Abstract
The successful implementation of solid state batteries not only requires the use of high-capacity anodes, but also high-performance composite cathodes. However, the production of solid state battery cathode composites with optimized microstructures remains a significant challenge, especially for large-scale fabrication. Here, we present a scalable high-intensity dry mixing process to create tailored functional coatings on single-crystalline LiNi0.82Mn0.07Co0.11O2 via mechanofusion. We investigate the coating of LiNi0.82Mn0.07Co0.11O2 with the malleable halide solid electrolyte Li3InCl6 under various process conditions, linking process parameters obtained from discrete element method simulations with experimentally accessible morphological properties to offer guidelines for further optimization. In this way nanometer-thin covering coatings as well as thick matrix coatings are successfully produced. Incorporating carbon black into the thick matrix coating results in well-performing mixed conducting matrices that can be used directly as composite cathodes without further treatment. The compositions investigated enable stable cycling with a specific capacity of up to qcomp = 100 mAh g−1 (based on the total mass of the composite cathode) at a C-rate of 1 C (60 min). While higher carbon black content is observed to improve CAM utilization, excessive amounts are detrimental for cell kinetics and chemo-mechanics, emphasizing the importance of the cathode mixing process and composition on overall cell performance.
Data availability
The source data used for all figures in this study are provided in the Source data File, which has been deposited, together with additional data, in Zenodo at https://doi.org/10.5281/zenodo.18493074.
References
Janek, J. & Zeier, W. G. A solid future for battery development. Nat. Energy 1, 16141 (2016).
Bates, A. M. et al. Are solid-state batteries safer than lithium-ion batteries? Joule 6, 742–755 (2022).
Wang, R., Cui, W., Chu, F. & Wu, F. Lithium metal anodes: present and future. J. Energy Chem. 48, 145–159 (2020).
Huang, W.-Z. et al. Anode-free solid-state lithium batteries: a review. Adv. Energy Mater. 12, 2201044 (2022).
Song, A. et al. A review on the features and progress of silicon anodes-based solid-state batteries. Adv. Energy Mater. 13, 2301464 (2023).
Janek, J. & Zeier, W. G. Challenges in speeding up solid-state battery development. Nat. Energy 8, 230–240 (2023).
Minnmann, P. et al. Designing cathodes and cathode active materials for solid-state batteries. Adv. Energy Mater. 12, 2201425 (2022).
Dixit, M. B. et al. Understanding implications of cathode architecture on energy density of solid-state batteries. Energy Storage Mater. 40, 239–249 (2021).
Han, Y. et al. Single- or poly-crystalline Ni-rich layered cathode, sulfide or halide solid electrolyte: Which will be the winners for all-solid-state batteries? Adv. Energy Mater. 11, 2100126 (2021).
Kamaya, N. et al. A lithium superionic conductor. Nat. Mater. 10, 682–686 (2011).
Kuhn, A. et al. A new ultrafast superionic Li-conductor: ion dynamics in Li11Si2PS12 and comparison with other tetragonal LGPS-type electrolytes. Phys. Chem. Chem. Phys. 16, 14669–14674 (2014).
Wang, Z.-Y. et al. Achieving high-energy and high-safety lithium metal batteries with high-voltage-stable solid electrolytes. Matter 6, 1096–1124 (2023).
Liu, J., Wang, S., Qie, Y. & Sun, Q. Identifying lithium fluorides for promising solid-state electrolyte and coating material of high-voltage cathode. Mater. Today Energy 21, 100719 (2021).
Dai, T. et al. Inorganic glass electrolytes with polymer-like viscoelasticity. Nat. Energy 8, 1221–1228 (2023).
Grube, M. et al. Solvent-free and scalable mechanochemical synthesis of high-performance sulfide solid electrolytes. J. Energy Storage 121, 116593 (2025).
Jo, Y.-S. et al. Engineering green and sustainable solvents for scalable wet synthesis of sulfide electrolytes in high-energy-density all-solid-state batteries. Green. Chem. 25, 1473–1487 (2023).
Kimura, Y. et al. Coating layer design principles considering lithium chemical potential distribution within solid electrolytes of solid-state batteries. Commun. Mater. 5, 1–13 (2024).
Nakamura, T., Amezawa, K., Kulisch, J., Zeier, W. G. & Janek, J. Guidelines for all-solid-state battery design and electrode buffer layers based on chemical potential profile calculation. ACS Appl. Mater. Interfaces 11, 19968–19976 (2019).
