The current Li-ion batteries with organic liquid electrolytes are limited by their safety and energy density. Therefore, ceramic electrolytes are proposed in developing next-generation, energy-dense Li-metal batteries by replacing organic liquid electrolytes to improve safety and performance. Among numerous ceramic Li-ion conductors, garnet-based solid electrolyte c-Li7La3Zr2O12 (c-LLZO) is considered one of the most promising candidates to enable Li metal batteries due to its high ionic conductivity, chemical stability, and wide electrochemical stability window against Li metal. However, synthesis and processing of c-LLZO through conventional solid-sate reaction methods requires long periods of calcination (> 6 h) at high reaction temperatures (> 1000 °C). The need for high reaction temperature results to attain cubic-LLZO phase results in large aggerated LLZO particles and causes Li-loss from the garnet structure, making them unfavorable to process further as bulk pellets or thin films. To overcome processing challenges with solid-state reaction method, two novel facile synthesis approaches molten salt (flux growth method), and solution combustion are employed to produce submicron-sized LLZO powders at low reaction temperatures (< 1000 °C) in a short time. In the first case, molten salt synthesis method with LiCl-KCl eutectic mixture is employed to produce sub-micron sized Ta-doped LLZO (LLZTO) powders at low temperatures (900 °C, 4 h). In addition, a detailed investigation on effect of sintering medium and sintering additives on the structural, microstructural, chemical, and Li-ion transport behavior of the LLZTO pellets are investigated. Sintered LLZTO pellets prepared using molten salt synthesis route exhibited high Li-ion conductivity up to 0.6 mS cm-1 and high relative density (> 95 %) using Pt-crucible. In the second case, a facile solution-combustion technique using an amide-based fuel source CH6N4O is utilized to produce submicron-sized Al-doped LLZO (Al-LLZO) powders at low reaction temperatures 600-800 °C in a short duration of 4 h. In addition, effect of fuel to oxidizer ratio on phase purity, particle growth size, and formation mechanism of conductive Al-LLZO are reported and discussed. The Al-LLZO pellets sintered at 1100 °C/ 6 h exhibited high Li-ion conductivity up to 0.45 mS cm-1 with relative densities (> 90 %).

Increasing demand for reducing the stress on fossil fuels has motivated automotive industries to shift towards sustainable modes of transport through electric and hybrid electric vehicles. Most fuel efficient cars of year 2016 are hybrid vehicles as reported by environmental protection agency. Hybrid vehicles operate with internal combustion engine and electric motors powered by batteries, and can significantly improve fuel economy due to downsizing of the engine. Whereas, Plug-in hybrids (PHEVs) have an additional feature compared to hybrid vehicles i.e. recharging batteries through external power outlets. Among hybrid powertrains, lithium-ion batteries have emerged as a major electrochemical storage source for propulsion of vehicles.

In PHEVs, batteries operate under charge sustaining and charge depleting mode based on torque requirement and state of charge. In the current article, 26650 lithium-ion cells were cycled extensively at 25 and 50 oC under charge sustaining mode to monitor capacity and cell impedance values followed by analyzing the Lithium iron phosphate (LiFePO4) cathode material by X-ray diffraction analysis (XRD). High frequency resistance measured by electrochemical impedance spectroscopy was found to increase significantly under high temperature cycling, leading to power fading. No phase change in LiFePO4 cathode material is observed after 330 cycles at elevated temperature under charge sustaining mode from the XRD analysis. However, there was significant change in crystallite size of the cathode active material after charge/discharge cycling with charge sustaining mode. Additionally, 18650 lithium-ion cells were tested under charge depleting mode to monitor capacity values.