Browsing by Author "Jacob, Martine"

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    Recycling of all‐solid‐state Li‐ion batteries : a case study of the separation of individual components within a system composed of LTO, LLZTO and NMC
    (2023) Waidha, Aamir Iqbal; Salihovic, Amila; Jacob, Martine; Vanita, Vanita; Aktekin, Burak; Brix, Kristina; Wissel, Kerstin; Kautenburger, Ralf; Janek, Jürgen; Ensinger, Wolfgang; Clemens, Oliver
    With the current global projection of over 130 million electric vehicles (EVs), there soon will be a need for battery waste management. Especially for all‐solid‐state lithium‐ion batteries (lithium ASSBs), aspects of waste management and circular economy have not been addressed so far. Within such ASSBs, the use of solid‐electrolytes like garnet‐type Li6.5La3Zr1.5Ta0.5O12 (LLZTO) may shift focus on strategies to recover not only the transition metal elements but also elements like La/Zr/Ta. In this work, we present a two‐step recycling approach using citric acid as the leaching agent to separate and recover the individual components of a model cell comprising of Li4Ti5O12 (LTO) anode, Li6.5La3Zr1.5Ta0.5O12 (LLZTO) garnet electrolyte and LiNi1/3Mn1/3Co1/3O2 (NMC) cathode. We observe that by adjusting the concentration of citric acid, it was possible to separate the materials from each other without strong mixing of individual phases and also to maintain their principle performance characteristics. Thus, the process developed has a potential for upscaling and can guide towards considering separation capability of battery components in the development of lithium ASSBs.
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    Towards recycling of all‐solid‐state batteries with argyrodite sulfide electrolytes : insights into electrolyte and electrode degradation in dissolution‐based separation processes
    (2025) Wissel, Kerstin; Hu, Zian; Wu, Xuebin; Jacob, Martine; Küster, Kathrin; Starke, Ulrich; Clemens, Oliver
    All‐solid‐state Li‐ion batteries (ASSBs) represent a promising leap forward in battery technology, rapidly advancing in development. Among the various solid electrolytes, argyrodite thiophosphates Li6PS5X (X=Cl, Br, I) stand out due to their high ionic conductivity, structural flexibility, and compatibility with a range of electrode materials, making them ideal candidates for efficient and scalable battery applications. However, despite significant performance advancements, the sustainability and recycling of ASSBs remain underexplored, posing a critical challenge for achieving efficient circular processes. This study investigates the dissolution‐based separation and recovery of argyrodite thiophosphate electrolytes and transition metal oxide electrode materials as a potential recycling strategy for ASSBs. A focus is set on the impact of solvent treatments on the recrystallization behavior of these electrolytes. Furthermore, the interactions between dissolved argyrodite thiophosphates and various transition metal oxide electrode materials (LiCoO2, LiMn2O4, LiNi0.8Mn0.1Co0.1O2, LiFePO4 and Li4Ti5O12) is examined to assess their influence on the functional properties of both the electrolytes and electrode materials. Structural, compositional and morphological changes are analyzed using X‐ray diffraction, scanning electron microscopy, energy‐dispersive X‐ray spectroscopy, inductively coupled plasma mass spectrometry and X‐ray photoelectron spectroscopy. Our findings provide insights into the complexities of recycling ASSBs, but also highlight the potential for developing efficient, sustainable recycling processes.
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    Towards recycling of LLZO solid electrolyte exemplarily performed on LFP/LLZO/LTO cells
    (2022) Ali Nowroozi, Mohammad; Iqbal Waidha, Aamir; Jacob, Martine; Aken, Peter A. van; Predel, Felicitas; Ensinger, Wolfgang; Clemens, Oliver
    All‐solid‐state lithium ion batteries (ASS‐LIBs) are promising due to their safety and higher energy density as compared to that of conventional LIBs. Over the next few decades, tremendous amounts of spent ASS‐LIBs will reach the end of their cycle life and would require recycling in order to address the waste management issue along with reduced exploitation of rare elements. So far, only very limited studies have been conducted on recycling of ASS‐LIBS. Herein, we investigate the recycling of the Li7La3Zr2O12 (LLZO) solid‐state electrolyte in a LiFePO4/LLZO/Li4Ti5O12 system using a hydrometallurgical approach. Our results show that different concentration of the leaching solutions can significantly influence the final product of the recycling process. However, it was possible to recover relatively pure La2O3 and ZrO2 to re‐synthesize the cubic LLZO phase, whose high purity was confirmed by XRD measurements.