Ruess, R. et al. Single-Crystalline LiNiO2 as High-Capacity Cathode Active Material for Solid-State Lithium-Ion Batteries. J. Electrochem. Soc. 170, 20533 (2023).
Wang, L. et al. High-energy all-solid-state lithium batteries enabled by Co-free LiNiO2 cathodes with robust outside-in structures. Nat. Nanotechnol. 19, 208–218 (2024).
Dai, Y. et al. Exploring of the upper limit of nickel content in cathode materials for PEO-based solid-state batteries. Chin. Chem. Lett. 111157, https://doi.org/10.1016/j.cclet.2025.111157 (2025).
Strauss, F. et al. Rational design of quasi-zero-strain NCM cathode materials for minimizing volume change effects in all-solid-state batteries. ACS Mater. Lett. 2, 84–88 (2020).
Liu, C., Roters, F. & Raabe, D. Role of grain-level chemo-mechanics in composite cathode degradation of solid-state lithium batteries. Nat. Commun. 15, 7970 (2024).
Koerver, R. et al. Chemo-mechanical expansion of lithium electrode materials—on the route to mechanically optimized all-solid-state batteries. Energy Environ. Sci. 11, 2142–2158 (2018).
Ryu, H.-H. et al. Microstrain alleviation in high-energy Ni-rich NCMA cathode for long battery life. ACS Energy Lett. 6, 216–223 (2021).
Kondrakov, A. O. et al. Anisotropic lattice strain and mechanical degradation of high- and low-nickel NCM cathode materials for Li-ion batteries. J. Phys. Chem. C 121, 3286–3294 (2017).
Conforto, G. et al. Editors’ Choice—quantification of the impact of chemo-mechanical degradation on the performance and cycling stability of NCM-based cathodes in solid-state Li-ion batteries. J. Electrochem. Soc. 168, 70546 (2021).
Payandeh, S., Goonetilleke, D., Bianchini, M., Janek, J. & Brezesinski, T. Single versus poly-crystalline layered oxide cathode materials for solid-state battery applications—a short review article. Curr. Opin. Electrochem. 31, 100877 (2022).
Ruess, R. et al. Influence of NCM particle cracking on kinetics of lithium-ion batteries with liquid or solid electrolyte. J. Electrochem. Soc. 167, 100532 (2020).
Trevisanello, E., Ruess, R., Conforto, G., Richter, F. H. & Janek, J. Polycrystalline and single crystalline NCM cathode materials—quantifying particle cracking, active surface area, and lithium diffusion. Adv. Energy Mater. 11, 2003400 (2021).
Bielefeld, A., Weber, D. A. & Janek, J. Microstructural modeling of composite cathodes for all-solid-state batteries. J. Phys. Chem. C 123, 1626–1634 (2019).
Bielefeld, A., Weber, D. A., Rueß, R., Glavas, V. & Janek, J. Influence of lithium ion kinetics, particle morphology and voids on the electrochemical performance of composite cathodes for all-solid-state batteries. J. Electrochem. Soc. 169, 20539 (2022).
Minnmann, P. et al. Editors’ Choice—visualizing the impact of the composite cathode microstructure and porosity on solid-state battery performance. J. Electrochem. Soc. 171, 60514 (2024).
Kissel, M. et al. Quantifying the impact of cathode composite mixing quality on active mass utilization and reproducibility of solid-state battery cells. Adv. Energy Mater. 15, 2405405 (2025).
Minnmann, P., Quillman, L., Burkhardt, S., Richter, F. H. & Janek, J. Editors’ Choice—quantifying the impact of charge transport bottlenecks in composite cathodes of all-solid-state batteries. J. Electrochem. Soc. 168, 40537 (2021).
Hendriks, T. A., Lange, M. A., Kiens, E. M., Baeumer, C. & Zeier, W. G. Balancing partial ionic and electronic transport for optimized cathode utilization of high-voltage LiMn2O4/Li3InCl6 solid-state batteries. Batter. Supercaps 6, e202200544 (2023).
Kaiser, N. et al. Ion transport limitations in all-solid-state lithium battery electrodes containing a sulfide-based electrolyte. J. Power Sources 396, 175–181 (2018).
Bielefeld, A., Weber, D. A. & Janek, J. Modeling effective ionic conductivity and binder influence in composite cathodes for all-solid-state batteries. ACS Appl. Mater. Interfaces 12, 12821–12833 (2020).
Kim, J. et al. High-performance all-solid-state batteries enabled by intimate interfacial contact between the cathode and sulfide-based solid electrolytes. Adv. Funct. Mater. 33, 2211355 (2023).
