WO2022205079A1 - 一种有机硅/石墨烯热界面材料的制备方法 - Google Patents

一种有机硅/石墨烯热界面材料的制备方法 Download PDF

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WO2022205079A1
WO2022205079A1 PCT/CN2021/084433 CN2021084433W WO2022205079A1 WO 2022205079 A1 WO2022205079 A1 WO 2022205079A1 CN 2021084433 W CN2021084433 W CN 2021084433W WO 2022205079 A1 WO2022205079 A1 WO 2022205079A1
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thermal interface
interface material
graphene
organosilicon
silicone
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French (fr)
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叶振强
曾小亮
李俊伟
张晨旭
张月星
许建斌
孙蓉
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中国科学院深圳先进技术研究院
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    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B37/00—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding
    • B32B37/12—Methods or apparatus for laminating, e.g. by curing or by ultrasonic bonding characterised by using adhesives
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B38/00—Ancillary operations in connection with laminating processes
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B7/00—Layered products characterised by the relation between layers; Layered products characterised by the relative orientation of features between layers, or by the relative values of a measurable parameter between layers, i.e. products comprising layers having different physical, chemical or physicochemical properties; Layered products characterised by the interconnection of layers
    • B32B7/04—Interconnection of layers
    • B32B7/12—Interconnection of layers using interposed adhesives or interposed materials with bonding properties
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B9/00—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B32—LAYERED PRODUCTS
    • B32B—LAYERED PRODUCTS, i.e. PRODUCTS BUILT-UP OF STRATA OF FLAT OR NON-FLAT, e.g. CELLULAR OR HONEYCOMB, FORM
    • B32B9/00—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00
    • B32B9/04—Layered products comprising a layer of a particular substance not covered by groups B32B11/00 - B32B29/00 comprising such particular substance as the main or only constituent of a layer, which is next to another layer of the same or of a different material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01L—SEMICONDUCTOR DEVICES NOT COVERED BY CLASS H10
    • H01L23/00—Details of semiconductor or other solid state devices
    • H01L23/34—Arrangements for cooling, heating, ventilating or temperature compensation ; Temperature sensing arrangements
    • H01L23/36—Selection of materials, or shaping, to facilitate cooling or heating, e.g. heatsinks
    • H01L23/373—Cooling facilitated by selection of materials for the device or materials for thermal expansion adaptation, e.g. carbon

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  • Thermal interface material is an indispensable thermal management material in the field of electronic packaging. It is used to fill the gap between the two interface contact areas and reduce the heat transfer resistance. It plays a crucial role in the performance, life and stability of electronic devices.
  • Thermal interface materials are usually composed of highly thermally conductive fillers and light and soft polymer substrates. Silicone [1] is currently one of the most widely used polymer substrates in the industry. The material is soft and stable in performance, and has been continuously recognized by the industry.
  • the traditional thermal conductive fillers are mainly ceramics (alumina, boron nitride), metals (aluminum powder, silver powder) and so on.
  • the prior art scheme adopts metal/organosilicon composite material, ceramic/organosilicon composite material and carbon-based filler/organosilicon composite material as thermal interface material.
  • Metal/organosilicon composite materials Inoue M[3] et al. studied the thermal conductivity of composite materials when silver flakes and silver particles are used as fillers. Silver flakes and silver particles are compounded in a certain proportion. When the mass fraction of silver is 85%, the in-plane thermal conductivity of the thermal interface material can reach 26W/(m ⁇ K). If the polymer is filled with silver particles randomly distributed, the thermal conductivity of the thermal interface material can reach 11W/(m ⁇ K).
  • the present invention proposes a preparation method of an organosilicon/graphene thermal interface material, and the prepared thermal interface material has a novel organosilicon/graphite film laminated structure.
  • the structure avoids direct contact between graphene and silicone, so there is no catalyst poisoning problem.
  • the schematic diagram of the laminated structure of the silicone/graphite film is shown in Figure 1.
  • Figure 1 a layer of adhesive is sprayed on both sides of the silicone pad, and the graphite film is bonded on the adhesive.
  • the silicone pad is cured Silicone, due to the poor viscosity of the silicone pad, cannot stick to the graphite film, so spray a layer of adhesive on both sides of the silicone pad.
  • step (3) the surface of one side of the silicone pad sample obtained in step (2) is coated with a layer of adhesive;
  • steps (1) to (3) are repeated to obtain an organosilicon/graphene thermal interface material with a stacked structure.
