This study explores the fabrication of composites involving polyimide (PI) and polyether ether ketone (PEEK) resins with Cu using chemical treatment and sandblasting, followed by plasma cleaning in a vacuum environment charged with Ar. To enhance the bonding strength of Cu to PI and PEEK, vacuum magnetron sputtering was used to deposit an intermediate transition layer of titanium and a plated seed layer of Cu onto the resin. For PI/copper composites, the copper layer’s highest bonding strength was achieved through sandblasting and plasma cleaning for 150 s at a bias voltage of 100 V. For PEEK/Cu composites, the optimal bonding strength of the copper layer was observed after 80 s of plasma cleaning. Surface roughness is important in the bonding strength of the copper layer. Additionally, the Ti transition layer strengthens bonding forces between Cu and both PI and PEEK. X-ray photoelectron spectroscopy revealed Ti–O bond formation with oxygen in the resins and Ti–C bonds within the carbon, indicating chemical interactions that bolstered Cu adhesion to resins. Adjusting the bias voltage had varying effects on the bonding strength of resin/Cu. For PI/Cu, the bonding force decreased with increasing bias voltage (20–150 V) owing to excessive bias voltage causing surface defects on the plated Cu layer, which reduced the density of the plated Cu layer. Conversely, the PEEK/Cu bonding force initially increased with increasing bias voltage due to enhanced surface bombardment. Beyond an optimal point, the bonding force in PEEK/Cu decreased due to unfavorable effects on layer density.
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