Environmental Research 150 (2016) 182–190

Contents lists available at ScienceDirect

Environmental Research
journal homepage: www.elsevier.com/locate/envres

Review article

Global demand for rare earth resources and strategies for green mining
Tanushree Dutta a, Ki-Hyun Kim a,n, Minori Uchimiya b, Eilhann E. Kwon c,
Byong-Hun Jeon d, Akash Deep e, Seong-Taek Yun f
a
Department of Civil & Environmental Engineering, Hanyang University, 222 Wangsimni-Ro, Seoul 04763, Republic of Korea
b
USDA-ARS Southern Regional Research Center, 1100 Robert E. Lee Boulevard, New Orleans, LA 70124, United States
c
Department of Environment and Energy, Sejong University, Seoul 05006, Republic of Korea
d
Department of Natural Resources & Environmental Engineering, Hanyang University, 222 Wangsimni-Ro, Seoul 04763, Republic of Korea
e
Central Scientific Instruments Organisation (CSIR-CSIO), Sector 30C, Chandigarh 160030, India
f
Department of Earth and Environmental Sciences and KU-KIST Green School, Korea University, Seoul 02841, Republic of Korea

art ic l e i nf o a b s t r a c t

Article history: Rare earth elements (REEs) are essential raw materials for emerging renewable energy resources and
Received 22 March 2016 ‘smart’ electronic devices. Global REE demand is slated to grow at an annual rate of 5% by 2020. This high
Received in revised form growth rate will require a steady supply base of REEs in the long run. At present, China is responsible for
28 May 2016
85% of global rare earth oxide (REO) production. To overcome this monopolistic supply situation, new
Accepted 30 May 2016
strategies and investments are necessary to satisfy domestic supply demands. Concurrently, environ-
Available online 10 June 2016
mental, economic, and social problems arising from REE mining must be addressed. There is an urgent
Keywords: need to develop efficient REE recycling techniques from end-of-life products, technologies to minimize
Rare earth ore deposits the amount of REEs required per unit device, and methods to recover them from fly ash or fossil fuel-
Ion-adsorption
burning wastes.
Urban mining
& 2016 Elsevier Inc. All rights reserved.
Preservation
Recycling

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 182
2. Rare-earth resources . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 185
3. Mining rare earths. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 186
3.1. Methods of extraction from major REE resources . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 186
3.1.1. Commercial REE ore concentration. . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 186
3.1.2. Ion-adsorption clays . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 186
3.1.3. Sedimentary phosphate deposits (phosphorites) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 186
3.1.4. Coal and coal by-products . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 187
3.1.5. Fly ash from fossil fuel and other wastes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 187
3.2. Consequences of rare earth mining . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 187
4. Preservation of rare earths and sustainability of material supply chain . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 187
4.1. Re-use of REEs through urban mining . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 188
4.2. Strategies for promoting the preservation of REEs . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 188
4.3. Sustainability of REE material supply chain . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 188
5. Conclusion and recommendations . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 188
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 189
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 189

1. Introduction

A gradual shift from traditional energy sources towards green

n
Corresponding author.
energy alternatives such as solar cells, electric vehicles, and wind
E-mail address: kkim61@hanyang.ac.kr (K.-H. Kim).

http://dx.doi.org/10.1016/j.envres.2016.05.052
0013-9351/& 2016 Elsevier Inc. All rights reserved.
 T. Dutta et al. / Environmental Research 150 (2016) 182–190 183

Fig. 1. Major areas of consumption of REEs worldwide. Percentage values indicate forecasted industry-level annual growth rate (Alonso et al., 2012) of each REE demand
category using the projections used for 2015–2035 (Kingsworth, 2010), assuming that each REE consumption market will grow at rates predicted by industry experts.

turbines is becoming realized on a global scale. The transition has

Fig. 2. REE usage (%) by types of application fields (adopted from Binnemans and
Jones, 2014).
led to a rapid surge in demand for a critical commodity: rare earth
elements (REEs). REEs are crucial for manufacturing a broad array
of high-tech products, devices, and technologies with widespread
applications in the medical, defense, aerospace, and automobile
industries (Figs. 1,2). International Union for Pure and Applied
Chemistry (IUPAC) defines REEs as the group of 17 elements
comprising 15 lanthanides plus Yttrium and Scandium (Table 1).
Rare earth elements are subdivided into heavy rare earth elements
(HREE) and light rare earth elements (LREE). Lanthanum, cerium,
praseodymium, neodymium, promethium, and samarium are
LREEs, while yttrium, europium, gadolinium, terbium, dysprosium,
holmium, erbium, thulium, ytterbium, and lutetium constitute
HREEs. The global market of REE-based products is estimated to be
worth 1.5–2 trillion US dollars, based on trade information and REE
contents of manufactured goods (Tukker, 2014). According to the
United States Geological Survey (USGS), 2016 report, the annual

Table 1
Summary of the usage of different REEs.

