The lithium (Li)‐metal anode offers a promising solution for high‐energy‐density lithium‐metal batteries (LMBs). However, the significant volume expansion of the Li metal during charging results in poor cycling stability as… Click to show full abstract
The lithium (Li)‐metal anode offers a promising solution for high‐energy‐density lithium‐metal batteries (LMBs). However, the significant volume expansion of the Li metal during charging results in poor cycling stability as a result of the dendritic deposition and broken solid electrolyte interphase. Herein, a facile one‐step roll‐to‐roll fabrication of a zero‐volume‐expansion Li‐metal‐composite anode (zeroVE‐Li) is proposed to realize high‐energy‐density LMBs with outstanding electrochemical and mechanical stability. The zeroVE‐Li possesses a sandwich‐like trilayer structure, which consists of an upper electron‐insulating layer and a bottom lithiophilic layer that synergistically guides the Li deposition from the bottom up, and a middle porous layer that eliminates volume expansion. This sandwich structure eliminates dendrite formation, prevents volume change during cycling, and provides outstanding flexibility to the Li‐metal anode even at a practical areal capacity over 3.0 mAh cm−2. Pairing zeroVE‐Li with a commercial NMC811 or LCO cathode, flexible LMBs that offer a record‐breaking figure of merit (FOM, 45.6), large whole‐cell energy density (375 Wh L−1, based on the volume of the anode, separator, cathode, and package), high‐capacity retention (> 99.8% per cycle), and remarkable mechanical robustness under practical conditions are demonstrated.
               
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