Science of the Total Environment 924 (2024) 171453

Contents lists available at ScienceDirect

Science of the Total Environment

journal homepage: www.elsevier.com/locate/scitotenv

Review

Can e-waste recycling provide a solution to the scarcity of rare earth

metals? An overview of e-waste recycling methods
Sai Sree Varsha Vuppaladadiyam a, Bennet Sam Thomas a, Chandan Kundu a, Arun
K. Vuppaladadiyam b, Huabo Duan c, Sankar Bhattacharya a, *
a
Department of Chemical and Biological Engineering, Monash University, Australia
b
School of Engineering, RMIT University, Melbourne, VIC 3000, Australia
c
School of Environmental Science and Engineering, Huazhong University of Science and Technology (HUST), Wuhan 430074, China

H I G H L I G H T S G R A P H I C A L A B S T R A C T

• Improper e-waste management is detri­

mental to human health and the
ecosystem.
• E-waste can be considered a secondary
resource of REEs.
• Recycling e-waste could facilitate the
recovery of REEs.
• Organic acids are emerging solvents
with minimum environmental impacts.

A R T I C L E I N F O A B S T R A C T

Editor: Daniel Alessi Recycling e-waste is seen as a sustainable alternative to compensate for the limited natural rare earth elements
(REEs) resources and the difficulty of accessing these resources. Recycling facilitates the recovery of valuable
Keywords: products and minimizes emissions during their transportation. Numerous studies have been reported on e-waste
E-waste recycling using various techniques, including thermo-, hydro- and biometallurgical approaches. However, each
Recycle approach still has technical, economic, social, or environmental limitations. This review highlights the potential
Recovery of recycling e-waste, including outlining the current unutilized potential of REE recycling from different e-waste
REEs
components. An in-depth analysis of e-waste generation on a global scale and Australian scenario, along with
Hydrometallurgy
various hazardous impacts on ecosystem and human health, is reported. In addition, a comprehensive summary
Solvometallurgy
Global GHG emissions of various metal recovery processes and their merits and demerits is also presented. Lifecycle analysis for

Abbreviations: ABS, acrylonitrile butadiene styrene; BFR, brominated flame retardants; CRTs, cathode ray tubes; DPDD, dibenzo-P-dioxins; DoEE, Department of
Energy and Environment; EEE, electronic and electrical equipment; ER, epoxy resin; HREEs, heavy rare earth elements; LABs, lead acid batteries; LCDs, liquified
crystal displays; LEDs, light-emitting diodes; LIBs, lithium ion batteries; LREEs, light rare earth elements; MOFs, metal-organic frameworks; NdFeB, neodymium
magnets; NiCd, nickel-cadmium; NiMH, nickel-metal hydride; PAHs, polycyclic aromatic hydrocarbons; PC, polycarbonate; PDBF, polybrominated di-benzo furans;
PE, polyethylene; PHAHs, polyhalogenated aromatic hydrocarbons; PP, polypropylene; PPM, parts per million; PR, phenolic resin; PTFE, polytetrafluoroethylene;
PVC, polyvinylchloride; REE, rare earth elements; WPCBs, waste printed circuit boards.
* Corresponding author.
E-mail address: [email protected] (S. Bhattacharya).

https://doi.org/10.1016/j.scitotenv.2024.171453
Received 8 November 2023; Received in revised form 27 February 2024; Accepted 1 March 2024
Available online 5 March 2024
0048-9697/© 2024 The Author(s). Published by Elsevier B.V. This is an open access article under the CC BY license (http://creativecommons.org/licenses/by/4.0/).
S.S.V. Vuppaladadiyam et al. Science of the Total Environment 924 (2024) 171453

Landfills recovering REEs from e-waste indicate a positive environmental impact when compared to REEs produced from
Mining virgin sources. In addition, recovering REEs form secondary sources eliminated ca. 1.5 times radioactive waste,
as seen in production from primary sources scenario. The review outcome demonstrates the increasing potential
of REE recycling to overcome critical challenges, including issues over supply security and localized dependency.

1. Introduction different industries has created more arguments regarding finding a

practical solution for reusing REEs. Thus, undertaking an appropriate
Rare earth elements (REEs) are among the primary raw materials in approach for recycling REEs can save huge space in landfills, reduce
manufacturing electronic devices and industrial applications. The environmental contamination from toxic substances and heavy metals
limited availability of REEs has become a critical concern in recent leaching into the soil (Dutta et al., 2016), and help recover critical
years. REEs comprise the following 17 elements of Lanthanides (fifteen metals.
metallic elements) lanthanum, cerium, praseodymium, neodymium, Electronic devices can be counted as a secondary resource for REEs in
promethium, samarium, europium, gadolinium, terbium, dysprosium, view of their concentrations. REEs are vital and critical contributors to
holmium, erbium, thulium, ytterbium, lutetium in the periodic table electronic devices’ performance (Fig. 1).
with atomic numbers (57–71) plus Scandium and Yttrium (Holgersson For example, REEs used in LED and fluorescent lamps are for lumi­
et al., 2018; Song and Li, 2014). Rare earth elements (REEs) exhibit nescent properties (Machacek et al., 2015). For electronic displays, REEs
similar chemical properties and predominantly exist in the trivalent are used for light and color adjustments (Song et al., 2013). REEs role in
oxidation state, except for two particular REEs, Europium and Cerium, strengthening permanent magnets and making them more resistant to
which occur as Eu2+ and Ce4+, respectively. REEs extraction and sepa­ demagnetization is another important application of these elements
ration procedures from their respective ores are intricate and typically (Gergoric et al., 2018). REEs help nickel-metal hydride batteries alloy to
involve significant expenses (Bai et al., 2021; Omodara et al., 2019). store, desorb and reabsorb hydrogen (Lucas et al., 2015), and REEs
REEs are divided into two essential categories: light (LREEs) and heavy application as catalytic converters in automotive industries (Schulz
rare earth elements (HREEs). LREEs include elements with atomic et al., 2017), further demonstrates the importance of these metals.
numbers ranging from 57 (lanthanum) to 63 (europium), while HREEs Batinic et al. (2018) state that the amount of REEs found in permanent
include elements with atomic numbers from 64 (gadolinium) to 71 magnets (mostly neodymium and praseodymium), nickel-hydride bat­
(lutetium), as well as scandium and yttrium. On a global scale, rare earth teries, and fluorescent lamps are high enough that implies the potential
oxide (REO) reserves are widely distributed, with the majority concen­ of these types of waste as secondary REEs resources (Batinic et al.,
trated in China, Brazil, and Vietnam. 2018).
The primary resources of REEs are the resources found in nature. Recycling e-waste components is considered an efficient approach to
Lazo (2019) explained that except for promethium produced by radio­ managing e-waste, and scientific and technological advancements in
active decay, almost all other REEs have stable natural resources in the recycling and reuse have made it possible to recover valuable materials
form of minerals (Lazo, 2019). Bastnasite, monazite, xenotime, allanite, from electronic components, such as plastics, waste toner powders, and
and gadolinite are the most common forms of REEs minerals. Lazo batteries. It should be noted that the metal content in e-waste, such as
(2019) states that only the first three have been used on the industrial printed circuit boards (PCBs), exceeds the metal content in ores (Hsu
scale thus far. Since the availability of REEs’ primary resources is un­ et al., 2019). Two fundamental stages are involved in processing e-waste
reliable, the sustainable management of REEs’ supplies has become a to retrieve metals: pre-processing and end-processing. Pre-processing
challenge in recent years. The continued growth of REEs demand in consists of dismantling, sorting, and shredding the e-waste, while end-

Fig. 1. Different industrial applications of REEs.

