Waste Management 60 (2017) 765–774

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Waste Management
journal homepage: www.elsevier.com/locate/wasman

Carbon footprint assessment of recycling technologies for rare earth

elements: A case study of recycling yttrium and europium from
phosphor
Allen H. Hu a,⇑, Chien-Hung Kuo a, Lance H. Huang a, Chao-Chin Su b
a
Institute of Environmental Engineering and Management, National Taipei University of Technology, Taiwan, ROC
b
Department of Molecular Science & Engineering, National Taipei University of Technology, Taiwan, ROC

a r t i c l e i n f o a b s t r a c t

Article history: Rare earth elements are key raw materials in high-technology industries. Mining activities and manufac-
Received 20 July 2016 turing processes of such industries have caused considerable environmental impacts, such as soil erosion,
Revised 19 October 2016 vegetation destruction, and various forms of pollution. Sustaining the long-term supply of rare earth ele-
Accepted 21 October 2016
ments is difficult because of the global shortage of rare earth resources. The diminishing supply of rare
Available online 31 October 2016
earth elements has attracted considerable concern because many industrialized countries regarded such
elements as important strategic resources for economic growth. This study aims to explore the carbon
Keywords:
footprints of yttrium and europium recovery techniques from phosphor. Two extraction recovery meth-
Life cycle assessment
Carbon footprint
ods, namely, acid extraction and solvent extraction, were selected for the analysis and comparison of car-
Rare earth recycling technologies bon footprints. The two following functional units were used: (1) the same phosphor amounts for specific
Phosphor Y and Eu recovery concentrations, and (2) the same phosphor amounts for extraction. For acid extraction
method, two acidic solutions (H2SO4 and HCl) were used at two different temperatures (60 and 90 °C). For
solvent extraction method, acid leaching was performed followed by ionic liquid extraction. Carbon foot-
prints from acid and solvent extraction methods were estimated to be 10.1 and 10.6 kg CO2 eq, respec-
tively. Comparison of the carbon emissions of the two extraction methods shows that the solvent
extraction method has significantly higher extraction efficiency, even though acid extraction method
has a lower carbon footprint. These results may be used to develop strategies for life cycle management
of rare earth resources to realize sustainable usage.
Ó 2016 Elsevier Ltd. All rights reserved.

1. Introduction economy (Tunsu et al., 2016). However, sustaining the long-term

Rare earth elements (REEs) consist of 17 elements in the peri-
odic table, 15 of which have atomic numbers within the range of
57–71. The REEs can be classified into light REEs (with atomic
number within the range of 57–62) and heavy REEs (with atomic
number within the range of 63–71). Promethium (61) is obtained
by synthetic methods and does not exist in nature (Damhus
et al., 2005). REEs have become among the most important strate-
gic resources and are called the ‘‘21st century industrial vitamins”
(Alonso et al., 2012). REEs are critical to high-technology applica-
tions, such as high-intensity magnets for electronic and electronic
motors, efficient lighting, wind power, and hybrid electric vehicles
(Hoenderdaal et al., 2013). REEs are also key ingredients in the
development of environmentally friendly energy technology and
⇑ Corresponding author.
E-mail address: allenhu@mail.ntut.edu.tw (A.H. Hu).
supply of these metals is difficult because of the global shortage
of REE resources, which have attracted considerable concern in
recent years.
According to the United States Geological Survey, approxi-
mately 99 million tons of REE reserves are available worldwide
(Chen, 2011). The gross volume of global export in REEs increased
from 259 t in 1990 to a peak of 111,373 t in 2004 but gradually
declined until 2012. Approximately 97% of the global REE supply
is produced by China, which has recently performed copious cuts
of its exports to protect its environment and national downstream
industries (Massari and Ruberti, 2013). The REE export quotas have
been sharply restricted, and the cut export quotas was almost 70%
in 2010. The total exports of REEs in 2014 reached 75,768 t, which
considerably increased from 64,000 t in 2013. In 2014, China
exported approximately 34,168 t of REEs, and this value was more
than 51% of the total REE worldwide. The price of REEs has sud-
denly increased because of the reduced export quotas. The average

