (en) * | 2018-01-19 | 2018-07-10 | 林荣铨 | A kind of preparation method and applications of graphene heat-conducting silicone grease |
| CN109851823A (en) * | 2018-12-21 | 2019-06-07 | 华中科技大学鄂州工业技术研究院 | A kind of graphene heat conductive silica gel and preparation method thereof |
| CN113801476B (en) * | 2020-06-11 | 2023-04-25 | 山东海科创新研究院有限公司 | Nano silicon dioxide composite graphene heat-conducting silicone grease for GPU and preparation method thereof |
| CN111825347A (en) * | 2020-07-03 | 2020-10-27 | 广东工业大学 | Device and method for orienting glass flakes by electric field |
| CN112063150A (en) * | 2020-09-05 | 2020-12-11 | 深圳市宝力新材料有限公司 | High-thermal-conductivity low-thermal-resistance high-heat-dissipation heat-conduction silica gel and preparation method thereof |
| CN114907698B (en) * | 2022-07-01 | 2023-08-15 | 深圳清华大学研究院 | Modified graphene oxide heat-conducting silicone grease and preparation method thereof |
Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102746670A (en) * | 2012-07-25 | 2012-10-24 | 广东工业大学 | Heat dissipation interface material used for packaging of high-power LED (light emitting diode) lamp and preparation method thereof |
-
2014
- 2014-01-16 CN CN201410021248.6A patent/CN103756325B/en active Active
Patent Citations (1)
| Publication number | Priority date | Publication date | Assignee | Title |
|---|---|---|---|---|
| CN102746670A (en) * | 2012-07-25 | 2012-10-24 | 广东工业大学 | Heat dissipation interface material used for packaging of high-power LED (light emitting diode) lamp and preparation method thereof |
Also Published As
| Publication number | Publication date |
|---|---|
| CN103756325A (en) | 2014-04-30 |
Similar Documents
| Publication | Publication Date | Title |
|---|---|---|
| CN103756325B (en) | A kind of low loading high thermal conductivity graphene/silicone grease composite and preparation method thereof | |
| CN107922743B (en) | Heat conductive resin composition | |
| CN103214848B (en) | Phase change heat-conducting thermal silicone grease composition for central processing unit (CPU) radiating and preparation method thereof | |
| CN105086950B (en) | A kind of high heat conduction cream | |
| CN101294067B (en) | Heat conductive silicone grease composition | |
| CN103497739B (en) | Heat-conducting cream and preparation method thereof | |
| CN105885418A (en) | Aluminum nitride/graphene composite thermally conductive silicone grease and preparing method thereof | |
| CN102250588B (en) | High-performance phase-change heat conduction material and preparation method thereof | |
| CN101985519B (en) | Moulded-in-place high molecular thermal conductive composite material and preparation method thereof | |
| CN102051049A (en) | Insulating and heat conducting silicon resin and preparation method thereof | |
| CN105400202A (en) | Boron nitride/graphene composite heat-conducting silicone grease and preparation method thereof | |
| CN103333494A (en) | Thermal-conductive insulation silicone rubber thermal interface material and preparation method thereof | |
| CN104140678A (en) | Self-adhesive heat-conducting silicone grease and preparation method thereof | |
| CN105062076A (en) | Heat-conducting graphene silicone grease and preparation method thereof | |
| CN105315968A (en) | Silicon-free phase-change heat transfer paste and preparation method thereof | |
| CN105315414A (en) | Preparation method for phase-change heat conduction silicon sheet | |
| CN102153955A (en) | Preparation method of heat conduction paster adopting fiber glass mesh as supporting structure | |
| CN108276612B (en) | Preparation and application of graphene/silicon composite heat-conducting silicone grease | |
| CN105348806A (en) | Carborundum/zinc oxide/graphene compounded heat-conducting silicone grease and preparation method thereof | |
| CN102250589B (en) | High performance silica-free heat conductive paste, and preparation method thereof | |
| CN105348807A (en) | Silicon dioxide/graphene/graphite compound heat-conducting silicone grease and preparation method thereof | |
| CN107099146A (en) | A kind of CPU high-efficiency heat conduction materials and preparation method thereof | |
| CN102532902A (en) | Macromolecule heat conduction material and preparation method thereof | |
| JP5755977B2 (en) | High thermal conductive resin composition | |
| CN103122237A (en) | Heat-conducting glue and preparation method thereof |
Legal Events
| Date | Code | Title | Description |
|---|---|---|---|
| C06 | Publication | ||
| PB01 | Publication | ||
| C10 | Entry into substantive examination | ||
| SE01 | Entry into force of request for substantive examination | ||
| C14 | Grant of patent or utility model | ||
| GR01 | Patent grant |