Active prelithiation strategies for advanced lithium storage systems: A perspective from electrochemical mechanism to structural design and application

Given the rising demand for high-energy–density devices in the commercial market, exploring new electrode materials is crucial for enhancing the energy density of lithium-ion batteries (LIBs). Novel electrode materials, which rely on conversion and alloy reactions, have attracted attention due to their high specific capacity and abundant resources. However, these materials often suffer from a large initial irreversible capacity and low- capacity retention, leading to significant active lithium consumption and a reduction in overall battery energy density. Consequently, a concise and efficient prelithiation technique is urgently needed to improve their electrochemical performance for commercial applications. Although various prelithiation methods have been developed, they predominantly remain experimental due to issues such as high reduction potential, poor prelithiation accuracy, and incompatibility with electrolytes, among others. From an industrial perspective, understanding the electrochemical reaction mechanisms and designing effective prelithiation technologies and electrode structures are vital for advanced lithium storage systems. This review first discusses the causes of active lithium loss and the electrochemical reaction mechanisms of different prelithiation methods. It summarizes the applications of advanced characterization methods in prelithiation technology. Then, various prelithiation strategies are reviewed and generalized according to the different components of LIBs. Additionally, the review examines the pathways for lithium replenishment and the recent developments in electrode structures within prelithiation strategies. Finally, the future perspectives and challenges of prelithiation technology in commercial applications are analyzed and projected.