Prelithiation in high-energy-density lithium-ion batteries: from fundamental mechanisms to next-generation system design.

Lithium-ion batteries (LIBs) constitute the core technology for the global transition to renewable energy. The use of silicon-based anodes, with theoretical capacities an order of magnitude higher than that of graphite, has become the most promising route to break through the energy density bottleneck of commercial LIBs. Nevertheless, the improvement of their energy densities is hampered by irreversible lithium consumption during solid electrolyte interphase formation, which typically reduces the full-cell usable capacity. Prelithiation, which introduces an external lithium reservoir to compensate for these losses, is widely recognized as the most effective solution to overcome this bottleneck. Despite extensive demonstrations of lab-scale prelithiation strategies, reviews predominantly focused on the materials-level electrochemical performance and lacked a unified, verifiable framework for industrial translation, creating a pronounced disconnect between academic research and manufacturing practice. Here, in this review, we systematically deconstruct the operating principles, electrochemical performance characteristics, and intrinsic failure modes of eight representative prelithiation strategies across three categories: electrochemical, chemical, and additive-based. We establish a semi-quantitative industrial evaluation framework covering eight core dimensions to enable rigorous, head-to-head, cross-strategy comparison by building on publicly available experimental data and mainstream battery-industry engineering consensus. We further quantify the intrinsic trade-offs between the electrochemical performance and manufacturability, distill five universal design rules for next-generation prelithiation systems, and propose an application-specific decision matrix to guide strategy selection across diverse use cases. This work bridges the divide between fundamental prelithiation chemistry and scalable battery engineering, and is expected to offer actionable guidance for both academic researchers and industrial practitioners.