Since the current volumes of collected end-of-life lithium ion batteries (LIBs) are low, one option to increase the feasibility of their recycling is to feed them to existing metals production processes. This work presents a novel approach to integrate froth flotation as a mechanical treatment to optimize the recovery of valuable metals from LIB scrap and minimize their loss in the nickel slag cleaning process. Additionally, the conventional reducing agent in slag cleaning, namely coke, is replaced with graphite contained in the LIB waste flotation products. Using proper conditioning procedures, froth flotation was able to recover up to 81.3% Co in active materials from a Cu-Al rich feed stream. A selected froth product was used as feed for nickel slag cleaning process, and the recovery of metals from a slag (80%)–froth fraction (20%) mixture was investigated in an inert atmosphere at 1350 °C and 1400 °C at varying reduction times. The experimental conditions in combination with the graphite allowed for a very rapid reduction. After 5 min reduction time, the valuable metals Co, Ni, and Cu were found to be distributed to the iron rich metal alloy, while the remaining fraction of Mn and Al present in the froth fraction was deported in the slag.

Innovative recycling routes are needed to fulfill the increasing demand for battery raw materials to ensure sufficiency in the future. The integration of battery scrap recycling and nickel slag cleaning by reduction with methane was experimentally researched for the first time in this study. Industrial nickel slag from the direct Outotec nickel flash smelting (DON) process was mixed with both synthetic and industrial battery scrap. The end products of the slag-scrap mixtures after reduction at 1400 °C in a CH4 (5 vol %)-N2 atmosphere were an Ni–Co–Cu–Fe metal alloy and FeOx–SiO2 slag. It was noted that a higher initial amount of cobalt in the feed mixture increased the recovery of cobalt to the metal alloy. Increasing the reduction time decreased the fraction of sulfur in the metal alloy and magnetite in the slag. After reduction, manganese was deported in the slag and most of the zinc volatilized. This study confirmed the possibility of replacing coke with methane as a non-fossil reductant in nickel slag cleaning on a laboratory scale, and the recovery of battery metals cobalt and nickel in the slag cleaning process with good yields.

One possible way of recovering metals from spent lithium-ion batteries is to integrate the recycling with already existing metallurgical processes. This study continues our effort on integrating froth flotation and nickel-slag cleaning process for metal recovery from spent batteries (SBs), using anodic graphite as the main reductant. The SBs used in this study was a froth fraction from flotation of industrially prepared black mass. The effect of different ratios of Ni-slag to SBs on the time-dependent phase formation and metal behavior was investigated. The possible influence of graphite and sulfur contents in the system on the metal alloy/matte formation was described. The trace element (Co, Cu, Ni, and Mn) concentrations in the slag were analyzed using the laser ablation-inductively coupled plasma-mass spectrometry (LA-ICP-MS) technique. The distribution coefficients of cobalt and nickel between the metallic or sulfidic phase (metal alloy/matte) and the coexisting slag increased with the increasing amount of SBs in the starting mixture. However, with the increasing concentrations of graphite in the starting mixture (from 0.99 wt.% to 3.97 wt.%), the Fe concentration in both metal alloy and matte also increased (from 29 wt.% to 68 wt.% and from 7 wt.% to 49 wt.%, respectively), which may be challenging if further hydrometallurgical treatment is expected. Therefore, the composition of metal alloy/matte must be adjusted depending on the further steps for metal recovery.

Demand for nickel and cobalt sulfate is expected to increase due to the rapidly growing Li-battery industry needed for the electrification of automobiles. This has led to an increase in the production of sodium sulfate as a waste effluent that needs to be processed to meet discharge guidelines. Using bipolar membrane electrodialysis (BPED), acids and bases can be effectively produced from corresponding salts found in these waste effluents. However, the efficiency and environmental sustainability of the overall BPED process depends upon several factors, including the properties of the ion exchange membranes employed, effluent type, and temperature which affects the viscosity and conductivity of feed effluent, and the overpotentials. This work focuses on the recycling of Na2SO4 rich waste effluent, through a feed and bleed BPED process. A high ion-exchange capacity and ionic conductivity with excellent stability up to 41 °C is observed during the proposed BPED process, with this temperature increase also leading to improved current efficiency. Five and ten repeating units were tested to determine the effect on BPED stack performance, as well as the effect of temperature and current density on the stack voltage and current efficiency. Furthermore, the concentration and maximum purity (>96.5%) of the products were determined. Using the experimental data, both the capital expense (CAPEX) and operating expense (OPEX) for a theoretical plant capacity of 100 m3 h−1 of Na2SO4 at 110 g L−1 was calculated, yielding CAPEX values of 20 M EUR, and OPEX at 14.2 M EUR/year with a payback time of 11 years, however, the payback time is sensitive to chemical and electricity prices.

In this study, industrial lithium-ion battery (LIB) waste was treated by a froth flotation process, which allowed selective separation of electrode particles from metallic-rich fractions containing Cu and Al. In the flotation experiments, recovery rates of ~80 and 98.8% for the cathode active elements (Co, Ni, Mn) and graphite were achieved, respectively. The recovered metals from the flotation fraction were subsequently used in high-temperature Cu-slag reduction. In this manner, the possibility of using metallothermic reduction for Cu-slag reduction using Al-wires from LIB waste as the main reductant was studied. The behavior of valuable (Cu, Ni, Co, Li) and hazardous metals (Zn, As, Sb, Pb), as a function of time as well as the influence of Cu-slag-to-spent battery (SB) ratio, were investigated. The results showcase a suitable process to recover copper from spent batteries and industrial Cu-slag. Cu-concentration decreased to approximately 0.3 wt.% after 60 min reduction time in all samples where Cu/Al-rich LIB waste fraction was added. It was also showed that aluminothermic reduction is effective for removing hazardous metals from the slag. The proposed process is also capable of recovering Cu, Co, and Ni from both Cu-slag and LIB waste, resulting in a secondary Cu slag that can be used in various applications.