CAS Key Laboratory of Molecular Nanostructure and Nanotechnology, Beijing National Laboratory for Molecular Sciences (BNLMS), Institute of Chemistry, Chinese Academy of Sciences (CAS), Beijing, 100190, P. R. China.
School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences (UCAS), 100049, Beijing, P. R. China.
Adv Mater. 2023 Jun;35(24):e2300350. doi: 10.1002/adma.202300350. Epub 2023 Apr 28.
The uncontrollable dendrite growth and unstable solid electrolyte interphase have long plagued the practical application of Li metal batteries. Herein, a dual-layered artificial interphase LiF/LiBO-Ag is demonstrated that is simultaneously reconfigured via an electrochemical process to stabilize the lithium anode. This dual-layered interphase consists of a heterogeneous LiF/LiBO glassy top layer with ultrafast Li-ion conductivity and lithiophilic Li-Ag alloy bottom layer, which synergistically regulates the dendrite-free Li deposition, even at high current densities. As a result, Li||Li symmetric cells with LiF/LiBO-Ag interphase achieve an ultralong lifespan (4500 h) at an ultrahigh current density and area capacity (20 mA cm , 20 mAh cm ). LiF/LiBO-Ag@Li anodes are successfully applied in quasi-solid-state batteries, showing excellent cycling performances in symmetric cells (8 mA cm , 8 mAh cm , 5000 h) and full cells. Furthermore, a practical quasi-solid-state pouch cell coupling with a high-nickel cathode exhibits stable cycling with a capacity retention of over 91% after 60 cycles at 0.5 C, which is comparable or even better than that in liquid-state pouch cells. Additionally, a high-energy-density quasi-solid-state pouch cell (10.75 Ah, 448.7 Wh kg ) is successfully accomplished. This well-orchestrated interphase design provides new guidance in engineering highly stable interphase toward practical high-energy-density lithium metal batteries.
不可控的枝晶生长和不稳定的固体电解质界面长期以来一直困扰着锂金属电池的实际应用。在此，我们展示了一种双层人工界面 LiF/LiBO-Ag，它可以通过电化学过程同时进行重构，以稳定锂金属阳极。这种双层界面由具有超快锂离子电导率的异质 LiF/LiBO 玻璃状顶层和具有亲锂性的 Li-Ag 合金底层组成，协同调节无枝晶锂沉积，即使在高电流密度下也是如此。结果，具有 LiF/LiBO-Ag 界面的 Li||Li 对称电池在超高电流密度和面积容量（20 mA cm −2 ，20 mAh cm −2 ）下实现了超长寿命（4500 h）。LiF/LiBO-Ag@Li 阳极成功应用于准固态电池，在对称电池（8 mA cm −2 ，8 mAh cm −2 ，5000 h）和全电池中表现出优异的循环性能。此外，一种实用的准固态软包电池与高镍正极耦合，在 0.5 C 下循环 60 次后，容量保持率超过 91%，其循环稳定性可与液态软包电池相媲美，甚至更好。此外，还成功完成了一种高能量密度的准固态软包电池（10.75 Ah，448.7 Wh kg −1 ）。这种精心设计的界面提供了在工程中实现高稳定性界面的新指导，以实现实用的高能量密度锂金属电池。
