Extended Electrochemical Window of Solid Electrolytes via Heterogeneous Multilayered Structure for High-Voltage Lithium Metal Batteries.

Duan, Hui; Fan, Min; Chen, Wan-Ping; Li, Jin-Yi; Wang, Peng-Fei; Wang, Wen-Peng; Shi, Ji-Lei; Yin, Ya-Xia et al. · Adv Mater · 2019

basic_science · Level V

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Abstract

In response to the call for safer high-energy-density storage systems, high-voltage solid-state Li metal batteries have attracted extensive attention. Therefore, solid electrolytes are required to be stable against both Li anode and high-voltage cathodes; nevertheless, the requirements still cannot be completely satisfied. Herein, a heterogeneous multilayered solid electrolyte (HMSE) is proposed to broaden electrochemical window of solid electrolytes to 0-5 V, through different electrode/electrolyte interfaces to overcome the interfacial instability problems. Oxidation-resistance poly(acrylonitrile) (PAN) is in contact with the cathode, while reduction tolerant polyethylene glycol diacrylate contacts with Li metal anode. A Janus and flexible PAN@Li<sub>1.4</sub> Al<sub>0.4</sub> Ge<sub>1.6</sub> (PO<sub>4</sub> )<sub>3</sub> (80 wt%) composite electrolyte is designed as intermediate layer to inhibit dendrite penetration and ensure compact interface. Paired with LiNi<sub>0.6</sub> Co<sub>0.2</sub> Mn<sub>0.2</sub> O<sub>2</sub> and LiNi<sub>0.8</sub> Co<sub>0.1</sub> Mn<sub>0.1</sub> O<sub>2</sub> cathodes, which are rarely used in solid-state batteries, the solid-state Li metal batteries with HMSE exhibit excellent electrochemical performance including high capacity and long cycle life. Besides, the Li||Li symmetric batteries maintain a stable polarization less than 40 mV for more than 1000 h under 2 mA cm<sup>-2</sup> and effective inhibition of dendrite formation. This study offers a promising approach to extend the applications of solid electrolytes for high-voltage solid-state Li metal batteries.