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processing involves chemical transformations that facilitate the sepa­ 2. Methodology of literature survey
ration and recovery of metals from distinct streams (Li et al., 2019).
Metallurgical processes (pyro, hydro, bio-metallurgy) are usually the A comprehensive three-step research process was undertaken to
end-processing technologies implemented for metal recovery (Alvarado- examine the diverse methods of recovering metals from e-waste. An
Hernández et al., 2019; de Oliveira et al., 2021; Hsu et al., 2021; Jadhao extensive search was conducted on web sources such as Google Scholar
et al., 2020). E-waste also contains precious and base metals in signifi­ and Science Direct. This search employed specific keywords like “e-
cant quantities. It is worth noting that e-waste, such as waste printed waste” and “metals,” “WPCB” and “recycle,” “recover” “rare earth
circuit boards, contains precious metals with 10 times higher purity than metals”, “battery wastes”, “e-waste generation trends”, and “metallur­
the rich ore content. Recovery of noble metals (such as Au, Ge, Pd, Pt, Se, gical technique,” etc. The search encompassed a range of sources,
etc.) from e-waste should be prioritized, but it should be realised that including peer-reviewed articles, reports, book chapters, and similar
recycling should be aimed at maximum resource recovery and negligible publications. Subsequently, recent studies published between 2017 and
negative environment impact. However, e-waste contains toxic and 2023 in esteemed journals were carefully selected and organized chro­
harmful compounds such as brominated flame retardants (BFRs), nologically. By screening the abstracts of these articles, relevant papers
dibenzofuran, dioxin, and heavy metals, and utmost care must be taken falling in the scope of the study were identified. The next step involved
while employing the methods to avoid negative environmental impacts. classifying various conventional and innovative techniques for extract­
In addition, the cost is another major obstacle to recovering metals from ing metals. Prominent examples from each method were chosen based
e-waste, which necessitates the need to identify an eco-friendly and cost- on their objective, concept, methodology, and experimental outcomes.
effective metal recovery process. It is worth noting that recycling of e- These selected examples were then summarized and thoroughly
waste is highly encouraged by the United Nations and is prioritized reviewed. Finally, a critical assessment and comparative analysis of the
under Sustainable Development Goals (SDGs). different metal recovery approaches were carried out to understand
The major problem of recovering precious metals from e-waste is its potential areas for future research in the appropriate field.
complex composition. Improper handling and discarding of e-waste can
result in severe environmental and human health issues as they contain 3. E-waste generation, global and Australian scenario
over 60 hazardous elements like Pb, Hg, Cd, Be, etc., threatening human
life and ecology. Similarly, uncontrolled thermal treatment, like incin­ Technological innovations in the electronic and electrical equipment
eration or combustion, will result in the release of toxic gases, such as (EEE) sector and consumers’ urge to use advanced devices resulted in
polybrominated di-benzo furans (PDBF), polycyclic aromatic hydro­ huge quantities of waste electronic and electrical equipment (WEEE) or,
carbons (PAHs), polyhalogenated aromatic hydrocarbons (PHAHs), and in simple terms, e-waste. Dealing e-waste is becoming increasingly
dibenzo-p-dioxins (DPDD) into the environment causing severe health cumbersome, especially in developing countries, because of the un­
implications (Pokhrel et al., 2020). Given the hazardous content avail­ availability of proper infrastructure to handle such huge quantities
able in the e-waste, improper treatment of e-waste could pose serious (Panda et al., 2020). Global e-waste generation is increasing by 20–40
concerns, including contaminating air, water and soil. In addition, million tons annually and presents huge potential to be recycled because
dismantling process with inadequate facilities and untrained people it contains valuable metals in substantial concentrations. Recycling e-
adds extra threat to human health and ecosystem. These issues are waste can levy the burden of the increasing demand for metals in
addressed by the United Nations SDGs under SDG3: Good Heath and different industrial applications. In 2019, >50 million tons of e-waste
Well-being, SDG6: Clean Water ad Sanitation, SDG14: Life Below Water, were generated across the globe. Such huge quantities of waste with
SDG11: Sustainable Cities and Communities, SDG12: Responsible Con­ huge potential for metals recovery and containing significant hazardous
sumption and Production and SDG8: Decent Work and Economic content could not be processed or discarded quickly. According to the
Growth (Vanessa et al., 2020). Currently, the research focus is mainly on USEPA, only 15–20 % of e-waste is recycled, and the balance is either
improving the economics of the metal recovery process and, at the same landfilled or incinerated (Udayakumar et al., 2022). E-waste is a valu­
time, developing an eco-friendly approach by introducing a controlled able and unconventional resource with very high metal content; the
thermal pre-treatment process followed by environmentally benign metals contribute to ca. 40 wt% (Hsu et al., 2019). The rate of e-waste
solvent extraction of precious metals. generation is an area of worry due to environmental concerns and the
Although there are numerous publications in this area, most studies complexity involved in the resource recovery process, often involving
have focused on a single conversion technology or highlighted a the application of toxic chemicals. According to Victoria-Environmental
particular approach as a sustainable solution. To the best of our Protection Authority (EPA), ‘Electronic waste (e-waste) is any waste item
knowledge, very few studies have reported recycling from a neutral that uses a plug, battery or power cord that is no longer working or wanted’
point of view and suggested a sustainable recycling approach. In addi­ (EPA-Victoria, 2023). Recycling e-waste requires an in-depth under­
tion, in the last 10 years, most of the research was carried out on using standing of the structure and constituents of e-waste. Recent reviews
conventional approaches such as precipitation, filtration and pyro- and classified e-waste into five categories, including waste printed circuit
hydrometallurgy. Although, these conventional approaches are still boards (WPCBs), battery wastes, light-emitting diodes (LEDs), liquified
considered promising for REEs recovery from e-waste, they cannot crystal displays (LCDs) and capacitors (Andooz et al., 2022; Tan and Li,
extract or recover REEs with low concentrations and low-affinity. High 2019).
energy consumption, exhaustive use of reagents, lack of economic ad­ E-waste has a very high potential to be a significant secondary supply
vantages often limit the application of recovery techniques. This revie is after mining REEs. Printed circuit boards (PCBs) are essential compo­
an all-inclusive analysis of critical aspects of e-waste management and nents of almost all EEEs and account for 3–6 % of the total weight of EEE
the way forward fo the REEs recovery for sustainable circular economy. (Holgersson et al., 2018; Işıldar et al., 2016). The diverse composition of
In this context, this review covers various global e-waste generation WPCBs is more complex than natural mines, and the metal recovery
scenarios, hazardous content and their ecological impacts and various processes are challenging. On the other hand, the availability of precious
strategies for recovering REEs from e-waste. In addition, various policies and base metals at elevated concentrations makes PCBs a valuable
and regulations applied in the Australian context for e-waste manage­ resource. Hence, effective and environmentally benign processing of
ment are summarized. Hence, this review provides a generic framework Waste PCBs needs an extensive understanding of the waste PCB’s
that could assist as a tool for future research in exploring an efficient, composition, scale of the recycling process, and techno-economics of the
economical and environmentally sustainable recovery method. extraction process (Birloaga et al., 2014). PCBs contain ceramics (30 %),
plastics (30 %) and metals (40 %), which are distributed in varying
percentages in metal layers, silkscreens, polymer substrates, adhesive

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materials and solder masks (Hao et al., 2020). The polymers in PCBs are toxicity, marine aquatic ecotoxicity, and terrestrial ecotoxicity. The
acrylonitrile butadiene styrene (ABS), epoxy resin (ER) or phenolic resin findings indicated a notable environmental impact associated with
(PR), brominated flame retardants (BFRs), polycarbonate (PC), poly­ NiMH batteries compared to LIBs. This impact primarily stemmed from
ethylene (PE), polypropylene (PP), polytetrafluoroethylene (PTFE), and using relatively larger quantities of toxic chemicals during production.
polyvinylchloride (PVC). In addition, refractory oxides, such as silica, Moreover, the shredding, treating, extraction, and refining of Cd for Ni-
alumina, etc., are also available in waste PCBs. In waste PCBs, precious Cd-based batteries and photovoltaic modules presented risks concerning
metals, like Au and Ag, and base metals, like Al, Cu, Zn, etc., are also groundwater contamination, food safety, and the well-being of workers
available in concentrations varying from 1 to 40 % on a weight basis. if exposed to these hazardous chemicals (Sovacool et al., 2020).
These metals are distributed in the multi-element alloys, and metal
joints and layers (Udayakumar et al., 2022). The metallic content in 3.1. Global scenario
waste PCBs largely relies on the waste type, manufacturing process and
equipment age. The metal fraction includes 7–38 % Fe, 10–27 % Cu, E-waste production is likely to continuously increase at an average of
2–19 % Al, 1–3 % Pb, 0.3–2 % Ni, 200–3000 parts per million (ppm) Ag, 20–50 million tons annually (Fig. 2a). The total e-waste production in
20–500 ppm Au, and 10–200 ppm Pd (Perkins et al., 2014). Besides, 2014 was 44.4 Mt, which increased to 55.5 Mt in 2020 and is expected to
non-metal fraction includes polymers and solder mask and contain 40 % reach ca. 75 Mt by 2030. In terms of per capita electronic waste gen­
as organic material, such as resins of thermoplastic and thermosetting, eration, there has been a steady annual increase worldwide (Fig. 2(a)).
and inorganic substances (SiO2 and Al2O3). The average global e-waste generated per capita in 2014 stood at 6.4 kg/
Another important category of e-waste is spent battery waste. Lead person, reached to 7.5 kg/person in 2020. This value is expected to reach
acid (LABs) and lithium-, and nickel-based batteries were the primary an alarming 9 kg/person by 2030. As shown in Fig. 2b, in 2019, Asia
players in the global battery market, accounting for a combined market emerged as the leading producer of e-waste, generating ca. 24.9 million
share of 94.8 %. Specifically, lithium-ion batteries (LIBs) were expected metric tons (MT). America followed closely with 13.1 MT, while Europe
to achieve a market value of ca. US $54 billion by 2024, exhibiting a contributed 12.0 MT to the overall e-waste production. Africa and
compound annual growth rate (CAGR) of 11 % from 2019 to 2024 (Zhao Oceania generated 2.9 MT and 0.7 MT of e-waste, respectively. When
et al., 2021). Despite the continuous growth of the battery market, examining the per capita e-waste generation, Europe claimed the top
managing end-of-life (EoL) batteries poses a significant challenge. The spot worldwide, with 16.2 kg/person. Oceania closely followed with
commonly utilized battery contains substantial amounts of heavy metals 16.1 kg/person, and America ranked third with 13.3 kg/person. On the
such as Mg, Pb, Cd, and Li, along with other contaminants widely other hand, Asia and Africa contributed significantly lower per capita e-
recognized for their high ecotoxicity (Guo et al., 2018). For instance, LIB waste generation, with 5.6 kg and 2.5 kg, respectively (Fig. 2(b))
batteries contain sulfuric acid, highly corrosive, and other highly toxic (Thakur and Kumar, 2022). From a per capita perspective, Europe and
heavy metals that are persistent in the environment and cause health Oceania demonstrate considerably higher levels of e-waste generation
issues such as brain, kidney, and nerve system damage and many other than other continents.
related complications (Ballantyne et al., 2018). In addition to Li, LIBs
contain metals, including Co, Ni, Mg, Al, and Cu, classified as toxic
3.2. Australian scenario
heavy metals and has high value and energy intensive ingredients (Kaya,
2022). Specifically, Co2+ ions can harm human and aquatic life. For
Australia’s total and per capita e-waste production has continuously
example, Li mining in Chile has resulted in local groundwater depletion
risen since the last decade. Australia is positioned as one of the leading
and destroyed fragile ecosystems. In most countries, the predominant
buyers of electronic products worldwide, resulting in the rapid expan­
battery types in the waste battery stream are NiCd (nickel‑cadmium)
sion of e-waste as a significant waste category in the country (Andeobu
and NiMH (nickel-metal hydride) batteries. Cadmium may cause health
et al., 2021). Over the past decade, Australia’s total and per capita e-
risks such as lung cancer and kidney damage. The potential elimination
waste generation have consistently increased from 410 kt in 2010 to
of Cd-containing batteries, like Hg batteries which have already been
554 kt in 2019 (Forti et al., 2020). According to research by Golev et al.
prohibited, is under careful consideration in certain countries (Zhao
(2016), Australia ranks among the nations with the highest per capita e-
et al., 2021). In a recent study conducted by Mahmud et al. (2019), a
waste generation. In 2014, Australia’s average e-waste generated per
comprehensive comparison was made between the environmental
person was close to 25 kg/capita, projected to increase to 30 kg/person
impact of lithium-ion batteries (LIBs) and nickel-metal hydride (NiMH)
by 2024. In a recent study, the generation trends of e-waste in Australia
batteries throughout their entire life cycles. Various factors include
were forecasted till 2024 considering three scenarios: (i) base case (fixed
eutrophication, freshwater aquatic ecotoxicity, global warming, human
consumption of EEEs at 35.2 kg/person), (ii) base case plus 5 kg/person

