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High Thermal Conductivity Diamond–Copper Composites Prepared via Hot Pressing with Tungsten–Coated Interfacial Layer Optimization

MetadataDetails
Publication Date2025-08-19
JournalMaterials
AuthorsQiang Wang, Zhijie Ye, Lei Liu, Jie Bai, Yuning Zhao
InstitutionsJi Hua Laboratory, Harbin Institute of Technology
Citations1
AnalysisFull AI Review Included
  • Peak Thermal Conductivity (TC): The fabricated diamond-copper composite achieved 640 W/(mK) at 50 vol% diamond content, representing the highest reported TC for hot-press sintered (HPS) composites with diamond content not exceeding 50%.
  • Interface Engineering: Tungsten (W) was deposited via magnetron sputtering and subsequently annealed at 1100 °C for 2 hours to form a carbide transition layer (W2C and WC).
  • Optimal Composition: The highest TC was achieved when the interfacial layer consisted of 2 wt.% W, 92 wt.% WC, and 6 wt.% W2C.
  • Microstructural Improvement: Annealing for 2 hours minimized the formation of low-conductivity amorphous carbon (a-C) regions and promoted a dense, ordered crystalline carbide structure, significantly reducing interfacial thermal resistance.
  • Interfacial Thermal Conductance (ITC): The optimal 2-hour annealed sample exhibited a peak ITC between 36 and 56 MW/(m2K), a substantial increase from the initial 9 MW/(m2K) (0h annealing).
  • Theoretical Validation: Acoustic Mismatch Model (AMM) and Diffusion Mismatch Model (DMM) calculations identified the optimal theoretical interface structure for phonon regulation as Diamond/W2C/WC/W2C/Cu.
  • Fabrication Method: Hot-press sintering (HPS) was confirmed as an effective method for producing high-performance composites, offering advantages in process control and uniformity over other methods like SPS or GPI.
ParameterValueUnitContext
Peak Thermal Conductivity (TC)640W/(mK)50 vol% diamond, 2h annealing
Diamond Volume Fraction50vol%Optimized content for peak TC
Diamond Particle Size400µmSubstrate material (HHD-90)
W Coating Thickness200nmDeposited via magnetron sputtering
Annealing Temperature1100°CVacuum tube furnace
Annealing Time (Optimal)2hYielded peak TC
Annealing Vacuum Pressure5 x 10-4PaMaintained during heat treatment
Peak Interfacial TC (H-J Model)56MW/(m2K)Calculated for 2h annealed composite
Lowest Interfacial TC (a-C/Diamond)2.59MW/(m2K)Calculated via AMM
W2C/WC Interfacial TC11,400MW/(m2K)Calculated via AMM (highest internal carbide ITC)
Diamond Intrinsic TC (Calculated)1717W/(mK)Based on 147 ppm Nitrogen content
Optimal Interface Composition92% WC, 6% W2C, 2% Wwt.%Composition after 2h annealing
HPS Composite Diameter30mmInitial HPS sample size
  1. Diamond Cleaning and Preparation:

    • Single-crystal diamond particles (400 µm) were sequentially cleaned using nitric acid, sodium hydroxide, acetone, and anhydrous ethanol.
    • Ultrasonic cleaning was applied to remove surface impurities before drying.
  2. Tungsten (W) Coating Deposition:

    • W coating (200 nm average thickness) was deposited onto the diamond particles using pulsed magnetron sputtering in an Argon atmosphere.
    • Particles were placed on a tilted rotating plate to ensure uniform coverage.
  3. Vacuum Annealing (Carbide Formation):

    • Coated particles were annealed at 1100 °C for varying durations (0 to 6 h) in a tube furnace.
    • A high vacuum (5 x 10-4 Pa) was maintained to prevent oxidation.
    • Annealing promoted the conversion of W into W2C and WC, with 2 hours yielding the optimal carbide ratio (92% WC, 6% W2C).
  4. Copper Plating:

    • Annealed diamond particles were activated and sensitized.
    • A copper layer was chemically deposited onto the metallized diamond surfaces using a rotary evaporator.
  5. Hot-Press Sintering (HPS):

    • The coated diamond powder was consolidated using HPS to form a dense composite material (50 vol% diamond).
    • The resulting composite was 30 mm in diameter and 1.5 mm thick, subsequently cut into 12.7 mm discs for characterization.
  6. Characterization and Modeling:

    • XRD, SEM, and Raman spectroscopy were used for phase identification and morphology analysis.
    • Thermal diffusivity was measured using the LFA467 HyperFlash method.
    • Thermal conductivity was calculated from density, specific heat, and diffusivity.
    • Interfacial thermal conductance was theoretically analyzed using the Acoustic Mismatch Model (AMM) and the Diffusion Mismatch Model (DMM).

The high thermal conductivity and robust interface bonding achieved by these diamond-copper composites make them ideal for demanding thermal management roles in high-tech sectors:

  • High-Power Electronic Devices: Used as heat sinks and spreaders for high-density components where traditional materials are inadequate.
  • Aerospace and Defense: Applications requiring lightweight materials with exceptional thermal stability and dissipation capabilities.
  • Mobile Chip Manufacturing: Thermal management solutions for high-integration, high-power density mobile processors and chips.
  • Thermal Management Systems: General use in cooling systems where efficient heat transfer is critical (e.g., high-frequency communications, radar).
  • Thermoelectric Conversion: Potential application in systems requiring efficient heat flow regulation.
View Original Abstract

Diamond-copper composites, due to their exceptional thermal conductivity, hold significant potential in the field of electronic device thermal management. Hot-press sintering is a promising fabrication technique with industrial application prospects; however, the thermal conductivity of composites prepared by this method has yet to reach optimal levels. In this study, tungsten was deposited on the surface of diamond particles by magnetron sputtering as an interfacial transition layer, and hot-press sintering was employed to fabricate the composites. The findings reveal that with prolonged annealing time, tungsten gradually transformed into W2C and WC, significantly enhancing interfacial bonding strength. When the diamond volume content was 50% and the interfacial coating consisted of 2 wt.% W, 92 wt.% WC, and 6 wt.% W2C, the composite exhibited a thermal conductivity of 640 W/(m·K), the highest value reported among hot-press sintered composites with diamond content below 50%. Additionally, the AMM (Acoustic Mismatch Model) and DMM (Diffusion Mismatch Model) models were utilized to calculate the interfacial thermal conductance between different phases, identifying the optimal interfacial structure as diamond/W2C/WC/W2C/Cu. This composite material shows potential for application in high-power electronic device cooling, thermal management systems, and thermoelectric conversion, providing a more efficient thermal dissipation solution for related devices.

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