Composite polymer electrolytes for all-solid-state lithium batteries with nanostructured garnet ceramic fillers

Conference Dates

November 10-14, 2019


The Li ion conducting garnet Li7La3Zr2O12 (LLZO) has attracted substantial interest as a solid electrolyte for next generation, all-solid-state lithium batteries on account of its relatively high ionic conductivity of ~10-4 S cm-1, non-reactivity with lithium, and wide voltage stability window (> 5 V vs. Li/Li+)1. Although more than a decade has passed since LLZO was first reported2, the application of LLZO as a ceramic electrolyte in all-solid-state batteries is still met with several practical challenges due to its brittle nature and the difficulty of forming good contacts or interfaces with electrodes3. Recently, the incorporation of LLZO as nanostructured ceramic fillers within solid polymer electrolytes has received great interest. The application of nano-sized particles as ceramic fillers has already been demonstrated to be effective for enhancing the mechanical stability and ionic conductivity of polymer-based solid electrolytes, but these fillers have mostly consisted of spherical particles of inert or “passive” components without intrinsic Li+ conductivity. Recent studies using LLZO-embedded into polymer films have revealed different degrees of effectiveness, indicating that more careful design of the composite polymer electrolytes (CPEs), including optimization of the LLZO filler properties and more detailed mechanistic study of the Li+ transport pathways, may be needed for the development of CPEs with high ionic conductivity. In our work4, we show that by incorporating only 5 wt% of electrospun LLZO nanowires into a polyacrylonitrile-LiClO4 matrix, the room temperature ionic conductivity of the composite is increased 3 orders of magnitude to 1.31 × 10-4 S/cm. CPEs made using LLZO nanoparticle and Al2O3 nanowire fillers are also studied to elucidate the role of filler type (active vs. passive), LLZO composition (undoped vs. doped), and morphology (nanowire vs. nanoparticle) on the CPE conductivity. It is demonstrated that both intrinsic Li+ conductivity and nanowire morphology are needed for optimum performance. Subsequent studies using solid-state nuclear magnetic resonance and synchrotron X-ray fluorescence microscopy are used to investigate the Li transport pathways and understand the dispersion of the nanowires within the composite films.

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