Fig. 2. (a) Global e-waste generation from 2014, projected till 2030, (b) amount of e-waste generated and per capita by region in 2019.

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and (iii) base case scenario minus 5 kg/person consumption. The au­ 2–3 kg of lead (Tsydenova and Bengtsson, 2011). Even though CRT
thors mentioned that e-waste generation is intensely linked to EEE sales, screens are replaced with liquid crystal display (LCD) and LED screens,
and the annual average growth rate of e-waste generation is projected at which contain much less lead content (<1 kg) (Bigum et al., 2017), a
3 ± 0.3 % till 2024, which was ca. 7 % between 2010 and 2014 (Golev huge amount of lead has recently been noticed entering the waste in­
et al., 2016). ventory. The plausible reason could be the previously installed CRT
Islam and Huda forecasted the generation trends of e-waste in screens reaching their end of life. However, LCD screens contain mer­
Australia from 2010 to 2030 (Islam and Huda, 2020). The study cury, which is highly toxic if mobilized. In addition, fluorescent lamps
considered 16 types of EES, their sales, and subsequent e-waste gener­ and alkaline batteries contain mercury, and mercury contamination is a
ation. The e-waste generation based on the sales value of EEE in 2010 significant issue in the associated recycling sector and occupational
was forecasted as 223 and 342 kt in 2010 and 2020, respectively. exposure (Lecler et al., 2018).
Moreover, the e-waste generation value is expected to reach 461 kt by Proper recycling methods can channel back rare metals, such as
2030, with an annual increase rate of 3.7 %. According to a consultation copper, gold or palladium, from e-waste into the supply chain. On the
report commissioned by the Australian government’s Department of contrary, primitive recycling approaches can pose serious environ­
Energy and Environment (DOEE), it was discovered that Australia mental and human health concerns by releasing contaminants into the
generated ca. 539 kt of e-waste in the year 2018–19 (Environment, ecosystem (Li and Achal, 2020). Pollutants in e-waste can be categorized
2020). This amount indicated a growth of ca. 3.7 % compared to the into two categories: the primary toxicants – hazardous substances that
previous year, which was similar to the value forecasted by Islam and are available in the e-waste, including heavy metals such as Pb, Cd, Hg,
Huda in their study (Islam and Huda, 2020). An interesting inference etc., and secondary toxicants – generated during processing and/or
that can be deduced by comparing the generation rate of municipal solid recycling e-wastes, including PAHs, difurans and dioxins (Ahirwar and
waste (6 %) against e-waste (3.8 %) is that e-waste is one of the fastest- Tripathi, 2021). Both primary and secondary toxicants are noticed in
growing waste streams in the global solid waste scenario. The authors major cities across the globe and have severe detrimental effects on
also projected the generation of different e-waste types till 2030 and human health, as shown in Fig. 3.
mentioned that these products would cover ca. 74 % of the entire e- For instance, unrecovered metals like As, Cu, Ni, Pb, Sb, Se, Sn, and
waste generation. Zn from discarded acid wastes have contaminated drains and surface soil
in Seelampur and Mandoli industrial areas in Delhi, India (Pradhan and
4. Hazardous content in e-waste and their impacts Kumar, 2014). In another study, elevated concentrations of PBDEs and
tetrabromobisphenol A were found in the indoor dust of television
E-waste contains a variety of hazardous metals, such as cadmium, recycling units in east China and Vietnam (Anh et al., 2017; Deng et al.,
mercury, etc., and chemicals, such as brominated compounds, poly­ 2014). Various PAHs such as anthracene, benzo(a)anthracene, chrysene,
aromatic hydrocarbons (PAHs), and plastics (Jadhao et al., 2022; Lecler phenanthrene, fluoranthene, and pyrene are detected in the recycling
et al., 2018). The content of e-waste and potentially toxic chemicals is and dumping sites of South China and Nigerian (Adeyi and Oyeleke,
expected to vary due to including electronic products with a short life­ 2017; Wang et al., 2012). Several studies indicated the presence of
span, such as mobile phones and computer products. Subsequently, the persistent organic compounds and heavy metals at the crude processing
e-waste shall contain a wider spectrum of metals besides tin, copper, and sites, including open burning and soil, water and other habitats exposed
lead, generally seen with PCBs. For instance, mobile phones contain ca. to the discharge of acidic effluents (Awasthi et al., 2016; Vaccari et al.,
1000 different components, most of which contain toxic heavy metals 2019). Fig. 4 presents the mechanism of various contaminant toxicity in
(Song and Li, 2014). A study by Cobbing in 2008 mentioned that 1450 humans.
tons of tetrabromobisphenol-A may have been used as a flame retardant Several researchers investigated the toxicological effects of e-waste
in manufacturing 990 million phones sold in 2006 (Cobbing, 2008). The and their potential impact on human and animal health and the
toxicity of e-waste depends, to a large extent, on the type of EEE. For ecosystem. Most metals are non-hazardous in their metallic form, but
instance, CRT screens, used in televisions a few decades ago, contain ca. they become hazardous when ingested/inhaled beyond a certain limit

Fig. 3. Hazardous impacts of heavy metals in e-waste on human health.

Adapted from Mitra et al. (2022) with permissions.

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S.S.V. Vuppaladadiyam et al. Science of the Total Environment 924 (2024) 171453

Fig. 4. Toxicity mechanism of various contaminants in humans.

