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Enabling "lithium-free" manufacturing of pure lithium metal solid-state batteries through in situ plating.

ABSTRACT: The coupling of solid-state electrolytes with a Li-metal anode and state-of-the-art (SOA) cathode materials is a promising path to develop inherently safe batteries with high energy density (>1000?Wh?L^-1). However, integrating metallic Li with solid-electrolytes using scalable processes is not only challenging, but also adds extraneous volume since SOA cathodes are fully lithiated. Here we show the potential for "Li-free" battery manufacturing using the Li₇La₃Zr₂O₁₂ (LLZO) electrolyte. We demonstrate that Li-metal anodes >20??m can be electroplated onto a current collector in situ without LLZO degradation and we propose a model to relate electrochemical and nucleation behavior. A full cell consisting of in situ formed Li, LLZO, and NCA is demonstrated, which exhibits stable cycling over 50 cycles with high Coulombic efficiencies. These findings demonstrate the viability of "Li-free" configurations using LLZO which may guide the design and manufacturing of high energy density solid-state batteries.

SUBMITTER: Wang MJ

PROVIDER: S-EPMC7567811 | biostudies-literature | 2020 Oct

REPOSITORIES: biostudies-literature

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Enabling "lithium-free" manufacturing of pure lithium metal solid-state batteries through in situ plating.

Wang Michael J MJ Carmona Eric E Gupta Arushi A Albertus Paul P Sakamoto Jeff J

Nature communications 20201015 1

The coupling of solid-state electrolytes with a Li-metal anode and state-of-the-art (SOA) cathode materials is a promising path to develop inherently safe batteries with high energy density (>1000 Wh L-1). However, integrating metallic Li with solid-electrolytes using scalable processes is not only challenging, but also adds extraneous volume since SOA cathodes are fully lithiated. Here we show the potential for "Li-free" battery manufacturing using the Li7La3Zr< ...[more]

PMID: 33060571

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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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Enabling "lithium-free" manufacturing of pure lithium metal solid-state batteries through in situ plating.

Publications

Enabling "lithium-free" manufacturing of pure lithium metal solid-state batteries through in situ plating.

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