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A Review of Current Progress of Recycling Technologies for Metals from Waste

Electrical and Electronic Equipment

Article in Journal of Cleaner Production · April 2016

DOI: 10.1016/j.jclepro.2016.04.004

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 Journal of Cleaner Production 127 (2016) 19e36

Contents lists available at ScienceDirect

Journal of Cleaner Production

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

Review

A review of current progress of recycling technologies for metals from

waste electrical and electronic equipment
Lingen Zhang, Zhenming Xu*
School of Environmental Science and Engineering, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai 200240, People's Republic of China

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

Article history: The development of the recycling technologies for waste electrical and electronic equipment (WEEE) has
Received 2 November 2015 entered a new stage. The WEEE disposing technologies have evolved from simple disassembly, classifi-
Received in revised form cation and sorting to high value-added utilization technologies. In the past decade, some modified and
3 April 2016
novel technologies have been developed to recover metals from WEEE. This paper focuses on the
Accepted 4 April 2016
Available online 12 April 2016
recycling of metals from WEEE. The recycling principle, separating process, and optimized operating
parameters of existing technologies are summarized and discussed in detail. Based on traditional recy-
cling technologies of WEEE, pyrometallurgical technology and some mild extracting reagent, such as
Keywords:
Recycling technology
chloride medium, ammoniaeammonium and non-cyanide lixiviants can effectively recycle metals.
Waste electrical and electronic equipment Compared with the conventional acid and cyanide leaching, they have vast improvements in aspect of
(WEEE) environmental protection. More than 98% of Cu and 70% of Au can be extracted. In addition, electro-
Metals chemical technology, supercritical technology, vacuum metallurgical technology, etc. are also applied to
Environmental assessment recycle WEEE. The recovery rate of Cu and Pb under optimum conditions is around 84.2% and 89.4%
respectively in supercritical water oxidation (SCWO) combined with electrokinetic (EK) technology.
Vacuum technology has good environmental performance due to its avoiding discharge of waste water.
Other new technologies such as ultrasound technology, mechanochemical technology, and molten salt
oxidation technology have also been tried to recycle metals from WEEE. Regrettably, although many
endeavors to develop recycling technologies have been attempted, these technologies are still relatively
single and limited because WEEE is a complex system. Hence, the shortages and defects of each tech-
nology are discussed from the perspective of technological promotion and environmental protection.
Furthermore, the outlook about the further development of recycling technologies for metals from WEEE
is presented.
© 2016 Published by Elsevier Ltd.

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 20
2. Selection and classification of research methods . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 22
3. Traditional methods to recycle metals from WEEE . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 23
4. Advanced technologies to recycle metals from WEEE . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 23
4.1. Pyrometallurgical technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 23
4.2. Mild extracting technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 24
4.3. Biometallurgical technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 25
4.4. Electrochemical technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 26
4.5. Supercritical technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 27

Acronyms and abbreviations: WEEE, waste electrical and electronic equipment; BFR, bromined flame-retardant; Waste PCBs, waste printed circuit boards; PMO, precious
metals operations; BMO, base metals operations; LIBs, lithium-ion batteries; SCW, supercritical water; BER, brominated epoxy resin; SCWO, supercritical water oxidation;
SCM, supercritical methanol; EK, electrokinetic; XRD, X-ray diffractometer; LCD, liquid crystal display; CRTs, cathode-ray tubes; TCLP, toxicity characteristic leaching pro-
cedure; MSO, molten salt oxidation.
* Corresponding author. Tel./fax: þ86 21 54747495.
E-mail address: zmxu@sjtu.edu.cn (Z. Xu).

http://dx.doi.org/10.1016/j.jclepro.2016.04.004
0959-6526/© 2016 Published by Elsevier Ltd.
20 L. Zhang, Z. Xu / Journal of Cleaner Production 127 (2016) 19e36

4.6. Vacuum metallurgical technology . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 28

4.7. Other novel technologies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 31
5. Environmental and practical defects of advanced technologies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32
6. Perspectives on recycling technologies . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32
6.1. Recycling technologies aspect . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32
6.2. Environmental protection aspect . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 32
7. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 33
Acknowledgments . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34
Supplementary data . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 34

