Prelithiation is widely recognized as a promising technology to enable the use of high capacity anode active materials such as silicon. Numerous prelithiation techniques have been proposed over the years, with a handful successfully undergoing pilot scale testing. Nevertheless, new challenges arise when moving from optimizing single processes to integrating them into the process chain. A major concern is the stability of prelithiated electrodes against moisture. In this study, we investigate the influence of industrially-relevant moisture levels on the electrochemical performance of prelithiated graphite/SiO_x composite anodes in 3-electrode half- and full-cells. We identify several indicators of electrode degradation such as an increase in open circuit potential, a decrease in graphite lithiation potential, and changes in specific charge/discharge capacity. The underlying degradation mechanisms are examined using electrochemical impedance spectroscopy, X-ray photoelectron spectroscopy, and time-of-flight secondary ion mass spectrometry, which show increased solid electrolyte interphase (SEI)-related interfacial resistances but no clear evidence of SEI degradation. Based on the experimental results, we define a process window for the stability of the investigated electrodes as a function of dew point and exposure time. Our results indicate an encouragingly high stability at dew points up to −40 °C for a realistic exposure time of 1 h.

Despite the variety of solid electrolytes available, no single solid electrolyte has been found that meets all the requirements of the successor technology of lithium-ion batteries in an optimum way. However, composite hybrid electrolytes that combine the desired properties such as high ionic conductivity or stability against lithium are promising. The addition of conductive oxide fillers to sulfide solid electrolytes has been reported to increase ionic conductivity and improve stability relative to the individual electrolytes, but the influence of the mixing process to create composite electrolytes has not been investigated. Here, we investigate Li₃PS₄ (LPS) and Li₇La₃Zr₂O₁₂ (LLZO) composite electrolytes using electrochemical impedance spectroscopy and distribution of relaxation times. The distinction between sulfide bulk and grain boundary polarization processes is possible with the methods used at temperatures below 10 °C. We propose lithium transport through the space-charge layer within the sulfide electrolyte, which increases the conductivity. With increasing mixing intensities in a high-energy ball mill, we show an overlay of the enhanced lithium-ion transport with the structural change of the sulfide matrix component, which increases the ionic conductivity of LPS from 4.1 × 10⁻⁵ S cm⁻¹ to 1.7 × 10⁻⁴ S cm⁻¹.

Niobium-containing diamond-like carbon films (a-C:H:Nb) were deposited in a hybrid plasma-enhanced chemical vapor deposition (PECVD) and direct-current magnetron sputtering (DCMS) process, using a niobium target in an argon/acetylene atmosphere on industrial polyimide foil, spin-coated polyimide foil, and alumina substrates. While the coating on the industrial foil tends to crack, the thin films on the spin-coated polyimide and the ceramic substrates showed good adhesion, as well as a smooth and dense topography. Investigations of the electrical properties revealed their suitability as biocompatible sensor materials in strain gauges, with a gauge factor of up to 3.2 and a temperature coefficient of the electrical resistance (TCR) of −200 ppm/K.

Among next-generation batteries, all-solid-state batteries (ASSB) promise increased energy densities, fast charging properties, and higher safety compared to traditional liquid-based systems. To achieve the demanded high energy densities high mass loadings of the composite cathodes are necessary. These consist of active material (AM), solid electrolyte (SE), and conductive additive as well as binder. Volume changes of intercalation AM and insufficient ionic percolation at low SE contents lead to an increased interfacial resistance and capacity loss. In order to promote cathode AM utilization the particle size ratio of the AM and the SE within the composite cathode needs to be optimized. Theoretical calculations have shown that for high AM utilization at high AM loadings particle size ratio is a crucial parameter [1, 2]. Experimentally, the influence of particle size ratio has so far only been studied at laboratory scale. However, scalable process routes have not considered this important aspect. In this work, we present a solvent-based process route for the preparation of sulfide-based solid-state composite cathodes with NCM622 as AM, starting from the adjustment of the particle size of a commercially available Li₆PS₅Cl SE by planetary ball mill. Further process steps include the dispersion of SE with AM and conductive additive and doctor blade coating of cathode films. We analyzed the composite cathodes with regard to their internal resistance as well as their microstructure and conducted electrochemical tests in lab-scale test cells. Optimization of the particle size ratio results in an increase of AM utilization by a factor of 5 as well as an enhanced AM-SE-particle contact area and lower porosity. References [1] Shi T, Tu Q, Tian Y, et al. High Active Material Loading in All‐Solid‐State Battery Electrode via Particle Size Optimization. Adv. Energy Mater. 2020; 10(1): 1902881 [https://doi.org/10.1002/aenm.201902881] [2] Bielefeld A, Weber DA, Janek J. Microstructural Modeling of Composite Cathodes for All-Solid-State Batteries. J. Phys. Chem. C 2019; 123(3): 1626–34 [https://doi.org/10.1021/acs.jpcc.8b11043]