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Battery Recycling Technologies: Recycling Waste Lithium Ion Batteries with the Impact on the Environment In-View

  • Crawford University (2007-2017)

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This survey is to review the advancement recorded so far in the lithium-ion battery recycling technologies in compliance with environmental laws. Amongst many of the technologies used to date, the best is the use of simple but scale-up dissolution technology involving non-toxic suitable organic solvents that can effectively dissolve toxic binder, PVdF in battery to avoid much pollution. Pollution through the hydrolysis of LiPF6 from the lithium-ion battery can also be minimized through conversion to useful compounds instead of using virgin materials for the synthesis. More environmentally friendly recycling technologies are still needed to meet the demands for materials, for scale-up processes and in compliance with environmental laws.
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Journal of Environment and Ecology
ISSN 2157-6092
2013, Vol. 4, No. 1
Battery Recycling Technologies: Recycling Waste
Lithium Ion Batteries with the Impact on the
Environment In-View
Oluwatosin Emmanuel Bankole (Corresponding author)
School of Chemistry and Chemical Engineering, Southeast University, Nanjing 211189,
Department of Chemistry, College of Natural Sciences, Crawford University, P.M.B
2001, Atan-Agbara Road, Ogun State, Nigeria
Chunxia Gong
Lixu Lei
School of Chemistry and Chemical Engineering
Southeast University, Nanjing 211189, China
Received: February 14, 2013 Accepted: March 18, 2012 Published: June 24, 2013
doi:10.5296/jee.v3i1.3257 URL:
This survey is to review the advancement recorded so far in the lithium-ion battery recycling
technologies in compliance with environmental laws. Amongst many of the technologies
used to date, the best is the use of simple but scale-up dissolution technology involving
non-toxic suitable organic solvents that can effectively dissolve toxic binder, PVdF in battery
to avoid much pollution. Pollution through the hydrolysis of LiPF6 from the lithium-ion
battery can also be minimized through conversion to useful compounds instead of using
Journal of Environment and Ecology
ISSN 2157-6092
2013, Vol. 4, No. 1
virgin materials for the synthesis. More environmentally friendly recycling technologies are
still needed to meet the demands for materials, for scale-up processes and in compliance with
environmental laws.
Keywords: Environmental pollution, Waste lithium-ion battery, Recycling, Technologies
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1. Introduction
The environmental pollution caused by the valuable chemical components such as cobalt,
copper, lithium, mixture of organic electrolyte and salts of either low quality or spent
lithium-ion batteries (LiBs) deposited into the environments necessitates responsive recovery
technologies. Since Sony made the first commercial lithium-ion cell in 1991, it has been
accorded more attention being superior to other types of batteries in terms of energy density,
which is a critical parameter for portable electronics as well as hybrid and electric vehicles.
Lithium ion batteries are the systems preferred as electrochemical power sources in portable
batteries segment such as mobile telephones, personal computers, video-cameras and other
modern-life appliances as well as in vehicles with electric drive due to its favorable
characteristics (Contestabile et al., 2001; Gaines, 2011; Nan et al., 2005; Wang et al., 2011).
As LiBs progressively dominate, the amounts of valuable chemical components that will be
deposited will be proportional to the number of LiBs used after their life-span has expired.
Therefore, recycling that constitutes the most generally acceptable environmentally friendly
method of managing these wastes must be taken serious, to minimize environmental toxicity,
for economic gains and reduction in dependence on foreign resources or on virgin materials
for productions in the industry as well as for sustainability of the natural resources
(Contestabile et al., 1999; Dewulf, et al., 2010; Graham-Rowe, 2010; Hitachi, 2011; Kumar,
2011; Wang et al., 2011). The methods could be on the laboratory scale, industrial or
commercial scale level. These as-recovered metals or their respective compounds (cobalt,
lithium, manganese, and nickel) are not only valuable metals but are alternative precursors
for new batteries formulations. Thus, several attempts have been made to review the old
processes considered green and non-green chemistries to either improve on the existing ones
or propose new recovery processes that are considered simple and of industrial-scale (Kondás
et al, 2006; Nan et al., 2005). However, the cells used in cell phones and laptops are not fully
recycled and consequently causing unsustainable open loop in the industrial cycle (Wang et
al., 2011).
Although according to the U.S. government, spent LiBs have been classified as
non-environmentally hazardous wastes or rather call “green batteries” and thus safe for
disposal in the normal municipal waste stream unlike other battery chemistries that contain
Cd, Pb or Hg, the presence of flammable and toxic elements or compounds may make their
safe disposal to become a serious problem. For instance, the mixture of dimethyl carbonate
(DMC) and ethylene carbonate (EC) used as solvent is flammable, while the polyvinylidene
fluoride (PVDF) used as binder irrespective of its percentage in the battery formulation is
toxic when burns consequent to the release of gaseous HF. Besides, the NMP commonly used
as a solvent for the electrode active materials (cathode and anode) fabrication during slurry
preparation has been reported as toxic and therefore environmentally incompatible (Alfonso
et al., 2004; Castillo et al., 2002; Mitchell, 2006; Robert, 2000; Roth and Orendorff, 2012;
Wang et al., 2011). As there is a general saying and belief that “health is wealth”, similarly,
“healthy environment is a wealthy environment”. On the other hand, “polluted environment is
an unhealthy and un-wealthy environment”. Therefore, recycling is of great importance to
save our immediate environment and for waste management sustainability.
