Recycling Strategies for Ceramic All-Solid-State Batteries—Part I: Study on Possible Treatments in Contrast to Li-Ion Battery Recycling

Abstract

In the coming years, the demand for safe electrical energy storage devices with high energy density will increase drastically due to the electrification of the transportation sector and the need for stationary storage for renewable energies. Advanced battery concepts like all-solid-state batteries (ASBs) are considered one of the most promising candidates for future energy storage technologies. They offer several advantages over conventional Lithium-Ion Batteries (LIBs), especially with regard to stability, safety, and energy density. Hardly any recycling studies have been conducted, yet, but such examinations will play an important role when considering raw materials supply, sustainability of battery systems, CO2 footprint, and general strive towards a circular economy. Although different methods for recycling LIBs are already available, the transferability to ASBs is not straightforward due to differences in used materials and fabrication technologies, even if the chemistry does not change (e.g., Li-intercalation cathodes). Challenges in terms of the ceramic nature of the cell components and thus the necessity for specific recycling strategies are investigated here for the first time. As a major result, a recycling route based on inert shredding, a subsequent thermal treatment, and a sorting step is suggested, and transferring the extracted black mass to a dedicated hydrometallurgical recycling process is proposed. The hydrometallurgical approach is split into two scenarios differing in terms of solubility of the ASB-battery components. Hence, developing a full recycling concept is reached by this study, which will be experimentally examined in future research.

Towards Recycling of LLZO Solid Electrolyte Exemplarily Performed on LFP/LLZO/LTO Cells**

“…However, most of the studies about recycling of LIBs are devoted to conventional liquid‐based electrolyte LIBs, while little attention has been paid to recycling of new emerging ASS‐LIBs. [7] Among these, the recycling of sulfide‐based ASS‐LIBs (e. g., Li|Li 6 PS 5 Cl|LiCoO 2 ) [8] and oxide‐based ASS‐LIBs such as LLZO (Li 7 La 3 Zr 2 O 12 ) [9] have been reported.…”

“…Theoretically, recycling of LLZO by a hydrometallurgical approach appears simple: the garnet‐type LLZO is somehow dissolved, then different elements will be extracted upon alkali precipitation at different pH levels, and finally Li could be recovered by a substitution reaction (e. g., using Na 2 CO 3 to substitute Na and Li and form Li 2 CO 3 ) at sufficiently high pH levels. [9] However, from a practical point of view, it is not as simple as it seems: First of all, apart from the solid electrolyte, a full cell of an ASS‐LIB contains cathode material, anode material, binder, an electron conductor such as graphite and current collectors. This makes the system highly complex.…”

Environmentally Friendly Recovery of Lithium from Lithium–Sulfur Batteries

“…Hereby, the transferability and robustness of a recycling procedure to another battery system with metallic lithium anodes is possible. In this context, direct shredding was examined for lithium-sulfur batteries too, since lithiumion batteries can also be directly shredded after an electric discharge [41]. However, the lithium-sulfur cells ignited during shredding and the thermally untreated black mass from lithium-sulfur batteries ignited during H 2 O leaching.…”

Transitioning solid-state batteries from lab to market: Linking electro-chemo-mechanics with practical considerations

“…As LIB recycling efforts are often made more difficult by the liquid electrolyte, solid-state cells may offer advantages, but only very few studies have approached this topic to date. 80,81 As has been demonstrated, the performance of SSBs is highly dependent on both the mechanical and electrochemical properties of its components. Therefore, the battery operating conditions, the manufacturing processes for each component, and the design of the battery pack, will all have major impacts on the viability of the technology.…”