High-voltage lithium-metal battery with three-dimensional mesoporous carbon anode host and ether/carbonate binary electrolyte

• Published in: Carbon (New York) 2021-10, Vol.184, p.752-763
• Main Authors: Adhitama, Egy, Rath, Purna Chandra, Prayogi, Achmad, Patra, Jagabandhu, Lee, Tai-Chou, Li, Ju, Chang, Jeng-Kuei
• Format: Article
• Language: English
• Subjects: Anode architecture; Anodes; Batteries; Carbon; Carbon nanotubes; Cathodes; Electrochemical analysis; Electrodes; Electrolyte design; Electrolytes; Full cell; Graphene; High energy density; Lithium; Lithium batteries; Ni-rich cathode; Open channels; Plating; Raman spectroscopy; Solid electrolytes; Structural stability; Studies
• ISSN: 0008-6223; 1873-3891
• DOI: 10.1016/j.carbon.2021.08.087

Electrolyte recipes and Li metal anode host materials are developed for lithium-metal batteries. 1,2-dimethoxyethane/ethylene carbonate mixed solvent with 1 M lithium bis(fluorosulfonyl)imide and 1 wt% LiNO3 is shown to form a robust solid electrolyte interphase and improve Coulombic efficiency and cyclability during Li metal plating/stripping. This electrolyte can withstand high potential, allowing the operation of a LiNi0.8Co0.1Mn0.1O2 (NMC-811) cathode. One-dimensional carbon nanotubes, two-dimensional graphene nanosheets, and three-dimensional ordered mesoporous carbon CMK-8 are used as the host materials for the accommodation of Li metal. The strong and continuous conducting network of CMK-8 with interpenetrating open channels is found to be a promising scaffold for Li metal. With the proposed electrolyte, the CMK-8 electrode enables uniform Li plating/stripping with a high Coulombic efficiency of 99.2% under a practical current density of 1 mA cm−2. Moreover, a long life of >550 charge-discharge cycles is achieved. The high structural stability of CMK-8 upon cycling is confirmed using electron microscopy and Raman spectroscopy. Finally, we use a Li-free CMK-8 electrode, an NMC-811 cathode, and the proposed electrolyte to construct a full cell. The electrochemical properties are evaluated. [Display omitted] •Electrolyte and anode host materials are developed for lithium-metal batteries.•The proposed electrolyte induces a robust SEI and withstands high potential.•1-D CNT, 2-D graphene, and 3-D CMK-8 carbon host materials are examined.•CMK-8 structure can minimize the dead Li amount and suppress Li dendrite formation.•Superior CE of 99.2% and great stability of up to 550 cycles are found for CMK-8.