Batteries reuse and direct production of high performances cathodic and anodic materials and other raw materials from batteries recycling using low cost and environmentally friendly technologies

Project Information

RHINOCEROS

Grant agreement ID: 101069685

DOI

10.3030/101069685

EC signature date 10 June 2022

Start date 1 September 2022

End date 31 August 2026

Funded under

• Climate, Energy and Mobility

Total cost

€ 8 943 026,25

EU contribution

€ 8 943 025,75

Coordinated by

FUNDACION TECNALIA RESEARCH & INNOVATION
Spain

Periodic Reporting for period 2 - RHINOCEROS (Batteries reuse and direct production of high performances cathodic and anodic materials and other raw materials from batteries recycling using low cost and environmentally friendly technologies)

Reporting period: 2024-03-01 to 2025-08-31

Summary of the context and overall objectives of the project

There is an urgent need for battery materials in Europe. Li-ion batteries (LIBs) have proven to be a reliable solution, especially for the production of batteries for EVs, followed by stationary storage market and consumer electronics. By 2030, the global demand for LIBs is estimated to increase 14 times and the EU could account for 17%, and the battery production in EU is expected to rise to 300 GWh/year.

According to an estimation from the Strategic research Agenda for batteries, the annual production of LIB will require high amounts of CRMs and Europe is currently dependent on imports to produce LIBs. Moreover, the extraction process of such materials usually comes with an environmental impact. In 2020 the Strategic Research Agenda for batteries released the EU Commission’s vision for 2030, which places Europe as the first recycler of LIB raw materials.
The development of closed loops in CRMs is required to secure their supply for the EU battery market. It currently depends on imports for LIBs production, EU needs innovative technologies that will recycle not only CRMs, but also all cell components.

RHINOCEROS aims at developing, improving and demonstrating, in an industrially relevant environment, an economically and environmentally viable route for re-using, re-purposing, re-conditioning and recycling of EoL EVs and stationary batteries. RHINOCEROS will first develop a smart sorting and dismantling system enabling automated classification and dismantling of LIBs and reassembly of still working modules in new repurposed batteries for second life applications. When direct reuse of batteries is not possible, a circular recycling route of materials present in LIBs will be followed closing materials loops. This route targets the pre-treatment, refining and the recovery of recycled materials.Through qualification by industrial end-users, RHINOCEROS will demonstrate the direct production of high performances cathodic and anodic materials and other raw materials at competitive costs from battery recycling.

Work performed from the beginning of the project to the end of the period covered by the report and main results achieved so far

On the automated sorting and dismantling, the robotic system adaptation is finished. A digital twin placed validated three operational scenarios that tested the reinforcement learning capacities with an autonomous congnitive agent. In parallel, the robotic system validation is an on-going work.

Concerning the mechanical pre-treatment of BM, a high purity BM was achieved using sieving and drying steps. The thermal pre-treatment process was also optimized recovering >95% of active materials and studied the impact of discharging and impurities on the recycling process. Supercritical CO2 treatment recovers electrolyte from mechanical BM with >90% yield. scCO2 technology recovered high purity (>95%) binder using a co-solvent system. A combination of scCO2 and ultrasonic washing recovered separator (PE/PP) with purities >98%. The ball milling with reducing agents achieved full metallization of the black mass and obtained Li-water-soluble salts, that were recovered as battery grade lithium carbonate after leaching. The integrated pre-treatment routes were defined with the validated technologies for each pre-treatment line (thermal and mechanical)

Potentioshthatic delithiation achieved recovery of Li as battery grade lithium hydroxide. The Hummer’s method produced rGO and LMR cathode materials with improved performance compared to commercial ones. The solvometallurgical process achieved its targets for extraction and recovery; apart from demonstrating system reusability. GDEx also achieved the recovery of CRMs with reduced power consumption for the systems tested. PIM membranes were developed and applied to secondary waste streams. An electrodialysis system for the recovery of remanent Li in secondary streams as carboante achieved >70% Li2CO3 precipitation with >94% purity. A pilot process flowsheet based on the solvometallurgical DES-based system route applied to the thermal BM was selected to be further scaled up. The basic engineering for scaling up has been defined.

The LCA and LCC were performed for all set of individual technologies in the project. It was also performed to all process flowsheet candidates wto reinforce the selection of the extraction process to be scaled up.

Progress beyond the state of the art and expected potential impact (including the socio-economic impact and the wider societal implications of the project so far)

The cognitive agent developed for robotic battery dismantling achieved an integration with a digital disassembly knowledge base, optimized to cut time and energy and going beyond the state of the art's reported efficiency for dismantling.

Mechanical pre-treatment was optimized via improved sieving combined with a drying process obtaining a high quality BM. Solvent distillation in the thermal BM process is demonstrated, recovering high purity EMC. sCO2 has proven versatile and effective to recover the electrolyte from BM without the use of further chemicals with selectivity towards its components. Also, it is able to recover the separator with high yield and >98% purity after washing. The scCO2 used with a co-solvent also recovers >60% of the PVDF binder with >98%.

The reductive reactive milling with followed by leaching of the water-soluble lithium phases recovers battery grade lithium carboante after recrystallization. Potentiostatic delithiation offers promising results and further steps in its research phase are required with regards of contamination of the obtained lithium hydroxide. The Hummer’s method approach demonstrated its capability for the synthesis of battery grade GO anode from black mass with proven high-performing working cathodic and anodic materials obtained. The solvometallurgical process applied to mechanical black mass yields very promising results in both extraction efficiency and purity of the obtained material, and further work in the DES recycling would be beneficial to benchmark with the current regeneration procedures. On another hand, this process applied to thermal black mass also yields positive results on extraction and purity while using different reducing agents than the analogous system applied to the mechanical black mass. PIMs were validated for secondary waste streams, both real and synthetic, showing good Mn and Li recovery, in real leachates, with low energy consumption and fast extraction.

The electrified membrane process was validated for Li extraction from DES black mass leachates achieving >70% Lithium extraction followed by a carbonation process that recovered >70% Li2CO3. On this last process, further work is still needed despite its promising results to enhance transfer efficiency from the waste leachate to the electrolyte that receives the extracted lithium.

Concept Diagram of the RHINOCEROS Process developed by TEC to be scaled up in JGI-HM facilities

Methodology of RHINOCEROS, a general depiction of the WPs and their responsibles