Serial No. REE Symbol Atomic number Use

1. Scandium Sc 21 Aerospace framework, high-intensity street lamps, high-performance equipment such as bicycle frames,
baseball bats
2. Yttrium Y 39 Television and computer screens, LED lights, cancer treatment drugs, enhances strength of alloys, catalyst
3. Lanthanum La 57 Camera lenses, carbon lighting applications such as studio lighting and projector lights, battery electrodes
4. Cerium Ce 58 Catalytic converters in cars, colored glass, steel production, refining crude oils
5. Praseodymium Pr 59 Strong magnets, welding goggles, lasers, aircraft engines
6. Neodymium Nd 60 Powerful magnets used in computed HD, microphones, wind turbines, and hybrid cars, lasers
7. Promethium Pm 61 Not usually found in nature
8. Samarium Sm 62 Cancer treatment, nuclear reactor control rods, X-ray lasers
9. Europium Eu 63 Color television screens, computer screens, fluorescent glass, genetic screening tests, control rods in nuclear
reactors
10. Gadolinium Gd 64 X-ray & MRI scanning systems, shielding in nuclear reactors, increases durability of alloys, green phosphors in
television screens
11. Terbium Tb 65 Television and computer screens, fuel cells, solar systems
12. Dysprosium Dy 66 Commercial lighting, hard disk devices, transducers
13. Holmium Ho 67 Lasers, glass coloring, high-strength magnets
14. Erbium Er 68 Glass colorant, signal amplification in fiber optic cables, metallurgical uses
15. Thulium Tm 69 High-efficiency lasers, portable X-ray machines, high temperature superconductors
16. Ytterbium Yb 70 Improves stainless steel, lasers, ground monitoring devices, industrial catalysts
17. Lutetium Lu 71 Cracking hydrocarbons in oil refineries
184 T. Dutta et al. / Environmental Research 150 (2016) 182–190
Fig. 3. Historical trend of the mine production of REO (in tons) in the world and China (according to USGS). The shaded area indicates the decreasing share of China in the
world production of REEs from more than 95% before 2012 down to 85% in 2015.
growth rate of global REE demand is expected to increase by 5% by
2020. Therefore, it has become obligatory for REE-consuming na-
tions to create align supply chains for REEs in order to maintain
current technologies and develop advanced technologies involving
renewable energy resources.
Rare earths are actually not rare to exhibit a broad geographical
distribution. The average levels of REEs in the earth's crust range
from 150 to 220 ppm (ppm) which exceed the level of many other
metals mined for industrial use (e.g. copper: 55 ppm and zinc: 70
ppm) (Long et al., 2010). Nonetheless, establishing and maintain-
ing a reliable supply chain of REEs are of great concern for a
number of reasons. Rare earths occur in geological deposits in
combination with other materials, which makes the extraction of
pure REEs challenging and expensive. The supply of standard
grade REEs depends upon the geology of the ores, cost of extrac-
tion, market demand, and price of individual REEs. A key concern
is whether the current supply base of REEs can keep pace with the
projected growth of REE markets worldwide. For example, there
was volatility in the rhenium market due to its under-supply in
2008, which caused an excessive price hike (10,500 USD/kg)
(Global Information Market Research Report, 2015). If these types
of situations arise for REEs, the resilience of the supply chain will
be decided by the supply chain's resistance, speed of response, and
flexibility to market fluctuations (refer to the case study of neo-
dymium by Sprecher et al. (2015). In addition, in order to ensure
zero surplus of any REEs, a maintenance of the right balance be-
tween the supply and demand is of paramount significance for
Fig. 4. Anticipated evolution of global rare earth demand and supply from 2016 to
2020. Data for this plot were extracted from Rollat et al. (2016).
economic reasons (Binnemans and Jones, 2015). The deviation of
balance can be caused by the reduced availability of the more
important REEs and vice versa. Recycling of the critical REEs could
be an appropriate solution for this problem.
Above-outlined concerns have motivated both developing and
developed nations to secure REE reserves. Most countries relied
heavily on imports for their current REE demands; in some cases,
100% of REEs were reported to be imported. However, this trend
has been changing rapidly most likely due to the restrictions re-
cently imposed by China on the export of metals and mineral
products (Mancheri et al., 2015). The USGS commodity report for
the fiscal year of 2015–2016 revealed that the United States de-
creased its import of rare earth metals and compounds from $190
million in 2014 to $150 million (estimated) in 2015. Up till 2010,
China controlled 98% of the global REE production (Chakhmour-
adian and Wall, 2012). Such market monopolies are detrimental
because even small changes in the foreign policy and export cri-
teria of one country can lead to inimical instabilities of global
market. The control of China over the world mine production of
rare earth oxides has indeed gone down significantly in the last
three years. Fig. 3 shows the decreasing share of China (85%
shareholder) in the world mine production of rare earths. Never-
theless, in various places, the mining of REEs in socially and en-
vironmentally unacceptable ways has placed this industry under
global scrutiny, further accentuating supply risk. The example of
Kvanefjeld, recognized as one of the world's largest REE resources,
illustrates the fact that even highly environmentally conscious and
progressive countries like Greenland (an autonomous Danish ter-
ritory) are loosening regulations to allow mining of REEs.
British Geological Survey Risk List (2015) described REEs as
critically at-risk marketable elements. Particularly, the five ele-
ments of dysprosium, terbium, yttrium, europium, and neody-
mium are critical commodities for emerging clean energy tech-
nologies. This is primarily due to the fact that the replacement of
such crucial components commonly used in emerging green en-
ergy technologies and smart devices with other more abundant
metals would require compromise for the quality of the finished
products. This review aims to provide an updated understanding
of the complex global scenario and risks (in social, environmental,
and economic) associated with the growth of the REE market and
possible ways to tackle these risks. Our ultimate goal is to assess
the future of REE supply chains (Fig. 4), highlight vulnerabilities
for REE-consumers, and propose ways to combat the environ-
mental impacts of REE mining. Alternatives and measures to
 T. Dutta et al. / Environmental Research 150 (2016) 182–190 185

