Periodic Reporting for period 2 - ROCHE (“Multilayer approach for solid-state batteries” - (ROCHE))
Berichtszeitraum: 2024-09-01 bis 2025-08-31
Solid electrolytes represent a significant advancement in battery technology, primarily due to their potential to address the key challenges faced by liquid electrolytes, such as safety risks associated with flammability, leakage, and thermal instability. Additionally, solid electrolytes can improve battery performance by enabling higher energy densities, longer life cycles, and better thermal management. The development of solid-state batteries, which utilize solid electrolytes, is considered one of the most promising approaches to meeting the growing global demand for safe, high-performance, and sustainable energy storage solutions.
ROCHE project will use a novel multilayer approach to fabricate solid-state batteries, in which solid inorganic material will be intercalated with MOFs layers. As novelty, three synergetic approaches of metal-organic frameworks (MOF) will be designed to improve and favour the ionic transport. It is expected that the use of the multilayer approach will increase the mechanical resistance compared to an individual one. Also the synergistic effect of the high ionic conductivity and nanowetted interface between the MOF and the cathode will entail a high-capacity and good dendrite suppression capability, allowing its implementation in next-generation solid-state batteries. The combined database and machine learning approach have been applied to design and predict material properties of electrodes such as voltage, crystallinity and chemical stability, from atomic scale to mesoscale.[5] Bearing this in mind, it can been applied to design new SSEs with fast Li-ion transport and mechanical properties. Providing an opportunity for exploring material properties at a lower cost and accelerating the material discovery processes.
Once aims have been established, the specific scientific objectives of the project are:
(1) The synthesis and optimization of materials with the objective to develop a multi-layer structure of SSEs.
(2) The assembly of SSEs in a battery structure and characterize their behaviour under long-test cycling.
(3) The understanding of the role of interfaces in the ionic transport in order to unravel a possible kinetic mechanism in solid-state batteries.
ROCHE project will use a novel multilayer approach to fabricate solid-state batteries, in which solid inorganic material will be intercalated with MOFs layers. As novelty, three synergetic approaches of metal-organic frameworks (MOF) will be designed to improve and favour the ionic transport. It is expected that the use of the multilayer approach will increase the mechanical resistance compared to an individual one. Also the synergistic effect of the high ionic conductivity and nanowetted interface between the MOF and the cathode will entail a high-capacity and good dendrite suppression capability, allowing its implementation in next-generation solid-state batteries. The combined database and machine learning approach have been applied to design and predict material properties of electrodes such as voltage, crystallinity and chemical stability, from atomic scale to mesoscale.[5] Bearing this in mind, it can been applied to design new SSEs with fast Li-ion transport and mechanical properties. Providing an opportunity for exploring material properties at a lower cost and accelerating the material discovery processes.
Once aims have been established, the specific scientific objectives of the project are:
(1) The synthesis and optimization of materials with the objective to develop a multi-layer structure of SSEs.
(2) The assembly of SSEs in a battery structure and characterize their behaviour under long-test cycling.
(3) The understanding of the role of interfaces in the ionic transport in order to unravel a possible kinetic mechanism in solid-state batteries.
The key objectives include synthesizing new solid electrolyte materials, evaluating their electrochemical performance, and optimizing their integration into next-generation battery systems. We have been particularly focused on two classes of solid electrolytes: three-components materials and organic ionic plastic crystals materials (OIPC). Each of these materials offers distinct advantages and challenges, and our goal has been to explore their properties in-depth to identify the most promising candidates for further development.
In summary, the main and specific objectives outlined in the ROCHE project have been successfully achieved, leading to valuable advancements in the understanding and development of electrolyte systems. Throughout the project, new research directions have also been identified to address the challenges encountered during implementation. These new lines of investigation provide promising opportunities for expanding the current knowledge base and improving the performance of next-generation electrochemical materials.
Although the simulation component did not yield the level of insight initially anticipated, it nonetheless contributed important progress toward understanding the interfacial behavior of ionic liquid electrolytes. The findings, while preliminary, have clarified several key aspects of ion transport and structural organization at the interface, offering a foundation for refining future simulation methodologies. Moreover, these results have opened possibilities for applying similar analytical frameworks to the study of quasi-solid electrolytes, where interfacial effects play an equally critical role.
Papers
- J.C. Barbosa, A. Fidalgo-Marijuan, J.C. Dias, R. Gonçalves, M. Salado, C.M. Costa, S. Lanceros-Méndez. Molecular design of functional polymers for organic radical batteries. Energy Storage Materials, Volume 60, June 2023, 102841
- Manuel Salado, Marco Amores, Cristina Pozo-Gonzalo, Maria Forsyth, Senentxu Lanceros-Méndez. Advanced and sustainable functional materials for potassium-ion Batteries. Energy Mater 2023;3:300037
- M. Salado, R. Fernández de Luis, T. H. Smith, M. Hasanpoor, S. Lanceros-Mendez, M. Forsyth. Dimensionality Control of Li Transport by MOFs Based Quasi-Solid to Solid Electrolyte (Q-SSEs) for Li−Metal Batteries.
-Carlos M Costa, Manuel Salado, Chiara Ferrara, et al. “The wide range of battery systems: From micro-to structural batteries, from biodegradable to high performance batteries” Progress in Materials Science, (2025)
-Manuel Salado, Mega Kar, Senentxu Lanceros‐Mendez, Maria Forsyth. “Progress and Perspective of Metal–Organic Frameworks as Solid Electrolyte Interphase Instability Mitigator in Magnesium Batteries”. Batteries & Supercaps 2500136.