http://dx.doi.org/10.1016/j.wasman.2016.10.032
0956-053X/Ó 2016 Elsevier Ltd. All rights reserved.
766 A.H. Hu et al. / Waste Management 60 (2017) 765–774
price of REEs in 2007 was approximately USD 13/kg, but this
amount increased to USD 70/kg in 2011 (Mancheri, 2015). In
2008–2011, the prices of REO and metals increased remarkably.
By comparison, their prices decreased sharply in the first half of
2012 and declined further in the second quarter of 2013 because
of low demands (Fig. 1). The price of europium metal increased
from $475/kg in 2008 to $2973/kg in 2011 but decreased from
$2074/kg in 2012 to $954/kg in 2013 (Humphries, 2012). Financial
markets could already have considered REE supply shortage into
clean energy companies (Baldi et al., 2014). This fact has signifi-
cantly increased REE prices, thus causing tension and high costs
among high-technology industries in Taiwan (Hou, 2011). There-
fore, improving the REE recycling technology in Taiwan is
necessary.
Recycling techniques for REE extraction and leaching from
waste products, such as phosphor, iron ore, coal fly ash, and other
by-products of rare-earth materials, include acid leaching, solvent
extraction, and ionic liquid (IL) methods (Gasser and Aly, 2013;
Resende and Morais, 2010; Vander Hoogerstraete et al., 2013).
The recovery methods of REEs via recycling of waste products, such
as batteries, computer monitors, magnets, and phosphor, are
shown to be promising at the laboratory scale. However, current
extraction methods have caused potential toxic damage and envi-
ronmental impact (Koltun and Tharumarajah, 2014). Moreover,
during the life cycle of REEs, all stages consume large amounts of
water, reagents, electricity, and fuel; these stages include extrac-
tion, separation, refining, and recovery from waste, specifically
ion-exchange, acid leaching, and liquid–liquid extraction phases
(Ecclestone, 2010). This observation illustrates that life cycle per-
spective plays an important role in assessing the environmental
impacts REEs (McLellan et al., 2013).
Fig. 1. Selected rare earth oxide prices, 2008–2013 (US/kg) (Humphries, 2012).
Almost 22% of global electricity consumption is used for light-
ing, and almost 10% of REEs are made for phosphor (Roskill
Information Services Ltd., 2011). The REO demand in phosphors
scale will increase in the future (Rollat et al., 2016). Following
the development of environmentally friendly lighting technology,
the demand for phosphor, which is applied to display screens,
LED, and OLED, will also increase rpidly. Therefore, developing a
more efficient recycling technology for REE from phosphor is crit-
ical, especially for yttrium. The significance of Y has increased the
development of technologies for recovery form virgin materials
and secondary sources in recent years (Innocenzi et al., 2014).
However, the current recycling technology focuses on existing
technologies, which often contradict environmental protection
and ignore sustainability. Thus, this technology should follow the
3R concept for actively solving technical bottlenecks and prioritize
environmentally friendly technology (Schüler et al., 2011).
In light of climate change phenomenon, REE recovery from
phosphor should focus on carbon footprint to reduce carbon emis-
sions (Binnemans et al., 2013). Carbon footprint assessment can
provide reference in selecting more environmentally friendly pro-
cesses for REE recycling from phosphor.
In the recent years, almost all articles on rare earth recycling
from phosphor have focused on the development of novel extract
technologies and discussed the efficiency of rare earth recovery.
However, few articles included LCA for rare earths at the rare earth
recycling scale, estimated the environment effect, performed car-
bon footprint analysis, and provided suggestions to make recycling
technologies more environmentally friendly. Most of the recent
analyses have been ‘‘cradle to gate” (Koltun and Tharumarajah,
2014; Weng et al., 2016). Therefore, this paper aims to assess the
carbon footprints of two recovery technologies, namely, acid
extraction and solvent extraction, for recycling two REEs (yttrium
 A.H. Hu et al. / Waste Management 60 (2017) 765–774
and europium) from phosphor. The main objectives of this study
are as follows: (1) to evaluate the carbon footprints of different
phosphor recycling techniques and compare the results with liter-
ature; (2) to investigate how the different experimental conditions
affect the results; and (3) to identify critical aspects for reducing
carbon emissions of the two recycling methods.
2. REE waste management and recycling methods from
phosphor
2.1. Current waste management strategy
Most mercury and REEs are contained in phosphor powder form
in fluorescent lamps. Failure to implement a suitable management
strategy may affect the environment seriously (Park and Rhee,
2016). Thus, spent fluorescent lamps management should be
developed to prevent environmental pollution. Waste phosphor
powders used to be landfilled. In the recent years, with the rapid
increase in prices of RE and the strong demand for phosphor
because of the growth of the LED industry, recycling and reusing
phosphors have been essential for sustainable development and
environmental protection (Zhang et al., 2013). In Taiwan, the gov-
ernment introduced the concept of extended producer responsibil-
ity (EPR) to promote recycling. Fluorescent lamps have been
recycled at a recycling rate of about 80% in the past five years
because of the recycling policy based on the EPR (Recycling Fund
Management Board, 2016). With the increase in recycled waste flu-
orescent lamps, large waste phosphors containing Y (24%), Eu
(4.2%), and so on are accumulated (Zhang et al., 2013). Establishing
a novel waste management perspective and developing recycling
technologies are necessary to enhance the resource efficiency of
REEs. Life cycle assessment (LCA) and material flow analysis
(MFA) can be combined with resource, waste, and environmental
management. Both approaches can be applied to evaluate waste
material transfer and environmental effect in the entire life cycle
of the product to strengthen the waste management strategy.
Recently, Swain et al. (2015) conducted MFA to investigate the sta-
tus of REEs in the Republic of Korea. They analyzed the detailed
mapping flow of Nd and provided certain recommendations for
an efficient recycling system. Rollat et al. (2016) used MFA to
determine the future demand for certain REs in Europe in 2020.
Their results explained how recycling to supply strongly depends
on the demand situation. Therefore, developing recycling technolo-
gies and adopting the life cycle perspective are important in waste
management and should be expanded to the circular economy,
which promotes recycling and the gradual decrease of waste
streams elimination in landfills.
2.2. REE recycling methods
Phosphor production and usage has increased in recent years,
and thus phosphor recycling and REE recovery are important
(Zhang et al., 2013; Castilloux, 2014). Several methods, mainly
