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Low concentration electrolyte with non-solvating cosolvent enabling high-voltage lithium metal batteries.

ABSTRACT: Developing low cost, yet high-voltage electrolyte is significant to improve the energy density and practicability of lithium metal batteries (LMBs). Low concentration electrolyte has significant merits in terms of cost and viscosity; however, their poor compatibility with high-voltage LMBs hinders its applications. Here, we develop a diluted low concentration electrolyte by replacing solvating cosolvent with a non-solvating cosolvent to facilitate the interaction between BF₄ ^- and Li⁺, resulting in optimized interfacial chemistry and suppressed side reaction. Thus, the high-loading Li-LiCoO₂ full cells (20.4 mg cm^-2) deliver outstanding cycling stability and rate performance at a cutoff voltage of 4.6 V. More impressively, a Li-LiCoO₂ pouch cell achieves an energy density of more than 400 Wh kg^-1 under practical conditions with thin Li (50 μm) and lean electrolyte (2.7 g Ah^-1). This work provides a rational approach to design a low concentration electrolyte, which can be extended to other high voltage battery systems.

SUBMITTER: Jiang Z

PROVIDER: S-EPMC8715189 | biostudies-literature | 2022 Jan

REPOSITORIES: biostudies-literature

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Low concentration electrolyte with non-solvating cosolvent enabling high-voltage lithium metal batteries.

Jiang Zhipeng Z Zeng Ziqi Z Zhang Han H Yang Li L Hu Wei W Liang Xinmiao X Feng Jiwen J Yu Chuang C Cheng Shijie S Xie Jia J

iScience 20211201 1

Developing low cost, yet high-voltage electrolyte is significant to improve the energy density and practicability of lithium metal batteries (LMBs). Low concentration electrolyte has significant merits in terms of cost and viscosity; however, their poor compatibility with high-voltage LMBs hinders its applications. Here, we develop a diluted low concentration electrolyte by replacing solvating cosolvent with a non-solvating cosolvent to facilitate the interaction between BF<sub>4</sub> <sup>-</s ...[more]

PMID: 35005528

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Project description:Safety and high-voltage operation are key metrics for advanced, solid-state energy storage devices to power low- or zero-emission HEV or EV vehicles. In this study, we propose the modification of single-ion conducting polyelectrolytes by designing novel block copolymers, which combine one block responsible for high ionic conductivity and the second block for improved mechanical properties and outstanding electrochemical stability. To synthesize such block copolymers, the ring opening polymerization (ROP) of trimethylene carbonate (TMC) monomer by the RAFT-agent having a terminal hydroxyl group is used. It allows for the preparation of a poly(carbonate) macro-RAFT precursor that is subsequently applied in RAFT copolymerization of lithium 1-[3-(methacryloyloxy)propylsulfonyl]-1-(trifluoromethylsulfonyl)imide and poly(ethylene glycol) methyl ether methacrylate. The resulting single-ion conducting block copolymers show improved viscoelastic properties, good thermal stability (T onset up to 155 °C), sufficient ionic conductivity (up to 3.7 × 10-6 S cm-1 at 70 °C), and high lithium-ion transference number (0.91) to enable high power. Excellent plating/stripping ability with resistance to dendrite growth and outstanding electrochemical stability window (exceeding 4.8 V vs Li+/Li at 70 °C) are also achieved, along with enhanced compatibility with composite cathodes, both LiNiMnCoO2 - NMC and LiFePO4 - LFP, as well as the lithium metal anode. Lab-scale truly solid-state Li/LFP and Li/NMC lithium-metal cells assembled with the single-ion copolymer electrolyte demonstrate reversible and very stable cycling at 70 °C delivering high specific capacity (up to 145 and 118 mAh g-1, respectively, at a C/20 rate) and proper operation even at a higher current regime. Remarkably, the addition of a little amount of propylene carbonate (∼8 wt %) allows for stable, highly reversible cycling at a higher C-rate. These results represent an excellent achievement for a truly single-ion conducting solid-state polymer electrolyte, placing the obtained ionic block copolymers on top of polyelectrolytes with highest electrochemical stability and potentially enabling safe, practical Li-metal cells operating at high-voltage.

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Low concentration electrolyte with non-solvating cosolvent enabling high-voltage lithium metal batteries.

Publications

Low concentration electrolyte with non-solvating cosolvent enabling high-voltage lithium metal batteries.

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