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To fabricate ceramic composite cathodes LiCoO2–Li6.6La3Zr1.6Ta0.4O12 (LCO-LLZTO) on an industrial scale, a water-based tape-casting process was developed, which is scalable and environmentally friendly. Additionally, the cosintering behavior of the two materials, often leading to poor electrochemical performance, was optimized via a Li2O-rich atmosphere. The resulting dense, free-standing, and phase-pure LCO-LLZTO mixed cathodes were assembled into full cells using a dual-layer solid polymer-ceramic separator and an In–Li anode. These cells show very high utilization rates for LCO of approximately 90% at a high areal capacity of over 3 mAh cm–2, demonstrating the potential of water-based tape-casting for a scalable and sustainable manufacturing of oxide-ceramic based solid-state Li batteries.

ChemSusChem : chemistry & sustainability, energy & materials (2021). doi:10.1002/cssc.202101178 special issue: "Chemistry Europe Reviews", Published by Wiley-VCH, Weinheim

All-solid-state sodium batteries (ASSNBs), which combine the benefits of high safety and low cost, are expectedto be an alternative or complementary storage technology to lithium ion batteries. Herein, we developed anaqueous tape casting technique for the continuous fabrication of ceramic sheets made of silicate-based Na5YSi4O12(NYS) Na+ ion superionic conductor for the first time. After sintering, the ceramics showed a total conductivityof 1.0 mS cm􀀀 1 at room-temperature, low total activation energy of 0.30 eV, and wide electrochemicalwindow of over 8 V. The critical current density of NYS tape against Na-metal electrodes can reach 2.2 mA cm􀀀 2and the galvanostatic cycling time is over 280 h under 0.8 mA cm􀀀 2 and 0.8 mAh cm􀀀 2. The obtained tape hashigh crystalline purity, dense microstructure, favorable mechanical properties (hardness H of 2 GPa and elasticmodulus E of 45 GPa). This work not only highlights the potential of the scarcely studied silicate-based NYS ionicconductor as a functional separator, but also presents a cost-efficient and eco-friendly continuous fabricationusing the aqueous tape casting technique, thus being expected to boost the practical application of NYS as solidstateelectrolyte in ASSNBs.

Several hydrophilic ionic liquids dissolved in water with different molalities are studied as “water-in-ionic liquid” supporting electrolytes. They exhibit wide electrochemical stability window from 3 to 4.4 V, high ionic conductivities and good flowability, making them promising supporting electrolytes for aqueous high-voltage rechargeable batteries. In such supporting electrolytes, enhanced redox activities of lithium insertion/extraction in anodic TiO2 film at low negative potential and Fe3+/Fe2+ couple at moderate positive potential were observed. Cyclability of an aqueous TiO2/Fe2+ hybrid battery is demonstrated with a voltage of 1.7 V.