chemical, are used to recycle REEs from waste phosphor. Fig. 2
shows a typical process for recovering REEs from fluorescent lamp.
The process includes dismantling and separation to collect useful
materials other than REEs, and physicochemical methods, such as
flotation and surfactant processes, to recover REEs from waste
phosphor. Wet methods, such as acid leaching and alkali fusion,
are used in REE dissolution and extraction for REE recovery (Wu
et al., 2014). Many researchers have extracted REEs and recovered
phosphor products in laboratory scale (Meyer and Bras, 2011). This
section summarizes the current development of recycling methods
from waste phosphor for REE recovery.
767
2.2.1. Physicochemical method
Flotation is a physicochemical method that separates powder
and valuable mineral particles based on the ability of air bubbles.
The use of flotation to separate phosphor powder is more difficult
than mineral particle separation because of complicated phosphor
components and small powder size. Hirajima et al. (2005a,b) tested
flotation for phosphor separation and found that the collector
types are pH-dependent. For example, at pH values of below 4.5,
halophosphate phosphor could be totally removed from the mix-
ture by flotation. The use of surfactants could also separate the
phosphor mixture, such as a two-step two-liquid flotation separa-
tion process, by using N,N-dimethylformamide as the polar and
non-polar phase (Otsuki et al., 2008). A phosphor mixture can also
separate in a dense medium (diiodomethane) (Hirajima et al.,
2005a,b). Phosphor powder separation through centrifugation
and pretreatment improves separation efficiency, but the process
is expensive and toxic. Differences in magnetic susceptibility are
also applied to separate phosphors in mixture phase (Horikawa
and Machida, 2011). Another chemical process is a photochemical
reduction in which photons are introduced to the medium and
emitted by a light source that assists in the electron transfer from
the solvent to the europium, causing the removal of Eu from waste
phosphor (Van den Bogaert et al., 2015).
2.2.2. Acid extraction method
Acid extraction method is an important wet technology in
extracting REEs from phosphor of waste-spent fluorescent tubes.
REEs are leached using different acids from phosphor. Nitric,
hydrochloric, and sulfuric acids are commonly used in the leaching
process. Compared with HCl and HNO3, sulfuric acid has high
leaching efficiency to recover REEs from waste phosphor (Li,
2010). Sulfuric acid is the priority when recovering REEs from
phosphor. Some parameters can improve REE leaching efficiency,
including acid class, acid concentration, pH, S/L ratio, and leaching
temperature and time; variations of these parameters affect REE
extraction rates, thereby producing different results (Jiang et al.,
2005; Liu et al., 2008). For example, Pietrelli et al. (2002) recovered
REEs from NiMH-spent batteries by sulfuric acid leaching and pre-
cipitation of rare earth sodium double sulphate. Chi et al. (2004)
roasted material that was leached by hot water (75 °C), and REEs
were extracted by oxalic acid precipitation. Shimizu et al. (2005)
recovered REEs from phosphor of spent fluorescent lamps by using
an extraction method based on supercritical carbon dioxide con-
taining tri-n-butyl phosphate complexes with HNO3 and H2O; the
recovery yield of yttrium and europium was up to 100% after
120 min under 15 MPa at 333 K. Rabah (2008) recovered yttrium
and europium from spent fluorescent lamps by pressure leaching
with a sulfuric/nitric acid mixture. The experiment condition was
at 120 °C, 5 MPa, and 4 M sulfuric/nitric acid; the highest extrac-
tion rate for Eu extraction was 92.8% and that for Y extraction
was 96.4%. De Michelis et al. (2011) showed that the highest
extraction of yttrium (
85%) is obtained by using 20% w/v S/L ratio
of 4 M H2SO4 at 90 °C. The results indicated that acid concentration
and interaction between acid and pulp density have important
positive effects on increasing the yttrium extraction yield for both
HCl and H2SO4 leaching. Innocenzi et al. (2013) achieved the high-
est extraction yield from yttrium (75–80%) under the best experi-
mental conditions following leaching tests: 3 M of sulfuric acid,
10% v/v of H2O2 concentrated solution at 30% v/v, 10% w/w pulp
density, 70 °C, and 3 h of reaction. Dual dissolution by hydrochloric
acid (DHA) can dissolve REEs from different phosphors during the
acid step. The total leaching rate of REEs is 94.6% by DHA. The
leaching rates of Y, Eu, Ce, and Tb reach 94.6%, 99.05%, 71.45%,
and 76.22%, respectively (Liu et al., 2014).
768 A.H. Hu et al. / Waste Management 60 (2017) 765–774
Waste
Dismantling and
fluorescent
seperation
lamp
Rare earth
phosphor
Fig. 2. Flow chart of a typical recycling process for REE recovery (Wu et al., 2014). (Dot line represents processes directly related to recycling of phosphor).
2.2.3. Alkali fusion method
Alkali fusion method is widely used under high-temperature
and high-pressure conditions, in which thermal decomposition of
insoluble substances occurs. Alkali fusion is applied to disintegrate
the structure of the substances and achieve the transition to sol-
uble substances. NaOH, Na2CO3, and Na2O2 are common alkali
fusion reagents (Manhique et al., 2011; Paulino et al., 2012; Wu
et al., 2014). Zhang et al. (2013) used alkali fusion to leach REEs
from waste phosphors after acid leaching. The mass ratio of NaOH,
waste phosphor, and calcination temperature and time were the
main influential factors in the experiment. The results indicate that
the leaching efficiency performance of NaOH at 800 °C for 2 h reac-
tion time is better than that of Na2CO3 in alkali fusion.
2.2.4. Solvent extraction method
Solvent extraction is a water-containing substance in contact
with an organic solvent that are mutually incompatible. Recently,
some different solvents and technologies can extract the REEs from
waste, for instance, lanthanum (III), europium (III), and lutetium
(III) were extracted by bis(4-acyl-5-hydroxypyrazoles) derivatives
(Bou-Maroun et al., 2006), N,N-dimethyl-diphenyl-malonamide,
and -3,6-dioxaoctane-diamide (Narita et al., 2004). The solvent
extraction is a liquid–liquid extraction and a promising technique
in the separation of REEs (Reddy et al., 1993). Liquid–liquid extrac-
tion has many desirable advantages: (1) simple equipment, (2)
quick and easy operation, (3) high recovery rate and good purity,
and (4) wide application range of features. However, it also has dis-
advantages: (1) high toxicity of the organic solvent, (2) expensive
reagents, and (4) high cost (Gao, 2002). When solvent extraction
is used to recover REEs, differences in distribution ratios, pH equi-
librium in the aqueous phase, phase comparison, logarithm of the
concentration, and the feed concentration should be considered. A
study in China showed that the optimal conditions to recover REEs
from phosphor are 25% naphthenic acid ratio, 20% isooctyl alcohol,
55% sulfonated kerosene, phase comparison 1:1, and balance water
phase pH 4.5; under such conditions, the REEs extraction yield is