1. Introduction advantages, such as less secondary waste and lower energy con-
sumption (He et al., 2006).
With new technological innovation, the replacement of equip- However, WEEE contains not only all kinds of metals, but other
ment is persistently accelerating the occurrence of serious pollu- chemical components which are also quite complicated, such as
tion problem resulting from waste electrical and electronic plastics and brominated flame retardants (BFRs). If WEEE is not
equipment (WEEE). The global amount of WEEE produced and disposed or recovered properly, it will cause serious environmental
disposed is sharply increasing over the past several decades. Ac- pollution and even jeopardize human health (Wang and Xu, 2015).
cording to statistics of Kiddee et al. (2013), 500 million tons of The main hazardous and useful materials of typical WEEE compo-
computers were discarded between 1997 and 2007 in the United nents are shown in Table 3. It has been reported that the occurrence
States and 610 million tons of computers became obsolete in Japan of recycling of WEEE by environment-unfriendly, hazardous and
by the end of 2010. The same statistics indicate more than 1.1 primitive technologies in China has increased in the past decades
million tons/year WEEE are generated in China, particularly from (Ni et al., 2010). Massive amounts of dumping or open burning of
manufacturing industry, end-of-life appliances and imports from WEEE took place in some cities of China.
developed countries (Hadi et al., 2015). Every year, 20e50 million Therefore, research on resource reutilization and safe disposal of
tons of WEEE are generated worldwide and this figure is growing the metals from WEEE has a great significance from the viewpoint
by about 45 million tons/year (Ogunseitan, 2013). of environmental protection. In the initial stage of WEEE recycling,
The waste electrical and electronic products are diverse, simple and rough recovery processes were widely adopted. As
including printed circuit boards (PCBs), television sets, re- shown in Fig. 2, ways of recycling metals from WEEE mainly include
frigerators, computers, cell phones, batteries, etc. Table 1 shows the manual dismantling, hydraulic shaking bed separation, strong acid
main components of typical WEEE, which were first listed in the leaching, etc. The defects of these methods are huge, as they not
Waste Electrical and Electronic Products Recycling Directory by only have low recovery efficiency, but also damage human health
Chinese government in 2011. and environment. Facing the serious issue resulting from crude
WEEE contains a variety of valuable materials, such as metals, recycling of WEEE, the European Union Council passed WEEE
glass, plastics and others. As can be seen in Fig. 1, WEEE is mainly Directive and the Restriction of Hazardous Substances (RoHS)
composed of metals (~60% weight), followed by plastics (~15.21% Directive to limit the harmful composition in electronic products in
weight), and CRT & LCD screen (11.87% weight). January 2003. In the last decade, China has followed the same
Although WEEE accounts for only 3e5% in solid waste, the va- legislative trends and developed WEEE laws and directives
rieties and contents of valuable metals in it are far more than other (Gottberg et al., 2006).
forms of municipal waste (Li et al., 2015). As shown in Table 2, Entering the 1970s, mechanicalephysical separation methods
WEEE such as printed circuit boards, TV scrap has high content of began to be utilized to treat the WEEE (Zhang and Forssberg, 1998).
base metals and the electronic devices such as personal computers Mechanicalephysical separation steps included selectively
and mobile phone scrap contains a large number of precious metals dismantling, crushing and physical separation methods. The
(Akcil et al., 2015; Cui and Zhang, 2008). Therefore, WEEE is worthy
of the name of “urban mine”. According to a survey by Environ-
mental Protection Agency, U.S., compared with primary metals
production, recycling metal resources from WEEE has significant

Table 1
Main components of typical WEEE (He and Xu, 2014).

Typical WEEE Main components

Refrigerator Tubes, liners, condenser, wires, refrigerant

Air conditioner Heat exchanger, motor, compressor,
copper pipe, PCBs, wires, refrigerant
Washer Tub, drain hose, motor, wires, salt waste
Television Deflection yoke, demagnetized coil,
speaker, PCBs, wires, CRTs, LCD
Computer Speaker, battery, storage medium,
PCBs, wires, CRTs, LCD
Cell phones Plastic enclosure, battery, storage
medium, PCBs, wires, LCD
Printer/duplicator Roller, toner, PCBs, wires, toner cartridge
Fig. 1. Typical material fractions in WEEE (Wang and Xu, 2014).
 L. Zhang, Z. Xu / Journal of Cleaner Production 127 (2016) 19e36 21

Table 2
Weight composition and value distribution of metals for different WEEE (Cui and Zhang, 2008).

