Direct joining molding of metals and polymers has received increasing attention in the field of lightweight fabrication. The aluminum alloy (Al) surface was modified by secondary anodizing and a special needle-like structure was formed on the Al surface. Then, the glass fiber-filling polyphenylene sulfide (PPS) was directly joined with Al by the hot pressing technique. The relationship between the interfacial structure and mechanical properties of Al/PPS hybrids was systematically investigated and discussed. The results showed that the generation of needle-like structures could improve the surface roughness and wettability, thus effectively improving the mechanical interlocking ability of the interface and forming the Al-O-C chemical bond with PPS. The maximum tensile strength of Al/PPS hybrids was 28.34 MPa, and their impact toughness (ak) reached 9.69 J/cm2. Even though the hybrids were exposed to a salt spray environment or 200 °C, the strength could still reach 25 MPa. This study has prepared a high-performance metal/plastic hybrid by secondary anodizing method, which can be applied in harsh environments.
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