(Grant et al., 2013; Ilankoon et al., 2018). Long-term exposure to e- hydrometallurgy or bio-metallurgy. Recycling involves several steps,
waste-based toxicants, such as PBDEs, PAHs, polychlorinated biphenyls, which include (i) disassembly and physical processes to recover non-
etc., may damage physiological systems, including the nervous, repro­ ferrous fractions, such as separation, (ii) enrichment of metals using
ductive, and endocrine systems. It is to be noted that chemical constit­ thermal or chemical processes and subsequent liberation using methods
uents derived from e-waste, such as PBDEs, PCDD/Fs, polychlorinated like pyrometallurgy, hydrometallurgy or electrochemical methods and
biphenyls, and PAH, are carcinogenic and also neurotoxic (Khan et al., (iii) purification and final recovery of metals. An overview of recovery
2019). Assessing the exposure of biomarkers and analyzing disease process is schematically presented in Fig. 5.
patterns among control and exposed participants can explain the risks
associated with human exposure to e-waste. A comprehensive review of 5.1. Pre-treatment methods
the health impacts of exposure to various toxicants associated with e-
waste recycling is available in the literature elsewhere (Ahirwar and Pre-treatment is required to optimize the efficiency by reducing the
Tripathi, 2021; Grant et al., 2013). In general, people living in the impurities, and it is essential in recycling operations to liberate targeted
proximity of e-waste recycling facilities are easily exposed to hazardous metals. Pre-treatment can include one or more steps of dismantling/
materials via all possible natural pathways (Khan et al., 2019; Li and disassembly, physical pre-treatment, thermal pre-treatment and chem­
Achal, 2020). For instance, a recent study in China revealed that ical pre-treatment (Dutta et al., 2023; Sethurajan et al., 2019). Accord­
compared to formal e-waste recycling facilities, people working at ing to Batinic et al. (2018), customized pre-treatment methods should be
informal recycling facilities had a higher potential for health risks from employed to have satisfactory separation and recovery of “mass rele­
toxicants such as heavy metals (Fang et al., 2013). vant” fractions in e-waste (Batinic et al., 2018). In addition, a significant
portion of REEs losses occur during the pre-treatment step, which affects
5. Recovery of REEs from e-wastes the final recycling efficiency.
Dismantling is a step to improve the recycling process by separating
Many researchers have studied the recovery of metals from WPCBs, the most valuable components containing metal parts from non-metallic
for instance, Oh et al. (Oh et al., 2003) separated magnetic and non- fractions and/or removing the hazardous components mentioned in
magnetic components of WPCBs through magnetic separation and WEEE Directive 2012/19 under Annex VII (Sethurajan et al., 2019).
then leached the non-magnetic metals, including Cu, Fe, Zn, and Al, Typically, after dismantling and disassembly, the metals and materials
using inorganic acids, such as H2SO4 and H2O2, and reported 95 % are separated one step further based on their physical characterization,
extraction efficiency. The recovery of metals generally happens in two such as electrical and magnetic features, weight, etc. (Batinic et al.,
stages: (i) magnetic separation for the removal of ferrous metals fol­ 2018). Sethurajan et al. (2019) mentioned that most of the pre-
lowed by (ii) pyrometallurgical or hydrometallurgical or electrodepo­ treatment process is manual, making it costly and labor-intensive, and
sition or a combination of these approaches to recover precious metals it is not technically and economically expected to become fully auto­
(Hsu et al., 2019; Kaya, 2016). Theoretically, combining different re­ mated soon(Sethurajan et al., 2019). Size reduction is the first step of the
covery processes will facilitate an effective recovery of precious metals physical pre-treatment, and the suitable size is determined based on the
with additional benefits such as creating revenue from each step, following treatment processes (Işıldar et al., 2018). Typically, for hy­
minimizing the use of toxic and hazardous chemicals, and operational drometallurgy processes, fine grinding (<200 μm) is more suitable,
ease and flexibility. By introducing pyrolysis as a pre-treatment step, it is while in pyrometallurgy, even relatively coarse materials can be used
possible to generate additional review by generating crude pyrolysis oil, (Sethurajan et al., 2019). In addition to the type of treatment process,
which can be processed to the required quality or directly used in boilers the degree of liberation is crucial and depends on both particle size and
to generate heat (Vuppaladadiyam et al., 2022). the type of e-waste (Sun et al., 2018) and it is a crucial factor in deter­
E-waste is often referred to as ‘urban mines’ as they are resource-rich mining separation efficiency (Sethurajan et al., 2019; Mudali et al.,
and contain REEs and other precious metals, especially Au, Ag, etc., at 2021). Primarily, shredder and hammer mills are used to reduce the size
significantly higher concentrations than their corresponding primary of e-waste (Sethurajan et al., 2019). Physical separation is the next
resources. The non-ferrous metals can be processed by pyrometallurgy, required step after size reduction that can be done through different

6
S.S.V. Vuppaladadiyam et al. Science of the Total Environment 924 (2024) 171453

Fig. 5. Overview of different steps and methods involved in the metal recovery process.

methods such as vibratory screening, density-based separation, electric complements pyrometallurgy and hydrometallurgy processes with more
conductivity-based separation, magnetic susceptibility, optical sorting, benefits (Binnemans and Jones, 2017). Each technique has some ad­
brittleness, and hydrophobicity of the phases (Cayumil, 2016; Sethur­ vantages and disadvantages. In this section, all methods are discussed in
ajan et al., 2019). Thermal treatment is generally applied on complex e- more detail.
waste containing many different components (de Marco et al., 2008),
including plastics mixed with precious, critical and rare earth metals 5.2.1. Pyrometallurgical process
(Hense et al., 2015). According to Işıldar et al. (2018) and Ramanayaka et al. (2020),
Roasting is another thermal pre-treatment method carried out in the pyrometallurgy is the most common industrial metal recovery process
presence of air used to oxidise solid metals. Forte et al. (2019), in a from waste electrical and electronic equipment (Işıldar et al., 2018;
recent study on the recovery of REEs from cathode-ray tubes (CRTs), Ramanayaka et al., 2020). A simple understanding of different steps
demonstrated that thermal roasting assisted in converting zinc sulphide involved in pyrometallurgy process considering waste printed circuit
to zinc oxide and facilitated selective leaching in the subsequent steps board as feed is presented in Fig. 6.
(Forte et al., 2019). In a recent study, Gergoric and his team investigated Pyrometallurgical process involves different approaches, which can
the effects of roasting on the leaching efficiency of REEs from NdFeB. be broadly categorized into thermal pre-treatment and extractive
The authors noticed that roasting improved the morphology of NdFeB metallurgical processes. Thermal pretreatment process includes incin­
powder and accelerated the leaching rate of REEs. In another study on eration and pyrolysis as pre-treatment steps, while extractive pyromet­
the recovery of REEs from neodymium magnets (NdFeB), Reisdörfer allurgical process involves smelting and roasting. Incineration involves
et al. (2019) noticed that roasting can convert all the available metals in burning carbon and binders at elevated temperatures in air or oxygen
NdFeB powder into metal oxides and increase the leaching selectivity as environment. It is worth noting that the selection of appropriate tem­
the solubility of rare earth oxides is significantly higher than the solu­ perature is crucial for the recovery of REEs from electronic wastes. Few
bility of cobalt and iron oxides (Gergoric et al., 2018; Reisdörfer et al., authors reported that maintaining an incineration temperature of 700 ◦ C
2019). Alkaline roasting can be utilized as a pre-treatment method to for 60 min resulted in an enhanced recovery rate of Li and Co (Liu et al.,
improve the selectivity for the recovery of metals in the leaching phase, 2023; Lombardo et al., 2020). The authors also mentioned that subse­
which is extensively used as a pre-treatment step for recovering REEs quent leaching rate also increased due complete removal of carbon,
from fly ash (Zhang et al., 2020). Chunfa et al. (2017) demonstrated that which otherwise may adsorb lithium salts. Pyrolysis allows the thermal
alkaline roasting can be applicable in some cases to recover REEs from e- decomposition of the e-waste in the absence of oxygen to produce high
waste and also conducted experimental investigations on alkaline calorific gas and oil, comparable to conventional fuels such as gasoline
roasting of waste fluorescent powder. The authors mentioned that and diesel, for energetic utilization (Evangelopoulos, 2014; Hense et al.,
alkaline roasting effectively converted Al2O3 into water-soluble NaAlO2, 2015). At the same time, pyrolysis takes the advantage of thermal
facilitating nearly 99 % of rare earth metals (REMs) recovery (Chunfa instability of organic compounds and acts as an extra separation stage
et al., 2017). that results in better REEs recovery (Vermeșan et al., 2019). In a recent
study, Khanna et al. (2018) used horizontal resistance and thermal
5.2. Existing REEs liberation technologies plasma furnaces to demonstrate that pyrolysis carried out under the
plasma furnace could achieve higher REEs recovery(Khanna et al.,
Pyrometallurgy and hydrometallurgy processes are the most widely 2018). Debnath et al. (2018) also explained that plasma technology
used approaches to recover metals from e-waste (Ambaye et al., 2020). provides a high-temperature and environmentally friendly approach for
Solvometallurgy has also attracted much attention as this approach metal recovery from e-waste(Debnath et al., 2018). Typically,

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S.S.V. Vuppaladadiyam et al. Science of the Total Environment 924 (2024) 171453

Fig. 6. An illustration with different steps involved in pyrometallurgy approach.

