Engineering the future of silicon-based all-solid-state lithium-ion batteries: Current barriers and innovative solutions

Abstract

As a leading contender for advanced energy storage systems, silicon-based all-solid-state lithium-ion batteries (Si-ASSLIBs) have garnered critical research frontier due to their demonstrated capacity to offer enhanced energy density and superior thermal stability and safety compared to conventional lithium-ion batteries. However, Si-ASSLIBs still faces challenges in practical applications, such as cell failure due to the significant volume expansion of silicon. Innovatively, we highlight that pressure plays two critical roles in Si-ASSLIBs. Herein, we systematically review the recent advances and challenges in Si-ASSLIBs, with a particular emphasis on their industrialization pathways. The research progress of Si-ASSLIBs is comprehensively summarized, and different silicon anodes and their electrochemical performance optimization strategies are presented. Next, we systematically summarize the mechanical properties, simulation, and morphological/structural characterization approaches pertaining to volume expansion in Si-ASSLIBs. Crucially, we propose that fabrication pressure pre-stabilizes electrode interfaces, while operational pressure dynamically regulates stress evolution. In order to promote the scaled-up industrial production of Si-ASSLIBs, we summarize the current state of research on the pre-lithiation process and present our views for industrialization. As a core enabler, pre-lithiation technology is rigorously evaluated via scalable production pathways, establishing design standards and an industrial roadmap. Finally, the challenges and opportunities for achieving high energy density Si-ASSLIBs and future developments are outlined. This review outlooks the challenges, opportunities, and future directions for advanced Si-ASSLIBs.