  • the preparation method of the above-mentioned organosilicon/graphene thermal interface material further comprises step (7) of grinding and polishing the obtained flake sample obtained in step (6).
  • the volume fraction of the graphite film or graphene film in the organic silicon/graphene thermal interface material of the stacked structure is 7.4% to 40%, preferably 17.2%.
  • the thickness of the silicone pad is 50-200 ⁇ m, preferably 100 ⁇ m.
  • the thickness of the adhesive is 5-20 ⁇ m, preferably 10 ⁇ m.
  • the thickness of the graphite film or graphene film is 17-40 ⁇ m, preferably 25 ⁇ m.
  • the thickness of the organic silicon/graphene thermal interface material of the stacked structure is 30 mm.
  • the binder is polybutadiene and polymethyl methacrylate, preferably polybutadiene, and the polybutadiene binder has strong viscosity and good elasticity.
  • the organic silicon is first cured into a silica gel pad, which is pressed into a film by a calendering device. Due to the poor viscosity of the silicone pad, it cannot stick to the graphite film. Polyolefin has strong viscosity and good elasticity, so spray polybutadiene adhesive on both surfaces of the silicone pad.
  • the present invention applies the graphite film to the thermal interface material of the organosilicon system, and the prepared organosilicon/graphene thermal interface composite material has good thermal conductivity, when the graphite volume fraction is 17.2vol% (graphite film thickness 25 ⁇ m, silica gel The pad thickness is 100 ⁇ m, the adhesive thickness is 10 ⁇ m), and the thermal conductivity is as high as 75.8 W/(m ⁇ K).
  • the organosilicon/graphene thermal interface composite material prepared by the present invention has good mechanical properties and certain resilience.
  • the test results show that when the maximum compressive strain is 40%, it can rebound to 20% strain in a short time, and the rebound rate is 50%.
  • the present invention belongs to a silica gel-based thermal interface material, which is one of the most widely used substrates in the field of electronic packaging at present. Therefore, the organosilicon/graphene thermal interface material provided by the present invention has good compatibility with the existing system.
  • FIG. 1 is a schematic diagram of the novel laminated structure of the present invention.
  • FIG. 2 is a flow chart of the preparation of the silicone pad/graphite film thermal interface material of the present invention.
  • FIG. 3 is a schematic diagram of a system for preparing a silica gel pad/graphite film thermal interface material according to the present invention.
  • FIG. 4 is a physical diagram of a sample of the silicone pad/graphite film thermal interface material of the present invention.
  • FIG. 5 is the detection signal output curve of the thermal interface material of the silica gel pad/graphite film of the present invention using a laser thermal conductivity meter.
  • FIG. 6 is the compression-resilience characteristic curve of the silicone pad/graphite film thermal interface material of the present invention.
  • FIG. 2 is a flow chart of the preparation of the silicone pad/graphite film thermal interface material of the present invention
  • FIG. 3 is a schematic diagram of the device of the preparation system of the silicone pad/graphite membrane thermal interface material of the present invention.
  • the specific preparation method is as follows: (1) First, a graphite film with a thickness of 25 ⁇ m and a fully cured silicone pad with a thickness of 100 ⁇ m are selected as raw materials. The incoming material is roll material with a width of 12cm. Spray the adhesive on one side of the graphite film.
  • polybutadiene is used as the binder, and the thickness of the sprayed binder is 10 ⁇ m.
  • the silicone pad is closely attached to the graphite film on the side of the adhesive sprayed by the roll-to-roll bonding device.
  • the function of the adhesive is to change the polarity of the surface of the silicone pad so that it can be closely attached to the graphite film.
  • steps (1) to (3) are repeated 206 times, and the thickness of the stack reaches 3 cm to obtain a stacked-structure organosilicon/graphene thermal interface material.
  • the in-plane dimensions of the laminate are 12cm*12cm.
  • the volume fraction of the graphite film is 17.2%.
  • step (6) Determine whether the laminate structure needs to be cured according to the type of adhesive.
  • the curing conditions of polybutadiene used in this example were placed at 120° C. for 4 hours.
  • the organic silicon/graphene thermal interface material sample of the stack structure obtained in step (5) is cut into thin slices along the thickness direction of the laminate by an ultrasonic cutting process, and the thickness of the thin slice is 0.3-3 mm.