Lee, D. et al. Shear force effect of the dry process on cathode contact coverage in all-solid-state batteries. Nat. Commun. 15, 4763 (2024).
Schnell, J. et al. All-solid-state lithium-ion and lithium metal batteries—paving the way to large-scale production. J. Power Sources 382, 160–175 (2018).
Batzer, M., Gundlach, D., Michalowski, P. & Kwade, A. Scalable production of separator and cathode suspensions via extrusion for sulfidic solid-state batteries. ChemElectroChem 10, e202300452 (2023).
Frankenberg, F. et al. Investigating the production of all-solid-state battery composite cathodes by numerical simulation of the stressing conditions in a high-intensity mixer. Powder Technol. 435, 119403 (2024).
Noh, S., Nichols, W. T., Cho, M. & Shin, D. Importance of mixing protocol for enhanced performance of composite cathodes in all-solid-state batteries using sulfide solid electrolyte. J. Electroceram 40, 293–299 (2018).
Titscher, P., Götz von Olenhusen, A., Arlt, T., Manke, I. & Kwade, A. Evaluation of a high-intensive mixing process in a ring shear mixer and its impact on the properties of composite particles for lithium–sulfur battery cathodes. Energy Technol. 7, 1801059 (2019).
Helmers, L. et al. Sustainable solvent-free production and resulting performance of polymer electrolyte-based all-solid-state battery electrodes. Energy Technol. 9, 2000923 (2021).
Fernandez-Diaz, L. et al. Mixing methods for solid state electrodes: techniques, fundamentals, recent advances, and perspectives. Chem. Eng. J. 464, 142469 (2023).
Puls, S. et al. Benchmarking the reproducibility of all-solid-state battery cell performance. Nat Energy 9, 1310–1320 (2024).
Maus, O. et al. Influence of post-synthesis processing on the structure, transport, and performance of the solid electrolyte Li5.5PS4.5Cl1.5 in all-solid-state batteries. Adv. Energy Mater. 15, 2403291 (2025).
Schlautmann, E. et al. Graded cathode design for enhanced performance of sulfide-based solid-state batteries. ACS Energy Lett. 10, 1664–1670 (2025).
Schlautmann, E. et al. Impact of the solid electrolyte particle size distribution in sulfide-based solid-state battery composites. Adv. Energy Mater. 13, 2302309 (2023).
Shi, T. et al. High active material loading in all-solid-state battery electrode via particle size optimization. Adv. Energy Mater. 10, 1902881 (2020).
König, C., Miß, V., Janin, L. & Roling, B. Mitigating the ion transport tortuosity in composite cathodes of all-solid-state batteries by wet milling of the solid electrolyte particles. ACS Appl. Energy Mater. 6, 9356–9362 (2023).
Park, C. et al. Electrochemical properties of composite cathode using bimodal sized electrolyte for all-solid-state batteries. J. Electrochem. Soc. 166, A5318–A5322 (2019).
Ruhl, J., Riegger, L. M., Ghidiu, M. & Zeier, W. G. Impact of solvent treatment of the superionic argyrodite Li6PS5Cl on solid-state battery performance. Adv. Energy Sustain. Res. 2, 2000077 (2021).
Wang, Y. et al. Mechanical milling-induced microstructure changes in argyrodite LPSCl solid-state electrolyte critically affect electrochemical stability. Adv. Energy Mater. 14, 2304530 (2024).
Choi, Y. E. et al. Coatable Li4SnS4 solid electrolytes prepared from aqueous solutions for all-solid-state lithium-ion batteries. ChemSusChem 10, 2605–2611 (2017).
Kim, D. H. et al. Infiltration of solution-processable solid electrolytes into conventional Li-ion-battery electrodes for all-solid-state Li-ion batteries. Nano Lett. 17, 3013–3020 (2017).
Lee, W. et al. Advanced parametrization for the production of high-energy solid-state lithium pouch cells containing polymer electrolytes. Nat. Commun. 15, 5860 (2024).
Kawaguchi, T., Nakamura, H. & Watano, S. Dry coating of electrode particle with model particle of sulfide solid electrolytes for all-solid-state secondary battery. Powder Technol. 323, 581–587 (2018).
Kawaguchi, T., Nakamura, H. & Watano, S. Parametric study of dry coating process of electrode particle with model material of sulfide solid electrolytes for all-solid-state battery. Powder Technol. 305, 241–249 (2017).
