ABSTRACT
The ever-growing needs for renewable energy demand the pursuit of batteries with higher energy/power output. A thick electrode design is considered as a promising solution for high-energy batteries due to the minimized inactive material ratio at the device level. Most of the current research focuses on pushing the electrode thickness to a maximum limit; however, very few of them thoroughly analyze the effect of electrode thickness on cell-level energy densities as well as the balance between energy and power density. Here, a realistic assessment of the combined effect of electrode thickness with other key design parameters is provided, such as active material fraction and electrode porosity, which affect the cell-level energy/power densities of lithium-LiNi0.6 Mn0.2 Co0.2 O2 (Li-NMC622) and lithium-sulfur (Li-S) cells as two model battery systems, is provided. Based on the state-of-the-art lithium batteries, key research targets are quantified to achieve 500 Wh kg-1 /800 Wh L-1 cell-level energy densities and strategies are elaborated to simultaneously enhance energy/power output. Furthermore, the remaining challenges are highlighted toward realizing scalable high-energy/power energy-storage systems.
ABSTRACT
The phase distribution of lithiated LVO in thick (â¼500 µm) porous electrodes (TPEs) designed to facilitate both ion and electron transport was determined using synchrotron-based operando energy dispersive X-ray diffraction (EDXRD). Probing 3 positions in the TPE while cycling at a 1C rate revealed a homogeneous phase transition across the thickness of the electrode at the 1st and 95th cycles. Continuum modelling indicated uniform lithiation across the TPE in agreement with the EDXRD results and ascribed decreasing accessible active material to be the cause of loss in delivered capacity between the 1st and 95th cycles. The model was supported by the observation of significant particle fracture by SEM consistent with loss of electrical contact. Overall, the combination of operando EDXRD, continuum modeling, and ex situ measurements enabled a deeper understanding of lithium vanadium oxide transport properties under high rate extended cycling within a thick highly porous electrode architecture.
ABSTRACT
To suppress dendrite formation in lithium metal batteries, high cation transference number electrolytes that reduce electrode polarization are highly desirable, but rarely available using conventional liquid electrolytes. Here, we show that liquid electrolytes increase their cation transference numbers (e.g., â¼0.2 to >0.70) when confined to a structurally rigid polymer host whose pores are on a similar length scale (0.5-2 nm) as the Debye screening length in the electrolyte, which results in a diffuse electrolyte double layer at the polymer-electrolyte interface that retains counterions and reject co-ions from the electrolyte due to their larger size. Lithium anodes coated with â¼1 µm thick overlayers of the polymer host exhibit both a low area-specific resistance and clear dendrite-suppressing character, as evident from their performance in Li-Li and Li-Cu cells as well as in post-mortem analysis of the anode's morphology after cycling. High areal capacity Li-S cells (4.9 mg cm-2; 8.2 mAh cm-2) implementing these high transference number polymer-hosted liquid electrolytes were remarkably stable, considering â¼24 µm of lithium was electroreversibly deposited in each cycle at a C-rate of 0.2. We further identified a scalable manufacturing path for these polymer-coated lithium electrodes, which are drop-in components for lithium metal battery manufacturing.
