Rechargeable batteries are regarded as the most promising candidates for practical applications in portable electronic devices and electric vehicles. In recent decades, lithium metal batteries (LMBs) have been extensively studied due to their ultrahigh energy densities. However, short lifespan and poor safety caused by uncontrollable dendrite growth hinder their commercial applications. Besides, a clear understanding of Li nucleation and growth has not yet been obtained. In this Review, the failure mechanisms of Li metal anodes are ascribed to high reactivity of lithium, virtually infinite volume changes, and notorious dendrite growth. The principles of Li deposition nucleation and early dendrite growth are discussed and summarized. Correspondingly, four rational strategies of controlling nucleation are proposed to guide Li nucleation and growth. Finally, perspectives for understanding the Li metal deposition process and realizing safe and high-energy rechargeable LMBs are given.
Solid state lithium metal batteries are the most promising next-generation power sources owing to their high energy density and safety. Solid polymer electrolytes (SPE) have gained wide attention due to the excellent flexibility, manufacturability, lightweight, and low-cost processing. However, fatal drawbacks of the SPE such as the insufficient ionic conductivity and Li + transference number at room temperature restrict their practical application. Here vertically aligned 2D sheets are demonstrated as an advanced filler for SPE with enhanced ionic conductivity, Li + transference number, mechanical modulus, and electrochemical stability, using vermiculite nanosheets as an example. The vertically aligned vermiculite sheets (VAVS), prepared by the temperature gradient freezing, provide aligned, continuous, run-through polymer-filler interfaces after infiltrating with polyethylene oxide (PEO)-based SPE. As a result, ionic conductivity as high as 1.89 × 10 −4 S cm −1 at 25 °C is achieved with Li + transference number close to 0.5. Along with their enhanced mechanical strength, Li|Li symmetric cells using VAVS-CSPE are stable over 1300 h with a low overpotential. LiFePO 4 in all-solid-state lithium metal batteries with VAVS-CSPE could deliver a specific capacity of 167 mAh g −1 at 0.1 C at 35 °C and 82% capacity retention after 200 cycles at 0.5 C.
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