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Abstract Anode‐free solid‐state lithium batteries promise high‐energy‐density storage but remain limited by unstable interfaces between the solid electrolyte and in situ‐formed lithium. In this work, a hybrid solid–liquid electrolyte strategy is developed using a localized high‐concentration electrolyte containing AlCl 3 and LiPO 2 F 2 , a trilayer garnet‐type Li 6.4 Ga 0.1 La 2.9 Ba 0.1 Zr 1.6 Ta 0.4 O 12 solid electrolyte. This configuration forms a mechanically stable and ionically conductive solid‐liquid electrolyte interphase, enabling 81% Coulombic efficiency after 300 cycles at 2 mA cm −2 and 1 mAh cm −2 in Cu/Li half‐cells. A single‐layer anode‐free hybrid solid‐state pouch cell demonstrated excellent long‐term cycling performance, retaining 75% of its initial capacity after 400 cycles at 1C (1.25 mA cm −2 ), with a Coulombic efficiency of 99% without external pressure and at room temperature. At the lab scale, this hybrid electrolyte approach shows both scalability and performance, providing a potential practical pathway to next‐generation anode‐free hybrid solid‐state lithium batteries.
Sarkar et al. (Fri,) studied this question.