Advancing Metallic Lithium Anodes: A Review of Interface Design, Electrolyte Innovation, and Performance Enhancement Strategies

Lithium (Li) metal is one of the most promising anode materials for next-generation, high-energy, Li-based batteries due to its exceptionally high specific capacity and low reduction potential. Nonetheless, intrinsic challenges such as detrimental interfacial reactions, significant volume expansion, and dendritic growth present considerable obstacles to its practical application. This review comprehensively summarizes various recent strategies for the modification and protection of metallic lithium anodes, offering insight into the latest advancements in electrode enhancement, electrolyte innovation, and interfacial design, as well as theoretical simulations related to the above. One notable trend is the optimization of electrolytes to suppress dendrite formation and enhance the stability of the electrode-electrolyte interface. This has been achieved through the development of new electrolytes with higher ionic conductivity and better compatibility with Li metal. Furthermore, significant progress has been made in the design and synthesis of novel Li metal composite anodes. These composite anodes, incorporating various additives such as polymers, ceramic particles, and carbon nanotubes, exhibit improved cycling stability and safety compared to pure Li metal. Research has used simulation computing, machine learning, and other methods to achieve electrochemical mechanics modeling and multi-field simulation in order to analyze and predict non-uniform lithium deposition processes and control factors. In-depth investigations into the electrochemical reactions, interfacial chemistry, and physical properties of these electrodes have provided valuable insights into their design and optimization. It systematically encapsulates the state-of-the-art developments in anode protection and delineates prospective trajectories for the technology's industrial evolution. This review aims to provide a detailed overview of the latest strategies for enhancing metallic lithium anodes in lithium-ion batteries, addressing the primary challenges and suggesting future directions for industrial advancement.