The microstructure and residual stress of polycrystalline diamond compact (PDC) play crucial roles in the performance of PDCs. Currently, in-depth research is still to be desired on the evolution mechanisms of microstructure and residual stress during high pressure high temperature (HPHT) synthesis process of PDCs. This study systematically investigated the influencing mechanisms of polycrystalline diamond (PCD) layer material design, especially the Co content of the PCD layer, on microstructure and residual stress evolution in PDCs via Raman spectroscopy and finite element micromechanical simulation. The research shows that when the original Co content of the PCD layer is higher than 15 wt.%, the extra Co in the PCD layer will migrate backwards towards the carbide substrate and form Co-enrichment regions at the PCD–carbide substrate interface. As the original Co content of the PCD layer increases from 13 to 20 wt.%, the residual compressive stress of diamond phase at the upper surface center of the PCD layer gradually decreases and transforms into tensile stress. When the original Co content of the PCD layer is as high as 30 wt.%, the residual stress transforms back into significant compressive stress again. The microstructure-based micromechanical simulation at the PCD–carbide substrate interface shows that the Co-enrichment region is the key for the transformation of the residual stress of the diamond phase from tensile stress into significant compressive stress.
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