Organic sulfurization interface enabled the long‐lifespan lithium metal anode for Ah‐class pouch cells

Abstract High‐energy‐density lithium metal batteries hold great promise for advancing low‐altitude economic development. However, the practical application of ultrathin lithium anodes remains challenging due to significant interfacial side reactions, dendrite formation, and substantial volume fluctuations. In this study, lithium metal electrodes were fabricated using a spin‐coating process, enabling an in situ reaction between lithium and phenyl disulfide (PDS). The resulting robust organic sulfurization interface, composed of lithium thiophenoxide, facilitates rapid lithium‐ion transport and effectively suppresses dendrite formation. Symmetric cells with a 50 μm Li@PDS anode exhibited an impressive lifespan exceeding 3000 h at 1 mA cm −2 and 1 mAh cm −2 . The Li@PDS anode demonstrated excellent structural stability in a practical LiNi 0.8 Co 0.1 Mn 0.1 O 2 (NCM811)||Li@PDS pouch cell, maintaining 94.8% of its initial capacity (1.45 Ah) over 260 cycles at a 0.4C rate and 87.30% of its initial capacity (1.1 Ah) over 360 cycles at a 2C rate (1C = 200 mA g −1 ). This work provides a promising pathway for developing durable lithium metal anodes suitable for scalable practical applications.