  • the in-plane size of the sheet was cut into 3cm*3cm for experimental testing.
  • FIG. 4 is a physical diagram of a sample of a silica pad/graphite film thermal interface material prepared in this example.
  • Example 1 The organosilicon/graphene thermal interface material prepared in Example 1 was tested and characterized, and the results were as follows:
  • Sample information of silicone/graphene thermal interface material graphite film thickness 25 ⁇ m, silicone pad thickness 100 ⁇ m, and adhesive thickness 10 ⁇ m.
  • the thermal conductivity test standard is shown in Table 1 below.
  • Test method The thermal diffusivity is tested with a laser thermal conductivity meter LFA467.
  • Figure 5 shows a schematic diagram of the detection signal of the laser thermal conductivity meter. The changing law of the detection curve indicates that the test results are credible.
  • the test results of the samples of the silicone/graphene thermal interface material are shown in Table 2 below:
  • Figure 6 shows the rebound of the thermal conductive gasket prepared in Example 1 with a maximum compressive strain of 40%. The results show that the sample rebounded to 20% compressive strain in a short time, and the rebound rate was 50%.

Abstract

本发明属于热界面材料技术领域，公开了一种有机硅/石墨烯热界面材料的制备方法，所述方法包括以下步骤：(1)、将石墨膜或石墨烯膜表面一侧涂覆一层粘结剂；(2)、将硅胶垫与涂覆有粘结剂石墨膜或石墨烯膜的一侧进行贴合；(3)、将步骤(2)得到硅胶垫样品的一侧的表面涂覆一层粘结剂；(4)、再将新的石墨膜或石墨烯膜与步骤(3)得到样品进行贴合；(5)在步骤(4)获得样品的基础上，重复步骤(1)～(3)，获得堆叠结构的有机硅/石墨烯热界面材料。本发明将石墨膜应用到有机硅体系的热界面材料中，该方法制备的热界面材料，具有高导热、机械性能良好、兼容性好的优点。

Description

一种有机硅/石墨烯热界面材料的制备方法 技术领域
本发明属于热界面材料技术领域，涉及一种有机硅/石墨烯热界面材料的制备方法。
背景技术
热界面材料是电子封装领域不可或缺的热管理材料，它用于填充两个界面接触区域的空隙，降低传热阻抗，对于电子器件的性能、寿命和稳定性起着至关重要的作用。热界面材料通常由高导热填料和材质轻软的聚合物基材复合而成。有机硅[1]，是目前工业界应用最广泛的聚合物基材之一，材料柔软、性能稳定，得到业界持续认可。传统的导热填料主要为陶瓷类(氧化铝、氮化硼)、金属类(铝粉、银粉)等。随着，芯片发热量日益增大，芯片散热问题成为制约芯片发展的关键因素之一，传统的热界面材料已经不能满足需求。石墨烯具有超高的热导率，实验测量结果高达5000+W/(m·K)[2]。其次，石墨烯国产程度较高，国内相关产品性能世界领先。成熟的商业化石墨膜热导率也可达1600W/(m·K)。因此，石墨烯有望成为热界面材料领域的新贵。但是，石墨烯与有机硅相结合时，有机硅经常发生不固化的现象。一种可能的解释是：石墨烯在制备过程中，引入一些氮、磷、硫元素，这些元素导致有机硅固化所需的铂金催化剂中毒，因此难以固化。
