Periodic Reporting for period 1 - OPERA (DEVELOPMENT OF OPERANDO TECHNIQUES AND MULTISCALE MODELLING TO FACE THE ZERO-EXCESS SOLID-STATE BATTERY CHALLENGE)
Reporting period: 2023-06-01 to 2024-11-30
Green, high-performing and safe batteries based on abundant materials are a key element in the transition to a carbonneutral future. However, to accelerate their development, a deep understanding of the complex electro-chemo-mechanical processes within the battery is required, which is only accessible through advanced experimental and computational methods. Zero-excess solid-state batteries, where the anode is formed in situ, have emerged as a promising new generation of environmentally friendly batteries with high energy density, improved safety and higher cost-efficiency, but only after solutions for non-uniform anode formation were found. In OPERA, seven leading research institutions, two synchrotron radiation facilities, a small-medium sized enterprise and a large technological company, all from complementary research fields such as batteries, surface and material science, and multiscale modelling, propose a unique strategy to face the current challenges of this technology. OPERA relies on the development of novel operando experimental techniques at the ESRF, ALBA and DESY synchrotrons and at the lab-scale, providing complementary information on multiaxial stress fields, chemical composition, nucleation and growth kinetics, structural defect formation and degradation of well-defined model cells with a resolution down to the atomic scale. The new insights and collected multiparameter data will be incorporated into a novel multiscale modelling approach supported by machine learning algorithms. This will ultimately lead to a conceptual understanding of the in-situ anode formation and, based on this, innovative improvement approaches to enable this type of energy storage technology, which will be an important step towards increasing the global competitiveness, resilience and independence of the EU.
Our main objective is to develop new methodologies that allow the experimental observation and further conceptual understanding to finally tailor the growth mechanisms involved in the Li anode formation in ZESSBs.
Our main objective is to develop new methodologies that allow the experimental observation and further conceptual understanding to finally tailor the growth mechanisms involved in the Li anode formation in ZESSBs.
During the project, the deposition of Li and Na is investigated by advanced electrochemical and operando techniques as well as by using modelling approaches. The main focus is on the use of single-crystal and polycrystalline Li₆.₅La₃Zr₁.₅Ta₀.₅O₁2 (LLZTO) samples as separator for ZESSB, in case of Na, NaRSiO (R = Sm or Gd) samples are used. To meet the requirements of several advanced operando characterization techniques, the samples are prepared and shaped in the required geometries, as well as produced as single layer thin film electrolytes.
Furthermore, two types of novel versatile stages for operando studies under (a) bending and (b) compressive loads are being developed. These hermetically sealed operando stages, built for different synchrotons, are suitable for applying stacking or bending loads through piezo drivers (up to 100 MPa), allowing for specialized electrochemical and polarization measurements.
Advanced electrochemical characterization of Li deposition is performed in a solid-state Hull cell, to investigate the morphology of Li deposition as a function of applied current and stack pressure.
Operando electrochemical dilatometry and nucleation studies using ultra-fast transient methods are used to further understand Li deposition and growth behavior. These methods are combined with post-mortem SEM analysis.
Advanced characterization methods developed and performed are operando TEM, in situ and operando AFM, spatially resolved optical spectroscopies, CSnanoXRD and DFXM, HAXPES and PEEM. These methods are used to characterize morphology and stress development during Li deposition at the Li-LLZTO interface as well as deepening the understanding of Li deposition using lithiophilic interphases.
Next to advanced characterization, comprehensive modelling approaches are used to simulate the dendrite growth at the Li-SE interface and deposition Li behavior on different CC and interlayer materials. While first principle calculations were performed to support the screening for possible metals as interlayer materials, the AI assisted multiscale modelling framework is still under development.
Lastly, a reference full cell set-up is designed consisting of an LFP/PEO-cathode, LLZTO separator and Cu-CC. The full cell serves to validate findings from modelling and characterization approaches. Optimization strategies based on the findings of the project are implemented and tested by using the reference cell as a starting point.
Furthermore, two types of novel versatile stages for operando studies under (a) bending and (b) compressive loads are being developed. These hermetically sealed operando stages, built for different synchrotons, are suitable for applying stacking or bending loads through piezo drivers (up to 100 MPa), allowing for specialized electrochemical and polarization measurements.
Advanced electrochemical characterization of Li deposition is performed in a solid-state Hull cell, to investigate the morphology of Li deposition as a function of applied current and stack pressure.
Operando electrochemical dilatometry and nucleation studies using ultra-fast transient methods are used to further understand Li deposition and growth behavior. These methods are combined with post-mortem SEM analysis.
Advanced characterization methods developed and performed are operando TEM, in situ and operando AFM, spatially resolved optical spectroscopies, CSnanoXRD and DFXM, HAXPES and PEEM. These methods are used to characterize morphology and stress development during Li deposition at the Li-LLZTO interface as well as deepening the understanding of Li deposition using lithiophilic interphases.
Next to advanced characterization, comprehensive modelling approaches are used to simulate the dendrite growth at the Li-SE interface and deposition Li behavior on different CC and interlayer materials. While first principle calculations were performed to support the screening for possible metals as interlayer materials, the AI assisted multiscale modelling framework is still under development.
Lastly, a reference full cell set-up is designed consisting of an LFP/PEO-cathode, LLZTO separator and Cu-CC. The full cell serves to validate findings from modelling and characterization approaches. Optimization strategies based on the findings of the project are implemented and tested by using the reference cell as a starting point.
Two high index papers were already published in journals "Small" and "Nature Communications" that present great results beyond state of the art.
The results will be updated during the second half of the project.
The results will be updated during the second half of the project.