Metalized Plastic Current Collectors Incorporated with Halloysite Nanotubes toward Highly Safe Lithium‐Ion Batteries

Abstract Metalized plastic current collectors (MPCCs) have shown potential in improving the energy density and safety of lithium‐ion batteries (LIBs). However, the poor mechanical strength, weak interfacial adhesion force, and surface metal corrosion have impeded the practical application of MPCCs. Here, an innovative engineering of MPCCs is proposed by incorporating halloysite nanotubes (HNTs) as fillers into polyimide (PI) polymer layer, which is further coated with two thin copper (Cu) layers. Because of the strong bonding between HNTs surface and the PI precursor, HNTs improve the mechanical strength of PI‐HNTs composite film, reinforce the interfacial adhesion force between the PI‐HNTs film and the coated Cu layer, and suppress the Cu corrosion by electrolyte. The prepared MPCCs exhibit a low mass density and only account about one‐fifth of the density of commercial Cu CCs. Furthermore, the PI‐HNTs‐Cu composite demonstrates significantly enhanced interfacial adhesion force doubled to 4 N cm −1 along with prolonged stability under electrolyte immersion and electrochemical reaction conditions, and delivers a high fracture strength of 125 MPa. LIBs assembled with MPCCs deliver a twice higher discharge capacity compared to battery with Cu CCs and reach a long‐term cycle capacity retention as high as 92.9% at 0.5 C after 500 cycles.