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Plastic Monolithic Mixed-Conducting Interlayer for Dendrite-Free Solid-State Batteries.

ABSTRACT: Solid-state electrolytes (SSEs) hold a critical role in enabling high-energy-density and safe rechargeable batteries with Li metal anode. Unfortunately, nonuniform lithium deposition and dendrite penetration due to poor interfacial solid-solid contact are hindering their practical applications. Here, solid-state lithium naphthalenide (Li-Naph(s)) is introduced as a plastic monolithic mixed-conducting interlayer (PMMCI) between the garnet electrolyte and the Li anode via a facile cold process. The thin PMMCI shows a well-ordered layered crystalline structure with excellent mixed-conducting capability for both Li⁺ (4.38 × 10^-3 S cm^-1 ) and delocalized electrons (1.01 × 10^-3 S cm^-1 ). In contrast to previous composite interlayers, this monolithic material enables an intrinsically homogenous electric field and Li⁺ transport at the Li/garnet interface, thus significantly reducing the interfacial resistance and achieving uniform and dendrite-free Li anode plating/stripping. As a result, Li symmetric cells with the PMMCI-modified garnet electrolyte show highly stable cycling for 1200 h at 0.2 mA cm^-2 and 500 h at a high current density of 1 mA cm^-2 . The findings provide a new interface design strategy for solid-state batteries using monolithic mixed-conducting interlayers.

SUBMITTER: Xiong BQ

PROVIDER: S-EPMC9218657 | biostudies-literature |

REPOSITORIES: biostudies-literature

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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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Plastic Monolithic Mixed-Conducting Interlayer for Dendrite-Free Solid-State Batteries.

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