-Manuel Salado, Thomas H. Smith, Nanditha Sirigiri, Fangfang Chen, Luke A. O’Dell, Jennifer M. Pringle and Maria Forsyth. “Ammonium-Based Plastic Crystals as Solid-State Electrolytes for Lithium and Sodium Batteries” JACS Au 2025, 5, 4, 1663–1676.
-Lixu Huang, Mahin Maleki, Manuel Salado, et al. “Interphase design from ionic liquid cation mixtures and multi-mode surface analysis for safe and stable Na metal batteries” EES Batteries, 2025,1, 853-866.
Conferences
- Oral presentation: 38th Australasian Polymer Symposium. “Dimensionality Control of Li Transport by MOFs Based Quasi-Solid to Solid Electrolyte (Q-SSEs)”
- Invited Oral presentation: TMS25. “Dimensionality Control of Li Transport by MOFs Based Quasi-Solid to Solid Electrolyte (Q-SSEs)”
- Oral presentation: 247th ECS Meeting “Solid-State Ammonium Based Electrolytes for Lithium and Sodium Batteries”
- Oral presentation: 6th ICEnSM “Solid-State Ammonium Based Electrolytes for Lithium and Sodium Batteries”
In summary, the main and specific objectives outlined in the ROCHE project have been successfully achieved, leading to valuable advancements in the understanding and development of electrolyte systems. Throughout the project, new research directions have also been identified to address the challenges encountered during implementation. These new lines of investigation provide promising opportunities for expanding the current knowledge base and improving the performance of next-generation electrochemical materials.
Although the simulation component did not yield the level of insight initially anticipated, it nonetheless contributed important progress toward understanding the interfacial behavior of ionic liquid electrolytes. The findings, while preliminary, have clarified several key aspects of ion transport and structural organization at the interface, offering a foundation for refining future simulation methodologies. Moreover, these results have opened possibilities for applying similar analytical frameworks to the study of quasi-solid electrolytes, where interfacial effects play an equally critical role.
Papers
- J.C. Barbosa, A. Fidalgo-Marijuan, J.C. Dias, R. Gonçalves, M. Salado, C.M. Costa, S. Lanceros-Méndez. Molecular design of functional polymers for organic radical batteries. Energy Storage Materials, Volume 60, June 2023, 102841
- Manuel Salado, Marco Amores, Cristina Pozo-Gonzalo, Maria Forsyth, Senentxu Lanceros-Méndez. Advanced and sustainable functional materials for potassium-ion Batteries. Energy Mater 2023;3:300037
- M. Salado, R. Fernández de Luis, T. H. Smith, M. Hasanpoor, S. Lanceros-Mendez, M. Forsyth. Dimensionality Control of Li Transport by MOFs Based Quasi-Solid to Solid Electrolyte (Q-SSEs) for Li−Metal Batteries.
-Carlos M Costa, Manuel Salado, Chiara Ferrara, et al. “The wide range of battery systems: From micro-to structural batteries, from biodegradable to high performance batteries” Progress in Materials Science, (2025)
-Manuel Salado, Mega Kar, Senentxu Lanceros‐Mendez, Maria Forsyth. “Progress and Perspective of Metal–Organic Frameworks as Solid Electrolyte Interphase Instability Mitigator in Magnesium Batteries”. Batteries & Supercaps 2500136.
-Manuel Salado, Thomas H. Smith, Nanditha Sirigiri, Fangfang Chen, Luke A. O’Dell, Jennifer M. Pringle and Maria Forsyth. “Ammonium-Based Plastic Crystals as Solid-State Electrolytes for Lithium and Sodium Batteries” JACS Au 2025, 5, 4, 1663–1676.
-Lixu Huang, Mahin Maleki, Manuel Salado, et al. “Interphase design from ionic liquid cation mixtures and multi-mode surface analysis for safe and stable Na metal batteries” EES Batteries, 2025,1, 853-866.
Conferences
- Oral presentation: 38th Australasian Polymer Symposium. “Dimensionality Control of Li Transport by MOFs Based Quasi-Solid to Solid Electrolyte (Q-SSEs)”
- Invited Oral presentation: TMS25. “Dimensionality Control of Li Transport by MOFs Based Quasi-Solid to Solid Electrolyte (Q-SSEs)”
- Oral presentation: 247th ECS Meeting “Solid-State Ammonium Based Electrolytes for Lithium and Sodium Batteries”
- Oral presentation: 6th ICEnSM “Solid-State Ammonium Based Electrolytes for Lithium and Sodium Batteries”
• Design easy-scalable solid-electrolytes: Considering the knowledge obtained during this period, the idea is to design electrolytes for use in larger battery systems, with the goal of testing in real-world applications by Q2 2025.
• Further Interface Studies: Conduct additional research on electrolyte-electrode interfaces to optimize contact and reduce resistance in metal-based systems.
• Simulation of electrolyte material: Modelling and simulations play an important role in understanding materials compositions and designing batteries. The optimal composition and nanostructure will be determined by the use of density functional theory (DFT) meanwhile the full battery behaviour will be simulated by finite element method (FE) modelling.
• Industrial Collaboration: Explore opportunities for collaboration with battery manufacturers to test solid electrolytes in commercial-scale applications.
• Further Interface Studies: Conduct additional research on electrolyte-electrode interfaces to optimize contact and reduce resistance in metal-based systems.
• Simulation of electrolyte material: Modelling and simulations play an important role in understanding materials compositions and designing batteries. The optimal composition and nanostructure will be determined by the use of density functional theory (DFT) meanwhile the full battery behaviour will be simulated by finite element method (FE) modelling.
• Industrial Collaboration: Explore opportunities for collaboration with battery manufacturers to test solid electrolytes in commercial-scale applications.