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CN-117566730-B - High-elasticity low-thermal-resistance graphene thermal interface material and preparation method thereof

CN117566730BCN 117566730 BCN117566730 BCN 117566730BCN-117566730-B

Abstract

The invention provides a graphene thermal interface material with high elasticity and low thermal resistance and a preparation method thereof, which are mainly characterized by high elasticity, low thermal resistance and extremely wide working temperature range, and are suitable for thermal management of 3C products, high-power electronic chips, new energy automobiles and extremely high and low temperature environments. The graphene aerogel film subjected to graphitization treatment is selected as a high heat conduction framework, graphene which is subjected to high-temperature annealing treatment but is not completely graphitized is in situ compounded in the graphene aerogel film to serve as an elastic component, and a micro buckling structure is introduced to further promote heat conduction of a vertical plane, so that the flexible graphene thermal interface material with high elasticity and low thermal resistance is prepared. The elastic thermal interface material is composed of graphene treated at different temperatures and different structures, can be used at a temperature range of-200 ℃ to 1000 ℃, is more resistant to chemical corrosion compared with a metal-based thermal interface material, and simultaneously solves the problem that the traditional graphene aerogel is difficult to achieve both high heat conduction and high elasticity.

Inventors

  • CAI SHENGYING
  • ZHAO WENBO
  • ZHAO BO
  • GAO CHAO

Assignees

  • 浙江大学绍兴研究院
  • 山西浙大新材料与化工研究院

Dates

Publication Date
20260505
Application Date
20230831

Claims (8)

  1. 1. The high-elasticity low-thermal-resistance graphene thermal interface material is characterized by having a density of 32-139 mg cm -3 and at least comprising a heat conducting framework and an elastic component filled in the heat conducting framework, wherein the heat conducting framework is a graphene aerogel film subjected to graphitization treatment, the density is 23-87 mg cm -3 , and the elastic component is graphene subjected to 1000-2000 ℃ annealing treatment.
  2. 2. The thermal interface material of claim 1, wherein the graphitizing treatment of the thermally conductive skeleton is performed at 2300-3150 ℃ for 1h.
  3. 3. The thermal interface material of claim 1, wherein the rebound rate is 50 to 99% when the compression rate is no more than 98%.
  4. 4. The thermal interface material of claim 1, wherein the vertical plane thermal conductivity ranges from 8 to 20 wtm -1 K -1 and the thermal impedance ranges from 0.02 to 2k cm 2 W -1 when a pressure of 10 to 1200kpa is applied.
  5. 5. The preparation method of the high-elasticity low-thermal-resistance graphene thermal interface material is characterized by comprising the following steps of: (1) The graphene oxide solution is coated to form a film, dried and then placed in hydrazine hydrate solution with the volume fraction of 5-85% to be foamed for 15-300 min, and graphitized treatment is carried out on the foamed graphene aerogel film, wherein the foaming temperature is 20-90 ℃; (2) And immersing the graphitized graphene aerogel film into a graphene oxide solution with the concentration of 0.2-5 mg -1 , carrying out vacuum infusion for 1-2 h, drying in an environment of 40-60 ℃, and then carrying out high-temperature annealing for 1-3 h at the annealing temperature of 1000-2000 ℃ to obtain the high-elasticity low-thermal-resistance graphene thermal interface material.
  6. 6. The preparation method of the high-elasticity low-thermal-resistance graphene thermal interface material is characterized by comprising the following steps of: (1) Spreading graphene oxide solution into a film, drying, placing the film in hydrazine hydrate solution with the volume fraction of 5-85% for foaming for 15-300 min, and carrying out graphitization treatment on the foamed graphene aerogel film, wherein the foaming temperature is 20-90 ℃; (2) Immersing the graphitized graphene aerogel film into a graphene oxide solution with the concentration of -1 g of 0.2-5 mg for 1-2 h, immersing in a hydrazine hydrate solution for 1-5 h to introduce a micro buckling structure on the surface of the graphene oxide sheet, replacing the hydrazine hydrate solution with ethanol, drying in an environment of 40-60 ℃, and carrying out high-temperature annealing treatment for 1-3 h at the annealing temperature of 1000-2000 ℃.
  7. 7. The method of claim 6, wherein the volume fraction of the hydrazine hydrate solution is 60-85%.
  8. 8. The method of claim 5 or 6, wherein the graphene oxide in the graphene oxide solution is a monolayer or multilayer.

