(WC–6wt%Co)/5Vol% diamond composites were successfully fabricated at 1150–1300 °C and 40 MPa for 5 minutes under the thermodynamically unstable conditions of the Spark Plasma Sintering method. The influence of on-off time, and frequency of the DC pulse of SPS on diamond stability, microstructure, and mechanical properties of WC–Co/diamond composites were investigated. The diamond particles are strongly bounded with the cemented carbide matrix by a transition layer composed of a solid solution of tungsten and carbon in cobalt. The amount of graphitization was low in the sintered composites at 1300 °C due to the low temperature and short sintering time. Reduction of SPS frequency effectively inhibited graphite preformation, and no graphite was detected in the sintered composites at 1150 °C. Diamond morphology was not affected during SPS as examined by SEM, and Raman scattering spectra. The uniform dispersion of the super-hard diamond phase in matrix which good bonded, caused the high hardness, fracture toughness and flexural strength of this composite. The reduction of pulse frequency of SPS leads to a significant enhancement in the hardness, fracture toughness, and flexural strength of the composites, overcoming the graphitization of diamond typically observed in SPS. The sample sintered with 4 Hz showed simultaneously the highest hardness (23.6 GPa), the highest fracture toughness (24.6 MPa.m½), and the highest flexural strength (2050 MPa).
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