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    Anion-Rectifying Polymeric Single Lithium-Ion Conductors

    Year: 2022

    Journal: Adv. Funct. Mater., Volume 32, FEB

    Authors: Cho, Seok-Kyu; Oh, Kyeong-Seok; Shin, Jong Chan; Lee, Ji Eun; Lee, Kyung Min; Cho, Junbeom; Lee, Won Bo; Kwak, Sang Kyu; Lee, Minjae; Lee, Sang-Young

    Organizations: Basic Science Research Program through the National Research Foundation of Korea (NRF) - Korean Government (MSIT) [2018M3D1A1058744, 2021R1A2B5B03001615]; Technology Innovation Program - Ministry of Trade, Industry & Energy (MOTIE, Korea) [20012216, 20010095]

    Keywords: accelerated li-ion transport; anion-rectifying capability; polymeric single-ion conductors; reticulated ion nanochannels; semi-interpenetrating polymer network

    Polymeric single lithium (Li)-ion conductors (SICs), along with inorganic conducting materials such as sulfides and oxides, have received significant attention as promising solid-state electrolytes. Yet their practical applications have been plagued predominantly by sluggish ion transport. Here, a new class of quasi-solid-state SICs based on anion-rectifying semi-interpenetrating polymer networks (semi-IPNs) with reticulated ion nanochannels are demonstrated. This semi-IPN SIC (denoted as sSIC) features a bicontinuous and nanophase-separated linear cationic polyurethane (cPU), which supports single-ion conducting nanochannels, and ultraviolet-crosslinked triacrylate polymer, which serves as a mechanical framework. The cPU phase is preferentially swollen with a liquid electrolyte and subsequently allows anion-rectifying capability and nanofluidic transport via surface charge, which enable fast Li+ migration through ion nanochannels. Such facile Li+ conduction is further enhanced by tuning ion-pair (i.e., freely movable anions and cations tethered to the cPU chains) interaction. Notably, the resulting sSIC provides high Li+ conductivity that exceeds those of commercial carbonate liquid electrolytes. This unusual single-ion conduction behavior of the sSIC suppresses anion-triggered interfacial side reactions with Li-metal anodes and facilitates electrochemical reaction kinetics at electrodes, eventually improving rate performance and cycling retention of Li-metal cells (comprising LiNi0.8Co0.1Mn0.1O2 cathodes and Li-metal anodes) compared to those based on carbonate liquid electrolytes.
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