Table 2 prevent steady declination of one of the earth's critical resources

Classification of rare earth-bearing mineral deposits. (Source: Long et al., 2010). are also suggested.
Serial No. Rocks and deposits Type

1. Peralkaline igneous rocks Magmatic (alkali-ultrabasic) 2. Rare-earth resources

Pegmatite dikes (alkali-ultrabasic)
Pegmatite dikes (peralkaline)
Rare earth elements occur in a number of mineral deposits;
Hydrothermal veins and stockworks
Volcanic however, they are not concentrated enough (typical concentration
Metasomatic-albitite range is 10 to a few hundred ppm by weight) to make their mining
2. Carbonatites Magmatic
easy or economic (Long et al., 2010). The most abundant mineral
Dikes and dialational veins sources of REEs, particularly light REEs (LREE), are bastnäsite
Hydrothermal veins and stockworks [(Ce,La)CO3(F,OH)] and monazite [(Ce,La,Nd,Th)PO4]. Bastnäsite
Skarn deposits in China and the United States constitute the largest
Carbonate rock replacement
percentage of the world’s rare-earth resources, while monazite
Metasomatic-fenite
deposits in Australia, Brazil, China, India, Malaysia, South Africa, Sri
3. Iron oxide-Copper Gold Magnetite-apatite replacement
Lanka, Thailand, and the United States constitute the second lar-
Hematite-magnetite breccia
gest segment (Long et al., 2010). Sources of HREEs include apatite,
4. Pegmatites Abyssal (heavy rare earth elements) cheralite, eudialyte, loparite, phosphorites, rare-earth-bearing (ion
Abyssal (light rare earth elements)
Muscovite (rare earth elements)
adsorption) clays, secondary monazite, spent uranium solutions,
Rare earth elements-allanite-monazite and xenotime (Long et al., 2010). Rare earth-bearing mineral de-
Rare earth elements-euxenite posits are mainly associated with igneous rocks (alkaline rocks and
Rare earth elements-gadolinite carbonatites) (Long et al., 2010). Furthermore, placer deposits,
Miarolitic-rare earth elements-topaz-
residual deposits from deep weathering of igneous rocks, peg-
beryl
Miarolitic-rare earth elements-gadoli- matites, iron oxide copper-gold deposits, and sedimentary marine
nite-fergusonite phosphate deposits (phosphorites) also contain economically vi-
5. Porphyry molybdenum Climax-type
able REE concentrations (Table 2). Recent studies of Aiglsperger
6. Metamorphic Migmatized gneiss et al. (2016) suggest nickel laterites of Cuba (Mao Bay area) and
Uranium-rare earth elements skarn Dominican Republic (Falcondo mines) as a worthy target of critical
7. Stratiform phosphate Platform phosphorite metals like REEs.
residual In addition to the occurrences in the form of ores and deposits,
Carbonatite-associated rare earths are also found in coal and coal by-products (in sedi-
Granite-associated laterite
mentary rocks) at a very low concentration. As such, their recovery
Baddeleyite bauxite
Karst bauxite from such sources is economically implausible. Several sources of
information concerning the REE contents in coal samples from
8. Paleoplacer Uraniferous pyritic quartz pebble
conglomerate
different countries are available (See Seredin et al., 2013 and
Auriferous pyritic quartz pebble Blissett et al., 2014). For example, Seredin et al. (2013) reported
conglomerate 0.002–0.8% of Ge, Ga, Se, and Li in coal deposits, wherein rare
9. Placer Shoreline Ti-heavy mineral placer metal contents were only reported from laboratorial ashes in high-
Tin stream placer temperature, e.g., between 600 and 850 °C (that excludes the vo-
latile fractions of the metals). Despite the low concentrations of