Electronic waste Content and value distribution for different WEEE (%) (in brackets)

Weight (%) Weight (g/t)

Fe Cu Al Pb Ni Ag Au Pd

TV board scrap 28 (4) 10 (39) 10 (13) 1 (2) 0.3 (5) 280 (6) 20 (25) 10 (6)
PC board scrap 7 (0) 20 (10) 5 (1) 1.5 (0) 1 (1) 1000 (64) 250 (5) 110 (15)
Mobile phone scrap 5 (0) 13 (8) 1 (0) 0.3 (0) 0.1 (0) 1380 (5) 350 (67) 210 (19)
DVD player scrap 62 (17) 5 (35) 2 (4) 0.3 (1) 0.05 (1) 115 (4) 15 (33) 4 (4)
PC mainboard scrap 4.5 (0) 14.3 (6) 2.8 (0) 2.2 (0) 1.1 (2) 639 (2) 566 (81) 124 (8)
Printed circuit boards scrap 12 (1) 10 (19) 7 (4) 1.2 (1) 0.85 (6) 280 (3) 110 (66) e
TV scrap (CRTs removed) e 3.4 (82) 1.2 (9) 0.2 (2) 0.038 (4) 20 (3) <10 (e) <10 (e)
Calculator scrap 4 (1) 3 (12) 5 (6) 0.1 (0) 0.5 (8) 260 (6) 50 (64) 5 (3)
Portable audio scrap 23 (3) 21 (78) 1 (1) 0.14 (0) 0.03 (0) 150 (3) 10 (12) 4 (2)
Typical electronic device scrap 8 (0) 20 (5) 2 (0) 2 (0) 2 (2) 2000 (3) 1000 (87) 50 (2)
E-scrap sample 27.3 (1) 16.4 (22) 11 (5) 1.4 (1) e 210 (2) 150 (65) 20 (4)

Table 3
Main hazardous and useful materials in components of typical WEEE (He and Xu, 2014).

Component Hazardous materials Useful materials

PCBs Heavy metals, brominated flame retardants Glass fiber, resin, copper
Refrigerator cabinet Freon Copper, aluminum, plastic
Toner cartridge Toner aluminum, steel, plastic Aluminum, steel, plastic
CRT Pb (PbO) Glass
LCD panel Liquid crystal, TAC, PVA Glass, In2O3
Wire Polychlorinated biphenyls Copper, aluminum, plastic
Li-ion battery LiPF6 Steel, Al, Cu, Li, Co
NieCd battery Cd Steel, Fe, Ni

Fig. 2. (a) Manual dismantling and (b) hydraulic shaking bed separation to recycle metals in WEEE.

Table 4
A summary of separating situation for the physical separation technologies (Ruan and Xu, 2016).

Physical separation method Character of separation Main advantages and disadvantages

Magnetic separation (MS)
Eddy current separation (ECS)
Air current separation (ACS)
Corona electrostatic separation (CES)
Separation of ferrous metals
Separation of ferrous and
non-ferrous materials
Separation of light particles
from heavy particles
Separate metallic particles
(size from 0.2 mm to 1 mm)
from non-metallic particles
MS was most suitable separating steel or iron but not suitable for
separating of non-ferrous metals
ECS was encouraged to recover non-ferrous metallic particles and
hard to separate ferrous metals/other metals
Wind velocity, particle size, particle density, etc. were the critical
influences for ACS
The movement trajectory and collection position of metallic particles
in CES were hard to predict and compute