99.78% (Guangjun and Xiaoqing, 2012). The solvent extraction
process usually has a large amount of volatile and toxic organic sol-
vents; thus, environmentally friendly methods should be devel-
oped (Kubota et al., 2008). IL efficiently improves solvent
extraction methods, including the extraction of REEs (Baba et al.,
2011). N,N-Dioctydiglycol amic acid frame (DODGAA) has been
synthesized as an environmentally friendly extractant for lan-
thanides (Naganawa et al., 2007); a high quality leaching from
the metal impurities was obtained by using an IL containing DOD-
GAA as the extractant system (Yang et al., 2013). DODGAA exhibits
Other materials
(Hg, Al, et al)
Chemical
Acid leaching Y, Eu, Ce, Tb
precipitation
Alkali fusion Extraction
high affinity for REE ions. High affinity does not exist in the tradi-
tional phosphorus extraction agent. A new recycling process
involving the IL extractant is proposed based on the use of the
functionalized IL betainium bis(trifluoromethylsulfonyl)imide,
[Hbet][Tf2N]. This innovative method allows the selective dissolu-
tion of the phosphor without leaching other constituents of the
waste powder, such as other phosphors, glass particles, and alu-
mina. The reusability of the IL provides an environmentally
friendly and efficient alternative to traditional acid leaching
(Dupont and Binnemans, 2015).
2.2.5. Hybrid method
Several kinds of recycling methods can be combined to improve
the recovery purity of REEs from waste phosphor. A single extrac-
tion method cannot complete the recovery of REEs from waste
phosphor. This part reviews typically combined recycling methods.
The recycling process that combines dismantling, acid leaching,
and solvent extraction can recycle Y and Eu from waste phosphor.
This combined method achieves high extraction rate and purity of
Y and Eu (Rabah, 2008). Moreover, the recycling process of crush-
ing, acid leaching, and chemical precipitation can also extract REEs
from waste phosphor. This method can obtain useful materials
other than REEs metals, but the recovery of REEs is still limited
(Mei et al., 2009). The methods for recovering REEs from waste
phosphor can adopt a first-step acid leaching, alkali fusion, and a
second-step acid leaching (Zhang et al., 2013). A ‘‘fire-wet” process
of recovering REEs from waste phosphor combines the alkaline
fusion, acid leaching, and chemical precipitation methods. Yang
et al. (2013) investigated a recycling process of REEs from waste
phosphor by a two-step process, which includes acid leaching
and solvent extraction with the use of ILs. The IL-based DODGAA
system presents a new direction for efficient recycling method.
Acid leaching and solvent extraction are promising hydrometal-
lurgy processes to extract rare earth elements (Wu et al., 2014).
Acid solution and solvent for good recovery efficiency, enhanced
purity, and easy dissolution of rare earth elements, especially Y
and Eu (Rabah, 2008; Jha et al., 2016). Acid and solvent extraction
methods involve chemical solutions, organic regents, heating treat-
ments, and high-energy-consuming equipment. High temperature
and energy are necessary to leach rare earth metals. However, this
phenomenon may elicit negative effects and induce carbon emis-
sion on the ecosystem because recycling technologies are not envi-
ronmentally friendly. Therefore, an LCA tool should be used to
determine the underlying mechanism of the whole recycling pro-
cess and to develop green technologies that support sustainable
development (Huang et al., 2015). Kubota et al. (2008) indicated
 A.H. Hu et al. / Waste Management 60 (2017) 765–774
that IL can be used as an environmentally friendly technology in
solvent extraction methods to recycle rare earth metals. Consider-
ing the convenient operation, high recycling efficiency, and envi-
ronmental effects, we selected acid and solvent extraction
methods to evaluate the carbon footprint and provided comments
and suggestions to improve their recycling processes. The main
REEs of the waste phosphor include light REEs (La, Ce, and Eu)
and heavy REEs (Y and Tb). Considering the leaching efficiency,
industrial applicability, and high demand for production of phos-
phor (Van den Bogaert et al., 2015), we chose Y and Eu for this
research.
3. Methodology
3.1. Experiments and materials
The acid extraction method was evaluated based on the recov-
ery efficiency of REEs from waste phosphor. Two acidic solutions
(H2SO4 and HCl) at two different temperatures (60 and 90 °C) were
employed. The raw materials included phosphor, acetone, and sul-
furic and hydrochloric acids, and the instruments in the experi-
ment included an oscillator, centrifuges, ovens, a magnetic
stirrer, and a pump. Approximately 5 g of waste phosphor was
used as the main raw material in the acid extraction methods. In
this method, the phosphor is first flushed by acetone. The wet