Fig. 5. Steps of REE ore concentration procedure and recycling.

186 T. Dutta et al. / Environmental Research 150 (2016) 182–190
REEs in coal by-products, they have been suggested to be im-
portant for their recovery; their presence can ultimately help ex-
pand REE reserve and production (Rozelle et al., 2016). Moreover,
fly ashes arising due to coal combustion and from municipal solid
waste incinerators (MSWI) have been found to comprise a sig-
nificant fraction of REEs. Hard coal fly ashes, for instance, re-
portedly contain 445 mg kg
1 REEs on an average global basis
(Ketris and Yudovich, 2009). On the other hand, the total con-
centration of REEs in the treated bottom ashes from MSWI was
estimated at 110 mg kg
1, with the preferential dominance of La,
Ce, and Nd at concentrations greater than 20 mg kg
1 (Allegrini
et al., 2014). Generally, these values are however two to three
orders of magnitude lower than the typical levels in REE-con-
centrated ores (mentioned before).
3. Mining rare earths
Rare earth resources are diverse in their geology, mineralogy,
and REE contents. A series of specific techniques are required to
process diverse REE resources to extract commercially viable
elements.
3.1. Methods of extraction from major REE resources
3.1.1. Commercial REE ore concentration
Rare earth ore mining and concentration are performed using a
complex (and often economically unrealistic) method that in-
cludes REE mining from ore deposits, grinding, cracking the mi-
nerals to produce mixed rare earth oxides (REO) concentrates,
separation, purification of oxides, and refining to produce in-
dustrial grade REEs (Fig. 5). It is difficult to obtain REE concentrates
from ore deposits (e.g. bastnäsite and monazite) because they
occur in solid-state mineral phase and are often laced with
radioactive elements such as uranium and thorium. Further details
of the REO present in rare earth minerals and the physical/che-
mical steps of their processing to obtain ore concentrates (mining,
physical beneficiation like floatation, gravity separation, electro-
static, and magnetic separation), processing of concentrates by
leaching in acidic or alkaline medium, pre-concentration, and re-
covery of REEs from each solution through precipitation and sol-
vent extraction methods, can be obtained in recent reviews of
Kumari et al. (2015) (Monazite) and Sinha et al. (2016) (Bastnasite
and Monazite). The system and process of selective REE extraction
from Bastnasite and Monazite has been patented by Teixeira et al.
(2015). In addition, many contemporary reports, like Quinn et al.
(2015) (solvent extraction), based exclusively on REE extraction
efficiencies by various precipitation and solvent extraction meth-
ods are also available.
Various techniques are available for the determination of
commercial REE ore concentration. Among those options, one can
rely on inductively coupled plasma-optical emission spectroscopy
(ICP-OES), neutron activation analysis (NAA), and inductively
coupled plasma-mass spectroscopy (ICP-MS) to produce the best
results due to high sensitivity (can detect up to a few ng (10
9 g)
L
1 levels) for multi-elements (Zawisza et al., 2016; Li et al., 2016).
Recently, in situ measurement techniques involving the use of
small, portable equipment for the detection of REEs have also
been developed. For instance, portable X-ray fluorescence (pXRF)
analyzers were used by Simandl et al. (2014) as field tools to
detect REEs in sedimentary phosphate deposits. The pXRF data
were correlated with inductively coupled plasma-atomic emission
spectroscopy (ICP-AES) and ICP-MS data. In addition, magnetic
susceptibility analyzers have also emerged as reliable alternative
tools for field measurement of REEs (Funari et al., 2016). Although
