Polymer-Mineral Composite Solid Electrolytes

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MRS Advances © 2019 Materials Research Society DOI: 10.1557/adv.2019.317

Polymer-Mineral Composite Solid Electrolytes Bo Wang Imerys, San Jose, CA 95134, U.S.A.

ABSTRACT

Polymer-mineral composite solid electrolytes have been prepared by hot pressing using lithium ion-exchanged bentonite (LIEB) and mineral derived LATSP (Li1.2Al0.1Ti1.9Si0.1P2.9O12) NASICON materials as solid electrolyte fillers in the polyethylene oxide (PEO) polymer containing LiTFSI salt. The mineral based solid electrolyte fillers not only increase ionic conductivity but also improve thermal stability. The highest ionic conductivities in the PEOLIEB and PEO-LATSP composites were found to be 9.4u10-5 and 3.1u10-4 S·cm-1 at 40°C, respectively. The flexible, thermal stable and mechanical sturdy polymer-mineral composite solid electrolyte films can be used in the all-solid-state batteries.

INTRODUCTION Inorganic ceramic solid electrolytes can overcome the concerns on safety, reliability, operation temperature, capacity loss and cycle life issues related to liquid organic electrolytes used in conventional lithium ion batteries [1-7]. However, the poor interfacial contact between the inorganic ceramic solid electrolytes and electrodes affects performance of all-solid-state batteries using inorganic ceramic solid electrolytes [8-12]. Soft polymer electrolytes can decrease the electrode-electrolyte interface resistance but polymers have low thermal stability and mechanical strength [13-16]. To combine the advantages of inorganic ceramic solid electrolytes and polymer solid electrolytes, polymer-ceramic composite solid electrolytes have been investigated with promising results [17-21]. For example, polymer-garnet composite solid electrolytes show good lithium ionic conductivity and mechanical strength [17, 18]. Similar results are also observed in the polymer-NASICON composite solid electrolytes [19-21]. Bentonite is a naturally abundant aluminosilicate mineral with good ion exchange capacity due to its sheet structure [22]. Lithium ions can be exchanged into the bentonite structure to enhance lithium ionic conductivity. Natural aluminosilicate kaolin clay mineral has been used as a starting material to synthesize ceramic NASICON solid electrolyte [23]. In this study, low cost minerals of lithium ion-exchanged natural bentonite and kaolin derived ceramic NASICON solid electrolyte are incorporated into the polymer matrix to form flexible composite solid electrolyte films. The impact of 2659

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these mineral derived solid electrolyte fillers on the ionic conductivity and thermal stability of the polymer-mineral composite solid electrolytes is discussed in this paper. EXPERIMENTAL DETAILS Lithium ion exchanged bentonite was prepared by activating a calcium bentonite (Imerys) with Li 2CO3 (Alfa Aesar, ACS, 99.0% min) us