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2. Structural Composition of Lithium-Ion Battery
All batteries consist of cathode, anode, electrolyte mixture and separator. The cathode has the
aluminium foils coated with a mixture of the active material, LiCoO2 or LiNi1/3Mn1/3Co1/3O2
depending on the type, PVdF or PTFE, carbon graphite, while the anode is a copper foil
coated with blended slurry of carbon graphite and PVdF or PTFE.
The electrolyte mixture consists of the water-proned electrolyte salt, LiPF6 and organic
solvents dissolved in varying ratios such as 1:1:1 (v/v) for 1M LiPF6, dimethyl carbonate
(DMC) and ethylene carbonate (EC) respectively. In addition, other lithium salts used for
lithium-ion battery are LiAsF6, LiClO4, and LiBF4, while the organic solvents among others
are propylenecarbonate with dimethoxyethane (PC–DME), γ-butyrolactone with
tetrahydrofuran (BL–THF) and dioxolane (1, 3-D) according to Contestabile et al (1999).
The separator is a non-conductor that separates the two electrodes from each other. The
structure of a cylindrical lithium-ion battery according to Nishi (2001) is represented in
Figure 1.
Figure 1. The structure of a cylindrical lithium-ion battery
2.1 The Chemical Reaction of a Typical Lithium-Ion Battery
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Lithium ions move from the negative electrode to the positive electrode during the discharge
process through the nonaqueous electrolyte and separator diaphragm and then undergo
reversible reaction when charging (Figure 2). The ionic chemical reactions are shown in
equations 1-3.
The cathodic half reaction:
LiMO2 Li
1-xMO2 + xLi+ + xe- (1)
The anodic half reaction:
xLi+ + xe- + 6C Li
xC6 (2)
The overall reaction:
LiMO2 + 6C Li
1-xMO2 + LixC6 (3)
Where M reprersents Mn, Ni or Co depending on the cathode active material.
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Figure 2. Schematic diagram of the chemical reaction of a lithium-ion battery
3. Processes for Recovery of Lithium Ion Batteries
According to Xu et al (2008), recycling technologies, irrespective of the processes must
amongst others achieve the reduction in the volume of the scraps or cases, selective
separation of the valuable components. The physical and chemical processes are generally the
two categories of processes employed in the laboratory and industry to recycle all kinds of
3.1 Physical Processes
The physical processes are generally dissolution, manual or mechanical separation and
pyrolysis. For instance, Contestabile et al (1999) and Bankole and Lei (2013) extracted the
electrolyte solution into organic solvents such as ethanol or iso-butylalcohol/water after
manually or mechanical dismantling LiBs and this enhanced reduction in the environmental
pollution caused by the hydrolysis of electrolyte salt, LiPF6 and also the toxic electrolyte
mixture. Interestingly, innovative conversion of LiPF6 to useful compound such as Li2SiF6
was achieved for the first time (Bankole and Lei, 2013).
3.1.1 Hydrometallurgical Process
In hydrometallurgical method, mechanical separation was employed as pretreatment by
subjecting LiBs to skinning, crushing removing of crust, sieving and separation of both anode
and cathode material for easy recovery of the valuable components of the batteries (Xu et al.,
2008; Zhou et al., 2010). However, safety precautions are required due to flammability of the
electrolyte mixture (Roth and Orendorff, 2012). Although the stress in manual separation will
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be reduced, the components of the batteries may not be fully separated from one another due
to the structural arrangement of the LiBs (Xu et al., 2008).
3.1.2 Dissolution Process
This process recently dominates and enhances effectiveness with maximum recovery of
valuable components from batteries. The adhesive force from the PVdF holding the electrode
active materials (anode and cathode) unto the current collectors is weakened. Therefore, the
choice of suitable organic solvents capable of dissolving the binder, PVdF or PTFE becomes
very important during recovery processes. Among these suitable solvents that have already
been tested and found effective are N, N-dimethylformamide (DMF), N, N-dimethyl
acetamide (DMAC), N-methylpyrrolidone (NMP) and dimethylsulfoxide (DMSO) with their
order of effectiveness in dissolving the adhesive investigated. For instance, LiCoO2 was
recovered from LiBs with the solubility of PVdF in the first three solvents recorded as
DMAC > DMF > NMP (Zhou et al., 2010). N-methylpyrrolidone separated both
LiMn1/3Ni1/3Co1/3O2 and LiCoO2, from LiBs at 40 oC for 15 minutes and at 100 C for 1 h,
respectively (Contestabile et al., 2001; Li et al., 2007). Although the powders were
effectively recovered, the cost of buying 1L of NMP which is about $ 207.90 makes its
application not cost-effective and suitable for a large scale recovery operation
(Sigma-Aldrich 2011; Xu et al., 2008). Among all these solvents, DMSO used at 60 ºC for 85
minutes could be the most suitable for its cheapness ($ 144.54/ L), non-toxicity and
environmental safety (MTI Corporation, 2009; Sigma-Aldrich 2011). Moreover, the clean
and shiny current collectors (Aluminium foils) obtained after the separation could be used for
other applications in the laboratory and industries. The flow-sheet for the recycling of LiBs
by dissolution method is shown in Figure 3.
