Understanding Interfaces at the Positive and Negative Electrodes on Sulfide-Based Solid-State Batteries.

Despite the high ionic conductivity and attractive mechanical properties of sulfide-based solid-state batteries, this chemistry still faces key challenges to encompass fast rate and long cycling performance, mainly arising from dynamic and complex solid-solid interfaces. This work provides a comprehensive assessment of the cell performance-determining factors ascribed to the multiple sources of impedance from the individual processes taking place at the composite cathode with high-voltage LiNi0.6Mn0.2Co0.2O2, the sulfide argyrodite Li6PS5Cl separator, and the Li metal anode. From a multiconfigurational approach and an advanced deconvolution of electrochemical impedance signals into distribution of relaxation times, we disentangle intricate underlying interfacial processes taking place at the battery components that play a major role on the overall performance. For the Li metal solid-state batteries, the cycling performance is highly sensitive to the chemomechanical properties of the cathode active material, formation of the SEI, and processes ascribed to Li diffusion in the cathode composite and in the space-charge layer. The outcomes of this work aim to facilitate the design of sulfide solid-state batteries and provide methodological inputs for battery aging assessment.

Rational Optimization of Cathode Composites for Sulfide-Based All-Solid-State Batteries.

All-solid-state lithium-ion batteries with argyrodite solid electrolytes have been developed to attain high conductivities of 10-3 S cm-1 in studies aiming at fast ionic conductivity of electrolytes. However, no matter how high the ionic conductivity of the electrolyte, the design of the cathode composite is often the bottleneck for high performance. Thus, optimization of the composite cathode formulation is of utmost importance. Unfortunately, many reports limit their studies to only a few parameters of the whole electrode formulation. In addition, different measurement setups and testing conditions employed for all-solid-state batteries make a comparison of results from mutually independent studies quite difficult. Therefore, a detailed investigation on different key parameters for preparation of cathodes employed in all-solid-state batteries is presented here. Employing a rational approach for optimization of composite cathodes using solid sulfide electrolytes elucidated the influence of different parameters on the cycling performance. First, powder electrodes made without binders are investigated to optimize several parameters, including the active materials' particle morphology, the nature and amount of the conductive additive, the particle size of the solid electrolyte, as well as the active material-to-solid electrolyte ratio. Finally, cast electrodes are examined to determine the influence of a binder on cycling performance.

Self-Assembled Novel BODIPY-Based Palladium Supramolecules and Their Cellular Localization.

Four new palladium metal supramolecules with triangular/square architectures derived from boron dipyrromethane (BODIPY) ligands were synthesized by self-assembly and fully characterized by 1H and 31P NMR, electrospray ionization mass spectrometry, and single-crystal X-ray diffraction. These supramolecules were more cytotoxic to brain cancer (glioblastoma) cells than to normal lung fibroblasts. Their cytotoxicity to the glioblastoma cells was higher than that of a benchmark metal-based chemotherapy drug, cisplatin. The characteristic green fluorescence of the BODIPY ligands in these supramolecules permitted their intracellular visualization using confocal microscopy, and the compounds were localized in the cytoplasm and on the plasma membrane.

Surface Modification of the LiFePO4 Cathode for the Aqueous Rechargeable Lithium Ion Battery.

The LiFePO4 surface is coated with AlF3 via a simple chemical precipitation for aqueous rechargeable lithium ion batteries (ARLBs). During electrochemical cycling, the unfavorable side reactions between LiFePO4 and the aqueous electrolyte (1 M Li2SO4 in water) leave a highly resistant passivation film, which causes a deterioration in the electrochemical performance. The coated LiFePO4 by 1 wt % AlF3 has a high discharge capacity of 132 mAh g-1 and a highly improved cycle life, which shows 93% capacity retention even after 100 cycles, whereas the pristine LiFePO4 has a specific capacity of 123 mAh g-1 and a poor capacity retention of 82%. The surface analysis results, which include X-ray photoelectron spectroscopy and transmission electron microscopy results, show that the AlF3 coating material is highly effective for reducing the detrimental surface passivation by relieving the electrochemical side reactions of the fragile aqueous electrolyte. The AlF3 coating material has good compatibility with the LiFePO4 cathode material, which mitigates the surface diffusion obstacles, reduces the charge-transfer resistances and improves the electrochemical performance and surface stability of the LiFePO4 material in aqueous electrolyte solutions.