Primary lithium (Li) metal batteries are widely used but are typically discarded after single-use operation, resulting in a dispersed and underutilized Li-containing waste stream. Here, we report an integrated electrochemical–chemical pathway for Li recovery from spent primary Li metal batteries. Residual Li is first reactivated through controlled electrochemical rejuvenation, inducing Li redeposition onto the anode-side casing. The regenerated Li is then selectively extracted and stabilized at the molecular level using a polycyclic aromatic hydrocarbon (PAH)–ether solution, followed by antisolvent-induced precipitation and moderate thermal conversion to lithium carbonate (Li2CO3). The effects of processing parameters, including drying atmosphere and calcination temperature, on phase evolution and Li content are systematically examined. The recovered Li2CO3 exhibits high crystallinity and Li purity, as further validated by the synthesis and electrochemical evaluation of lithium cobalt oxide (LiCoO2) cathodes. The resulting cathode materials demonstrate crystallographic integrity and electrochemical performance comparable to those derived from commercial Li sources. By coupling electrochemical control, solution-phase Li leaching, and materials regeneration, this work establishes a process-oriented framework for valorizing Li from primary battery waste and demonstrates a closed-loop Li utilization pathway that bridges recovery and functional material regeneration, highlighting an underexplored opportunity for sustainable Li resource recovery.
Silicon monoxide (SiOx) is a promising anode material for lithium-ion batteries owing to its high theoretical capacity, yet its application is limited by low initial Coulombic efficiency (ICE) caused by irreversible lithium consumption. Prelithiation is an effective strategy to address this issue, although the influence of binder chemistry during prelithiation has not been systematically clarified. In this work, the effects of binder formulation and prelithiation strategy on SiOx anodes are investigated by comparing five binder systems under direct-contact prelithiation (DCP) and chemical prelithiation (CP). Electrochemical results show that binder engineering strongly impacts lithiation efficiency, reversible capacity, and cycling stability. Among all systems, electrodes employing the PAA+SBR binder consistently deliver the best performance, achieving high ICE (>95%), high reversible capacity (up to ~1900 mAh g−1), and stable capacity retention over extended cycling under both DCP and CP. Morphological and interfacial analyses reveal that PAA+SBR effectively suppresses electrode cracking, limits thickness expansion, and maintains low interfacial impedance. X-ray photoelectron spectroscopy further indicates that PAA+SBR forms a relatively thinner, inorganic-rich interphase dominated by Li2CO3 and Li2O, in contrast to the organic and silicate-rich interphase observed for PAA+CMC. These findings demonstrate that binder engineering plays a critical role in enabling high-performance prelithiated SiOx anodes.
