Search for: All records

Abstract Practical applications of lithium metal batteries are often limited by low cycling efficiencies and uncontrolled lithium dendrite growth caused by unstable and heterogeneous lithium‐electrolyte interfaces. To address this issue, a calix[4]pyrrole‐based wavy covalent organic framework (WCOF) is developed that acts as a protective layer to suppress Li dendrite growth and reduce side reactions on the Li anode. The presentWCOFis porous and contains calix[4]pyrrole units acting as “molecular traps” that allow efficient PF₆⁻anion capture while allowing for uniform Li⁺diffusion. This provides structurally stable artificial protective layers that permit high Li⁺transference numbers. The resulting solid electrolyte interphases permit ultralong‐term stable cycling at a current density of 1 mA cm⁻²and reversible lithium plating/stripping (over 2500 h) at an areal capacity of 2 mAh cm⁻². The protected anodes of this study also demonstrated excellent cell stability through 260 cycles when paired with high‐voltage cathodes (NCM811 with high mass loading: 20 mg cm⁻²).