Planetary ball mills are well known and used for particle size reduction on laboratory and pilot scales for decades while during the last few years the application of planetary ball mills has extended to mechanochemical approaches. Processes inside planetary ball mills are complex and strongly depend on the processed material and synthesis and, thus, the optimum milling conditions have to be assessed for each individual system. The present review focuses on the insight into several parameters like properties of grinding balls, the filling ratio or revolution speed. It gives examples of the aspects of grinding and illustrates some general guidelines to follow for modelling processes in planetary ball mills in terms of refinement, synthesis' yield and contamination from wear. The amount of energy transferred from the milling tools to the powder is significant and hardly measurable for processes in planetary ball mills. Thus numerical simulations based on a discrete-element-method are used to describe the energy transfer to give an adequate description of the process by correlation with experiments. The simulations illustrate the effect of the geometry of planetary ball mills on the energy entry. In addition the imaging of motion patterns inside a planetary ball mill from simulations and video recordings is shown.

Lithium‐ion battery (LIB) manufacturing requires a pilot stage that optimizes its characteristics. However, this process is costly and time‐consuming. One way to overcome this is to use a set of computational models that act as a digital twin of the pilot line, exchanging information in real‐time that can be compared with measurements to correct parameters. Here we discuss the parameters involved in each step of LIB manufacturing, show available computational modeling approaches, and discuss details about practical implementation in terms of software. Then, we analyze these parameters regarding their criticality for modeling set‐up and validation, measurement accuracy, and rapidity. Presenting this in an understandable format allows identifying missing aspects, remaining challenges, and opportunities for the emergence of pilot lines integrating digital twins. Finally, we present the challenges of managing the data produced by these models. As a snapshot of the state‐of‐the‐art, this work is an initial step towards digitalizing battery manufacturing pilot lines, paving the way toward autonomous optimization.

The synthesis of sulfide solid electrolytes in ball mills by mechanochemical routes not only is efficient but also can enable the upscaling of material synthesis as required for the commercialization of solid-state battery materials. On a laboratory scale, the Emax high energy ball mill accounts for high stresses and power densities, as well as for temperature control, to prevent damage to the material and equipment even for long process times. To overcome the merely phenomenological treatment, we characterized the milling process in an Emax by DEM simulations, using the sulfide solid electrolyte LPS as a model material for the calibration of input parameters to the DEM, and compared it to a planetary ball mill for a selected parameter set. We derived mechanistic model equations for the stressing conditions depending on the operation parameters of rotational speed, media size and filling ratio. The stressing conditions are of importance as they determine the outcome of the mechanochemical milling process, thus forming the basis for evaluating and interpreting experiments and for establishing scaling rules for the process transfer to larger mills.

To achieve the commercialization of solid‐state‐batteries (SSBs), solid electrolyte properties need to be further improved. The hybrid solid electrolyte (HSE) approach is expected to combine the favorable properties of different solid electrolyte classes and is therefore systematically investigated. Mixing low amounts of thiophosphate or oxide filler particles (FP) into a polyethylene oxide (PEO) polyethylene glycol (PEG) and lithium salt bis(trifluoromethane)sulfonimide (LiTFSI) matrix cannot improve the electrochemical properties. Silanization of the thiophosphate FPs significantly increases the ionic conductivity to 0.1 mS cm⁻¹ at room temperature compared to 0.017 mS cm⁻¹ for a pure PEO solid electrolyte. Moreover, a correlation between the intrinsic conductivity of the FPs and the resulting conductivity of the HSE is observed. Also, the functionalization is successfully transferred to oxide FPs. In addition to an equally significant increase in ionic conductivity, a strong influence of the crystallite size of the FPs on the resulting ionic conductivity of the HSE was found. The discovered effect of FP surface structure on overall HSE conductivity indicates a participation of the FP surface in ion transport and emphasizes the need for tailored filler design in HSE applications.