Open-air APPJ/rubbing combined deposition of MoS₂/graphene composite/LLZTO anode bilayers for all-solid-state Li-ion batteries

An atmospheric, oven-free and vacuum-free route is used to fabricate multilayer Li-ion anodes by combining atmospheric-pressure plasma jet (APPJ) with rubbing. MoS₂, graphene, conductive carbon black (CB) and spent anode material from NCR18650 cells are deposited on Cu, then overcoated with an APPJ LLZTO garnet layer. Optical/SEM images show that APPJ combined with rubbing produces leveled, percolated coatings, and that the garnet layer gives the most continuous surface. Adhesion is quantified by ASTM D3359 cross-cut/tape and percent material loss. The composite base (~11.02 μm) scores 0B with ~65% loss. After LLZTO, thickness rises to 40.53 μm, adhesion to 2B, and loss falls to ~15% at <100 °C. The garnet layer thus acts as a solid electrolyte and mechanical reinforcement, yielding an ASSB-ready composite/LLZTO anode bilayer for LiFePO₄ cells and linking circular-economy anode feedstocks to all-solid-state Li-ion architectures. • Open-air APPJ/rubbing route for MoS₂/graphene composite anode bilayers. • Composite/Ta-LLZTO bilayer acts as ASSB-ready anode-side module. • APPJ Ta-LLZTO top-coat improves cross-cut adhesion from 0B to 2B. • Material loss under tape test drops from ~65% to ~15% at <100 °C. • Defines adhesion–thickness–loss triad as a manufacturability descriptor.