As the field of all-solid-state battery (ASSB) cells rapidly develops, both from the perspective of new materials as well as processing and cell assembly methods, the necessity for standardized benchmarking protocols that enable interlaboratory comparability increases. At an academic level there are no well-established nor unified protocols for quantifying ASSB cell performance. The latter is in larger part due to the lack of standardized cell setups, processing and cycling parameters among the groups, sometimes limited by accessibility to similar equipment.To evaluate the interlaboratory reproducibility of ASSB cell performance, we coordinated and report on a Round Robin study that involves 21 experienced groups* across Asia, Europe, and North America. We provided state-of-the-art, commercially-sourced battery materials, namely single crystal LiNi0.6Mn0.2Co0.2O2, (NMC-622) positive electroactive material (CAM), a thiophosphate-based (Li6PS5Cl) solid electrolyte (SE), and indium foil for the preparation of an In/(InLi) x alloy negative electrode. All groups were asked to assemble three ASSB cells with the provided materials at specified CAM- and SE-loadings as well as to use the same electrochemical cycling procedure. Moreover, all groups were asked to provide detailed information on their cell assembly protocols and results, including (but not limited to) applied pressures to prepare the battery electrodes, cell dimensions, weighed amounts of materials, and raw electrochemical data.Massive differences were observed in the specific discharge capacities, which initially ranged from 23.7 to 143.1 mAh⋅g-1, and showed large variabilities in capacity retention (ranging from 0 to 107%). This result is not surprising considering that each group reports its own materials’ processing and cell assembly protocol in which different uniaxial pressures, compression times and cycling (stack) pressures are applied. Although challenging to correlate differences in cycling performance to a single parameter, we identified the initial open circuit voltage, the initial polarization and the cycling pressure as main contributors. We report that 43% of the attempted cells failed. This was mainly due to issues during cell assembly but also due to errors during cycling, suggesting that lab scale ASSB research is challenging and error prone. These problems may have a negative impact on reproducibility if they are not detected during assembly. Considering all the obtained results, we emphasize that triplicate cell data should always be reported by all groups. Due to the large available dataset, we identify important parameters that, if reported, would help improve the interlaboratory reproducibility and comparability of ASSB cell cycling data.*The total number of researchers involved in this study is 108, representing 26 institutions and will be duly acknowledged in the presentation. Due to space limitations, they are not included in the abstract.
Read full abstract