phosphor was subjected to shock while stirring, and then oven-
dried. Second, the leaching process was conducted by using sulfu-
ric and hydrochloric acids at two different temperatures. Third, the
solution was separated using a centrifuge and a pump. This process
completes the first step of acid extraction. The second step for the
acid extraction was repeated, and finally an aqueous solution
(approximately 180 ml) was obtained. An inductively coupled
plasma (ICP) instrument was used to analyze the concentration
of REEs. The amount of phosphor residue was not included in the
scope of this study. A flow chart of the acid extraction method is
shown in Fig. 3.
A solvent extraction method was used to recovery efficiency of
the REEs from waste phosphor with the use of an IL. This method
Phosphor
Washed with acetone
Centrifugal drying
H2SO4 1st Acid leaching
HCl
Heating and stirring
filtration
H2SO4
2st Acid leaching
HCl
Heating and stirring
filtration
RE solution
Fig. 3. Flow chart of the acid extraction method.
769
was divided into two stages, one is acid leaching, and the other
one is IL extraction. The input of raw materials included phosphor
and sulfuric acid. After the acid leaching step, the IL and extractant
were added into the extract; the IL ([C4mim][Tf2N]) with DODGAA,
sodium hydroxide, and sulfuric acid were used. The instruments
were shock, heating mixer, temperature machines and centrifuge.
One gram of phosphor consumption was used in the solvent
extraction method. In this method, sulfuric acid was used to leach
waste phosphor, and the leach residue was collected and washed
with pure water and then dried. Second, the IL ([C4mim][Tf2N])
with DODGAA was added in the leach residue, and the pH was
adjusted using 1 M sodium hydroxide solution. Third, shock and
temperature machines and centrifuge were used, and then sulfuric
acid solution was added to perform back extraction. Finally, an
aqueous solution (approximately 17.6 ml) was obtained, and then
an ICP instrument was used to analyze the concentration of REEs.
The flow chart of the IL extraction method is shown in Fig. 4.
3.2. Life cycle assessment and carbon footprint
Life cycle assessment (LCA) is a method used for evaluating con-
sumption of resources, such as water, electronics, and other mate-
rials, and estimating the cumulative environmental impacts
associated with the entire life cycle of a product (Corporation
and Curran, 2006). The methodological framework of all LCA tech-
niques is based on the ISO standards 14040 (Europe, 2009). The
evaluation of the structure and processes can be divided into goal
and scope definition, inventory analysis, impact assessment, and
interpretation. The carbon footprint calculation in this study is
based on the ISO standard 14067-1, which is the accumulated
activity date of the entire LCA multiplied by carbon emission factor
(f) [Eq. (1)]. The carbon footprint denotes the total carbon emission
for the entire life cycle.
X
CF of activities ¼ ðActivity data i  Emission factor f Þ ð1Þ
The activity data i denotes the intensity of the activity, which is
expressed by volume or mass. The carbon emission factors are con-
stants, which depend on the linear relation between the activity
intensity and carbon emission. The calculation methodology of
2007 GWP 100a is based on the Intergovernmental Panel on Cli-
mate Change (IPCC) factors. Environmental data (materials con-
sumption and emissions) related to the various analyzed material
options were obtained from the Ecoinvent v3 database. These elec-
tricity data were adapted from the 101 annual electricity carbon
emission factor (i.e., 0.532 kg CO2 eq/kW h) of the Taiwan Bureau
of Energy, Ministry of Economic Affairs (Bureau of Energy, 2013).
Carbon footprint was estimated using SimaPro 8.0.2, and the IPCC
2007 GWP 100a methodology was applied.
3.3. System boundary and scope definition
The main goal of this study was to estimate the carbon footprint
of the acid and solvent extraction methods by LCA under different
conditions. The system boundary is a recovery process from waste
phosphor, which includes raw material and manufacturing stages,
and all raw material, energy, and resource use are quantified over
the whole life cycle from ‘‘gate to gate” (B2B). The raw material
stage means the material transportation from supplier and the
manufacturing stage indicates the REE recycling experiment. The
manufacturing stage includes the energy and material inputs, recy-
cling experiment and outputs. In this study, the LCA of the resource
consumption includes waste phosphor, chemical solution, and
electricity. The analysis equipment is not included in this study
because the test duration is limited. Other factors involved in the
process structures such as equipment maintenance and operation
770 A.H. Hu et al. / Waste Management 60 (2017) 765–774