Figure 3. Flow sheet for the recovery of valuable components from LiBs by dissolution
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3.1.3 Pyrolysis or Pyrometallurgical Process
The name comes from the two words “pyro” and “lysis” meaning “fire” and “decomposition”,
respectively. Therefore, this process decomposes the components of the LIBs by heating to
high temperatures under heat and pressure. Pyrometallurgical process has been associated
with high air emission of dioxins, chloride compounds and mercury, and therefore requires
strict standard for air filtration systems to avoid pollution. It was used as pre-treatment for
waste batteries before leaching process, especially to remove Hg, papers and plastics under a
controlled atmosphere (Bernardes et al., 2004; Johnson and Derrick, 2010; Pietrelli et al.,
3.2 Chemical Processes
The chemical processes are mainly hydrometallurgical methods involving acid or base
leaching, solvent extraction, chemical precipitation, bioprocess and electrochemical process
or combination of the processes. The multiple-steps will consume more chemicals.
3.2.1 Hydrometallurgical Processes
The scraps of the spent LiBs were put in either acid or alkaline solution to dissolve the
metallic fraction of the batteries to recover valuable components (Bernardes et al., 2004).
Hydrometallurgical was used on the basis of its simplicity, environmentally friendly due to
waste water and air emission minimization, adequate recovery of valuable metals with high
purity and low energy requirements (Li et al., 2010a, 2010b; Pietrelli et al., 2005). For
instance, cobalt-containing slag was treated through hydrometallurgical process by Lain
(2002) and Espinosa et al (2004).
This process also used the mixture of H2SO4 and H2O2 to recover Li and Co from LiBs and
achieved full recovery of the metals within 10 min at 75 oC with an agitation of 300 rpm.
However, the thermal pretreatment of LiCoO2 particles to remove carbon and organic binder
before chemical leaching significantly reduced the leaching efficiency. Also, LiPF6
decomposed into lithium fluoride and phosphorus pentafluoride during crushing process
(Shin et al., 2005).
Also, with an enhanced leaching efficiency, mixture of an easily degradable organic acid
DL-malic acid and H2O2 was used to recover Co and Li from LiBs (Li et al, 2010a). Instead
of DL-malic acid with H2O2, both Co and Li were effectively recovered using citric acid and
H2O2 (Li et al., 2010b). Kang et al (2010a) leached cobalt-containing powder from LiBs with
H2SO4 and H2O2 to recover cobalt sulfate, while addition of oxalic acid to the filtrate from
another powder produced crystalline cobalt oxalate, which was then heated to produce Co3O4
(Kang et al., 2010b). Zhang et al (1998) recovered Co and Li using HCl solution. The Co in
the leached liquor was selectively extracted with PC-88A in kerosene and then as cobalt
sulfate with high purity, while Li was obtained as LiCO3.
A combination of ultrasonic washing, acid leaching and precipitation was proposed by Li et
al (2009a, 2009b) to recover Co from spent LIBs. The ultrasonic washing improved the
recovery efficiency of Co, reduced energy consumption as well as environmental pollution.
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This process was considered feasible for recycling spent LIBs for scale-up operation (Li et al.,
2009a). A recycling process that combined hydrometallurgical and sol–gel steps in addition
to other general steps was also used to recover Co and Li from LiBs. The acid media
(hydrogen peroxide in HNO3) used enhanced the leaching efficiency. A gelatinous precursor
was prepared by adding citric acid to the leaching liquor to obtain amorphous citrate
precursor process (ACP), followed by pyrolysis to obtain pure crystalline LiCoO2 (Lee and
Rhee, 2002).
3.2.2 Combined Acid-Alkaline with Organic Solvents Process
As a means of advancing the process of recycling spent lithium-ion batteries, combined
acids-alkaline and organic solvents was used for safety, simplicity and other benefits
observed in other methods. Lithium, Ni, Mn and Co were leached from LiMnNiCoO2 using
HNO3 and then precipitant, NaOH by Castillo et al (2002), while Consestabile et al (2001)
also leached LiCoO2 with HCl and then precipitated the cations with NaOH solution. In
similar steps, the batteries inner rolls were treated with NaOH to dissolve the aluminium foil
to separate the cathode material powders from other components. The powder obtained was
burnt to remove PVdF, followed by dissolution to produce sulfate solution. Cobalt in the
solution was deposited as oxalate, while Acorga M5640 and Cyanex272 (di-(2,4,4 trimethyl
pentyl) phosphoric acid) were used to selectively extract small quantities of Cu2+, Co2+ (Nan
et al, 2005) and Ni2+ ions (Nan et al., 2006) in the solution. Wang et al (2009) selectively
used KMnO4 to recover Mn as MnO2 and manganese hydroxide from the leaching liquor,
while dimethylglyoxime was used to recover Ni. Cobalt was precipitated as cobalt hydroxide,
while addition of a saturated Na2CO3 solution to the liquor precipitated Li as Li2CO3. The
process can be represented by the flow-sheet in Figure 4.
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Figure 4. Flow sheet for general acid-alkaline with selective recovery and recycling of LiBs.