现有技术方案采用的有金属/有机硅复合材料、陶瓷/有机硅复合材料以及碳基填料/有机硅复合材料作为热界面材料。其中，1、金属/有机硅复合材料：Inoue M[3]等研究银片、银颗粒作为填料时的复合材料导热性能。银片和银颗粒按一定比例进行复配，当银质量分数为85％时，热界面材料的面内热导率可达26W/(m·K)。如果采用银颗粒随机分布的形式进行填充聚合物，热界面材 料的热导率可达11W/(m·K)。热界面材料在应用过程中，热量通过垂直方向进行传递，因此垂直方向的热导率指标更为重要。2、陶瓷/有机硅复合材料：陶瓷颗粒有氧化铝、氮化硼、氮化铝、碳化硅、氧化锌等。通常用于电绝缘性能要求较高的领域。氧化铝最常用，成本最低，但是本征热导率较低，约30W/(m·K),氮化铝本征热导率很高，达170W/(m·K)，但是成本高。王红玉等[4]将氧化铝和氮化铝按照89:11的质量比例进行复配，制备复合材料，当填料质量分数为90％时，热导率达4.0W/(m·K)。3、碳基填料/有机硅复合材料：碳纤维是一种高导热填料，热导率可达700W/(m·K)。Uetani等[5]利用静电植绒方法，制备碳纤维基热界面材料，垂直方向热导率可达23.3W/(m·K)，填料含量13.2wt％。
现有技术中上述热界面材料存在以下缺点：1、现有的采用氧化铝作为填料的热界面材料，导热性能不足，难以适应5G时代的散热需求。而采用银、氮化铝等高导热填料的热界面材料，制备成本高昂，且并未有完全利用好自身的高导热性能，譬如银的本征热导率可达429W/(m·K)，而当银质量分数85％时，热界面材料的热导率也仅为26W/(m·K)。2、碳基填料中，性能好、技术成熟的材料主要有碳纤维，但是碳纤维成本高昂，且主要进口自日本，存在原材料被国外控制的风险。生产石墨膜的国内厂商众多，导热性能高于碳纤维，石墨膜导热性能>1600W/(m·K)，碳纤维约900W/(m·K)。但是石墨膜难以在有机硅体系的热界面材料中推广应用的主要原因是，石墨膜容易导致硅胶催化剂中毒不固化。
参考文献：
[1]苏俊杰,李苗,冯乙洪,曾幸荣,程宪涛,吴向荣.制备工艺对有机硅导热垫片性能影响分析[J].有机硅材料,2020,34(06):54-57.
[2]Tong X C(2011)Thermal Interface Materials in Electronic Packaging.In:Advanced Materials for Thermal Management of Electronic Packaging.Springer Series in Advanced Microelectronics,vol 30.Springer,New York,NY.
[3]Inoue M,Liu J.Effects of Multi-modal Filler Size Distributions on Thermal Conductivity of Electrically Conductive Adhesives Containing Ag Micro and Nanoparticles[J].Transactions of the Japan Institute of Electronics Packaging,2010,2(1):125-133.
[4]王红玉,万炜涛,陈田安.高性能有机硅导热材料的制备与研究[J].有机硅材料,2017,31(02):82-85.
[5]Uetani K,Ata S,Tomonoh S,et al.Elastomeric Thermal Interface Materials with High Through‐Plane Thermal Conductivity from Carbon Fiber Fillers Vertically Aligned by Electrostatic Flocking[J].Advanced Materials,2015,26(33):5857-5862.
发明内容