separating situations for the physical separation technologies are particles. Mechanicalephysical separation technologies have ach-
summarized Table 4. ieved good effects in aspect of practice and environmental pro-
The methods of magnetic separation and eddy current separa- tection. They have been adopted by most of the recycling
tion are usually chosen to separate ferrous and non-ferrous metal enterprises in China. An integrated mechanical-physical recycling
22 L. Zhang, Z. Xu / Journal of Cleaner Production 127 (2016) 19e36
technology for WEEE was established by Xu and his team (Li et al.,
2007; Li and Xu, 2010), including two-step crushing, corona elec-
trostatic separation, to recover metallic and non-metallic materials
(Huang et al., 2009a). Eddy current and electrostatic separation
methods have achieved recovery for magnetic metals, such as Fe,
Ni, Co etc (Habib et al., 2013; Jujun et al., 2014; Menad et al., 2013).
Furthermore, non-metal materials from WEEE also achieved recy-
cling as padding (Guo et al., 2010a, b). Fig. 3 shows an automatic
production line of corona electrostatic separation and eddy sepa-
ration equipment.
Regrettably, mechanicalephysical recycling technology for the
most of single metal from WEEE cannot achieve effective recycling.
Now, one of the biggest challenges in terms of the recycling tech-
nologies for WEEE is how to further classify and recycle high value-
added metals from WEEE through scientific and effective ways/
methods.
As a matter of fact, WEEE is a complex system, containing
various organic substances, and metals. Therefore, the methods and
technologies of recycling metals from WEEE are totally different
from technologies of mineral separation. In order to develop and
implement both environmentally friendly and economically viable
recycling processes of metals, a large number of novel technologies
are proposed in recent years and mainly include: pyrometallurgical
technology, mild extracting technology, electrochemical technol-
ogy and vacuum metallurgical technology etc (Rocchetti et al.,
2013; Weeden et al., 2015).
Pyrometallurgy has been successfully realized industrialization.
Its principle involves metals enrichment by smelting and convert-
ing, refining and other processes to remove the non-metallic ma-
terial from WEEE. In this process, the crushed scraps are burned in a
furnace or in a molten bath to remove plastics. The refractory ox-
ides form a slag phase together with some metal oxides (Cui and
Zhang, 2008; Flandinet et al., 2012). Traditional hydrometallurgi-
cal process is associated with acid or alkaline solutions to solubilize
crushed WEEE. This process is called leaching. But in recent decade,
hydrometallurgical technology has begun to pay more attention to
environment-friendly recycling metals. Some mild leaching agents
and modified technologies are proposed, which offer more exact,
relatively low construction costs and a certain recovery rate of
metals with their suitability for small scale applications. In recent
years, extensive studies and practices have been carried out on
recycling metals from WEEE by vacuum metallurgical technology
which separates and recycles materials through several kinds of
means like vacuum evaporation, vacuum sublimation (Zhan and
Xu, 2009, 2011, 2012), vacuum reduction (He et al., 2014), vacuum
pyrolysis (Zhou and Qiu, 2010; Zhou et al., 2011), etc. Vacuum
metallurgical technology has some advantages on the separation of
Fig. 3. (a) An automatic production line of corona electrostatic separation and (b) eddy separation equipment.
metals, such as low energy consumption and significant economic
benefits.
Although special advantages come from these technologies,
defects accompany also. These recycling processes for metals are
relatively single, limited, and some methods still have negative
effects on environment. Therefore, it is necessary to summarize and
discuss in detail the current status of recovery technologies for base
and precious metals from WEEE. This paper focuses on the recy-
cling of metals from WEEE, reviews features and defects of the
existing technologies. Based on environmental protection and
resource recycling utilization for the metals, some novel and
environment-friendly ideas are proposed in this article. Meanwhile,
the outlook on the further development of recycling technology is
presented for the metals from WEEE.
2. Selection and classification of research methods
Selection and classification of research methods were divided
into three steps:
(1) Selection and classification of literature: the first step of this
research is to conduct literature reviews by a comprehensive
search on the Scopus, Elsevier and Web of Science database,
using as key words “WEEE” AND “metals” AND “recycle”
AND “technology” AND “metallurgical” and so forth. The
abstracts of the most relevant papers according to their title
were assessed to examine whether they fall under the scope
of the study. In addition, already published reviews on
recycling areas of e-waste were identified and utilized to get
available methods and technologies. The literature was
classified according to different recycling technologies,
metals type (base metals and precious metals) and the
means of pollution control.
(2) Selection and classification of recycling technologies: for
traditional recycling technologies, such as pyrometallurgical
and hydrometallurgical technology, we chose the technolo-
gies which had prominent improvement in the aspects of
environmental protection. In addition, some new/novel
technologies in recent decades were also focused. These
technologies had great significance for recycling metals in
the view of pollution control and recovery efficiency. They
included biometallurgical technology, electrochemical tech-
nology, supercritical technology, and vacuum metallurgical
technology etc.
(3) Evaluation of technological processes: these methods/tech-
nologies were classified into seven specific categories to
facilitate their analysis and evaluation. We focus on each
 L. Zhang, Z. Xu / Journal of Cleaner Production 127 (2016) 19e36 23