3.2.3 Bio-Metallurgical Process
Compared with the aforementioned pyrometallurgical, hydrometallurgical processes,
bioprocess was considered as having higher efficiency, low cost and environmentally
compatible (Bernardes et al., 2004; Xin et al., 2009). The process used bacteria and inorganic
chemical solutions. For example, acidithiobacillus ferrooxidans utilized elemental sulfur and
ferrous ion to produce metabolites, H2SO4 and ferric ion in the leaching medium to recover Li
and Co from LiCoO2 of LiBs. The metabolites enhanced the dissolution of metals from the
batteries. Comparatively, bio-dissolution of Co was faster than Li (Mishra et al., 2008). Xin
et al (2009) also recovered Co and Li from the spent LiBs through the same processes.
However effective the procedure may be, the cost of culturing the enzymes or bacteria may
somehow hinder its commercial operation.
3.2.4 Electrochemical Process
Electrochemical methods have been used to recover metals from the leached liquor of the
cathode active materials of LiBs. Meanwhile, it was impossible to recover Ni directly by the
method from the liquor obtained. Therefore, Ni was first separated from Co by solvent
extraction, followed by its recovery through galvanostatic and potentiostatic electrowinning
(Lupi and Pasquali, 2003). Also, Freitas and Garcia (2007) electrochemically recovered Co,
while combination of the electrochemical and hydrothermal methods were used to recover
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both Co and Ni from LiCoO2 and (LiCoxNi(1-x)O2 in the Li ion and Li polymer batteries,
respectively (Lupi et al, 2005). The ionic equations for the electrochemical reactions of a
divalent cation during electrolytic recycling process could follow:
Anode: M2++ 2H2O MO
2 + 4H+ + 2e-
Cathode: 2H+ + 2e- H
Overall: M2++ 2H2O MO
2 + 2H+ + H2
3.2.5 Pyrometallurgical Process
The process chemically recovered valuable components of the waste materials or
concentrates at elevated temperatures (Espinosa et al, 2004). Pauline et al (2008) fused the
mixture of active mass (cathode and anode) and electrolyte with KHSO4 in a furnace.
Although precaution was taking to avoid reduction of sulfate to SO2 of sulfide, industrial
dumps like CaF2, Ca3(PO4)2 and other byproducts were generated along with the desired
4. Conclusion
From the review so far, several attempts have been made to clean the environment and
achieve the general objectives of waste sustainability and management. The chemical
processes have been improved upon with great success recorded. However, the amount of
chemicals involved in most of the multiple-steps used could render them economically
unsuitable beside the effect of byproducts or other wastes generated that must be properly
treated in conformity with the acceptable limit for the environments.
The use of suitable non-toxic organic solvents capable of dissolving the PVdF in the batteries
to maximize the recovery values and enhance the reduction in the amount of HF gas released
by pyrolysis before leaching has proved more environmentally compatible. We suggest that
the inner materials of the LiBs be washed with suitable organic solvents to extract the toxic
electrolyte mixture to avoid pollution caused by hydrolysis of LiPF6. Also, conversion of the
electrolyte salt to useful products is achievable to minimize wastes generation.
We appreciate the
support received from the School of Chemistry and Chemical Engineering,
Southeast University, China. The expertise whose works are adopted is greatly appreciated.
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Electrode Materials from Spent Lithium-ion Batteries, IEEE, 1-4. ISSN: 2151-7614. http://
... Laboratories and companies recycle all types of batteries using chemical and physical processes. Physical processes often include pyrolysis, manual or mechanical separation, and dissolution, for example, [57,62] extracting the electrolyte solution into organic solvents like ethanol or iso-butyl alcohol/water after manually or mechanically dismantling LiBs. This reduces environmental pollution caused by the hydrolysis of electrolyte salt, LiPF6, and the toxic electrolyte mixture. ...
... This reduces environmental pollution caused by the hydrolysis of electrolyte salt, LiPF6, and the toxic electrolyte mixture. LiPF6 was creatively converted for the first time by the authors of [62] into a useful chemical like Li2SiF6. Wang and Yu [60] used LCA and discovered that recycling waste batteries can significantly minimize their environmental impact. ...
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Due to an extensive usage of heavy machinery, the construction sector is criticized as one of the major CO2 emitters. To address climate concerns, mitigating these greenhouse gas (GHG) emissions is important. This study aimed to strategize for “zero emission construction” by assessing the life cycle environmental impacts of diesel, electric, and hybrid construction machinery. By applying life cycle assessment (LCA) principles with adherence to ISO 14040/44 methodologies, this study scrutinizes the environmental repercussions of a standard excavator over 9200 effective operational hours, from raw material acquisition to end-of-life disposal. The results demonstrate a significant reduction in global warming potential (GWP), ozone depletion potential (ODP), and acidification potential (AP) in transitioning from diesel to hybrid and fully electric machines. A nominal increase due to this shift also occurred and impacted categories such as human carcinogenic toxicity (HT), freshwater eutrophication (EP), and marine ecotoxicity (ME); however, a more significant upsurge was noted in terrestrial ecotoxicity (TE) due to battery production. Thus, this study highlights the need for a careful management of environmental trade-offs in the shift toward electrified machinery and the importance of centering on the environmental profile of the battery. Future work should focus on enhancing the environmental profile of battery production and disposal, with policy decisions encouraging holistic sustainability based on green energies in construction projects.
... When using the battery, lithium ions (Li + ) move from the negative electrode to the positive electrode, while the current moves in the opposite direction Figure 1(b). The oxidation-reduction reactions taking place at the anode and cathode are given in Equations 1-3, [14], [19]- [21]. ...
