Scalable manufacturing and processing of high-aspect ratio multi-material solid-state electrolytes are important for advanced energy storage and conversion systems. Recently, there has been a push toward all solid-state batteries to eliminate flammability issues in portable electronics. Several solid conductors exist and broadly fall into two material categories: (1) polymers and (2) ceramics. Polymer ionic conductors are advantageous because they can be manufactured easily into thin films, are mechanically robust, and flexible. However, polymer conductors have lower ionic conductivities when compared with their ceramic counterpart. Ceramic conductors boast outstanding ionic conductivities (>10 mS/cm) but processing the electrolyte into thin films (50-100μm) for efficient device integration still remains a challenge because of the brittle nature of the ceramic. There have been a few studies which have investigated a hybrid approach which combines the polymer and ceramic into a composite electrolyte^1,2,3. Fundamentally, if achieved, the polymer/ceramic electrolyte could be an effective means for meeting manufacturing requirements for battery systems. Herein, we focus on understanding and building structure-processing-property relationships for scalable manufacturing of high performing polymer/ceramic composite electrolytes. Colloidals suspensions composed of LLZO, PEO, and a range of solvents are explored as inks systems for advanced printing applications^4,5. A range of electrolyte architectures are examined for fundamental transport properties and electrochemical performance metrics and synchrotron nanotomography⁶ is used to discern the local structure of the ceramic within the polymer.

[1] Yang, Ting, et al. "Composite Polymer Electrolytes with Li7La3Zr2O12 Garnet-Type Nanowires as Ceramic Fillers: Mechanism of Conductivity Enhancement and Role of Doping and Morphology." ACS applied materials & interfaces 9.26 (2017): 21773-21780.

[2] Zheng, Jin, and Yan Yan Hu. "New Insights into Compositional Dependence of Li-Ion Transport in Polymer-Ceramic Composite Electrolytes." ACS applied materials & interfaces(2018)

[3] Zheng, Jin, et al. "Li-ion transport in a representative ceramic–polymer–plasticizer composite electrolyte: Li 7 La 3 Zr 2 O 12–polyethylene oxide–tetraethylene glycol dimethyl ether." Journal of Materials Chemistry A 5.35 (2017): 18457-18463.

[4] Hatzell, Kelsey B., et al. "Understanding inks for porous-electrode formation." Journal of Materials Chemistry A 5.39 (2017): 20527-20533.

[5] Dixit, Marm B., et al. "Catalyst Layer Ink Interactions That Affect Coatability." Journal of The Electrochemical Society165.5 (2018): F264-F271.

[6] Hatzell, Kelsey B., et al. "Direct observation of active material interactions in flowable electrodes using X-ray tomography." Faraday discussions 199 (2017): 511-524.