阅读说明：本技术 一种含sic绒毛的石墨烯纸热界面材料 (Graphene paper thermal interface material containing SIC fluff ) 是由 周敏 黄新 姚海英 魏俊杰 于 2020-12-08 设计创作，主要内容包括：本发明公开了一种含SIC绒毛的石墨烯纸热界面材料,包括SiO-2浆料,所述SiO-2浆料包括55-65％的水、0-1％的润湿剂、0-1％的消泡剂、5-15％的水性树脂、0-1％的分散剂、15-25％的纳米SiO-2、0-1％的PH调节剂和5-15％的防沉剂,按照上述各重量组分的配比材料,依次将水、分散剂、润湿剂、纳米Si0-2粉体、消泡剂、pH调节剂、防沉剂和水性树脂加入到容器中,并在加入原料的同时进行机械搅拌。该含SIC绒毛的石墨烯纸热界面材料采用改良hummers法制备的氧化石墨烯溶液(GO)和SiO-2水溶胶作为原材料,简单易得,采用超声混合、真空抽滤、电磁感应快速退火、真空烘干等简便的方法,用几个简单的步骤就可以制得高性能的热界面材料。(The invention discloses a graphene paper thermal interface material containing SIC fluff, which comprises SiO 2 Slurry of said SiO 2 The slurry comprises 55-65% of water, 0-1% of wetting agent, 0-1% of defoaming agent, 5-15% of water-based resin, 0-1% of dispersing agent and 15-25% of nano SiO 2 0-1% of PH regulator and 5-15% of anti-settling agent, and water, dispersant, wetting agent and nano Si0 are sequentially mixed according to the mixture ratio of the components 2 Adding the powder, the defoaming agent, the pH regulator, the anti-settling agent and the water-based resin into a container, and mechanically stirring while adding the raw materials. The graphene oxide paper thermal interface material containing SIC fluff is prepared by adopting an improved hummers methodSolution (GO) and SiO 2 The hydrosol is used as a raw material, is simple and easy to obtain, and can be prepared into the high-performance thermal interface material by adopting a simple and convenient method such as ultrasonic mixing, vacuum filtration, electromagnetic induction rapid annealing, vacuum drying and the like through a plurality of simple steps.)

1. A graphene paper thermal interface material containing SIC fluff comprises SiO₂The slurry is characterized in that: the SiO₂The slurry comprises 55-65% of water, 0-1% of wetting agent, 0-1% of defoaming agent, 5-15% of water-based resin, 0-1% of dispersing agent and 15-25% of nano SiO₂0-1% of PH regulator and 5-15% of anti-settling agent, and water, dispersant, wetting agent and nano Si0 are sequentially mixed according to the mixture ratio of the components₂Adding powder, defoaming agent, pH regulator, anti-settling agent and water-base resin into a container, mechanically stirring while adding raw materials, and after the raw materials are added, dispersing by 3 means of high-speed dispersion, sanding and ultrasonic dispersion until the fineness is less than 50um to obtain the nano SiO₂The preparation process of the graphene paper thermal interface material of the SIC fluff is as follows:

a. dispersing 1mg-1000mg of Graphene Oxide (GO) in a mixture of 1ml-300ml of ethanol and 1ml-30ml of deionized water for ultrasonic treatment;

b. 100-1000uL of SiO were added to the dispersion₂The slurry is subjected to ultrasonic mixing treatment, wherein the dropping speed cannot be too high, the dropping speed is required to be 10-100uL/s, and ultrasonic dispersion is assisted during the dropping so as to ensure that SiO is dispersed₂Can be uniformly dispersed on the GO surface;

c. vacuum filtering the product after ultrasonic treatment, collecting, washing with deionized water for several times until neutral pH value is reached, drying the product at 60 deg.C, and adding SiO₂Nanoparticle-modified graphene oxide paper (SiO)₂@ GO paper) is peeled off from a Polytetrafluoroethylene (PTFE) filter membrane;

d. SiO to be obtained₂The @ GO paper is pre-annealed for 4-12h at 140 ℃ in a vacuum oven to remove residual moisture and partial oxygen-containing groups in the paper;

e. and treating the thin paper at 1300-1500 ℃ by using a 2000 ℃ temperature-controlled induction heating furnace with the crystal model of SP-50KTC in the fertilizer combination department to obtain the SiC hybridized graphene paper.