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Wastes with high metal content are an important secondary source. Utilisation of these wastes is important offering environmental and economic advantages as well as the conservation of natural resources. Due to the widespread use of portable electrical and electronic devices (mobile phones, laptops, video cameras, etc.) and electric cars, the consumption of lithium and cobalt, which are used as main components in lithium-ion batteries/batteries (LIB), has increased. Because LIBs contain lithium (1.5-7%), cobalt (5-20%), manganese (15-20%), copper (8-10%), aluminium (5-8%), and nickel (5-10%), they are considered as an important secondary source. Industrially, mechanical pretreatment, pyrometallurgical and hydrometallurgical methods as alone or in combination are used to recover metals from waste LIBs. After mechanical pretreatment and physical separation processes, hydrometallurgical methods, including solution purification, precipitation and solvent extraction methods, are used after leaching with inorganic such as H2SO4, HCI and HNO3 or organic acids. In this study, processes for recovery of metals from LIBs are discussed with a critical review of studies carried out on this. In addition, flowsheets of industrial applications for lithium/cobalt recovery in the world are presented. Yüksek metal içeriklerine sahip olan atıklar önemli bir ikincil kaynak konumundadırlar. Bu atıkların değerlendirilmesi, çevresel ve ekonomik avantajlarının yanı sıra doğal kaynakların korunması açısından da önemlidir. Taşınabilir elektrikli ve elektronik cihazların (cep telefonları, dizüstü bilgisayarlar, video kameralar vb.) ve elektrikli otomobillerin yaygınlaşmasına bağlı olarak bunların temel bileşeni olan lityum-iyon pillerde/bataryalarda (LIB) kullanılan lityum ve kobalt tüketimleri de artmıştır. LIB'ler, lityum (%1,5-7), kobalt (%5-20), manganez (%15-20), bakır (%8-10), alüminyum (%5-8) ve nikel (%5-10) gibi metalleri içermesinden dolayı önemli bir ikincil kaynak olarak değerlendirilmektedirler. Atık LIB'lerden metallerin geri kazanımında endüstriyel olarak mekanik ön-işlem, pirometalurjik, hidrometalurjik veya bunların birleşimden oluşan yöntemler kullanılmaktadır. Mekanik ön-işlem ve fiziksel ayırma işlemlerinden sonra H2SO4, HCI ve HNO3 gibi inorganik ya da organik asitlerle liç sonrası çözelti saflaştırma, çöktürme ve solvent ekstraksiyon yöntemlerini içeren hidrometalurjik yöntemler kullanılmaktadır. Bu çalışmada, LIB'lerden metallerin geri kazanım prosesleri ve yapılmış farklı çalışmalar tartışılmıştır. Ayrıca, Dünya'da lityum/kobalt kazanımının gerçekleştirildiği endüstriyel uygulamalardan akım şemaları sunulmuştur.
... The influence of ultrasonic treatment on the separation of cathodic active materials was also reported in (Yang et al., 2015). In addition to N-methylpyrrolidone, other organic solvents including dimethylsulfoxide (DMSO) (Bankole et al., 2013), N, N-dimethylformamide (DMF) , N, N-dimethylacetamide (DMAC) (Zheng et al., 2016a), and ionic liquid (Zeng and Li, 2014a) are also utilized to separate the active cathodic substances. ...
Lithium-ion batteries (LIBs) with high power density are commonly used in electric vehicles and portable electronic devices. Their applications have been soaring in recent years resulting in an increasing number of used LIBs. Spent LIBs containing heavy metals and toxic hazardous are becoming a severe threat to the environment and human health which must be addressed properly. Recycling is an option for end-of-life LIBs, which not only prevents the pollution of toxic components but also saves natural sources. This paper introduces battery structures and gives an overview of the current state of waste LIBs and their recycling status. Moreover, recent advancements in hydrometallurgy, pyrometallurgy, and direct recycling at both research and industrial levels are deeply analyzed. This document can serve as a useful reference resource for researchers or engineers, who might profit from applying the concept to the examples summarized in the comprehensive review paper.
... The roughly estimated relative efficiency order of different solvents for PVDF runs as NMP > DMAC > DMF > DMSO > H 2 O > DCM > CCl 4 > acetone > ethanol. [103][104][105] Conversely, tetrauoroacetic acid (TFA) is a better choice for the more polar PTFE binder. 106 Due to the higher cost and hazardous nature of NMP, other solvents such as DMSO and DMF are also exploited as cheaper and safer alternatives. ...
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The advent of lithium-ion battery technology in portable electronic devices and electric vehicle applications results in the generation of millions of hazardous e-wastes that are detrimental to the ecosystem. A proper closed-loop recycling protocol reduces the environmental burden and strengthens a country with resource sustainability, circular economy, and the provision of raw materials. However, to date, only 3% of spent LIBs have been recycled. The recycling efficiency can be further increased upon strong policy incentives by the government and legislative pressure on the collection rate. This review sheds light on the pretreatment process of end-of-life batteries that includes storage, diagnosis, sorting, various cell discharge methods (e.g., liquid medium, cryogenic and thermal conditioning, and inert atmosphere processing), mechanical dismantling (crushing, sieving, sequential, and automated segregation), and black mass recovery (thermally and solvent leaching). The advantage of the stagewise physical separation and practical challenges are analyzed in detail. Disassembling the battery module pack at the cell level with the improved technology of processing spent batteries and implementing artificial intelligence-based automated segregation is worth it for high-grade material recovery for battery applications. Herein, we outline an industry-viable mechanochemical separation process of electrode materials in a profitable and ecofriendly way to mitigate the energy demand in the near future.