Hayakawa, E., Nakamura, H., Ohsaki, S. & Watano, S. Dry mixing of cathode composite powder for all-solid-state batteries using a high-shear mixer. Adv. Powder Technol. 33, 103705 (2022).
Hayakawa, E., Nakamura, H., Ohsaki, S. & Watano, S. Design of active-material/solid-electrolyte composite particles with conductive additives for all-solid-state lithium-ion batteries. J. Power Sources 555, 232379 (2023).
Friebel, J. M., Ditscherlein, R., Ditscherlein, L. & Peuker, U. A. Three-dimensional characterization of dry particle coating structures originating from the mechano-fusion process. Microsc. Microanal. 30, 179–191 (2024).
Jin, F. et al. Elucidating the impact of Li3InCl6-coated LiNi0.8Co0.15Al0.05O2 on the electro-chemo-mechanics of Li6PS5Cl-based solid-state batteries. Chem. Mater. 36, 6017–6026 (2024).
Kissel, M. et al. Engineering the artificial cathode-electrolyte interphase coating for solid-state batteries via tailored annealing. Chem. Mater. 37, 2192–2203 (2025).
Kim, J. S. et al. Synergistic halide-sulfide hybrid solid electrolytes for Ni-rich cathodes design guided by digital twin for all-solid-State Li batteries. Energy Storage Mater. 55, 193–204 (2023).
Tanno, K. Current status of the mechanofusion process for producing composite particles. KONA Powder Part. J. 8, 74–82 (1990).
Kwade, A. A stressing model for the description and optimization of grinding processes. Chem. Eng. Technol. 26, 199–205 (2003).
Burmeister, C. F. & Kwade, A. Process engineering with planetary ball mills. Chem. Soc. Rev. 42, 7660–7667 (2013).
Schlem, R. et al. Energy storage materials for solid-state batteries: design by mechanochemistry. Adv. Energy Mater. 11, 2101022 (2021).
Burmeister, C. F., Hofer, M., Molaiyan, P., Michalowski, P. & Kwade, A. Characterization of stressing conditions in a high energy ball mill by discrete element simulations. Processes 10, 692 (2022).
Zheng, L., Wei, C., Garayt, M. D. L., MacInnis, J. & Obrovac, M. N. Spherically smooth cathode particles by mechanofusion processing. J. Electrochem. Soc. 166, A2924–A2927 (2019).
Rumpf, H. C. H. Zur Theorie der Zugfestigkeit von Agglomeraten bei Kraftübertragung an Kontaktpunkten. Chem. Ing. Tech. 42, 538–540 (1970).
Tavares, L. & King, R. Single-particle fracture under impact loading. Int. J. Miner. Process. 54, 1–28 (1998).
Frankenberg, F. et al. Tailoring composite microstructure through milling for dry-processed sulfide-based solid-state battery cathodes. Small 21, e07279 (2025).
Reisacher, E., Kaya, P. & Knoblauch, V. Percolation behavior of a sulfide electrolyte–carbon additive matrix for composite cathodes in all-solid-state batteries. Batteries 9, 595 (2023).
Puls, S., Ketter, L., Zeier, W. G. & Vargas-Barbosa, N. M. Opportunities and limitations of partial transport quantification in all-solid-state composite electrodes. ACS Electrochem. 1, 2432–2447 (2025).
Yanev, S. et al. Rapid determination of all-solid-state battery performance via chronoamperometry. J. Electrochem. Soc. 169, 90519 (2022).
Wang, C. et al. Interface-assisted in-situ growth of halide electrolytes eliminating interfacial challenges of all-inorganic solid-state batteries. Nano Energy 76, 105015 (2020).
Ma, T. et al. In-situ cathode coating for all-solid-state batteries by freeze-drying technology. Nano Energy 124, 109522 (2024).
Mayer, J. K. et al. Investigation of moisture content, structural and electrochemical properties of nickel-rich NCM based cathodes processed at ambient atmosphere. J. Electrochem. Soc. 169, 60512 (2022).
Lechner, M., Wölfl, S., Kurz, E. & Daub, R. Identification of critical moisture exposure for nickel-rich cathode active materials in lithium-ion battery production. J. Power Sources 626, 235661 (2025).
Zhang, L. et al. Elucidating the humidity-induced degradation of Ni-rich layered cathodes for Li-ion batteries. ACS Appl. Mater. Interfaces 14, 13240–13249 (2022).
Li, X. et al. Water-mediated synthesis of a superionic halide solid electrolyte. Angew. Chem. 131, 16579–16584 (2019).
