Luo Chao, Hu Hong, Zhang Tian, Wen Shujing, Wang Ruo, An Yanan, Chi Shang-Sen, Wang Jun, Wang Chaoyang, Chang Jian, Zheng Zijian, Deng Yonghong
Department of Materials Science and Engineering, Academy for Advanced Interdisciplinary Studies, Shenzhen Key Laboratory of Solid-State Batteries, Southern University of Science and Technology, Shenzhen, 518055, China.
Institute of Textiles and Clothing, The Hong Kong Polytechnic University, Kowloon, Hong Kong SAR, China.
Adv Mater. 2022 Sep;34(38):e2205677. doi: 10.1002/adma.202205677. Epub 2022 Aug 22.
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 . Pairing zeroVE-Li with a commercial NMC or LCO cathode, flexible LMBs that offer a record-breaking figure of merit (FOM, 45.6), large whole-cell energy density (375 Wh L , 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.
锂金属阳极是高能量密度锂金属电池（LMB）的一个很有前景的解决方案。然而，充电过程中锂金属的显著体积膨胀会导致枝晶沉积和固态电解质界面破裂，从而造成较差的循环稳定性。在此，我们提出一种简便的一步卷对卷制造方法，制备零体积膨胀锂金属复合阳极（zeroVE-Li），以实现具有出色电化学和机械稳定性的高能量密度LMB。zeroVE-Li具有类似三明治的三层结构，由上层电子绝缘层和下层亲锂层组成，二者协同作用引导锂从底部向上沉积，中间层为多孔层，可消除体积膨胀。这种三明治结构消除了枝晶形成，防止了循环过程中的体积变化，即使在实际面积容量超过3.0 mAh cm时，也为锂金属阳极提供了出色的柔韧性。将zeroVE-Li与商用NMC或LCO阴极配对，展示了具有创纪录品质因数（FOM，45.6）、高全电池能量密度（基于阳极、隔膜、阴极和封装的体积，为375 Wh L）、高容量保持率（每循环>99.8%）以及在实际条件下显著机械稳健性的柔性LMB。
