A Low‐Strain Cathode by sp‐Carbon Induced Conversion in Multi‐Level Structure of Graphdiyne

Abstract A multi‐level architecture formed alternatively by the conformal graphdiyne (GDY) and CuS is well engineered for Li‐free cathode. Such a proof‐of‐concept architecture efficiently integrates the advantages of GDY and produces new functional heterojunctions ( sp −C−S−Cu hybridization bond). The layer‐by‐layer 2D confinement effect successfully avoids structural collapse, the selective transport inhibits the shuttling of active components, and the interfacial sp −C−S−Cu hybridization bond significantly regulates the phase conversion reaction. Such new sp −C−S−Cu hybridization of GDY greatly improves the reaction dynamics and reversibility, and the cathode delivers an energy density of 934 Wh kg −1 and an unattenuated lifespan of 3000 cycles at 1 C. Our results indicate that the GDY‐based interface strategy will greatly promote the efficient utilization of the conversion‐type cathodes.