Phosphor Filtrate(H2SO4)

H2SO4
[C4mim][Tf2N] /DODGAA
NaOH aq(pH control)
Acid leaching

Liquid-Liquid The other

Exreaction metals
Soild/Liquid
Separation
IL Recycle Y,Eu loading

Back Extraction Y,Eu

Fig. 4. Flow chart of the IL extraction method (Yang et al., 2013).

belong to indirect emission. The waste stage of the extraction pro-
cess was not included because waste treatment is not included in
the process. The system boundary and scope of the recycling pro-
cess is shown in Fig. 5.
3.4. Functional unit
The functional units were defined based on the addition of two
acidic solutions (H2SO4 and HCl) at two different temperatures (60
and 90 °C) in the acid extraction process, which produced different
REE recovery concentrations and carbon emissions. To compare the
carbon footprint of the different conditions, the average recovery
concentrations of yttrium and europium were adopted as the func-
tional units: 14645.55 ppm for yttrium and 1557.17 ppm for euro-
pium. Furthermore, we assumed two functional units to compare
the two extraction methods: the same amounts of phosphor
(
1 g) for input, and the same amounts of recovery concentrations
of yttrium (
16,100 ppm) for output.
3.5. Inventory data collection
Inventory data of the acid extraction methods were collected to
investigate the laboratory settings; primary data were collected
through experiments. In the raw material stage, we surveyed the
information of supplier background and the input weight of exper-
iments, and then locations were searched and the transport dis-
tance was estimated using Google Maps; the concept of ton–
kilometer was used. Material transport was assumed to be a 3.5-
ton truck. In the manufacturing stage, the experimenter provided
the energy resources input data and the experiment equipment
model, and information from the Internet was used to collect the
operating power for the equipment. Table 1 presents the inventory
data of the acid extraction methods.
The solvent extraction method in this study refers to Japan’s
REEs recycling technical literature ‘‘Selective extraction and recov-
ery of REEs from phosphor powders in waste fluorescent lamps
using an IL system” (Yang et al., 2013). We contacted the author
of the paper, Yang Fan, who worked at the Chinese Academy of
Sciences Institute of Xiamen REE materials. The research was
focused on environmentally friendly technology. In this study,
inventory data were collected by contacting the author through
mails. The raw material inventory data was provided by the paper
in the text, and material transport of vehicle was assumed to be a
3.5-ton truck. Google map was used to measure the distance. The
experimental instrument was provided by the author. An experi-
mental instrument model was assumed in this study, and informa-
tion from the Internet was used to collect the operating power for
the equipment. Table 2 presents the inventory data of the solvent
extraction methods.

