Abstract

In the upcoming years, todaýs e-mobility will challenge the capacity of sustainable recycling. Due to the presence of organic components (electrolyte, separator, casings, etc.), future recycling technologies will combine thermal pre-treatment followed by hydrometallurgical processing. Despite the ongoing application of such treatment, there is still a lack of information on how applied parameters affect subsequent metal recovery. In this study, both oxidative and reductive conditions in dependence on temperature and time were studied. Qualitative and quantitative characterizations of the samples after treatment were performed followed by leaching with 2 M sulphuric acid at ambient temperature to determine the leachability of valuable metals such as Co, Mn, Ni and Li. Moreover, the negative or positive effect of treatment on the leachability of the main impurities (Cu and Al) was determined. Since the presence of carbon affects the degree of active material reduction, it's content after each thermal treatment was determined as well. If all variables, temperature and time of thermal processing are taken into account, pyrolysis at 700 °C for 30 min is the optimal treatment. Under these conditions, full recovery is reached after 2 min for Li, 5 min for Mn and 10 min for both Co and Ni. In the case of the incineration, only processing at 400 and 500 °C promoted higher recovery of metals, while the treatment at 600 and 700 °C led to the formation of less leachable species.

Highlights

  • Modern processing of spent lithium-ion batteries (LiBs) applies combined methods to achieve higher material recovery

  • Leaching yield increased from 10% to over 70% after the incineration at 400 ◦C

  • Incineration re­ duces the feasibility of carbothermic reduction of Co, Mn and Ni oxides into more soluble oxides or even into their metallic forms, which are easier to leach

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Summary

Introduction

Modern processing of spent lithium-ion batteries (LiBs) applies combined methods to achieve higher material recovery. The presence of some reducing agent like H2O2 requires a lower acid concentration in the leaching media to yield the same concentration of lithium and cobalt in the leaching liquor (Porvali et al, 2020). This is because of the reduction of Co3+ to Co2+, which can be readily dissolved (Lee and Rhee, 2003). The effect of such thermal treat­ ments on the impurities (Cu and Al) is barely reported, but their removal causes significant losses of valuable metals If their presence in the leachate can be eliminated by proper thermal pretreatment, it brings remarkable simplification of the processing as well as environmental impact. The effect of the thermal treatment can be more precisely defined

Materials and methods
Thermal pre-treatment
Leaching
Samples analysis
Material characterization
Thermodynamic considerations for leaching process
Leaching of untreated samples
Leaching of incinerated samples
Leaching of the impurities after incineration
Leaching of pyrolyzed samples
Leaching of the impurities after pyrolysis
Comparison between incineration and pyrolysis
Conclusions

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