these portable tools may be less accurate than laboratory
measures, the above-discussed portable tools are useful enough to
detect the presence of REEs in waste heaps. Moreover, bio-ad-
sorption of REEs from primary ores with the aid of genetically
engineered microbial probes is also a promising technique to as-
sess REE enrichment and/or separation. Park et al. (2016) have
recently made a remarkable breakthrough in this emerging re-
search area by engineering the aerobic bacterium Caulobacter
crescentus that exhibited high specificity toward REEs with small
atomic radii through the cell surface display of lanthanide binding
tags (LBT).
3.1.2. Ion-adsorption clays
The recovery of REEs from ion-adsorption clays involves rela-
tively easy processing steps. These resources are commonly found
in Madagascar, Brazil and the southern provinces of China (Rocha
et al., 2013; Yang et al., 2013; SGS, 2014). Chemical weathering and
dissolution of granite and granite porphyry, where REEs become
absorbed on the clay surface, result in the formation of ion-ad-
sorption clays. Unlike ores, ion-adsorption clays contain REEs in an
easily extractable trivalent cationic state. Extraction of rare earths
from these clays is accomplished by surface/mountain-top mining,
followed by tank or heap leaching with aqueous electrolyte solu-
tion (sodium chloride (NaCl)) or ammonium sulfate ((NH4)2SO4),
and finally use of ion-exchangers. The ion exchange reaction be-
tween kaolinite (a hydrated aluminosilicate crystal with chemical
formula: Al2Si2O5(OH)4 and (NH4)2SO4) can be chemically re-
presented as
2(Kaolin)3- RE3 þ þ3(NH4)2SO4-2(Kaolin)3-(NH4 þ )3
þ(RE3 þ )2(SO42
)3
The above type of ion exchange processing is of industrial
significance despite limited use of ion-adsorption clays as a rare
earth reserve. Ion-adsorption rare earths constitute only 2.9% of
China's REE reserves, yet accounting for 26% of China's total REE
production during 1988–2007. The figure increased to 35% after
2009 (Su, 2009; Yang et al., 2013). Nonetheless, a strong reliance
upon such small reserve could be detrimental, especially from
China's point of view as it could result in the fast depletion of their
important natural resources.
3.1.3. Sedimentary phosphate deposits (phosphorites)
REEs are also found to be significantly enriched sedimentary
marine phosphate deposits or phosphorites. According to Emsbo
et al. (2015), the concentration of REEs, particularly of HREEs, in
phosphorites is high enough to be considered, as a primary source
of REEs. For example, some U.S. phosphorites are considerably
enriched in REEs (relative to Chinese clay-type of deposits) with
total REE contents in 500–2000 mg Kg
1 (Kato et al., 2011). Most
importantly, unlike primary ore concentrates, phosphorites are
easily extractable. It is noteworthy that the world's fertilizer in-
dustry used phosphorites to produce 150 metric ton phosphate
fertilizer per year (Zhang et al., 2006). Phosphate rock is dissolved
in dilute sulfuric acid to produce phosphoric acid used for the
production of fertilizer, animal feed, and chemicals. The same
process can be used to dissolve 100% of REEs contained in the
phosphate deposits (Emsbo et al., 2015). An additional benefit of
phosphate mining is that it does to lead to radioactive thorium or
uranium-rich waste commonly associated with REE mining (Zie-
linski et al., 1997). Collectively, all these factors can make phos-
phorites a very useful future resource. Another phosphate ore
deposit used in the preparation of phosphorus fertilizer, named
apatite (containing 0.1–1 mg Kg
1 REO), was tested recently for
REE recovery (Ogata et al., 2016) in which up to 70% leaching ef-
ficiency of REE was achieved with 2(M) sulfuric acid.
 T. Dutta et al. / Environmental Research 150 (2016) 182–190 187