Zhang, Z. et al. One-step solution process toward formation of Li6PS5Cl argyrodite solid electrolyte for all-solid-state lithium-ion batteries. J. Alloys Compd. 812, 152103 (2020).
Nikodimos, Y., Huang, C. J., Taklu, B. W., Su, W. N. & Hwang, B. J. Chemical stability of sulfide solid-state electrolytes: stability toward humid air and compatibility with solvents and binders. Energy Environ. Sci. 15, 991–1033 (2022).
Park, K. H. et al. Design strategies, practical considerations, and new solution processes of sulfide solid electrolytes for all-solid-state batteries. Adv. Energy Mater. 8, 1800035 (2018).
Emley, B. et al. On the quality of tape-cast thin films of sulfide electrolytes for solid-state batteries. Mater. Today Phys. 18, 100397 (2021).
Nikodimos, Y. et al. Unveiling the chemical stability and solvent compatibility of halide solid-state electrolytes: insights from isothermal calorimetric titration and synchrotron spectroscopy. Chem. Mater. 37, 7622–7634 (2025).
Wang, C. et al. A universal wet-chemistry synthesis of solid-state halide electrolytes for all-solid-state lithium-metal batteries. Sci. Adv. 7, eabh1896 (2021).
Hofer, M. et al. Effective mechanochemical synthesis of sulfide solid electrolyte Li3PS4 in a high energy ball mill by process investigation. Adv. Powder Technol. 34, 104004 (2023).
Mayer, J. K. et al. Influence of the carbon black dispersing process on the microstructure and performance of Li-ion battery cathodes. Energy Technol. 8, 1900161 (2020).
Weber, M., Mayer, J. K. & Kwade, A. The Carbon Black Dispersion Index DI CB: a novel approach describing the dispersion progress of carbon black containing battery slurries. Energy Technol. 11, 2201299 (2023).
Bockholt, H., Haselrieder, W. & Kwade, A. Intensive powder mixing for dry dispersing of carbon black and its relevance for lithium-ion battery cathodes. Powder Technol. 297, 266–274 (2016).
Zhang, W. et al. Interfacial processes and influence of composite cathode microstructure controlling the performance of all-solid-state lithium batteries. ACS Appl. Mater. Interfaces 9, 17835–17845 (2017).
Rosenbach, C. et al. Visualizing the chemical incompatibility of halide and sulfide-based electrolytes in solid-state batteries. Adv. Energy Mater. 13, 2203673 (2022).
Acknowledgements
M.K., F.F., J.J., and A.K. acknowledge financial support by Deutsche Forschungsgemeinschaft (DFG, German Research Foundation) through the priority program 2289 (project 462470125) and by BMFTR through the projects 03XP0430A, 03XP0430C (FestBatt Cluster of Competence, FB2-Thio) and 03XP0590D (FoFeBat). Language and grammar of the manuscript have partially been improved with the help of DeepL Write and ChatGPT4.0 (by OpenAI).
Funding
Open Access funding enabled and organized by Projekt DEAL.
Author information
Authors and Affiliations
Contributions
M.K. and F.F. contributed equally to this work. M.K., F.F., A.K., and J.J. conceived the project. M.K. and F.F. designed and coordinated the experiments. F.F. prepared the mixtures with the help of N.L., measured the porosities, carried out DEM simulations of the mixing process and analyzed the data. M.K. carried out the electrochemical investigations with help of A.L., measured and analyzed the EDX-SEM and XPS data. T.D. carried out the STEM-EDX and TEM investigations. D.W. analyzed the XRD data. M.K. and F.F. wrote the first version of the manuscript which was edited by all authors.
Corresponding authors
Ethics declarations
Competing interests
The authors declare no competing interests.
Peer review
Peer review information
Nature Communications thanks Bohua Wen and the other, anonymous, reviewer(s) for their contribution to the peer review of this work. A peer review file is available.
Additional information
Publisher’s note Springer Nature remains neutral with regard to jurisdictional claims in published maps and institutional affiliations.
Supplementary information
Rights and permissions
Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons licence, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons licence, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons licence and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this licence, visit http://creativecommons.org/licenses/by/4.0/.
About this article
Cite this article
Kissel, M., Frankenberg, F., Demuth, T. et al. Mechanofusion-derived cathode composite microstructures with scalable mixed conducting matrix coatings for solid state batteries. Nat Commun (2026). https://doi.org/10.1038/s41467-026-71305-2
Received:
Accepted:
Published:
DOI: https://doi.org/10.1038/s41467-026-71305-2