... In other words, testing, and sorting of EOL LIBs by their state and remaining utilization are needed for determining the appropriate activities after. At this stage, a triage is necessary to determine the level of quality and (Bankole et al., 2013;Li et al., 2010;Zhang et al., 2018). Disassembly of the battery package is a significant activity-and obstacle-in achieving CE for LIBs. ...
... Dissolution treatment weakens the adhesive substance using a special organic solvent (Song et al., 2013). The solvents that have been successful at this stage include N,N-dimethylformamide (DMF), N,N-dimethylacetamide (DMAC), N-methylpyrrolidone (NMP) and dimethylsulfoxide (DMSO) (Bankole et al., 2013;Zhou et al., 2010). However, due to the high cost of organic solvents and devices (He et al., 2015), this process is impractical on an industrial scale. ...
Electrifying transportation through the large-scale implementation of electric vehicles (EVs) is an effective route for mitigating urban atmospheric pollution and greenhouse gas emissions and alleviating petroleum-derived fossil fuel reliance. However, huge dumps of spent lithium-ion batteries (LIBs) have emerged worldwide as a consequence of their extensive use in EVs. With the increasing shortage in LIB raw materials, the recycling of spent LIBs has become a fundamental part of a sustainable approach for energy storage applications, considering the potential economic and environmental benefits. In this mini-review, we will provide a state-of-the-art overview of LIB recycling processes (e.g., echelon utilization, pretreatment, valuable metal leaching and separation). We then discuss the sustainability of current LIB recycling processes from the perspectives of life cycle assessment (LCA) and economic feasibility. Finally, we highlight the existing challenges and possibilities of LIB recycling processes and provide future directions that can bridge the gap between proof-of-concept bench demonstrations and facility-scale field deployments through mutual efforts from academia, industry, and government. It is expected that this review could provide a guideline for enhancing spent LIB recycling and facilitating the sustainable development of the field.
... Because of the limited lifetime of LIBs, 11 million tons of spent batteries are estimated to be produced by 2030 [7,8]. Recently, a report by the United Nations University revealed that a high percentage of electronic waste, including spent LIBs, is highly polluting because it often contains Li, Co, Mn, and Ni, among others. ...
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The abundant use of lithium-ion batteries (LIBs) in a wide variety of electric devices and vehicles will generate a large number of depleted batteries, which contain several valuable metals, such as Li, Co, Mn, and Ni, present in the structure of the cathode material (LiMO2). The present work investigates the extraction of lithium, as lithium chloride, from spent LIBs by carbochlorination roasting. The starting samples consisted of a mixture of cathode and anode materials from different spent LIBs known as black mass. Calcium chloride was used as a chlorinating agent, and carbon black was used as a reducing agent. The black mass, calcium chloride, and carbon black were mixed in 50:20:30 w/w % proportions. Non-isothermal thermogravimetric tests up to 850 °C and isothermal tests at 350, 500, and 700 °C were carried out in an inert atmosphere. It was observed that the carbochlorination reaction starts at 500 °C. An extraction percentage of 99% was attained through carbochlorination at 700 °C. The characterization results indicate that CaCO3, Ni, and Co and, to a lesser extent, CoO, NiO, and MnO2 are present in the roasted sample after the processes of washing, filtering, and drying.
... Because of the limited lifetime of LIBs, 11 million tons of spent batteries are estimated to be produced by 2030 [7,8]. Recently, a report by the United Nations University revealed that a high percentage of electronic waste including spent LIBs is highly polluting because they contain i.e. ...
The abundant use of lithium-ion batteries (LIBs) in a wide variety of electric devices and vehicles will generate a large number of depleted batteries, which contain several valuable metals such as Li, Co, Mn, and Ni present in the structure of the cathode material (LiMO2). The present work investigates chemical, technological, and environmental aspects in the treatment of such wastes, development of a methodology for the extraction of lithium, cobalt, nickel, manganese, and graphite by a carbochlorination pyrometallurgical process. Mixtures of cathode and anode materials (called black mass, mixed oxides of Li, Co, Ni, Mn, and graphite) from different LIBs, carbon black (as reducing agent), and CaCl2 (as chlorinating agent) were used. Non-isothermal thermogravimetric tests up to 850°C and isothermal tests at 700°C of the mixtures in an inert atmosphere were carried out. It was experimentally observed that the LiMO2-C-CaCl2 reaction takes place at 700°C. LiCl, Ni, and Co were obtained as final products, and to a lesser extent, CoO, NiO, and MnO2. CaCO3 was also obtained as a by-product. The obtained results show that carbochlorination is an efficient and effective alternative route for the extraction and recovery of metals from different LIBs, focused on the sustainability and circular economy
... The electrolyte is usually sandwiched between the negative and positive electrodes, which plays an important role in transporting the positive lithium ions between the cathode and anode. Electrolyte is also insulating electronic conduct-manage safety issues and eliminate waste production ( Bankole et al., 2013 ). It has been reported that 13% of LIB cost per kWh could be saved through metals recycling. ...