3.1.4. Coal and coal by-products
Rozelle et al. (2016) reported a recovery rate of 71–89% based
on extraction of REEs from high ash-containing by-products of coal
mining collected from a surface coal-mine of the Allegheny group
in Central Pennsylvania. REE concentration profiles above and
below the coal bed were also assessed. The chemical steps for the
recovery of REEs involved the use of ammonium sulfate, which
leached out 89% of the REEs into the filtered solution. Subsequent
applications of an ionic liquid (1-butyl 3-methylimidazolium
chloride) and a deep eutectic solvent (2:1 urea/choline chloride,
M/M) as lixiviants resulted in 80% and 71% recovery of REEs, re-
spectively. Quantitative analysis of the different REEs was per-
formed using ICP-AES, which allowed detection of the various
REEs (with the exceptions of Dy, Eu, Ho, Lu, Tb, and Tm) with a
detection limit (DL) of 5 mg kg
1. In another study, Phuoc et al.
(2016) used laser-induced breakdown spectroscopy (LIBS) for
qualitative detection of REEs in ash samples of Powder River Basin
bituminous coal. Labutin and Popov (2016), however, pointed out
the presence of Fe may have led to overlapping spectral lines, thus
bringing into question the validity of the spectroscopic data pre-
sented by Phuoc et al. (2016).
3.1.5. Fly ash from fossil fuel and other wastes
As stated earlier in Section 2, fly ash from MSWI and coal
combustion comprise of extractable amounts of REE (Hower et al.,
2015; Yuzhuang et al., 2015; Funari et al., 2016). However, those
materials are not routinely analyzed due to their low REE content
and apprehensions about the economic viability of the extraction
process. Chemical analyses (using Na2O2 sintering technique cou-
pled with ICP-MS) of samples of MSWI fly ashes from incineration
plants have indicated that they are promising alternative waste-
derived sources of REEs. Study of fly ash from Jungar power plant,
Inner Mongolia, China by Dai et al. (2014), revealed that the con-
centration of the critical REEs were greater in the finer sized
fractions (454 LREE mg g
1 in o25 mm fraction) of fly ash than the
coarser ones (156 mg g
1 in 4125 mm fraction). However, the
feasibility of recovering REEs from fly ash on an industrial scale
needs to be explored.
3.2. Consequences of rare earth mining
Rare earth mining and extraction procedures constitute mas-
sive exploitation of earth's resources and destabilize/deteriorate
soil and water ecosystems. One of the biggest concerns of REE
mining from the primary ore deposits such as bastnasite and
monazite is the resultant radioactive stockpiles. Rare earths fre-
quently co-exist with radioactive minerals like thorium and
uranium imparting radiological effects during their recovery
(Binnemans et al., 2013; Ault et al., 2015). The release of the
radionucleotides along with other contaminants like dust and
heavy metals may also bear serious environmental costs. Proces-
sing one ton of REEs is associated with the generation of 2000 t of
toxic waste and 1000 t of wastewater contaminated with ammo-
nium sulfate and heavy metals (Su, 2009). Immediate negative
effects of REE mining include severe soil erosion, biodiversity loss,
land use change, flooding, pollution of air, soil, and water, and crop
uptake of REEs, consequentially leading to human health issues
(Tang and Li, 2000; Liu, 2002; Chen, 2010; Anonymous, 2011;
Carpenter et al., 2015). Using satellite imagery, Guo (2012) de-
picted the visual changes in the landscape caused by the surface/
mountaintop mining in the Ganzhou area of the Jianxi province of
China. Biological, environmental, and human health effects of
mountaintop mining activities have been well documented (Gil-
bert, 2010; Holzman, 2011; Beggs, 2012; Bernhardt et al., 2012).
Alarmingly, some of these human health and environmental im-
pacts are irreversible and persistent even after reclamation of the
mine site (Palmer et al., 2010).
China adopted an alternative technique in 1997, which is re-
ferred to as in-situ leaching of clays. This technique deploys
leaching holes 0.8 m in diameter and 1.5–3 m in depth at an in-
termittent distance of 2–3 m. Leaching occurs over a prolonged
period of time (150–400 days) with application of 3–5% ammo-
nium sulfate solution (Yang et al., 2013). This in-situ leaching
protects the soil and vegetation. Nevertheless, enforcement of
such in-situ leaching must be preceded by a thorough geotechnical
survey of the mining area and nearby locations. Otherwise, there
may be low REE recovery (up to 5%), groundwater contamination,
an increase in soil and water pH, and nutrient pollution of
downstream rivers (Liu, 2002; Palmer et al., 2010).
4. Preservation of rare earths and sustainability of material
supply chain
Preservation of rare earth resources calls for the development
of efficient recycling techniques at the pilot-plant scale. Due to the
economic and environmental costs of REE mining, it is desirable to
promote the recycling and reuse of rare earths, while also mini-
mizing the dependency on such resources. Recycling of REEs may
help reduce the imbalance in REE supply by enforcing the primary
supply chain for some REEs that are crucial in particular for in-
dustrial applications (Binnemans and Jones, 2015; Machacek et al.,
2015). On the other hand, development of new technologies to
make use of lower amounts of the materials is also of great