2. The SIC fluff-containing graphene paper thermal interface material of claim 1, wherein: the pore size of the Polytetrafluoroethylene (PTFE) filter membrane is 0.22 um.

3. The SIC fluff-containing graphene paper thermal interface material of claim 1, wherein: the specific temperature rise parameters in the step e are as follows: the heating rate of 25-1000 ℃ is 1 ℃/s, the temperature is kept for 10min at 1000 ℃, the heating rate of more than 1000 ℃ is 0.5 ℃/s, and the temperature is kept for 4-10min at the final target temperature.

4. The SIC fluff-containing graphene paper thermal interface material of claim 1, wherein: the preparation method of the graphene paper thermal interface material containing SIC fluff comprises the following basic formula:

SiO₂(s)+3C(s)＝SiC(s)+2CO(g)

SiO₂(s)+CO(g)＝SiO(s)+CO2(g)

3SiO(g)+CO(g)＝SiC(S)+2SiO₂(s)。

Technical Field

The invention relates to the technical field of thermal management, in particular to a graphene paper thermal interface material containing SIC fluff.

Background

Graphene Oxide (GO) is prepared from natural graphite by a modified Hummers method, as a precursor material of graphene, GO is easily dispersed in water due to a plurality of oxygen-containing functional groups (such as hydroxyl, carbonyl and epoxy) existing on the surface of the graphene, because hydrogen bonds can be formed between the oxygen-containing groups and water molecules, and is more easily prepared into a high-toughness macroscopic thin film compared with the weak water dispersibility of graphene, however, the thermal conductivity of GO is not ideal due to surface defects, edge disorder or surface functional groups of GO, therefore, graphene oxide (RGO) is reduced by a reduction method subsequently, the thermal and electrical properties of the Graphene Oxide (GO) are improved, (a graphene-based thin film is prepared by reducing Graphene Oxide (GO) by a chemical reducing agent or high-temperature treatment, wherein the most common method is that RGO thin film is prepared by reducing GO in situ by hydrazine hydrate, but hydrazine hydrate is extremely toxic, the method is usually an environmental problem, and therefore, how to design the graphene paper thermal interface material containing the SIC fluff, which has high surface thermal conductivity and proper mechanical property, becomes a problem to be solved currently.

Disclosure of Invention

The invention aims to provide a graphene paper thermal interface material containing SIC fluff, so as to solve the problems in the background technology.

In order to achieve the purpose, the invention provides the following technical scheme: a graphene paper thermal interface material containing SIC fluff comprises SiO₂Slurry of said SiO₂The slurry comprises 55-65% of water, 0-1% of wetting agent, 0-1% of defoaming agent, 5-15% of water-based resin, 0-1% of dispersing agent and 15-25% of nano SiO₂0-1% of PH regulator and 5-15% of anti-settling agent, and water, dispersant, wetting agent and nano Si0 are sequentially mixed according to the mixture ratio of the components₂Adding powder, defoaming agent, pH regulator, anti-settling agent and water-base resin into container, and simultaneously adding raw materialMechanically stirring, after the raw materials are added, dispersing by 3 means of high-speed dispersion, sand grinding and ultrasonic dispersion until the fineness is less than 50um to obtain the nano SiO₂The preparation process of the graphene paper thermal interface material of the SIC fluff is as follows:

a. dispersing 1mg-1000mg of Graphene Oxide (GO) in a mixture of 1ml-300ml of ethanol and 1ml-30ml of deionized water for ultrasonic treatment;