Energy, material
inputs
Phosphor Transport

Process outputs

Chemical
Transport
reagents

waste XRF ICP

Raw material Manufacturing

Fig. 5. System boundary and scope of this study.
 A.H. Hu et al. / Waste Management 60 (2017) 765–774 771

Table 1
Inventory data of the acid extraction methods.

Acid extraction methods Transport distance (T-km) Electricity consumption (kW h) Water consumption (g) Reagent consumption (g) Resource depletion (g)
Phosphor powder 0.000354 – – – 5.447
Acetone 0.0113 – – 118.5 –
Sulfuric acid 0.0710 – – 736 –
ID water – – 1000 – –
Shaker – 0.3625 – – –
Centrifuge – 0.758 – – –
Oven – 9.55 – – –
Magnet stirrer – 6.312 – – –
Filter – 0.15 – – –

Table 2
Inventory data of the solvent extraction methods.

Solvent extraction methods Transport distance Electricity consumption Water consumption (g) Reagent consumption (g) Resource depletion (g)
(T-km) (kW h)
Phosphor powder 0.0000753 – – – 1
DODGAA 0.0047 – – 77.445 –
[C4mim][Tf2N] 9.5E6 – – 1.44 –
Sulfuric acid 0.00223 – – 36.8 –
Sodium hydroxide 0.00129 – – 21.3 –
Water – – 2000 – –
Shaker – 0.00955 – – –
Centrifuge – 0.033 – – –
Heating mixer – 7.2 – – –
Temperature machines – 12 – – –

4. Results and discussion
4.1. Results of acid extraction method
Sulfuric acid leaching and 90 °C heating were employed in the
raw material and manufacturing stages. The carbon footprint is
0.0396 kg CO2 eq in the raw material stage and 10.03 kg CO2 eq
in manufacturing stage. The carbon footprints of acetone washing,
first sulfuric acid leaching, and second sulfuric acid leaching are
5.57, 2.25, and 2.21 kg CO2 eq, respectively. Main contributors to
the carbon footprint emission in the manufacturing stage include
the oven and magnet mixer, with approximately 5.08 and
1.68 kg CO2 eq emissions, respectively. The results of carbon foot-
prints of the acid extraction are shown in Fig. 6.
4.2. Results of solvent extraction method
The manufacturing stage was divided into two stages, namely,
first sulfuric acid leaching and IL stage. The carbon footprint in
the raw material stage is 0.00175 kg CO2 eq. The carbon footprint
in the manufacturing stage is 10.64 kg CO2 eq, and that in the first
sulfuric acid leaching and IL stage are 3.89 and 6.75 kg CO2 eq,
respectively. The main contributor to the carbon footprint in the
acid leaching stage was the heating mixer, with approximately
3.84 kg CO2 eq emission. In the IL stage, the main contributor to
the carbon footprint emission was the constant-temperature
machine, with approximately 6.4 kg CO2 eq emission. The results
of carbon footprints of the solvent extraction method are shown
in Fig. 7.
4.3. Comparison of the methods under different condition
The main parameters of acid extraction methods are acid solu-
tion and stirring temperature. Sulfuric acid was first used in the
acid extraction methods at 60 and 90 °C. After adjusting the exper-
imental parameters, the sulfuric acid was replaced with hydrochlo-
ric acid and the temperature was adjusted to 60 and 90 °C.
Different experimental parameters produced different carbon foot-
prints and extraction rates. The inventory data of the acid leaching
at 90 °C are shown in Table 3.

Acid extraction

12 Total emission
10 Raw material transport
8 Washed with acetone
10.0696
6 1st Sulfuric acid leaching
4 2nd Sulfuric acid leaching
5.57
2 0.0396 2.25 2.21
0
Total Raw Washed 1st 2nd
emission material with Sulfuric Sulfuric
transport acetone acid acid
leaching leaching

Fig. 6. Carbon footprints of the acid extraction according to the IPCC 2007.
772 A.H. Hu et al. / Waste Management 60 (2017) 765–774

Solvent extraction

12
Total emission
10
Raw material transport
8
Sulfuric acid leaching
6 10.64175
Ionic Liquid extraction
4 6.75
2 0.00175 3.89

0
Total Raw Sulfuric acid Ionic Liquid
emission material leaching extraction
transport

Fig. 7. Carbon footprints of the solvent extraction according to the IPCC 2007.

Table 3
Inventory data of the acid leaching in 90 °C.