Table 3
List of 2016 studies on recycling of REEs from end-of-life products.

Order Recycle REE Method used % Recovery Reference

1 Motors Nd, Pr, Dy Hydrometallurgy 82 (99% purity) Bandara et al., 2016

2 Permanent Magnet Nd, Pr Vacuum Induction melting, hydrolysis & magnetic 93 (99.7% purity) Bian et al., 2016
separation
3 Fuel cell catalyst Pt Hydrometallurgy 76 Duclos et al. 2016
4 Phosphor (lamps) Eu, Y Hydrometallurgy 100 (99.9% purity) Dupont and Binnemans,
2015
5 Oil refining Catalyst La, Ce Hydrometallurgy NA Ferella et al. 2016
(Review)
6 NiMH magnets Nd, Sm, Pr, Hydrometallurgy 98.1 (Nd), 95.5 (Sm), 95.5 (Pr), Meshram et al. 2016
Ce 89.4 (Ce)
7 NiMH magnets (Review) La, Nd Hydrometallurgy NA Sinha et al., 2016
8 Permanent Magnet REE Hydro & Pyrometallurgy NA Sun et al., 2016
(Review)
9 Phosphor (lamps) Tb, Eu, Y Mechanical Activation & leaching 89.4 (Tb), 93.1 (Eu), 94.6 (Eu) Tan et al., 2016
10 Fluorescent lamp Eu, Y Hydrometallurgy 99.9 Tunsu et al., 2015
188 T. Dutta et al. / Environmental Research 150 (2016) 182–190
significance, particularly for some critical REEs, e.g., dysprosium
(Dy) and neodymium (Nd). Such rare earth metals are in high
demand, as they are used in clean energy technologies (e.g., wind
turbines and electric vehicles) (Fig. 2) (Alonso et al., 2012).
4.1. Re-use of REEs through urban mining
Recovery of REEs from scraps formed during production pro-
cesses, landfills, and end-of-life consumer products (e.g., used
cars) is referred as ‘urban mining’ and rightly regarded as an im-
portant component of resource management (Simoni et al., 2015;
Bandara et al., 2016). A recent work of Zeng et al. (2016) has also
uncovered newly the potential of waste electronic and electrical
equipment (WEEE) or e-waste. The recycling of REEs is also
deemed necessary to counter the harmful effects of extensive
mining on the environment (Simoni et al., 2015). In fact, REEs
contained in non-recycled waste materials may end up in surface
waters and oceans. Recently, significantly high concentrations of
rare earths were detected in the surface water of San Francisco Bay
area presumably due to the wastewater treatment plant dis-
charges of refractory magnetic resonance imaging (MRI) contrast
agents used in hospitals and medical research centers (Hatje et al.,
2014, 2016). Urban mining might be a useful solution to tackle
some of these undesired effects of REE mining and discharge
(Ongondo et al., 2016; Sun et al., 2016). Besides, unlike the primary
REE ores, REE recyclates do not contain radioactive substances,
implying that health problems can be partially avoided by means
of recycling (Binnemans et al., 2013).
A major challenge in REE recycling has been their low yield rate
due to the lack of appropriate recycle design along with the te-
dious steps involved in their separation. Likewise, there is a
common belief that it is virtually impossible to recycle REEs in any
appreciable quantity, as they are used in very minute quantities. In
this review, a contradictory viewpoint on this generic belief is
discussed by presenting contemporary examples regarding re-
covery of rare earth metals and oxides from a range of end-of-life
(EoL) products (including spent fluorescent lamps, motors, NiMH
batteries, fluid catalysts, fuel cell catalysts, etc).
Table 3 lists 2016 studies on REE recovery from spent products.
Similar studies conducted up to 2015 were reviewed by Binne-
mans et al. (2013, 2015) and Tunsu et al. (2015). Most importantly,
many of these studies confirm a reasonably good yields (i.e., up to
99%) of re-usable REEs and their oxides, which further exemplifies
that recent technological advancements have been able to par-
tially, if not fully, cross the barriers of REE recycling processes. As a
good example of this scenario, recovery of REE oxides (of neody-
mium, praseodymium, and dysprosium) has actually been made
from commercial NdFeB magnets and industrial scrap magnets by
employing membrane-assisted solvent extraction (MSX: Kim et al.,
2015). The demonstrated process was capable of selectively re-
covering pure REE oxides (e.g., based on the XRD and SEM-EDX
analysis) from scrap magnets at good yields without any co-ex-
traction of non-REEs over the 120 h run.
It should be noted that although many lab-scale experiments
reported a very high recovery for REEs, full proof recycling tech-
nologies of REEs are still non-existent at industrial-scale (Sun
et al., 2016). However, nowadays, some chemical and electrical
companies are tackling the challenge of developing steps and
processes to recover high purity REEs from wastes. For instance,
the 2013 joint venture between Honda and Japan Metals and
Chemicals (JMC) explored the use of molten salt electrolytes to
recycle REEs into usable oxides from used nickel-metal hydride
(NiMH) batteries. Likewise, Umicore and Solvay Rhodia (chemical
companies) developed a similar initiative (Forbes, 2014). Other
multinational corporations have also joined forces in REE recovery,
e.g., Mitsubishi Electric (recycling REEs from air conditioners) and
Veolia Environmental Services (recycling REEs from e-waste and
lamps) (Forbes, 2014). Such efforts are critical for the sustainable
supply of REEs in green energy technologies and smart electronic
devices.
4.2. Strategies for promoting the preservation of REEs
Another significant challenge in REE primary mining and re-
cycling is the development of effective administrative policies to
establish and implement recycling programs at governmental or