Description

High-elasticity low-thermal-resistance graphene thermal interface material and preparation method thereof Technical Field The invention belongs to the technical field of thermal management materials, and particularly relates to a high-elasticity low-thermal-resistance graphene thermal interface material and a preparation method thereof. Background With the rapid development of information technology and the high miniaturization and integration of electronic components, the problem of heat dissipation is becoming a bottleneck for limiting the development of various fields. Local heating caused by heat unable to be transferred in time can lead to chip down-conversion, increased battery side reactions and reduced life/reliability of electronic products. The thermal interface material is a flexible material with high thermal conductivity and low modulus, and the thermal interface material is filled between the heat generating element and the radiating fin to improve the interface environment between the heat generating element and the radiating fin and enhance heat transfer. The development of the high-performance thermal interface material is important to promote the rapid development of technologies such as smart phones, new energy automobiles, 5G and the like, and has extremely high market value. The traditional thermal interface material is mainly formed by compounding an elastic polymer matrix with a metal filler, an inorganic filler or a carbon material, has relatively low thermal conductivity (5-10W -1K-1), is narrow in applicable temperature range (-40-200 ℃), and is difficult to meet the heat dissipation requirements of a high-power chip, a high-energy-density battery cell and an extremely high-low temperature environment. Although graphene is used for preparing high-performance thermal interface materials at present, the graphene is mainly used as a heat conducting filler, and few thermal interface materials completely composed of graphene cannot combine heat conduction and physical and mechanical properties. Whether to prepare a pure graphene thermal interface material with high elasticity and low thermal resistance, strengthen heat conduction and physical and mechanical properties, widen the working temperature range, and provide a new solution for the thermal management problem is a problem and a huge challenge to be solved urgently. Disclosure of Invention The invention aims to provide a high-elasticity low-thermal-resistance graphene thermal interface material, which at least comprises a high-low-temperature-resistant high-elasticity low-thermal-resistance thermal interface material which is formed by taking a graphitized graphene aerogel film as a high-heat-conductivity framework and taking high-temperature annealed but incompletely graphitized graphene as an elastic component. The elastic graphene component is filled in the high-heat-conductivity graphene foam film, so that the problem that the heat conduction and elasticity of the single graphene aerogel are difficult to be combined can be effectively solved, and the preparation of the low-thermal-resistance high-elasticity graphene thermal interface material is realized. The high-elasticity low-thermal-resistance graphene thermal interface material at least comprises a graphene aerogel film subjected to graphitization treatment as a high-thermal-conductivity skeleton, wherein the density is 23-87 mg cm -3, high-temperature annealed graphene which is not completely graphitized is used as an elastic component, and the elastic component is filled on the inner surface of the high-thermal-conductivity skeleton in a non-close stacking mode, so that the density of the whole material is 32-139 mg cm -3, and the high-low temperature-resistant high-elasticity low-thermal-resistance thermal interface material is formed. In some embodiments of the present invention, the high thermal conductivity skeleton mainly refers to a graphene aerogel film subjected to graphitization treatment at 2300-3150 ℃, and the graphitization treatment time is generally 1h. The invention also provides a preparation method of the graphene thermal interface material with high elasticity and low thermal resistance, which comprises the following steps: (1) And (3) carrying out knife coating on the graphene oxide solution to form a film, drying, then placing the film in a hydrazine hydrate solution with the concentration of 5-85% to foam for 15-300 min, and carrying out graphitization treatment on the foamed graphene aerogel film. Wherein the foaming temperature is 20-90 ℃. (2) And immersing the graphitized graphene aerogel film into a graphene oxide solution with the concentration of 0.2-5 mg -1, carrying out vacuum infusion for 1-2 h, drying in a 40-60 ℃ environment, and then carrying out high-temperature annealing treatment for 1-3 h at the annealing temperature of 1000-2000 ℃ to obtain the high-elasticity low-thermal-resistance graphene thermal interface material. The invention