针对上述背景技术中提到的的技术问题，本发明提出一种有机硅/石墨烯热界面材料的制备方法，所制备得到的热界面材料具有新型的有机硅/石墨膜叠层结构，这种结构中避免石墨烯与有机硅进行直接接触，因此无催化剂中毒的问题。有机硅/石墨膜叠层结构示意图如图1所示，图1中，将硅胶垫两侧分别喷涂一层粘结剂，在粘结剂上粘接石墨膜，其中，硅胶垫是固化后的有机硅，由于硅胶垫粘性差，无法黏住石墨膜，所以在硅胶垫两侧各喷涂一层粘结剂。
本发明目的是提供一种有机硅/石墨烯热界面材料的制备方法，所述方法包括以下步骤：
(1)、将石墨膜或石墨烯膜表面一侧涂覆一层粘结剂；
(2)、将硅胶垫与涂覆有粘结剂石墨膜或石墨烯膜的一侧进行贴合；
(3)、将步骤(2)得到硅胶垫样品的一侧的表面涂覆一层粘结剂；
(4)、再将新的石墨膜或石墨烯膜与步骤(3)得到样品进行贴合；
(5)在步骤(4)获得样品的基础上，重复步骤(1)～(3)，获得堆叠 结构的有机硅/石墨烯热界面材料。
上述有机硅/石墨烯热界面材料的制备方法，还包括步骤(6)，将步骤(5)获得的堆叠结构的有机硅/石墨烯热界面材料样品沿着叠层厚度方向切割成薄片，薄片厚度0.3～3mm。
上述有机硅/石墨烯热界面材料的制备方法，还包括步骤(7)，将步骤(6)获得的获得的薄片样品进行打磨抛光处理。
在本发明的技术方案中，所述堆叠结构的有机硅/石墨烯热界面材料中石墨膜或石墨烯膜的体积分数为7.4％～40％，优选为17.2％。
在本发明的技术方案中，所述硅胶垫的厚度为50～200μm，优选为100μm。
在本发明的技术方案中，所述粘结剂的厚度为5～20μm，优选为10μm。
在本发明的技术方案中，所述石墨膜或石墨烯膜的厚度为17～40μm，优选为25μm。
在本发明的技术方案中，所述堆叠结构的有机硅/石墨烯热界面材料的厚度为30mm。
在本发明的技术方案中，所述切割采用超声切割或者线切割。
在本发明的技术方案中，所述粘结剂为聚丁二烯、聚甲基丙烯酸甲酯，优选为聚丁二烯，聚丁二烯粘结剂的粘性强、弹性好。
需要说明的是，本发明在硅胶与石墨膜或石墨烯膜接触之前，先将有机硅固化成为硅胶垫，经过压延设备压成薄膜。由于硅胶垫粘性差，无法黏住石墨膜。聚烯烃粘性强、弹性好，所以在硅胶垫两个表面喷涂聚丁二烯粘结剂。
本发明所构思的技术方案与现有的技术相比，具有以下有益效果：
1、本发明将石墨膜应用到有机硅体系的热界面材料中，制备得到的有机硅/石墨烯热界面复合材料的导热性能好，当石墨体积分数17.2vol％时(石墨膜厚度25μm，硅胶垫厚度100μm，粘结剂厚度10μm)，热导率高达75.8 W/(m·K)。
2.本发明制备得到的有机硅/石墨烯热界面复合材料具有良好的力学性能，具备一定的回弹能力。测试结果表明最大压缩应变为40％时，短时间可回弹至20％应变，回弹率50％。
3.本发明属于硅胶基热界面材料，是目前在电子封装领域最广泛应用的基材之一，因此本发明提供的有机硅/石墨烯热界面材料对于现有的体系具有良好的兼容性。
附图说明
图1为本发明新型叠层结构示意图。
图2为本发明硅胶垫/石墨膜热界面材料制备流程图。
图3为本发明硅胶垫/石墨膜热界面材料制备系统装置示意图。
图4为本发明硅胶垫/石墨膜热界面材料试样实物图。
图5为本发明硅胶垫/石墨膜热界面材料采用激光导热仪的检测信号输出曲线。
图6为本发明硅胶垫/石墨膜热界面材料的压缩回弹特性曲线。
具体实施方式
下面结合实施例，对本发明作进一步地详细说明，但本发明的实施方式不限于此。
下述实施例中所使用的实验方法如无特殊说明，均为常规方法；下述实施例中所用的试剂与材料等，如无特殊说明，均可从商业途径得到。
为了更好的解释本发明，以便于理解，下面结合附图，通过具体实施方式，对本发明作详细描述。
实施例1
如图2所示为本发明硅胶垫/石墨膜热界面材料制备流程图，如图3所示为本发明硅胶垫/石墨膜热界面材料制备系统装置示意图。
具体制备方法为，(1)首先，选用25μm厚度的石墨膜和100μm厚度已固化完全的硅胶垫作为原材料。来料为卷料，宽度均为12cm。在石墨膜一侧喷涂粘结剂。在本实施例中采用聚丁二烯作为粘结剂，喷涂的粘结剂的厚度为10μm。
(2)通过滚对滚贴合装置将硅胶垫和喷涂粘结剂的一面的石墨膜紧密贴合，粘结剂的作用是改变硅胶垫表面极性，使其能够与石墨膜紧密贴合。
(3)贴合之后得到的有机硅/石墨复合膜样品，在该样品的硅胶垫一侧表面再次喷涂一层粘结剂，粘结剂厚度10μm。
(4)再将新的一层石墨膜贴合到步骤(3)得到样品的带有粘结剂的一侧；
