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Solubility-mediated sustained release enabling nitrate additive in carbonate electrolytes for stable lithium metal anode

2018; Nature Portfolio; Volume: 9; Issue: 1 Linguagem: Inglês

10.1038/s41467-018-06077-5

2041-1723

Yayuan Liu, Dingchang Lin, Yuzhang Li, Guangxu Chen, Allen Pei, O. Nix, Yanbin Li, Yi Cui,

Advanced battery technologies research

Abstract The physiochemical properties of the solid-electrolyte interphase, primarily governed by electrolyte composition, have a profound impact on the electrochemical cycling of metallic lithium. Herein, we discover that the effect of nitrate anions on regulating lithium deposition previously known in ether-based electrolytes can be extended to carbonate-based systems, which dramatically alters the nuclei from dendritic to spherical, albeit extremely limited solubility. This is attributed to the preferential reduction of nitrate during solid-electrolyte interphase formation, and the mechanisms behind which are investigated based on the structure, ion-transport properties, and charge transfer kinetics of the modified interfacial environment. To overcome the solubility barrier, a solubility-mediated sustained-release methodology is introduced, in which nitrate nanoparticles are encapsulated in porous polymer gel and can be steadily dissolved during battery operation to maintain a high concentration at the electroplating front. As such, effective dendrite suppression and remarkably enhanced cycling stability are achieved in corrosive carbonate electrolytes.