category of method/technology to further search in data-
bases. A filtered work of literature for a certain technical
process was carried out. And then, according to the ideas,
devices and results of experiments in literature, we selected
representative examples from each recycling technology to
summarize and review. Finally, some shortages and im-
provements of these recycling processes were proposed from
relevant research papers, review papers and some produc-
tion processes. Hence, this paper reviewed representative
and innovative technologies to clarify current progress of
recycling metals in WEEE.
3. Traditional methods to recycle metals from WEEE
Traditional methods of recycling WEEE are incineration, hy-
draulic shaking bed separation and acid leaching process. For
incineration process, WEEE is directly burned in the blast furnace.
The product in the blast furnace contains 70e85 wt.% black copper.
This black copper is fed into the converter to be oxidized and then is
reduced in the anode furnace. The recovered anode copper can be
further purified in H2SO4 electrolyte with other elements, such as
Ni, Zn, and Fe (Kang and Schoenung, 2005). The hydraulic shaking
bed separation was widely used for recycling metals in waste PCBs
in the past. Crude copper particles can be obtained by this process.
However, this process generates huge amounts of waste water and
residues (Huang et al., 2009a). If not handled properly, waste water
and residues can cause serious secondary pollution. In addition, it is
hard to recover other metals except copper, and non-metal mate-
rials cannot be recycled.
Traditional hydrometallurgy processes are acid leaching to
recover metals (Watling, 2013). HNO3/HCl/HClO4 is used as leach-
ing solvent to extract metals such as Cu, Pb, Zn, etc. from WEEE. In
the past, nitric acid was also used in combination with hydrochloric
acid in the form of aqua regia for non-selective and aggressive
digestion of base and precious metals (Cu, Pb, Zn, Ag, etc.) from
WEEE (Bas et al., 2014; Castro and Martins, 2009; Sheng and Etsell,
2007). Cyanide leaching precious metal Au has been used for more
than one century due to the selectivity and stability of dicyanoau-
rate complex (Kulandaisamy et al., 2003; Quinet et al., 2005). The
cyanide as leaching agent has a major issue, its toxicity, that may
cause environmental and workers safety problems if used
improperly. These traditional methods are not only inefficient but
also greatly damaging to the environment. In recent years, on the
basis of traditional technologies, some advanced recycling tech-
nologies are put forward and have gained considerable progress.
process is most important process for pyrometallurgy. The two
basic and widely applied smelting processes include flash smelting
and bath smelting. Flash smelting employs oxygenated gas to
promote autogenous conditions while bath smelting depends on
the roasting and smelting steps, and reaction occurs in a molten
pool containing both melts and slag phases (Montenegro et al.,
2013). Some advanced smelting equipments have been used in
pyrometallurgy, such as Outokumpu flash smelting, Noranda
reactor system and Mitsubishi continuous smelting (Kucharski
et al., 2014; Moskalyk and Alfantazi, 2003). The next step is con-
verting process. In the copper converters, matte can be obtained
from the converting unit by blowing in air from tuyeres. This step
can oxidize the iron sulfide and convert copper sulfide to metallic
copper. The last procedure is refining units with the purpose to get
high purity copper in the reverberatory or rotary furnaces
(Hagelüken, 2006). The pyrometallurgical process of recycling
copper in WEEE is shown in Fig. 4.
An application for pyrometallurgical process to recover metals
from WEEE was practiced at the Boliden Ltd. Ro €nnskår Smelter,
Sweden. The schematic diagram for the Ro € nnskår Smelter is shown
in Fig. 5a. More than 100,000 t of e-scraps including WEEE were fed
into Kaldo Furnace every year (Cui and Zhang, 2008). The e-scraps
can be fed into the process in different steps according to their
purities. Some e-scraps containing high content of copper were fed
into converting process directly, but low grade e-scraps were fed
into Kaldo Furnace. And further the mixed copper alloys produced
in Kaldo Furnace were sent to the converting process to recover
metals (Cu, Ag, Au, Pd, Ni, Se, and Zn). The dusts containing Pb, Sb,
In and Cd were sent to other operations to further recover (Cui and
Zhang, 2008; Ek and Olsson, 2005; Isaksson and Lehner, 2000).

