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Journal of Environmental Management
journal homepage: www.elsevier.com/locate/jenvman
Research article
Optimization of metals extraction from spent lithium-ion batteries by
sulphuric acid and sodium metabisulphite through a techno-economic
evaluation
Nathália Vieceli
a,*
, Carlos A. Nogueira
b
, Manuel F.C. Pereira
c
, Fernando O. Durão
c
,
Carlos Guimarães
c
, Fernanda Margarido
a
a
Center for Innovation, Technology and Policy Research – IN+, Instituto Superior Técnico, University of Lisbon, 1049-001, Lisboa, Portugal
b
LNEG - Laboratório Nacional de Energia e Geologia, I.P., Campus do Lumiar, 1649-038, Lisboa, Portugal
c
CERENA – Centro de Recursos Naturais e Ambiente, Instituto Superior Técnico, University of Lisbon, 1049-001, Lisboa, Portugal
ARTICLE INFO
Keywords:
Lithium-ion batteries
Economic evaluation
Optimization
Acid leaching
ABSTRACT
The main factors that affect the extraction of metals from spent lithium-ion batteries by acid leaching using
H
2
SO
4
, and sodium metabisulphite, were evaluated and optimized through a set of experiments, framed by a
techno-economic approach.
The maximum value of the profit response was obtained with the highest possible values of acid con-
centration (2.5 M) and time (2 h), a liquid/solid ratio of 5 L/kg, and the lowest possible value of temperature
(40 °C). After leaching, the electrodes active material contained in the metals decreased, while it was still sig-
nificant in the graphite, as observed by scanning electron microscopy-energy dispersive spectrometry and x-ray
powder diffraction. Even though the performed economic evaluation was a summarized outline it can be con-
sidered suitable to compare different leaching conditions and to determine the possible best combinations of
factors that can optimize the profit response.
1. Introduction
Disposed electrical and electronic equipment (WEEE) is one of the
fastest growing waste-management problems worldwide. Within the
European Union (EU) represents 3–5% of the total waste produced
every year (European Commission, 2017). In 2014, 11.6 Mt of WEEE
were generated in Europe, corresponding to 15.6 kg/inhabitant (Baldé
et al., 2015).
The high energy density of lithium-ion batteries (LIBs), associated
with other properties, boosted their use on the market of portable
electronic devices such as mobile phones, laptops, MP3s and others, as
well as in electric vehicles, amounting to billions the number of LIBs
units produced every year, thus increasing their wasting (Zeng and Li,
2014; Scrosati and Garche, 2010).
A LIB cell includes two electrodes (positive and negative), a se-
parator, an electrolyte and a steel can. The negative electrode consists
of a Cu foil coated with graphite, while the positive electrode consists of
an Al foil coated with a Li-transition metal mixed oxide, such as LiCoO
2
,
LiMn
2
O
4
, or LiNiO
2
. Graphite and the mixed oxide are overlaid on the
foils using a polymer binder, such as polyvinylidene fluoride (PVDF).
The electrolyte is normally a lithium salt, LiPF
6
, LiBF
4
, LiClO
4
, or LiSO
2
,
dissolved in an organic solvent (a mixture of several alkyl carbonates).
The separator is made of microporous polypropylene (PP) (Al-Thyabat
et al., 2013). Alternative materials for Li-based batteries have been
studied and a remarkable recent development is the all-solid-state re-
chargeable Na or Li battery developed by Braga et al. (2017). This is a
noncombustible device with a long life span, fast rates of charge/dis-
charge, and higher energy density than conventional lithium-ion bat-
teries (The University of Texas at Austin and UT News, 2017).
For several years, LiCoO
2
has been the most common LIBs active
cathode material. Due to some drawbacks such as its high cost and
cobalt toxicity, LiCoO
2
has been partially replaced by LiMn
2
O
4
and Li
(Mn,Ni,Co)O
2
, particularly in high energy/power applications. As such,
active cathode materials in LIBs can contain a variable concentration of
Co, Ni, and Mn, making their recovery more complex (Chen et al.,
2011), and more unreliable the attribution of a recycling value (Waste
Management World, 2011).
Even though in theory LIBs could be totally recycled with an effi-
ciency rate above 90% using hydrometallurgical processes, a pyr-
ometallurgical procedure is generally applied, with Li being lost in the
https://doi.org/10.1016/j.jenvman.2018.08.085
Received 25 January 2018; Received in revised form 12 July 2018; Accepted 23 August 2018
*
Corresponding author.
E-mail address: nathalia.vieceli@tecnico.ulisboa.pt (N. Vieceli).
Journal of Environmental Management 228 (2018) 140–148
0301-4797/ © 2018 Elsevier Ltd. All rights reserved.
T