Acid extraction methods Electricity consumption (kW h) Water consumption (g) Reagent consumption (g) Resource Depletion (g)
Sulfuric acid 17.132 1000 854.5 5.447
Hydrochloric acid 12.104 1000 196.38 5.43

The functional units of four different parameters in the acid
extraction method are expressed in terms of the average values
of extraction concentrations: 14,645.55 ppm for yttrium and
1557.18 ppm for europium. LCA results indicate that when the
extraction concentration of yttrium and europium were the same,
the use of 2 M sulfuric acid at 60 °C had lower carbon emission
than at 90 °C. The use of hydrochloric acid as the leaching solution
produced lower carbon footprint than the use of sulfuric acid at the
same temperature. The carbon footprints of the different condi-
tions are shown in Table 4.
4.4. Discussion on the two extraction methods
Acid and solvent extraction methods were compared in this
study with regard to carbon footprint emission, in which two sce-
narios of functional units were employed. In the first scenario, the
phosphor consumption was assumed to exhibit a linear relation-
ship with the extraction concentration of yttrium, which was used
as the functional unit. In addition, the amount of phosphor con-
sumption was 1 g, which was the same as that in the solvent
extraction methods, and the carbon footprint would have ratio
relationship. In the second scenario, the same extraction concen-
tration was assumed as the baseline for comparison. The extraction
concentration of yttrium in solvent extraction methods was con-
sidered the functional unit, in which 16,100 ppm was applied for
yttrium.
In the first scenario, we selected 2 M, H2SO4, and 90 °C for the
comparison baseline. The amount of phosphor consumption was
assumed to be 1 g and the original phosphor consumption was
5 g; therefore, the phosphor consumption in acid extraction meth-
ods was adjusted to 1 g so that the carbon footprint would gener-
ate originally 0.2 times, according to the linear relationship. In the
2 M, H2SO4, and 90 °C condition, the carbon footprint was
2 kg CO2 eq. The solvent extraction had higher carbon footprint
than the acid extraction. In the second scenario, the functional
units assumed a 16,100 ppm concentration for yttrium. The acid
extraction methods should employ 5.5 g phosphor for consump-
tion, 404.5 g of sulfuric acid, and 42.83 g hydrochloric acid to reach
16,100 ppm extraction concentration. The more resources are con-
sumed, the higher the carbon footprint. Therefore, the solvent
extraction method had higher carbon footprint than the acid
extraction method.
The carbon footprints under the same functional units allows
for comparison of the two scenarios to arrive at a reasonable con-
clusion. Whether phosphors input or extraction concentration was
applied as the functional unit, the solvent extraction method had
higher carbon emission than the acid extraction method. However,
the acid extraction method should consume more phosphors than
the solvent extraction method to produce 16,100 ppm yttrium.
Therefore, solvent extraction had much higher extraction effi-
ciency than acid extraction. The carbon footprints of the two
extraction methods are shown in Table 5.
5. Conclusion
Results showed that solvent extraction exerted higher levels of
carbon emission than acid extraction and provided guidance for
selecting high-efficiency and low-carbon emission conditions for
recycling. The instruments operation had caused the highest
carbon footprint, which exhibited a close relationship with the

Table 4
Carbon footprints under different condition.

Sample list Extraction concentration Average concentration SimaPro

Y (ppm) Eu (ppm) Y (ppm) Eu (ppm) Carbon emission (kg)
2M H2SO4 60 °C 16874.748 1354.9145 14645.55 1557.18 9.76
2M H2SO4 90 °C 14109.461 1542.8455 10
2M HCl 60 °C 14132.356 1637.6435 9.26
2M HCl 90 °C 13465.613 1653.3035 9.54
 A.H. Hu et al. / Waste Management 60 (2017) 765–774
Table 5
Carbon footprints of two extraction methods.
Two extraction methods Functional unit
Phosphor consumption (g)
H2SO4 (60 °C/90 °C) 1 1.95/2
HCl (60 °C/90 °C)
Solvent extraction
operating wattage and operating time of instruments. For future
studies on REEs recycling technology, low-power equipment may
be used to achieve an environmentally friendly technology with
low carbon emission and the effect of adopting different duration
of equipment operation on the recycling efficiency and carbon
footprint should be determined.
This study also helps expand various perspectives from a labo-
ratory scale to an industrial scale. In industrial scale, a high amount
of recovered materials should be collected and transported, and
such a high amount corresponds to a high carbon footprint. There-
fore, mechanisms should be established to collect large amounts of
recovered materials from recycle bins, shorten transportation dis-
tance, and improve transport efficiency. In the manufacturing
stage, carbon footprint can be reduced when low-power equip-
ment is used, green extractant is utilized, and chemical substance
emission is decreased. Thus, rare earth recycling strategies with
low carbon footprint and green chemical technologies can be
improved.
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