b. 100-1000uL of SiO were added to the dispersion₂The slurry is subjected to ultrasonic mixing treatment, wherein the dropping speed cannot be too high, the dropping speed is required to be 10-100uL/s, and ultrasonic dispersion is assisted during the dropping so as to ensure that SiO is dispersed₂Can be uniformly dispersed on the GO surface;

c. vacuum filtering the product after ultrasonic treatment, collecting, washing with deionized water for several times until neutral pH value is reached, drying the product at 60 deg.C, and adding SiO₂Nanoparticle-modified graphene oxide paper (SiO)₂@ GO paper) is peeled off from a Polytetrafluoroethylene (PTFE) filter membrane;

d. SiO to be obtained₂The @ GO paper is pre-annealed for 4-12h at 140 ℃ in a vacuum oven to remove residual moisture and partial oxygen-containing groups in the paper;

e. and treating the thin paper at 1300-1500 ℃ by using a 2000 ℃ temperature-controlled induction heating furnace with the crystal model of SP-50KTC in the fertilizer combination department to obtain the SiC hybridized graphene paper.

Preferably, the pore size of the Polytetrafluoroethylene (PTFE) filter membrane is 0.22 um.

Preferably, the specific temperature-raising parameters in step e are as follows: the heating rate of 25-1000 ℃ is 1 ℃/s, the temperature is kept for 10min at 1000 ℃, the heating rate of more than 1000 ℃ is 0.5 ℃/s, and the temperature is kept for 4-10min at the final target temperature.

Preferably, the basic formula in the preparation method of the graphene paper thermal interface material containing SIC fluff is as follows:

SiO₂(s)+3C(s)＝SiC(s)+2CO(g)

SiO₂(s)+CO(g)＝SiO(s)+CO2(g)

3SiO(g)+CO(g)＝SiC(S)+2SiO₂(s)。

compared with the prior art, the invention has the beneficial effects that: the graphene paper thermal interface material containing SIC fluff adopts graphene oxide solution (GO) and SiO prepared by an improved hummers method₂The hydrosol is used as raw material, is simple and easy to obtain, adopts simple and convenient methods of ultrasonic mixing, vacuum filtration, electromagnetic induction rapid annealing, vacuum drying and the like, can prepare the high-performance thermal interface material by using a plurality of simple steps, and uses the composite SiO₂The SiC villus is grown by the particles and assisted by a rapid annealing process, so that a bridge between graphene layers is built, the axial thermal conductivity of the graphene is greatly improved, meanwhile, villous SiC is generated by the unique method, covalent bonds are generated between the SiC and the graphene, and the SiC is mutually wound through the villus, so that the thermal conductivity of the SiC is improved.

Drawings

FIG. 1 is a graph of the present invention through SiO before annealing₂Schematic view of modified GO;

FIG. 2 is a diagram showing a spherical SiO particle having a diameter of about 2 μm agglomerated with large particles before annealing in the present invention₂A schematic diagram;

FIG. 3 is a schematic vertical cross-sectional view of SiC fluff after 1400 ℃ annealing in accordance with the present invention;

FIG. 4 is a schematic cross-sectional view of SiC fluff after 1400 ℃ annealing in the present invention;

FIG. 5 shows the triple agglomerated SiO after 1400 ℃ annealing in the present invention₂Reducing and growing into a schematic diagram of the SiC nanowire.

Detailed Description

The technical solutions in the embodiments of the present invention will be clearly and completely described below with reference to the drawings in the embodiments of the present invention, and it is obvious that the described embodiments are only a part of the embodiments of the present invention, and not all of the embodiments. All other embodiments, which can be derived by a person skilled in the art from the embodiments given herein without making any creative effort, shall fall within the protection scope of the present invention.

In the description of the present invention, it should be noted that the terms "upper", "lower", "inner", "outer", "front", "rear", "both ends", "one end", "the other end", and the like indicate orientations or positional relationships based on those shown in the drawings, and are only for convenience of description and simplicity of description, but do not indicate or imply that the referred device or element must have a specific orientation, be constructed in a specific orientation, and be operated, and thus, should not be construed as limiting the present invention. Furthermore, the terms "first" and "second" are used for descriptive purposes only and are not to be construed as indicating or implying relative importance.