pyrometallurgy is used to recover non-ferrous metals through smelting, atmosphere at a temperature of 1000 ◦ C for 30 min and noticed the
incineration, and roasting in the presence of selective gases at a very residue obtained after roasting presented excellent recovery rate for Li
high temperature (Li et al., 2019; Ramanayaka et al., 2020). According and Co when subjected to leaching (Liu et al., 2019a). Salt assisted
to Sethurajan et al. (2019) and Ambaye et al. (2020), despite the high roasting and microwave roasting are two commonly used methods
desirability of the pyrometallurgical process in regards to high reaction under roasting approach. Smelting is another effective pyrometallurgi­
rate, which makes a very efficient separation for any e-waste, it has some cal approach to recover REEs from e-waste. In smelting process, the
economic and environmental disadvantages such as high energy con­ material is heated above its melting point and the metals are separated
sumption, the release of toxic gases and volatile metals, high GHG in the liquid phase by reduction and subsequent formation of immiscible
emission, high capital cost, and slag generation(Ambaye et al., 2020; molten layers (Makuza et al., 2021). The advantage of smelting process
Sethurajan et al., 2019). In addition, it is to be noted that pyrometallurgy over roasting lies in direct use of unsorted and untreated e-waste into the
is unsuitable for low-volume streams such as PCBs and LEDs (Sethurajan high-temperature reactor. Among the available pyrometallurgy pro­
et al., 2019). Both incineration and pyrolysis are carried out at tem­ cesses, smelting is considered as a vigorous process, which includes
peratures between 600 and 900 ◦ C. Whille incineration is done in the modern equipment such as Mitsubishi continuous smelter, Noranda
presence of air/oxygen, pyrolysis is carried out in an inert atmosphere. reactor system, and Outokumpu flash smelting. Smelting is generally
Roasting and smelting are two important extractive pyrometallur­ carried out in the range of 600 to 1200 ◦ C in a combustion chamber
gical processes that are used to process e-waste at temperatures (Dutta et al., 2023). Recently, Chen and his team developed a novel
>1000 ◦ C, in the absence of aqueous media (Makuza et al., 2021). strategy of Cu matte smelting in e-waste recycling. The authors inves­
Similar to the other thermal processes, roasting is also an exothermic tigated the behaviour of trace metals between iron-silicate slag and
process generally requires a pre-treatment step. Carbothermic reduction copper matte at 1250 ◦ C. The operational conditions for different pre­
roasting method employs a reducing agent such as carbon/coke and treatment and pyrometallurgical processes are mentioned in Table 1.
heats the cathode material leaving carbon residue and mixture of alloys
and impure metal oxides. The mixture is then refined to produce 5.2.2. Hydrometallurgical process
precious metals (Fig. 6). Liu and Xiao carried out carbothermal reduc­ Hydrometallurgy is a two-step process including (i) leaching, in
tion roasting of NMC cathode material at a roasting temperature and which metals from e-waste dissolve in a chemical aqueous media, and
time of 650 ◦ C and 30 min and carbon dosage of 10 %. High recovery (ii) recovery, in which the dissolved metals are selectively extracted
rates for Ni, Mn and Co were noticed, which were 98.68 %, 98.08 %, and from leachate (Sethurajan et al., 2019). Although compared to pyro­
93.33 %, respectively (Liu et al., 2019a). Li and his co-workers inves­ metallurgy, hydrometallurgy has some drawbacks, such as sludge gen­
tigated roasting approach on a mixture of LiCoO2 and graphite under N2 eration, heavy metal pollution, and toxicity (Sethurajan et al., 2019),

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S.S.V. Vuppaladadiyam et al. Science of the Total Environment 924 (2024) 171453

Table 1
Summary of operational conditions for different thermal pre-treatment and pyrometallurgical processes (Bose and Singh, 2019; Chen et al., 2018; Kaya and Kaya,
2019; Liu et al., 2020).
Treatment Technique Media Temperature Emission
range (◦ C)
Particles Heavy Non-metallic fumes
metal
fumes

Desoldering General General 225–265 – Pb Acetaldehyde, benzene, xylene, styrene

Incineration Uncontrolled Air/oxygen 600–950 Fly ash (as carbon and Cd, Hg, Polybrominated biphenyls (PBBS),
metals) Cr, Pb, Zn, bromobenzene series and bromophenol
Sn, Sb (PBPh), polycyclic aromatic hydrocarbons
(PAHs), polychlorinated dioxins, furans, acid
fumes, brominated hydrocarbons, aliphatic
hydrocarbon
Controlled Air/oxygen 1000–1250 H2O, CO2
(modern)
Sorting and Dry methods of General 25 Dust (include metals and – –
upgrading size reduction and non-metals)
sorting
Pyrolysis Without halogen Inert 200–1150 – – CO, CO2, SO2, NOx, HBr, CH3Br, C2H5Br,
stabilization brominated aromatics, PBDD, BFs
(fixation)
With halogen 200–1150 – – CO, H2, CO2, H2O
stabilization
(fixation)
Roasting Roasting Reducing agent (Coke/ 170–470 – – CO, SO2, NOx
coal)
Salt-assisted Sulfation agents such as – – SOx
roasting SO2(g), MgSO4, NH4SO4,
NaHSO4⋅H2O, or Na2SO4
Smelting Smelting Reducing agent (Coke/ 1200–1300 Dust of carbon and metals Zn, Pb, Sn CO2, CO, SO2, NOx, Br2, HBr, chlorinated and
coal) (Zn, Pb, Sn, Cu, Ag, Cd, Sb. brominated polycyclic aromatic hydrocarbons
in different forms of
elemental, bromine, or
oxide)

hydrometallurgy is the preferable technique as it has lower GHG, toxic phase. In the leaching step, a suitable chemical lixiviant is introduced to
gas, and dust emission and lower energy consumption (Diaz et al., the slag, leading to the mobilisation of metals (Priya and Hait, 2017).
2016). At the same time, it has higher efficiency, no slag generation, Acids are the main solvents in this step, which convert metals into sol­
lower capital cost, and easier working conditions(Diaz et al., 2016). uble salts in aqueous media (Habib et al., 2020). In this section, the most
Different steps involved in hydrometallurgy to liberate REEs from e- important leaching parameters are discussed. Lixiviant is generally a
waste and their subsequent recovery are presented in Fig. 7. The first liquid medium (mostly acids) used to selectively extract the targeted
step of the hydrometallurgical process is the leaching of metals from e- metals from the electronic waste. The lixiviant type can significantly
waste. Leaching is, in fact, the mass transfer from a solid to a liquid affect the efficiency of REEs leaching depending on the type of e-waste

Fig. 7. Summary of hydrometallurgical leaching and metal recovery techniques.

Source: NCBI (2023).

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S.S.V. Vuppaladadiyam et al. Science of the Total Environment 924 (2024) 171453

and ions introduced (Yang and Honaker, 2020). Summaries of using recovery from e-waste since these acids are not as strong as inorganic
different acids in leaching REEs from different e-waste have been pro­ acids and are benign to the environment. Moreover, the low cost of some
vided in the following tables. organic acids, such as citric acid, can help develop more cost-effective
The data in Table 2 summarizes studies that considered different leaching approaches (Astuti et al., 2016). Oxalic acid is also a good
acids as leaching agents in recovering REEs from different types of e- candidate for leaching as it has fungi origin (Wang et al., 2015) and its
waste. Yan et al. (2014), demonstrated that inorganic acids are more hydrogen liberation degree is higher than other acids (Kareem et al.,
effective leaching agents in leaching heavy metals from contaminated 2010). The data collected from the literature review show that although
sediments than inorganic acids (Yan et al., 2014). In addition, the au­ organic acids have demonstrated the ability to leach REEs from elec­
thors also mentioned that different organic acids have different effec­ tronic waste, these acids have been employed for leaching REEs from
tiveness in leaching heavy metals. For example, acetic acid showed a only a few types of e-waste. Since hydrometallurgy has been a desirable
higher leaching efficiency than citric, maleic, and succinic acids. Liu way to recover REEs, many patents have used this technique along with
et al. (2019c) studied the efficiency of organic acids in leaching Li and new modifications for one or more steps of pre-treatment, leaching, and/
Co from the cathodic material of spent lithium-ion batteries and re­ or recovery to enhance the entire approach for the recovery of REEs. A
ported different leaching efficiencies (Liu et al., 2019c). In another summary of these patents has been provided in Table 3.
study, Jadhav et al. (2017) explained that a specific acid can show
different leaching efficiencies depending on the type of targeted mate­ 5.3. Recovery
rial, indicating that choosing an appropriate acid for targeted metals is
crucial because of impurities in targeted materials(Jadhav et al., 2017). After leaching as the first step of hydrometallurgy, the recovery of
According to the studies mentioned in Table 2, it is worth noting that metals from the leachate solution is the next step. The recovery step is
the acid concentration has a significant impact on REEs leaching from e- the final and critical step in extracting and purifying targeted metals in
waste. In the study done by Lee et al. on NdFeB magnet waste, the au­ metallurgical processes. The most common methods for metal recovery
thors demonstrate that an increase in sulfuric acid and hydrochloric acid from leachate include precipitation, electrochemistry, and solvent
concentration increased the amount of Nd leached (Lee et al., 2013). extraction (Priya and Hait, 2017). Since each method has strengths and
Behera and Parhi (2016) also demonstrated that organic acid concen­ weaknesses, a combination might be employed in some cases to maxi­
tration showed similar behaviour on Nd leaching from NdFeB magnet mize the recovery of targeted metal/metals. A summary of the most
waste (Behera and Parhi, 2016). Liu et al. (2021) demonstrated that common recovery techniques has been presented to understand their
using oxalic acid as a leaching reagent can simplify the process of REEs merits, demerits and challenges.
recovery from NdFeB magnets and achieve good precipitation results. In
addition, the authors also mentioned that using oxalic acid as a leaching 5.3.1. Solvent extraction
agent can leach iron into the solution and precipitate the REEs in their As stated by Lazo (2019), solvent extraction is the most common
oxalate form (Liu et al., 2021). recovery approach used for REEs in industry. Solvent extraction is a
It is worth noting that a comparison between pyrometallurgy and selective liquid-liquid method for complex mixture separation. In this
hydrometallurgy techniques may provide meaningful insights to un­ technique, there are two immiscible liquids (Lazo, 2019). Typically, one
derstand the potential merits and demerits of each process. After pre- of the liquids is an aqueous phase, and the other is an organic phase. The
treatment processes (shown in Fig. 5), both pyro- and hydrometallur­ principle of solvent extraction is based on differential solubilities in
gy processes are needed for an effective recovery process. It is to be those two immiscible liquids. In this method, the targeted solute pre­
noted that a single process could not be considered as an effective re­ sented in the first liquid is soluble in the second immiscible solvent. The
covery process and both pyro- and hydro-metallurgy approaches are solvent extraction method is generally employed where distillation is
highly encouraged in this context. In summary, the merits and demerits not applicable when materials are non-volatile, have very close boiling
of both the techniques are as follows. Pyrometallurgy offers high purity points, and are sensitive to heat. The criteria of choosing the appropriate
yields and simple in operation. Approaches such as roasting and solvent for the solvent extraction process include low cost, non-
smelting offers flexibility in the recovery process. However, pyromet­ corrosive, non-flammable, and have a high-density difference, which
allurgy is an energy intensive process and the residue required further facilitates using gravity to maintain a counter current flow of the phases
processing. On the other side, hydrometallurgy is less energy intensive (Thornton, 2011). According to Rao et al. (2021), the solvent extraction
and the metals can be separated with high purity. Also, hydrometallurgy is highly sustainable since it needs fewer extraction stages than other
offers good extraction kinetics and high selectivity. For instance, hallow methods. Rao et al. (2021) explained that solvent extraction is a very
fibre membranes offer high selectivity, which facilitates in single stage selective method that separates targeted metals from a mixture of metals
extraction. However, hydrometallurgy is highly criticized for the in an aqueous solution (Rao et al., 2021).
exhaustive use of reagents that are toxic and hazardous in nature. A Solvent extraction has three steps: extraction, scrubbing and strip­
summary of advantages and disadvantages is presented in Table S1 of ping. Solvent extraction has many advantages over other extraction
Supplementary Information. methods, including being a faster technique, continuous process,
Based on the experiments conducted on NiMH batteries waste to economical and highly concentrated solutions. However, the major
study the change of acid concentration on leaching REEs, Yang et al. disadvantage of of solvent extraction method is the requirement of a
(2014) demonstrated that an increase in hydrochloric acid concentra­ high number of stages (sometimes >100) to achieve the desired sepa­
tion has a direct relationship with REEs leached (Yang et al., 2014), ration efficiency (Lazo, 2019). According to Jha et al., the most common
while Korkmaz et al. (2018) showed an increase in sulfuric acid con­ organic solvents used for REEs extraction include Cyanex 272, D2EHPA,
centration from 2 M to 14 M resulted in an increase first and then a PC 88A, TBP, Kelex 100, LIX 84, Versatic 10 and Aliquat 336 (Jha et al.,
decrease in different REEs leached from the NiMH batteries (Korkmaz 2016). Table 4 shows that solvent extraction has been used in many
et al., 2018). Alonso et al. (2012) and Liu et al. (2019a) showed that an studies with a very high efficiency for REEs recovery.
increase in sulfuric acid concentration lead to an increase in REEs and La
leaching from NiMH battery waste (Alonso et al., 2012; Liu et al., 5.3.2. Precipitation
2019b). Comparing the results of leaching via organic acids with the After completing the leaching stage, the precipitation method can
results gained from inorganic acids demonstrates that organic acids, purify the targeted metal/metals as an extraction technique. For pre­
including citric acid, acetic acid, oxalic acid, maleic acid and glycolic cipitation, a precipitating agent is a driver which converts the targeted
acid, can effectively leach REEs by >90 % from electronic waste. These metal or impurity to an insoluble compound. The most common
results are promising in developing eco-friendly approaches for REEs precipitating agents for REEs precipitation are sulphate, carbonate,

