Sustained-Release Nanocapsules Enable Long-Lasting Stabilization of Li Anode for Practical Li-Metal Batteries

A robust solid-electrolyte interphase (SEI) enabled by electrolyte additive is a promising approach to stabilize Li anode and improve Li cycling efficiency. However, the self-sacrificial nature of SEI forming additives limits their capability to stabilize Li anode for long-term cycling. Herein, we demonstrate nanocapsules made from metal–organic frameworks for sustained release of LiNO(3) as surface passivation additive in commercial carbonate-based electrolyte. The nanocapsules can offer over 10 times more LiNO(3) than the solubility of LiNO(3). Continuous supply of LiNO(3) by nanocapsules forms a nitride-rich SEI layer on Li anode and persistently remedies SEI during prolonged cycling. As a result, lifespan of thin Li anode in 50 μm, which experiences drastic volume change and repeated SEI formation during cycling, has been notably improved. By pairing with an industry-level thick LiCoO(2) cathode, practical Li-metal full cell demonstrates a remarkable capacity retention of 90% after 240 cycles, in contrast to fast capacity drop after 60 cycles in LiNO(3) saturated electrolyte. [Image: see text] ELECTRONIC SUPPLEMENTARY MATERIAL: The online version of this article (10.1007/s40820-020-00514-1) contains supplementary material, which is available to authorized users.