(5)以步骤四得到的样品为基础，重复(1)～(3)步骤重复206次，叠层厚度达到3cm，获得堆叠结构的有机硅/石墨烯热界面材料。叠层的面内尺寸为12cm*12cm。
在本实施例中，石墨膜的体积分数为17.2％。
(6)根据粘结剂的类型，确定是否需要固化叠层结构。本实施例所采用的聚丁二烯固化条件是120℃下放置4小时。将步骤(5)得到堆叠结构的有机硅/石墨烯热界面材料样品，用超声切割工艺切割沿着叠层厚度方向切割成薄片即为热界面材料，薄片厚度0.3～3mm。薄片的面内尺寸切割成3cm*3cm，用于实验测试。
(7)将(6)中获得的样品进行打磨抛光处理即可。图4为本实施例制备得到硅胶垫/石墨膜热界面材料试样实物图。
一、测试与表征：
将实施例1制备得到的有机硅/石墨烯热界面材料进行测试表征，结果如下：
(1)热导率测试
有机硅/石墨烯热界面材料的试样信息：石墨膜厚度25μm，硅胶垫厚度100μm，粘结剂厚度10μm。
热导率测试标准如下表1所示。
表1
Figure PCTCN2021084433-appb-000001
测试方法：热扩散系数有激光导热仪LFA467进行测试，图5给出激光导热仪的检测信号示意图。检测曲线的变化规律表明测试结果可信。有机硅/石墨烯热界面材料的试样的检测结果如下表2所示：
表2
检测项目 结果
密度ρ 2.25g/cm 3
比热容c 0.92J/(g·K)
热扩散系数α 36.6mm 2/s
热导率λ(λ＝α·c·ρ) 75.8W/(m·K)
厚度s 2.75mm
(2)力学性能测试
回弹性是导热垫片的重要性能指标要求。图6给出实施例1制备得到的导 热垫片最大压缩应变40％的回弹情况，结果显示短时间内样品回弹至20％压缩应变，回弹率50％。
上述实施例只为说明本发明的技术构思和特点，其目的在于让熟悉此项技术的人士能够了解本发明的内容并据以实施，并不能以此限制本发明的保护范围，凡根据本发明精神实质所作的等效变化或修饰，都应涵盖在本发明的保护范围之内。
上述实施例为本发明较佳的实施方式，但本发明的实施方式并不受所述实施例的限制，其他的任何未背离本发明的精神实质与原理下所作的改变、修饰、替代、组合、简化，均应为等效的置换方式，都包含在本发明的保护范围之内。

Claims (10)

  1. 一种有机硅/石墨烯热界面材料的制备方法，其特征在于，所述方法包括以下步骤：
    (1)、将石墨膜或石墨烯膜表面一侧涂覆一层粘结剂；
    (2)、将硅胶垫与涂覆有粘结剂石墨膜或石墨烯膜的一侧进行贴合；
    (3)、将步骤(2)得到硅胶垫样品的一侧的表面涂覆一层粘结剂；
    (4)、再将新的石墨膜或石墨烯膜与步骤(3)得到样品进行贴合；
    (5)在步骤(4)获得样品的基础上，重复步骤(1)～(3)，获得堆叠结构的有机硅/石墨烯热界面材料。
  2. 根据权利要求1所述的有机硅/石墨烯热界面材料的制备方法，其特征在于，还包括步骤(6)，将步骤(5)获得的堆叠结构的有机硅/石墨烯热界面材料样品沿着叠层厚度方向切割成薄片，薄片厚度0.3～3mm。
  3. 根据权利要求1所述的有机硅/石墨烯热界面材料的制备方法，其特征在于，还包括步骤(7)，将步骤(6)获得的获得的薄片样品进行打磨抛光处理。
  4. 根据权利要求1所述的有机硅/石墨烯热界面材料的制备方法，其特征在于，所述堆叠结构的有机硅/石墨烯热界面材料中石墨膜或石墨烯膜的体积分数为7.4％～40％，优选为17.2％。
  5. 根据权利要求1所述的有机硅/石墨烯热界面材料的制备方法，其特征在于，所述硅胶垫的厚度为50～200μm，优选为100μm。
  6. 根据权利要求1所述的有机硅/石墨烯热界面材料的制备方法，其特征在于，所述粘结剂的厚度为5～20μm，优选为10μm。
  7. 根据权利要求1所述的有机硅/石墨烯热界面材料的制备方法，其特征在于，所述石墨膜或石墨烯膜的厚度为17～40μm，优选为25μm。
  8. 根据权利要求1所述的有机硅/石墨烯热界面材料的制备方法，其特征 在于，所述堆叠结构的有机硅/石墨烯热界面材料的厚度为30mm。
  9. 根据权利要求1所述的有机硅/石墨烯热界面材料的制备方法，其特征在于，所述切割采用超声切割或者线切割。
  10. 根据权利要求1所述的有机硅/石墨烯热界面材料的制备方法，其特征在于，所述粘结剂为聚丁二烯、聚甲基丙烯酸甲酯，优选为聚丁二烯。
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