4. Advanced technologies to recycle metals from WEEE

4.1. Pyrometallurgical technology

Pyrometallurgical technology has been significantly improved in

terms of the recycling technologies and the treatment of pollutant.
Pyrometallurgy can successfully realize industrialization, including
a series of steps, such as dismantling, smelting in a plasma arc
furnace, drossing, sintering, melting and reactions in a gas phase at
high temperatures. In this process, the crushed scraps containing
metals (including base and precious metals) are burned in a high
temperature furnace, and then the metals are volatilized by a
chemical reaction or by heat, and impurities are converted into slags.
Generally, WEEE needs to be treated firstly through the
mechanicalephysical pretreatment: dismantling main parts;
shredding/grinding processes for size reduction, liberation of
components, etc. And then, enriched metals are smelted in furnaces Fig. 4. A schematic flow sheet showing recycling copper in WEEE by pyrometallurgy
and coarse metal ingot can be obtained. In most cases, smelting processes.
24 L. Zhang, Z. Xu / Journal of Cleaner Production 127 (2016) 19e36
Another application for pyrometallurgical process was the plant
of Umicore integrated smelter and refinery. This process mainly
focused on recovery of precious metals from WEEE including Ag,
Au, Pt, Pd, Rh, Ru and Ir. The schematic diagram for the Umicore
Smelter is shown in Fig. 5b. Its procedures included: firstly, WEEE
was pretreated (i.e. dismantling, shredding and physical process-
ing) and then the precious metals operations (PMO) were smelted
in an Isa Smelt furnace. Almost all other metals were concentrated
in the slag after smelting; thirdly, the slag was further treated at the
base metals operations (BMO). The base metals were the byprod-
ucts from the PMO which were subjected to electrolytic refining to
gain high purity base metals, such as copper (Le Ret and Briel, 2011;
Tuncuk et al., 2012).
A crushing-pyrometallurgical process of waste fluorescent
lamps was applied by Nomura Kohsan in Japan (the flow sheet as
shown in Fig. 5c). This process concentrated on the extraction of
base metals, rare earth metals and mercury in the recycling of
fluorescent lamps. The waste fluorescent lamps were calcinated in
vertical calcinatory and then underwent refining process to get rare
earth metals and mercury (Yufeng et al., 2014).
4.2. Mild extracting technology
Modified and new hydrometallurgical technologies have
becoming a hot spot of recent researches. They are more targeted
towards metals recovery or pretreatment, easier to control chemical
reaction, and make relatively less pollution than pyrometallurgical
€nnskår Smelter; (b) plant of Umicore and (c) recycling process of fluorescent lamps (Cui and Zhang, 2008; Tuncuk et al., 2012; Yufeng et al.,
Fig. 5. Schematic diagram for (a) Ro
2014).
technology (Ghosh et al., 2015). Some mild leaching agent for hy-
drometallurgy was proposed, such as leaching process of chlorinate
(He and Xu, 2015), ammoniaeammonium (Koyama et al., 2006; Sun
et al., 2015; Xiao et al., 2013) and non-cyanide lixiviants for leaching
Au (Akcil et al., 2015), etc.
Several chloride-based leaching processes were developed and
presented at the lab/pilot scale. A chloride medium
(HCleCuCl2eNaCl) to extract copper were utilized. Cupric ion
(Cu2þ) acting as an oxidant can form stabilization of cuprous (Cuþ)
when a suitable ligand such as chloride ion (Cl) was added to
sulfate solution (Yazici and Deveci, 2015). Cu2þ also might present
as chloro-complexes ðCuCl2n n Þ in chloride solutions (Yazici and
Deveci, 2013). The equations of reactions are described:
Cu0 þ Cu2þ /2Cuþ
Cuþ þ nCl /CuCl1n
n
(1)
Cu0 þ Cu2þ þ 2Cl /2CuClðsÞ ðDG298 K ¼ 41 kJ=molÞ
Cu0 þ Cu2þ þ 4Cl /2CuCl
2 ðDG298 K ¼ 25 kJ=molÞ
The results showed that increasing the initial concentration of
Cu2þ to 79 mmol/l can improve the extraction of metals with