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With the significant rise in the application of lithium-ion batteries (LIBs) in electromobility, the amount of spent LIBs is also increasing. LIB recycling technologies which conserve sustainable resources and protect the environment need to be developed for achieving a circular economy. Recycling of LIBs will reduce the environmental impact of the batteries by reducing carbon dioxide emissions in terms of saving natural resources to reduce raw materials mining. This work reviewed the most advanced and ongoing LIB recycling technologies, and categorized the reviewed technologies according to the components of the LIB cells, including cathodes, anodes, electrolyte and separators. Most recycling technologies focus on the recovery of valuable metals, particular for cobalt by hydrometallurgical method from the cathodes. The commercial process based on the combination of the pyrometallurgical and hydrometallurgical technologies which was commercially developed by Umicore, and Retriev, is mainly focusing on the developed hydrometallurgical technology for optimizing the recovering efficiency. There is research undergoing to recover graphite from anodes through Fenton oxidation, froth flotation and thermal treatment with a combination of hydrometallurgical process. As LIB recycling technologies are under development, there is great potential to reduce emission of carbon dioxide and this should be a focus in research. There is also a high need to develop a more advanced LIB recycling technology to recover more valuable materials with reduced carbon emission, therefore to contribute to “Net zero” ambition.
In this study, we address the most recent innovations in the field of sustainable and environment friendlier binders for electrochemical energy storage devices such as, supercapacitors and batteries accompanied by the explanation, how they could reduce the impacts of environment and cost and enhance the efficiency of the energy equipment. Hitherto, the number of sustainable and environment friendlier binders are categorized according to their chemical composition, processability and natural availability. Different electrochemical devices are being employed to investigate their wide‐ranging advantages. Among them the most commonly employed devices are lithium‐ion batteries (LIBs) and electrochemical double layer supercapacitors (ECDSs). A detailed insight into the anodic half as well as cathodic half has been presented. The Si derived anodes exhibit enhanced capacitive performance as a result of increased cycling ability. This feature owes from the greater interactions between the functionalities and surface of the active particles of the anode material for example, polysaccharides such as carboxymethyl cellulose (CMC)/nanocellulose (NC). On the other hands the transition to water‐processable cathodes is more complicated compared to anodes. Among various polysaccharides, the NC has gained considerable attention as a sustainable and environment friendlier class of greener materials. Herein, we have discussed the role of NC based electrode materials with applications in supercapacitors and batteries. Finally, a comprehensive overview based on the documented work and current views for the further development of NC based aqueous electrodes in the field of electrochemical energy storage devices are discussed. Sustainable and environment friendly binders for electrochemical energy storage devices such as, supercapacitors and batteries. The review also elaborates on ways to reduce the environmental impacts, cost and enhance the energy efficiency.
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An alternative method for preparing lithium hexafluorosilicate regarded as an important anode active material in lithium ion battery is proposed. The compound was obtained from lithium ion battery by washing the electrolyte mixture with ethanol and distillation in a glassware reactor. The investigation showed that there was an exchange reaction between the silicon from the glassware and phosphorus of LiPF6 in the ethanol used as the extractant. Ethanol proved suit-able for the synthesis of Li2SiF6 in glassware to enhance water requirement as a condition for the reaction. The compounds obtained from both simple plastic and glassware were characterized using XRD. The results of the X-ray diffraction patterns confirmed that both Li2SiF6 and LiF were obtained from glassware and plastic respectively. The lattice parameter analysis has the hexagonal structure with space groups P321 and P-3M1 as well as the orthogonal structure with space groups P222 and P2221. It has been successfully shown that the electrolyte solution from the Li-ion battery can be economically and effectively used for the preparation of Li2SiF6 for immediate demand besides the virgin materials and still re-use the ethanol by distillation.
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Preparation of LiCoO2 cathode materials from spent lithium–ion batteries are presented. It started with the reclaim/recycle of metal values from spent lithium–ion batteries, which involves the separation of electrode materials by ultrasonic treatment, acid dissolution, precipitation of cobalt and lithium, followed by the preparation of LiCoO2 cathode materials. Co (99.4%) and Li (94.5%) were recovered from spent lithium–ion batteries. The LiCoO2 cathode materials prepared from the reclaimed cobalt and lithium compounds showed good elecrtochemical performance. The reclaiming of cobalt and lithium has a promising outlook for the recycling of cobalt and lithium from spent Li–ion batteries, thus reducing the cost of Li–ion batteries.
Lithium batteries use organic electrolytes because of the wide operating voltage. For lithium ion rechargeable batteries, these electrolytes are almost universally based on combinations of linear and cyclic alkyl carbonates. These electrolytes make possible the use of Li as the anodic active component and results in the high power and energy densities characteristic of the Li-ion chemistries. However, these organic electrolytes have high volatility and lammability that pose a serious safety issue for their use in the consumer and transportation markets. If exposed to extreme conditions of elevated voltage and temperature, these electrolytes can react with the active electrode materials to release signiicant heat and gas.
Lithium/cobalt/nickel oxide (LiCox Ni1-xO2, 0 < x < 1) is one of the cathode materials currently used in commercial Li-ion batteries. The direct Ni recovery by electrochemical methods from leach liquor obtained by dissolution of this cathode is not possible because of cobalt anomalous co-deposition. After separating Ni from Co by SX methods, nickel has been recovered by means of both galvanostatic and potentiostatic electrowinning. Operative conditions such as solution pH, temperature, Ni concentration, bath agitation and, in the case of galvanostatic operation, current density have been determined for the selected cathode and anode material. The use of galvanostatic conditions enables a good Ni metal deposit to be obtained, while potentiostatic conditions result in an almost complete depletion of nickel in the electrolyte..