In the description of the present invention, it is to be noted that, unless otherwise explicitly specified or limited, the terms "mounted," "disposed," "connected," and the like are to be construed broadly, such as "connected," which may be fixedly connected, detachably connected, or integrally connected; can be mechanically or electrically connected; they may be connected directly or indirectly through intervening media, or they may be interconnected between two elements. The specific meanings of the above terms in the present invention can be understood in specific cases to those skilled in the art.

Referring to fig. 1-5, an embodiment of the present invention is shown:

a graphene paper thermal interface material containing SIC fluff comprises SiO₂Slurries of SiO₂The slurry comprises 55-65% of water, 0-1% of wetting agent, 0-1% of defoaming agent, 5-15% of water-based resin, 0-1% of dispersing agent and 15-25% of nano SiO₂0-1% of PH regulator and 5-15% of anti-settling agent, and water, dispersant, wetting agent and nano Si0 are sequentially mixed according to the mixture ratio of the components₂Adding powder, defoaming agent, pH regulator, anti-settling agent and water-base resin into a container, mechanically stirring while adding raw materials, and after the raw materials are added, dispersing by 3 means of high-speed dispersion, sanding and ultrasonic dispersion until the fineness is less than 50um to obtain the nano SiO₂The preparation process of the graphene paper thermal interface material of the aqueous slurry and SIC fluff is as follows:

a. dispersing 1mg-1000mg of Graphene Oxide (GO) in a mixture of 1ml-300ml of ethanol and 1ml-30ml of deionized water for ultrasonic treatment;

b. 100-1000uL of SiO were added to the dispersion₂The slurry is subjected to ultrasonic mixing treatment, wherein the dropping speed cannot be too high, the dropping speed is required to be 10-100uL/s, and ultrasonic dispersion is assisted during the dropping so as to ensure that SiO is dispersed₂Can be uniformly dispersed on the GO surface;

c. vacuum filtering the product after ultrasonic treatment, collecting, washing with deionized water for several times until neutral pH value is reached, drying the product at 60 deg.C, and adding SiO₂Nanoparticle-modified graphene oxide paper (SiO)₂@ GO paper) is peeled off from a Polytetrafluoroethylene (PTFE) filter membrane;

d. SiO to be obtained₂The @ GO paper is pre-annealed for 4-12h at 140 ℃ in a vacuum oven to remove residual moisture and partial oxygen-containing groups in the paper;

e. and treating the thin paper at 1300-1500 ℃ by using a 2000 ℃ temperature-controlled induction heating furnace with the crystal model of SP-50KTC in the fertilizer combination department to obtain the SiC hybridized graphene paper.

Further, the pore size of the Polytetrafluoroethylene (PTFE) filter membrane was 0.22 um.

Further, the specific temperature-raising parameters in the step e are as follows: the heating rate of 25-1000 ℃ is 1 ℃/s, the temperature is kept for 10min at 1000 ℃, the heating rate of more than 1000 ℃ is 0.5 ℃/s, and the temperature is kept for 4-10min at the final target temperature.

Further, the preparation method of the graphene paper thermal interface material containing SIC fluff has the following basic formula:

SiO₂(s)+3C(s)＝SiC(s)+2CO(g)

SiO₂(s)+CO(g)＝SiO(s)+CO2(g)

3SiO(g)+CO(g)＝SiC(S)+2SiO₂(s)。

it will be evident to those skilled in the art that the invention is not limited to the details of the foregoing illustrative embodiments, and that the present invention may be embodied in other specific forms without departing from the spirit or essential attributes thereof. The present embodiments are therefore to be considered in all respects as illustrative and not restrictive, the scope of the invention being indicated by the appended claims rather than by the foregoing description, and all changes which come within the meaning and range of equivalency of the claims are therefore intended to be embraced therein. Any reference sign in a claim should not be construed as limiting the claim concerned.