10
 S.S.V. Vuppaladadiyam et al.
Table 2
Leaching of REEs from different e-waste sources.
Leaching E-waste Pre-treatment Acid concentration Reducing Time (min) Temp. S/l Pulp density Particle size rpm Leaching yield Ref.
agent category agent ratio

Inorganic acids
Nitric acid Nd magnet 1M 0.3 H2O2 20 80 ◦ C 83.3 g/l 98 % Nd (Rabatho et al.,
81 % Dy 2013)
Fluorescent Drying at 100 ◦ C. 2M ≥24 h 20 ◦ C 10 % w/v 200 >95 % Y, >80 % Eu (Pavon et al.,
lamps 2019)
Sulfuric acid Nd magnet 0.1/0.5/1/3/6 N 15 27 ◦ C 1:50 <0.297 mm 5.02/5.64/8.14/100/ (Lee et al., 2013)
100 % Nd
Fluorescent 4N 24 h 90 ◦ C 20 % >90 % 200 85 % of Y (De Michelis
lamps between 40 et al., 2011)
and 500 mm
NiMH waste Roasting at 850 ◦ C for 2 2/4/6/8/10/12/14 M 1h 25 ◦ C 1:5 <38 μm 500 90.5/93.4/91.4/ (Korkmaz et al.,
h 93.8/92.3/93.8/84 % 2018)
La
Hydrochloric Nd magnet Roasting in 850 ◦ C 0.5 M 300 368 K 100 g/l 500 98 % REEs (Kumari et al.,
acid 2015)
NiMH Drying at 100 C for 1 h
◦
5/15/20 % 100 min 70 C
◦
1:10 74 450 45.67/87.12/98.89 % (Yang et al.,
battery REEs 2014)
Fluorescent Alkaline leaching with 3M 8 % H2O2 1.5 h 75 ◦ C 1:11 99.8 % REEs (Chunfa et al.,
lamps NaOH (850 ◦ C, 2 h and S: 2017)
L equal to 1:1.6)
Phosphoric Nd magnet 3M 0.3 M 120 80 ◦ C 100 g/l 94 % Nd (Rabatho et al.,
11

acid H2O2 99 % Dy 2013)

Organic acids
Citric acid Nd magnet Roasting at 900 ◦ C for 1M 60 90 ◦ C 1:20 400 72.8 % Nd (Reisdörfer et al.,
480 min 2019)
Acetic acid Nd magnet Roasting at 400 ◦ C for 1M 1440 23 ± 1 ◦ C 1/30 g/ml <355 μm 400 >95 % REEs (Behera and
1.5 h Parhi, 2016)
CRT Roasting at 850 ◦ C for 1 M acetic acid/2 M 2 h 1st 25 C 1st
◦
10 ml/g 1st <425 2500 24.8 wt% Y and 1.4 wt (Forte et al.,
20 min methanesulphonic acid step/24 h step/90 ◦ C step/20 ml/ % Eu 1st step/90 wt% 2019)
2nd step 2nd step g 2nd step of Y and Eu
NiMH Evaporation/ 5 % v/v 600 min 25 ◦ C 230 9.6 % m/m (Zambrano-
battery crystallization in an oven Colmenares
at 70 ◦ C et al., 2018)

Science of the Total Environment 924 (2024) 171453

Formic acid NiMH Drying at 105 ◦ C for 3 h 5 M/10 M 3h 40 ◦ C 100 g/l <100 40 wt%/100 wt% La (Gismonti et al.,
battery 2021)
Malic acid Nd magnet – 1M 60–360 90 ◦ C 1:20 400 79.9 %/99 % Nd (Reisdörfer et al.,
2019)
Ascorbic acid Nd magnet 1M 400 25/70 ◦ C 1/80 400–1000 50 %/95 % Nd (Gergoric et al.,
2018)
Glycolic acid Nd magnet 1M 400 25 ◦ C 1/80 g/ml 400–1000 95 % Nd (Gergoric et al.,
2018)
Oxalic acid Nd magnet 2M 360 90 C
◦
60 ml/g 400 93.17 % precipitation (Liu et al., 2021)
rate of rare earth
oxalate
S.S.V. Vuppaladadiyam et al. Science of the Total Environment 924 (2024) 171453

Table 3
List of patents using leaching for REEs recovery.
Feed Leaching Recovery Efficiency Patent Number Ref.

Fluorescent powder e- HCl 1st, HNO3 2nd & H2SO4 3rd Bis-2-ethylhexyl‑hydrogen phosphate in toluene 1st/ 96.2 % Y EP 3556873A1 (Patil, 2018)
wastes methyltrioctyl ammonium chloride 2nd/bis-2- 95.6 % Tb
ethylhexyl‑hydrogen phosphate in toluene 3rd 55.1 % Gd
Waste phosphor H2SO4 Di-(2-ethylhexyl) phosphoric acid/2-ethylhexyl 2- >95 % and >99 US20130309150A1 (Thakur and
powders ethylhexylphosphonic acid % Y, Eu, Ce and Kumar, 2022)
Tb
Luminescent HCl Na2SO4 >90 % REEs WO2014023092A1 (Zhang, 2012)
materials
NdFeB HCl <70 % & <80 % WO2014013929A1 (Hino EaS,
2015)
Fluorescent powder H2SO4, glacial acetic acid >99.99 % Eu CN102115822B (Wu, 2010)
and polishing oxide
powder waste
Ore H2SO4 bake and water leaching/ Precipitation by adding Na2CO3/after re-leaching, re- >70 % REOs WO 2016/011540 (Dreisinger and
re-leaching after first precipitation by adding oxalic acid recovery Al Verbaan, 2016)
precipitation with HCI, HNO3 or
H2SO4
Neodymium iron HCl, then air oxidation pre- Precipitating by adding H2CO3 >98 % REEs CN102206755B (Jian, 2011)
boron waste treatment carried out leaching
A waste and old rare Ultrasonic immersion of NaOH Filtering, adding Na2SO4 into the filtrate for reaction; >92 % REEs CN103233123A (Jiang, 2013)
earth capacitor then leaching with H2SO4 with filtering the reaction solution recovery
batteries H2O2
Waste phosphor HCl, H2SO4, or HNO3 with H2O2 Solid-liquid separation, then precipitation by adding 91 %–98.8 % CN102312098B (Mei, 2011)
powder oxalic acid Y2O3 recovery
Rare earth polishing HCl Precipitating by adding oxalic acid >90 % REOs CN103103361A (Liu, 2013)
powder waste recovery