intergovernmental levels. A low level of community awareness
regarding recycling, lack of recycling design, and collection of
scrap products are the major roadblocks (Reck and Graedel, 2012).
However, some of these limitations have been overcome in the
recent years. This was also reflected in the recycling forecasts by
Rollat et al. (2016) who projected increased possibilities of re-
cycling by 2020. Altogether, there are a number of possible stra-
tegies for preserving primary REE resources (Sprecher et al., 2015;
Yang et al., 2013). These include: i) establishing stringent industrial
standards and laws for the REE industry, ii) reducing red tape to
promote faster system response, iii) centralizing management of
REE resources by eliminating illegal mining, iv) developing in-
tegrated REE market pricing and distribution systems, v) en-
couraging investment in environmental programs to combat the
environmental consequences associated with the REE industry, vi)
promoting the participation of nations with high annual con-
sumption of REEs worldwide, and vii) encouraging REE recycling
from enriched waste materials, EoL products, and other under-
utilized resources (e.g., Liu and Diamond, 2005).
4.3. Sustainability of REE material supply chain
As mentioned earlier, sudden disruptions in the demand-sup-
ply chain of the critical materials may create serious market vo-
latilities. Such raw material threats took place in Re and Nd mar-
kets in 2008 and 2010, respectively; their material prices sky-
rocketed within a span of a few months but geared back to normal
levels in the following months. Sprecher et al. (2015) examined the
case of Nd market crisis of 2010 using an approach based on
market resilience theory combined with market flow analysis.
Socio-economically, any material production system embeds three
levels: societal needs, machinery of production, and the system
that augments the supply of the materials required by the pro-
duction machinery (Daigo et al., 2014). The resilience of the pro-
duction system against supply chain disruptions is thus dictated
by the strength of the system (Sprecher et al., 2015).
Key components of the sustainability in the production system
and material supply chain include: i) resistance, i.e., the ability to
combat the disturbances without any substantial loss of function,
ii) speed of recovery, and iii) flexibility, i.e., the ability to switch
between alternative supply systems. According to Binnemans et al.
(2015), such supply chain resilience in REEs market has been
achieved either by substituting critical REEs with less critical
metals or by augmenting the supply by sustainable primary
mining and recycling. The rapidity of the system response could be
further buttressed by additional interventions from the govern-
ment and/or other regulatory agencies, as discussed in Section 4.2.
5. Conclusion and recommendations
REE-based devices and renewable energy technologies are ex-
pected to drive tremendous growth in REE demand. However,
there are also critical challenges, because the costs of mining and
extracting primary REE resources are high. Because richer deposits
are highly localized in a limited number of counties, the supply
 T. Dutta et al. / Environmental Research 150 (2016) 182–190
and price of REEs could face tactical monopoly. As such, every
country needs a constant REE supply to support automobile,
electronic, and allied industries. Indeed, some REE-consuming
nations have ramped up domestic REE production (e.g., Molycorp
Inc, USA and Lynas Corporation, Australia) to avoid large ex-
penditures of REE imports. However, the number of such cases are
still sparse. China still has the maximum control over the entire
REE value chain and it has overtaken nearly all developed nations
in the REE industry. Therefore, further domestic investments by all
rare earth-consuming nations in primary mining will be needed to
overcome this situation. Perhaps, researchers and industrialists
can thoroughly analyze China's approaches as a case study to build
up on the existing framework. Nevertheless, caution should be
practiced to ensure that the mining approaches adopted by most
nations are well backed up by geotechnical survey data for the
mine site and adjacent areas to help reduce the possibility of any
environmental problems. Nonetheless, it is important to empha-
size that a landmark in the REEs industry has been achieved
through successful recovery of REEs (99% purity) from end-of-life
products (urban mining). Our survey confirmed that, in last few
years, lab-scale REE recovery has increased sporadically, although
mature procedures for industrial REE recycling are virtually non-
existent. An integrated approach that considers ecology, resource
management, mining techniques, scale of production, market, and
state legislature needs to be implemented. In future, such recovery
methods need to be implemented at the industrial-scale.
Exploring alternative commercially viable REE resources, e.g., fly
ash and other waste materials, should also be a major research
focus.
Acknowledgments
This study was supported by a grant from the National Re-
search Foundation of Korea (NRF) funded by the Ministry of Edu-
cation, Science and Technology (MEST) (No. 2009-0093848). E
Kwon also acknowledges the support made by a National Research
Foundation of Korea (NRF) Grant funded by the Korean Govern-
ment (MSIP) (No. 2914RA1A004893).
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