Cathode structural design enabling interconnected ionic/electronic transport channels for high-performance solid-state lithium batteries

Great achievements have been accomplished for high performance solid-state electrolytes, however, the poor electrode/electrolyte interfacial contact severely impedes the development of solid-state lithium batteries (SSLBs). Herein, we design a 3D structural composite cathode based on cross-linked electrospun LiNi 0.5 Co 0.2 Mn 0.3 O 2 (ES-NCM) network and ductile Li + conductive polymer electrolyte. Improved electrochemical kinetics and intimate interface are realized through infiltrating polymer precursor into ES-NCM network followed by in-situ polymerization. Assembled with Li 1.3 Al 0.3 Ti 1.7 (PO 4 ) 3 -polyvinylidene fluoride (LATP-PVDF) solid electrolyte, the composite ES-NCM || LATP-PVDF || Li battery exhibits satisfactory electrochemical performance (with an initial discharge capacity of 143.2 mAh g −1 at 0.1C and a capacity retention of 74.0% after 80 cycles) since continuous Li + /e − conduction channels are generated by ES-NCM skeleton and Li + conductive polymer. Besides, the high areal capacity of 1.19 mAh cm −2 at a high ES-NCM loading of 9.28 mg cm −2 further supports the feasibility of our composite cathode design in the application of high energy-density SSLBs. Additionally, the flexible solid-state pouch cell exhibits excellent electrochemical performance (with a discharge capacity of 131.6 mAh g −1 ) and reliable safety characteristics under mechanical abuse. This work is anticipated to provide a new perspective in overcoming solid-solid contact issues in SSLBs. • Intimate interface between ES-NCM network and solid electrolyte is constructed. • Improved electrochemical kinetics is realized by continuous Li + /e − conduction. • High NCM loading of 9.28 mg cm −2 is obtained for composite cathode. • Solid-state lithium batteries exhibit satisfactory electrochemical performances. • Solid-state pouch cell with high safety and flexibility is demonstrated.