fluoride, phosphate, and oxalate (Han, 2020). In general, the precipi­ current flows from the cathode and the anode is placed in the leaching
tation process is either selective precipitation or coprecipitation. In the solution, anions move toward the anode and cations move toward the
selective precipitation method, it is possible to precipitate the impurities cathode, then targeted metals as cations deposit in the cathode (Xu et al.,
and targeted metals separately and, as a result, achieve a higher purity of 2020). The electrowinning method has been used for many years in the
targeted metals at the end, even though it can also lead to the loss of industry for metals separation since the electrowinning process has been
some of the REEs during the removal of impurities. Zhang and his team a more economical approach than the other separation methods for
mentioned that using selective precipitation for extraction of REEs from purifying metals from leaching solutions (Robinson et al., 2003) Kondos
NdFeB magnets, by adding NaOH as the first precipitating agent, Fe is and his team noted the advantages of electrowinning, including no
precipitated as Fe (OH)3 and Nd and Dy are also precipitated later and sludge generation, no need for chemicals, easy maintenance, easy
after adding H2C2O4 as the second precipitating agent (Zhang et al., operation conditions, low capital cost, and low operation cost. The au­
2020). By using this method, authors reported a recovery of 91.5 % of thors alos mentioned that the feasibility of combining electrowinning
Nd and 81.8 % of Dy. In coprecipitation, valuable metals recover with other techniques, which can achieve a more efficient and cost-
simultaneously, and usually, the powder achieved as precipitation of effective metal separation process (Kondos et al., 1991). Some factors
this process is used as the raw materials for other applications. In such as pH, temperature, metal ion purity and concentration, acid
addition, Zhang et al. (2020) stated that using the coprecipitation concentration, plus current density have crucial impacts on the final
method on the leaching solution from NdFeB magnets ends up with a product metal composition and yields (Holm and O’Keefe, 2000).
composite powder containing REEs, Co, and Fe elements, which can be
used as raw material for recycled NdFeB magnets preparations(Zhang 5.3.4. Metal-organic framework (MOF)
et al., 2020). According to Han (2020), pH has a crucial role in REEs Metal-organic frameworks (MOFs) have recently gained much
precipitation, and the appropriate pH range for REEs precipitation attention in the recovery of metals from complex water mixtures due to
strongly depends on the precipitator or precipitating agent type (Han, their extraordinary ability to selectively adsorb a high amount of tar­
2020). geted metals (Li et al., 2018). One reason MOFs are more favourable is
the possibility of post-synthetic modification of their adsorption sites
5.3.3. Electrochemical (Wang and Cohen, 2009). According to Kavun et al., unlike other
Electrochemical metal recovery is a selective metal recovery methods used for recovering REEs from e-waste, which have high
approach that can be used to recover REEs from e-waste. The electro­ operating costs and high REEs losses, adsorption with MOF is a more
chemical approach needs much less chemical, is easily controlled, re­ effective, selective and low-cost method (Kavun et al., 2021). In a study
quires less energy, and is more environmentally friendly than other by Sun and his co-workers, the authors reported a 90 to 99 % efficiency
methods (Rai et al., 2021). Higher sustainability in the electrochemical in recovering gold from different complex solutions, including medium
method due to avoiding the extensive use of toxic chemicals and obtained from e-waste by using MOFs (Sun et al., 2018). Elsaidi et al.
external energy requirements, no secondary waste generation and harsh noticed a 99.99 % recovery of REEs from aqueous and brine solutions by
pH conditions (Kim et al., 2021). using magnetic MOFs (Elsaidi et al., 2018). Kavun et al. (2021) stated
Based on the studies conducted by Kim et al. (2021), there is the that despite all the advantages of using MOFs as an adsorber, there are
potential to design suitable platforms for the selectivity of the targeted still some uncertainties regarding the effectiveness of using MOFs for
minor ions mixed with the excess competing ions, making the electro­ separating REEs in the presence of other metals (Kavun et al., 2021).
chemical recovery approach a desirable method for the recovery of REEs
(Kim et al., 2021). Electrowinning is an electrochemical process and a 5.3.5. Solvometallurgy
separation technique that utilizes a direct current to separate metal ions Solvometallurgy has recently emerged as a metallurgical metal re­
present in the leaching solution. In the electrowinning method, when the covery technique with high similarity to hydrometallurgy. However,

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S.S.V. Vuppaladadiyam et al. Science of the Total Environment 924 (2024) 171453

Table 4 Table 4 (continued )

Extraction methods used for recovery of REEs from e-waste. Recovery E-waste Conditions Recovery Reference
Recovery E-waste Conditions Recovery Reference method yield
method yield
Multi-metal Using aqueous, 86–96 % (O’Connor
Precipitation Fluorescent Oxalic acid 20 % 97 % for all (Ippolito waste 100 mM Eu, Nd, Ga, et al.,
lamps in excess, at REE et al., Na2SO4. Ga was and Sc 2018)
room 2017) prepared in100
temperature for mM NaCl as a
1 h. supporting
NdFeB 10 % excess 2 M 91.7 %, (Diaz electrolyte
magnet NaOH, 2 h at 66.7 %, and et al., composition
70 ◦ C. 54.9 % for 2016) Unaligned
Pr, Nd, and carbon
Dy nanotubes
CRT Using oxalic acid (>99 wt%) (Forte encapsulated in
phosphor At 25 ◦ C and for mixed Y/Eu et al., polyvinyl
waste 30 min and 500 oxalate 2019) alcohol filters
rpm
Nickel- Adding 300 % 95 wt% of (Korkmaz
metal excess of oxalic REEs et al., Solvometallurgy has a fundamental difference from hydrometallurgy.
hydride acid at 25 ◦ C for 2018) Solvometallurgy does not need an aqueous solution for metal extraction;
batteries 24 h
it uses non-aqueous solvents instead (Li et al., 2018). The absence of the
Solvent CRTs DEHPA at a 68 % (De la
extraction concentration of yttrium Torre water phase in solvometallurgy has led to different extracting mecha­
0.5 mol/l with a oxide et al., nisms compared to hydrometallurgy. Solvometallurgy has shown more
contact time of 5 2018) advantages than hydrometallurgy, such as process intensification, high
min and using n- selectivity in the leaching stage, no gel silica formation, and water, acid,
heptane as a
diluent.
and energy consumption reduction (Binnemans and Jones, 2017). The
Extraction of capability of metals recovery even with low concentration, suitability
europium using for urban waste treatment, and compatibility with bioleaching are the
HNO3 of 120 g/l other advantages of solvometallurgy (Binnemans and Jones, 2017). The
concentration,
list of advantages and disadvantages for various recovery methods dis­
extraction of
yttrium using cussed above is given in Table 5.
HCl of 300 g/l
concentration,
four times the
stoichiometric
amount of oxalic
acid for yttrium
precipitation
Flat Panel Di-(2- 99 % (Yang Table 5
Display Ethylhexyl) yttrium et al.,
Advantages and disadvantages of various recovery methods based on our anal­
waste phosphoric acid 2016)
(DEHPA) was
ysis of literature review.
used as the Method Advantages Disadvantages
extractant and
kerosene was Solvent extraction • Targeted recovery of • Large amounts of harsh
used as the metals solvents required
diluent followed • Established industry • Number of recovery stages
by stripping with practise is usually very high
HCl at room Precipitation • Targeted metal recovery • Co-precipitation of
temperature (21 has been achieved only competing metal ions is
± 1 ◦ C), after numerous recovery observed leading to loss of
NdFeB D2EHPA in 129 ± 55 (Gergoric steps quality
magnets Solvent 70 separation et al., • Can be achieved using • Lack of industrial
At 25 ± 1 ◦ C and factors Nd/ 2018) milder, less toxic solvents applicability due to this
1500 rpm Fe such as sodium hydroxide technique now replaced
Hard disc Using 1 M NaOH 72.3 % Nd (Erust in low strengths entirely with solvent
drives for 99.8 % iron and 66.3 % et al., extraction followed by
precipitation at Dy 2021) precipitation.
pH 4.5 and 25 ◦ C Electrochemical • Highly selective recovery • Requires relatively less
in 1.5 h. Using recovery of metals has been competing metal ions to
(D2EHPA) and achieved through electro achieve high recovery.
(CYPHOS® dialytic techniques
IL101), with 0.2 • Low capital cost in • Industrial applicability is
M ionic liquid in comparison with solvent yet to be fully realised and
30 min extraction technique is subject to the cost of
Electrochemical NdFeB Using 99.4 % (Xu et al., recovering a mixed metal
magnets (NH4)2SO4, purity of 2020) feedstock
Na3Cit, H2SO4 as Nd, Dy and Metal organic • Selective and low-cost • Not effective in the
supporting Pr frameworks technique presence of large number
electrolyte (MOF) of competing metal ions
composition • Surface functionalized • Cost of MOF
The magnet is MOF’s can reduce capital manufacturing is still quite
used as anode costs often associated high and will take time for
with solvent extraction this technique to be fully
technique. realised at industrial scale

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S.S.V. Vuppaladadiyam et al. Science of the Total Environment 924 (2024) 171453

6. Lifecycle assessment for REEs recovered from secondary adapt to the ever-evolving challenges posed by e-waste (Adeyi and
sources Oyeleke, 2017).