In this work, cobalt from spent cellular telephone Li-ion batteries was recovered by electrochemical techniques. According to X-ray diffraction results, the composition of the positive electrode is LiCoO2, Co3O4, C, and Al. The largest charge efficiency found was 96.90% at pH 5.40, potential applied of −1.00 V and a charge density of 10.0 °C cm−2. The charge efficiency in the electrochemical recycling of cobalt decreases with the decrease in pH. The energy dispersive X-ray analysis (EDX) measurements of the electrodeposits showed that the surface is constituted of 100% cobalt. Scanning electron microscopy (SEM) showed a three-dimensional nucleus growth.The application of nucleation models to the initial stages of electrodeposit growth shows that at pH 5.40 electrodeposition happens with progressive nucleation. With the decrease in pH to 2.70, nucleation becomes instantaneous.
In this paper, based on the structure of lithium-ion batteries, the electrode materials were separated from spent lithium-ion batteries (LIBs) with aim to recycle all valuable components as possible. The spent LIBs were dismantled first, then the mechanical pulverization and sieving process was adopted in the separation of anodes, and dissolution method was used to partition active components from cathodes. Owing to low bonding force between graphite carbon particles and copper foil, graphite carbon can easily drop off and be separated when anode materials were struck. The results showed that after shredding and sieving, most copper was concentrated in the size range above 0.30 mm at the condition of 3 min pulverization, which led to a favorite recovery rate for copper, reaching 95.9%. The selected organic solvent N,N-dimethylformamide (DMF) could be successfully applied to dissolve the polyvinylidene fluoride (PVDF) adhesive that the cathode active materials LiCoO2 be effectively separated from the aluminum current collector.
A recycling process involving mechanical, thermal, hydrometallurgical and sol–gel steps has been applied to recover cobalt and lithium from spent lithium-ion batteries and to synthesize LiCoO2 from leach liquor as cathodic active materials. Electrode materials containing lithium and cobalt can be concentrated with a two-step thermal and mechanical treatment. The leaching behavior of lithium and cobalt in nitric acid media is investigated in terms of reaction variables. Hydrogen peroxide in 1M HNO3 solution is found to be an effective reducing agent by enhancing the leaching efficiency. Of the many possible processes to produce LiCoO2, the amorphous citrate precursor process (ACP) has been applied to synthesize powders with a large specific surface area and an exact stoichiometry. After leaching used LiCoO2 with nitric acid, the molar ratio of Li to Co in the leach liquor is adjusted to 1.1 by adding a fresh LiNO3 solution. Then, 1M citric acid solution at a 100% stoichiometry is added to prepare a gelatinous precursor. When the precursor is calcined at 950°C for 24h, purely crystalline LiCoO2 is successfully obtained. The particle size and specific surface-area of the resulting crystalline powders are 20μm and 30cm2g−1, respectively. The LiCoO2 powder is found to have good characteristics as a cathode active material in terms of charge–discharge capacity and cycling performance.
Cobalt oxide was prepared from spent lithium ion batteries (LIBs) by reductive leaching, copper sulfide precipitation, cobalt oxalate precipitation and thermal decomposition. The cobalt rich non-magnetic −16mesh fraction obtained from spent LIBs by mechanical separation was leached using 2M H2SO4, 6vol% H2O2, reaction temperature 60°C, agitation speed 300rpm, pulp density 100g/L, reaction time 1h. The leaching efficiency of cobalt was more than 99% and its concentration was 27.4g/L. Copper was removed (99.9%) as CuS by precipitating with Na2S. The crystalline solid CoC2O4·2H2O selectively precipitated by treating the copper-free liquor with oxalic acid was calcined to produce crystalline Co3O4, of which primary average particle size was 340nm.
A laboratory process based on a simple and environmentally friendly operation, aimed to recycle spent Li/MnO2 batteries, is described in this study. This process involves roasting batteries under reduced pressure at 650°C, selective leaching of Li2CO3 from calcined electrode material in distilled water at ambient temperature and controlled crystallization of pure Li2CO3 from the aqueous solution.
A novel process was conducted with experiments which separated and recovered metal values such as Co, Mn, Ni and Li from the cathode active materials of the lithium-ion secondary batteries. A leaching efficiency of more than 99% of Co, Mn, Ni and Li could be achieved with a 4 M hydrochloric acid solution, 80 °C leaching temperature, 1 hour leaching time and 0.02 gml− 1 solid-to-liquid ratio. For the recovery process of the mixture, firstly the Mn in the leaching liquor was selectively reacted and nearly completed with a KMnO4 reagent, the Mn was recovered as MnO2 and manganese hydroxide. Secondly, the Ni in the leaching liquor was selectively extracted and nearly completed with dimethylglyoxime. Thirdly, the aqueous solution in addition to the 1 M sodium hydroxide solution to reach pH = 11 allowed the selective precipitation of the cobalt hydroxide. The remaining Li in the aqueous solution was readily recovered as Li2CO3 precipitated by the addition of a saturated Na2CO3 solution. The purity of the recovery powder of lithium, manganese, cobalt and nickel was 96.97, 98.23, 96.94 and 97.43 wt.%, respectively.