Recyclability assessment and design for recycling recommendations of end-of-life NMC811 lithium-ion batteries

Improving the recyclability of lithium-ion batteries (LIBs) is a key requirement for closing material cycles, reducing dependence on primary resource extraction and enabling the recovery of critical elements such as lithium, nickel, cobalt and manganese. This case study addresses that challenge directly by providing quantitative design for recycling (DfR) recommendations for NMC811 LIBs, grounded in a rigorous process model developed within the HydroLiBRec project. The methodology integrates empirical analytical measurements with thermodynamic simulation (FactSage 8.2 and HSC Chemistry 10.3.7.1) to trace material and substance flows through the complete recycling chain: manual dismantling, mechanical and metallurgical processing of end-of-life NMC811 cells. Separated cells constituted 63.7 percent of total battery pack weight. The process yields an overall mass-weighted recyclability index of 59.4 percent across all elements, with a specific lithium recovery of 59.7 percent, under current design conditions. Critically, the study demonstrates that targeted modifications to battery design, including dismountable casings, water-dispersible binders and fluorine-free electrolytes, combined with process-level adaptations such as a delamination step and froth flotation, are projected to raise the recyclability index from 59 percent to 90 percent while reducing global warming potential by up to 19 percent. The main takeaway for industry and policymakers is that recyclability is not just about processing methods — it is largely decided during the design stage. Applied in practice, these DfR recommendations provide battery manufacturers with a concrete, simulation-backed roadmap to design cells that are inherently easier and more efficient to recycle, thereby reducing dependence on primary mining, lowering the environmental footprint of the battery supply chain and supporting the transition toward a circular economy for LIBs. Background LIBs are central to the global energy transition, particularly in applications such as electric vehicles and large-scale energy storage systems. Demand is expected to increase between 2030 and 2050, which will intensify the need for critical raw materials (CRMs), especially lithium, cobalt, nickel and manganese used in cathode materials such as nickel manganese cobalt (NMC), nickel cobalt aluminum (NCA) and lithium cobalt oxide (LCO). The supply of these materials is geographically concentrated, with lithium production largely occurring in Chile, Argentina and Australia; cobalt production dominated by the Democratic Republic of the Congo; and nickel processing strongly associated with China and Indonesia. This concentration raises concerns about long-term availability and price stability. As a result, the recycling of end-of-life LIBs has become increasingly important, not only as a supply strategy but also as a way to reduce environmental impacts. Life cycle assessment (LCA) is widely used to evaluate the environmental performance of different recycling pathways, including their greenhouse-gas emissions relative to conventional mining and refining. In parallel, DfR has gained attention as a strategy that considers end-of-life treatment during the product design stage. By influencing factors such as disassembly, material separation and recovery efficiency, DfR directly affects the environmental outcomes captured in LCA studies. Methodology Bosch Power Tube 500 e-bike battery packs (500 Wh, 2.9 kg) were used as input material. Manual dismantling separated the pack into its main fractions, yielding 40 LG CHEM ING18650MJ1 round cells containing NMC811 active material (63.7 weight percent), which were used as feedstock for the recycling process. Fig. 1 Block flow diagram of recovery of lithium salt from LiB (NMC811). As shown in Fig.1, the process consisted of manual, mechanical and metallurgical processing stages. Mechanical processing included blade cutting to weaken the casing, followed by electrohydraulic fragmentation at 40 kV, and 1.5 Hz in water to delaminate the multistructure material.Skimming and sieving then separated materials by density and size, producing black mass enriched in lithium, nickel, cobalt and manganese. Metallurgical treatment involved pyrolysis at 500 °C under inert atmosphere to remove organic components, followed by hydrometallurgical processing. Formic acid leaching at 70 °C dissolved lithium and partially extracted other metals. Copper was recovered by cementation, and precipitation using calcium hydroxide (Ca(OH)2) and ammonia (NH3) enabled the production of lithium-containing products. The process was modeled and simulated with FactSage and HSC Chemistry, assuming thermodynamic equilibrium conditions. Based on these results, a gate-to-gate LCA was conducted using the EF 3.0 method with Ecoinvent v3.8 data. DfR was evaluated using a product-centric approach, with the recyclability index calculated from element-specific recovery rates. Results and discussion As illustrated in Fig. 2, the Sankey diagram shows the distribution of material flows across the different stages of the recycling process, leading to the recovery of lithium salt from NMC811 LIBs.The recycling index is a crucial metric for assessing the effectiveness of recycling, both for products and their constituent materials. Derived by calculating individual elemental recovery rates relative to total weight, this index (Fig. 3) offers a granular evaluation of sustainability impact. These results reinforce the necessity of shifting toward a product-centric recycling strategy. Fig. 2 Quantitative flow analysis of NMC811 battery recycling via Sankey visualization. The DfR assessment confirms that recycling performance is strongly dependent on material compatibility and product design. The applied process is product-specific for NMC811, and the metal wheel analysis shows that processing anode and cathode materials together leads to unavoidable losses. Fig. 3 Recycling efficiency label for NMC 811 battery cell. DfR analysis indicates that although the investigated cell design follows sustainability criteria, several design modifications can significantly improve recycling performance. A dismountable casing enables direct processing of the electrode assembly during pyrolysis, facilitating access to critical components and reducing environmental impacts, with reductions of 17 percent in global warming potential, 14 percent in acidification, 26 percent in human toxicity and 13 percent in eutrophication. Binder selection also plays a key role, as conventional polyvinylidene fluoride (PVDF) limits material separation; replacing it with water-dispersible alternatives such as carboxymethyl cellulose (CMC) or styrene-butadiene rubber (SBR) improves liberation and recovery. Similarly, fluorine-containing electrolytes increase process complexity and reagent demand, and their elimination reduces environmental impacts, including a 19 percent reduction in global warming potential and up to 27 percent in human toxicity. Process-related improvements further enhance recovery efficiency. Specifically, the integration of a delamination step prior to metallurgical treatment prevents contamination of hydrometallurgical streams by copper and aluminum, increasing the recyclability index from 59 percent to 71 percent.To prevent further contamination from anode dissolution and dendrite formation, cells must be properly pre-discharged using salt solutions. Finally, implementing froth flotation for active material separation, alongside these design modifications, further drives the recyclability index upward. Conclusion The present study shows that integrating DfR, thermodynamic simulation and LCA provides a framework for assessing LIB recyclability. The investigated process achieves a recyclability index of 59.4 percent, with potential improvement to 90 percent through combined design and process modifications. Ultimately, recyclability is largely determined at the design stage, requiring closer alignment between battery manufacturers and recyclers. The findings represent idealized theoretical potentials, as the steady-state equilibrium models used here omit kinetic and mass transfer variables. Bridging the gap from these laboratory-scale results to industrial implementation will require addressing inherent challenges in process integration and large-scale operational dynamics. Funding The HydroLiBRec project was funded by the German Ministry of Education and Research (grant number: 03XP0339B). References A list of all references is available in the full paper.

Recyclability assessment and design for recycling recommendations of end-of-life NMC811 lithium-ion batteries

Authored by: Felipe Alejandro Garcia Paz, Christine Nadine Prado Goerlach, Chanchan Li, Monika Keutmann, Tobias Necke, Mohsin Sajjad, Karl Gerald van den Boogaart and Ashak Mahmud Parvez

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