Life cycle assessment (LCA) is a well-known methodology to under­ 8. Gaps and recommendations
stand the environmental impacts of products/commodities over the
entire lifecycle (Hengevoss et al., 2024). LCA takes in to account the Insights into developing new and novel recycling technologies for
material processing, usage and end-of-life (EoL) stages and involves the recovery of REEs from electronic waste encounters the challenges
material and energy flow of upstream and downstream processes over and issues encountered during the processing of raw materials and with
the product complete lifecycle (Jyothi et al., 2020). In general, LCA is the limited availability against demand. Based on the literature survey,
composed of three basic steps: (i) identifying environmental loads such the basic challenge in the recovery of REEs from e-waste includes the
as raw material and energy, (ii) evaluating the environmental impacts of application of existing processes, which are designed for the recovery of
loads identified in step 1 and (iii) accessing environmental protection base and precious metals, for the recovery of REEs. Investigations on
and prospects of generating valuable products from wastes. Several integrating REEs recovery with the recovery of base and precious metals
studies are reported on identifying the environmental impacts of are crucial for the commercial-scale application. Based on the under­
recovering REEs from secondary sources. However, it is worth noting standing gained from this review, we stress the need to understand the
that authors reported contradicting opinions, which can be attributed to techno-economic and environmental viability of previously validated
the variations in scope and boundary considered in their studies. For lab-scale processes at a large scale.
instance, Liu and Keoleian conducted an LCA based study for lighting Although the pyrometallurgical approach is beneficial in recovering
waste management and subsequent recovery of REEs and critical metals some metals, it cannot recover the REEs lost in slag. In addition, the
from LED bulbs. The authors reported that recovering REEs and other pyrometallurgical processes, despite being straightforward, emit toxic
critical metals from lamp waste via hydrometallurgy route had more gases during the thermal degradation of organic compounds. Further­
environmental impacts than producing from primary resources. The more, the high energy demand and corrosion problems make the process
global warming impact and CO2eq for every kg gallium (Ga) recovered costly. It is worth noting that, although pyrometallurgical processes
was significantly high and were noticed to be 74 kg and 3687 kg. The offer excellent recovery rates for feedstock with high REE concentra­
higher impact was mainly due to the low Ga concentrations in lamp tions, it may not be suitable for low-grade e-waste. In addition, the
waste (Liu and Keoleian, 2020). Borrirukwisitsak et al. conducted the availability of inherent toxic elements may generate harmful emissions.
LCA for a variety of electronic wastes including refrigerator, air condi­ Therefore, it is worth noting that pyro-processing routes cannot be
tioner, smart phone, personal computers and LCD TVs. The authors considered as effective stand-alone recovery pathways. Hydrometallur­
noticed that ecotoxicity and human toxicity were identified as potential gy, on the other side, is considered as a promising approach for the re­
impact categories during dismantling stage (Borrirukwisitsak et al., covery of REEs from e-waste. However, several issues are to be
2023). Sprecher and his team conducted LCA study on recovering per­ addressed on upstream (leachate) and downstream (solvent extraction)
manent magnets from computer hard disks and compared the environ­ stages of operation. It is worth noting that e-waste contains REEs in
mental impacts against virgin permanent magnet (VPMs) LCA. The diverse forms, from oxides to alloys, and majority of them are insoluble
authors compared human toxicity and climate change under both the even under strong acidic or alkali conditions. Pre-treatments such as
scenarios. While the human toxicity value was reported as 150 for VPMs, roasting at high temperatures is beneficial before leaching. Most of the
the value was 3.6 and 28 for unit kg 1,4-DCB-Eq. for permanent magnets leaching studies have been focused on identifying alternatives to inor­
recycled via handpicking and shredding, respectively. Similarly, climate ganic acids, and the other options include organic acids and ionic liq­
change values were 27, 3.3 and 10 CO2eq. for VPMs and permanent uids. The application of alternative leaching agents is limited to NdFeB
magnets recycled via hand picking and shredding, respectively magnets. However, there is a need to extend these leaching agents to
(Sprecher et al., 2014). other forms of e-waste and test their potential under varied operational
conditions. There is an immediate need to focus on innovative modifi­
7. E-waste legislation in Australia cations, such as using ionic liquids and liquid membranes in hydro­
metallurgical processes to develop a technically superior,
To combat the escalating challenges associated with e-waste, a Na­ environmentally benign, and economical recycling process. In addition,
tional Waste Policy was brought into existence by the Australian gov­ given their chemical similarities, novel separation techniques need to be
ernment in 2019. By integrating existing policies and regulatory developed to isolate individual REEs. Thus, further studies must
frameworks, the National Waste Policy aimed to enhance the effec­ emphasize the need to develop a unified process capable of dealing with
tiveness of e-waste management in Australia (Adeyi and Oyeleke, 2017). different e-waste types economically and environmentally stable.
The National Product Stewardship Scheme, in association with in­ Another key challenge is the unavailability of stringent norms for
dustries and the State and Territory Governments, was also introduced recycling e-waste, which are not in consistency with time or are not
in 2011 (Zhao et al., 2021). Implementing the National Waste Policy in properly enforced. It is worth mentioning that recycling REEs from
2019 set a path for Australia’s resource recovery and management of e- secondary sources can help avoid 1.5 times radioactive waste per ton of
waste over 10 years between 2010 and 2020. Several objectives, such as REEs. However, current REE recovery processes are difficult and costly.
agreements with international accords, like the Basel and Stockholm For instance, neodymium rubidium iron boron products often contain a
Conventions, minimize e-waste generation and ensure the safe and metal layer coated on the surface to avoid oxidation, therefore, making
environmentally sound treatment, disposal, recovery, and reuse of e- the extraction of neodymium a difficult and costly task. In addition, it
waste (Ahirwar and Tripathi, 2021). Furthermore, the Product Stew­ also contains a metal layer. Such issues can be addressed by combining
ardship Act enacted in 2011 established a framework for effectively pyrometallurgy and hydrometallurgy, which is not yet mature. How­
managing the health, safety and environmental impacts of electrical and ever, research in this direction would certainly lead to the development
EEEs and recycling and disposal (Pradhan and Kumar, 2014). Presently, of minimal chemical and energy intensive ideas in the future. Further­
the e-waste management system in Australia is still developing. While more, initiatives from the governments, such as promoting a technology
significant progress has been made since the inception of the National by providing subsidies or by investing in specific research, could pro­
Waste Policy and the Product Stewardship Act, there has been a three- mote recycling as an effective tool among the general public. However,
fold increase in the e-waste generation rate in Australia compared to the major challenge in recycling e-waste is the low quantity of REEs
other waste streams. Hence, it is imperative to enhance the capacity and available in each device.
technology of the nation’s systems to effectively accommodate and

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S.S.V. Vuppaladadiyam et al. Science of the Total Environment 924 (2024) 171453

9. Conclusions electronic wastes: a review on progress, challenges, and perspectives. Environ. Sci.
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metallurgy. J. Sustain. Metall. 3, 570–600.
Sai Sree Varsha Vuppaladadiyam: Writing – review & editing, Birloaga, I., Coman, V., Kopacek, B., Vegliò, F., 2014. An advanced study on the
hydrometallurgical processing of waste computer printed circuit boards to extract
Writing – original draft, Validation, Methodology, Formal analysis, Data
their valuable content of metals. Waste Manag. 34, 2581–2586.
curation, Conceptualization. Bennet Sam Thomas: Writing – review & Borrirukwisitsak, S., Khwamsawat, K., Leewattananukul, S., Rewlay-ngoen, C., 2023.
editing, Formal analysis. Chandan Kundu: Writing – review & editing, Material flow analysis and life cycle assessment of WEEE dismantling into recycled
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Huabo Duan: Writing – review & editing, Formal analysis. Sankar 1–12.
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Formal analysis, Data curation, Conceptualization. fixation in co-pyrolysis of non-metallic fractions of waste printed circuit boards with
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Declaration of competing interest
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Acknowledgment Diaz, L.A., Lister, T.E., Parkman, J.A., Clark, G.G., 2016. Comprehensive process for the
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Hub for the micro recycling of battery and consumer wastes Inc.
(IH190100009). Monash University funded the living scholarship of Dutta, T., Kim, K.H., Uchimiya, M., Kwon, E.E., Jeon, B.H., Deep, A., Yun, S.T., 2016.
Vuppaladadiyam Sai Sree Varsha Global demand for rare earth resources and strategies for green mining. Environ.
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