XUE Zhenghang, ZHANG Shouyang, ZHANG Ruoqian, et al. Preparation and Properties of High Emissivity Coatings on the Surface of High Thermal Conductivity Cabon/carbon Composites[J]. Acta Materiae Compositae Sinica, 2025, 42(6): 3366-3376.
Citation: XUE Zhenghang, ZHANG Shouyang, ZHANG Ruoqian, et al. Preparation and Properties of High Emissivity Coatings on the Surface of High Thermal Conductivity Cabon/carbon Composites[J]. Acta Materiae Compositae Sinica, 2025, 42(6): 3366-3376.

Preparation and Properties of High Emissivity Coatings on the Surface of High Thermal Conductivity Cabon/carbon Composites

Funds: Key project of National Natural Science Foundation of China(U21 B2067)
More Information
  • Received Date: June 19, 2024
  • Revised Date: August 15, 2024
  • Accepted Date: August 15, 2024
  • Available Online: September 05, 2024
  • The infrared emissivity of high thermal conductivity carbon/carbon (HTC-C/C) composite surface is low, resulting in poor radiative heat dissipation ability. In order to further improve its thermal control ability, it is necessary to coat its surface with high emissivity coating. Carbon nanotube (CNTs)/carbon black (CB) composite coating with high infrared radiation and thermal shock resistance was prepared on the surface of HTC-C/C composite material by compressed air spraying method. After a certain amount of pyrogenic carbon (PyC) was deposited, the coating obtained stronger interface bonding performance while maintaining high infrared emissivity. The effects of thermal shock and high temperature heat treatment on the microstructure and properties of high emissivity coatings were investigated. The results showed that When the mass ratio of CNTs to CB reached the optimal ratio, the emissivity of the prepared coating reached more than 0.94, and no cracking and spalling occurred after 60 thermal shock resistance tests at 300℃↔−196℃, indicating good thermal stability. After heat treatment, the microstructure order of the nano-carbon materials in the coating changes, resulting in wavelength dependence of the coating emissivity. However, due to the synergistic effect of each band, the emissivity of the whole test band (1-22 μm) fluctuates little.

  • Objectives 

    The surface of high thermal conductivity carbon/carbon (HTC-C/C) composite has low infrared emissivity, resulting in poor radiative heat dissipation ability. In order to further improve its thermal control ability, it is necessary to coat its surface with high emissivity coating. In this paper, a coating with high emissivity and strong binding force was prepared on the surface of HTC-C/C composite by using compressed air spraying method.

    Methods 

    First, sodium dodecyl benzene sulfonate (SDBS) was added into isopropyl alcohol (IPA) and mixed evenly to obtain isopropyl alcohol dispersion solution. Then carbon nanotubes (CNTs) and carbon black nanoparticles (CB) were added into IPA dispersion solution successively for 30 min, and then phenolic resin (PF) was added to achieve uniform ultrasonic dispersion. The HTC-C/C sample was preheated on the 85℃ heating plate for five minutes, and the above fully dispersed paint was sprayed on the surface of the HTC-C/C composite material with an air compressor to obtain a porous and high-emissivity coating. Chemical vapor deposition (CVD) was used to deposit pyrolytic carbon in the surface pores of the coating to improve the binding force, and finally the coating with high microporous emissivity and strong binding force was obtained. The coatings prepared with different proportions of CB and CNTs were successively named CNTs/ CB-PYC-1, CNTs/ CB-PYC-2, CNTs/ CB-PYC-3 and CNTs/ CB-PYC-4, and the changes in the emissivity and binding force of the coatings at different proportions were studied. The effects of thermal shock and high temperature heat treatment on the microstructure and properties of high emissivity coatings were investigated.

    Results 

    (1) Affected by rough surfaces of different scales, the uniform mesh jagged undulation structure formed by CNTs and CB can effectively improve the emissivity. With the increase of roughness, the emissivity also increases gradually. CNTs/CB coatings with different morphology and structures were prepared by a simple spraying process. When the proportion of CB is too large, the pores of the coating are small, resulting in the sealing phenomenon during the deposition of pyrolytic carbon (PyC), which is not conducive to the deposition of PyC inside the coating, and the binding force between the coating and the substrate is poor. When the proportion of CNTs is too large, the specific surface area of the coating surface is reduced, and the surface reflection site is reduced, resulting in a decrease in emissivity. When the mass fraction of CNTs and CB reached the optimal ratio, the emissivity reached more than 0.97, which increased by more than 40% compared with the non-sprayed high thermal conductivity carbon/carbon (HTC-C/C) matrix. (2) After the deposition of PyC, CNTs and CB were covered with a considerable amount of PyC and bonded to each other. The CNTs mesh structure with stronger connection was formed in the composite coating, which made the coating have better bonding force. When the deposition time of PyC was 15 min, the bonding force measured by nanoscratch method was above 25 N. After 60 thermal cycles at 300℃↔-196℃, CNTs/CB-PyC composite coating can maintain no cracking while the emissivity is above 0.94, and has good thermal shock resistance. (3) Under the argon atmosphere, after heat treatment above 1500℃, the microscopic order degree of the nano-carbon materials in the coating changes, resulting in a wavelength dependence of the coating emissivity, the emissivity in the short wavelength range increases, and the emissivity in the long wavelength range decreases. However, due to the synergistic effect of various bands, The emissivity of the whole test band (1-22 μm) has little fluctuation.Conclusion: Based on the principle of matching thermal and physical properties, a method of preparing carbon coating on the surface of HTC-C/C composite was developed. Using low cost industrial carbon black and multi-wall carbon nanotubes as the main raw materials of the coating, the high infrared emissivity coating can be prepared on a large scale and at low cost by using air spraying method. The process is simple and the cost is low. The coating has strong binding force and good thermal stability while ensuring high emissivity. The nano-carbon material in the coating has a small emissivity fluctuation in the whole test band (1-22 μm) after heat treatment, which can be well applied in the high temperature oxygen free environment in space.

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