almost complete extractions (98%) for Cu at a leaching period of
more than 120 min. Yazici and Deveci (2013, 2015) used
H2SO4eCuSO4eNaCl leaching system to extract the metals from
waste PCBs. The effect of initial concentration of cupric (0.5e7.5 g/l
Cu2þ), chloride (4.7e46.6 g/l Cl) and temperature (20e80  C) on
the leaching of copper was investigated. The results demonstrated
 L. Zhang, Z. Xu / Journal of Cleaner Production 127 (2016) 19e36
that the extraction of metals had significantly improved with
increasing temperature and Cu2þ concentration. The Cl/Cu2þ
molar ratio was importance for the extraction process, because Cl
and Cu2þ had a strong interaction in leaching process.
The method of ammoniaeammonium leaching has superiority
in terms of selectivity towards copper (Liu et al., 2009). An
ammoniaeammonium sulfate and chloride systems were used to
recover Cu from waste PCBs. Ammoniaeammonium salt solution
containing Cu(I) and Cu(II) ammine complexes were used as the
leaching agent. The process consisted of two stages: leaching and
purification. In the stage of leaching, Cu in the waste PCBs was
oxidized by Cu(II) to form Cu(I)eammine complex ions, resulting
from the decreased oxidationereduction potential during the
leaching. The leaching reaction can be expressed as:
þ
Cu þ CuðNH3 Þ2þ
4 /2CuðNH3 Þ2
The Cu(II)eammine complex significantly enhanced the leach-
ing rate of Cu (leaching rate >95%). In the stage of purification, an
electro-winning technology had been proposed to recycle Cu in the
Cu(I)eammine complex ðCuðNH3 Þþ 2 Þ (Koyama et al., 2006; Oishi
et al., 2007). They focused on the leaching mechanism and
behavior of copper by electro-winning. Lim et al. (2013) tried to use
NH3/NH4Cl with oxidants CuCl2 leaching to recover metals Cu from
alloy obtained from smelting reduction process of mobile phone
PCBs. It was observed that 98% Cu can be leached under the
following conditions: 2 kmol/m3 NH4Cl and 5 kmol/m3 NH3 solu-
tion, 0.1 kmol/m3 CuCl2 at 30  C.
In order to overcome the disadvantages of cyanide leaching
precious metals, considerable efforts have been made to research
for non-cyanide systems. Hence, several non-cyanide lixiviants
have been proposed and are regarded as being the most realistic
substitutes in recent years, such as thiourea (Li et al., 2012a),
thiosulfate (Chandra and Jeffrey, 2005; Ha et al., 2010; Jeffrey and
Brunt, 2007).
Thiourea ((NH2)2CS) used as a gold extracting agent for WEEE
has shown significant advantage due to its high rate of leaching,
lower toxicity and eco-efficiency (Gurung et al., 2013; Ubaldini
et al., 1998; Vinh Hung et al., 2010; Wronski and Luczak, 2010).
The content of leaching of gold is contingent upon careful optimi-
zation and control of pH, redox potential, thiourea concentration,
and leaching time. The reaction follows the equation:

þ
Au þ 2SCðNH2 Þ2 /Au SC½NH2 2 2
þ e
In addition, the combination of lixiviants can produce a syner-
gistic effect. The effect was evident using ferric sulfate as the
oxidant for leaching Au (Broadhurst and Dupreez, 1993; Li and
Miller, 2007). The gold leaching reaction in acid thioureaeferric
sulfate solution can be represented by the following reaction:

þ
Au þ 2SCðNH2 Þ2 þ Fe3þ /Au SC½NH2 2 2
þ Fe2þ
The conclusion showed that the ferric ion presented in acidic
thiourea solutions can significantly affect the reaction kinetics of
gold cementation. The leaching rate of gold depended on ferric
concentration; ferric ion increased significantly the redox potential
of the solutions, but the leaching rate kept constant with time when
thiourea concentration was below 12 g/l and ferric was above 0.1 g/l
(Birloaga et al., 2013). Birloaga et al. (2014) utilized two chemical
leaching systems to recycle the base and precious metals from
waste PCBs, that is, the first step was the leaching system of sulfuric
acid with hydrogen peroxide, meantime thiourea with the ferric ion
in sulfuric acid medium was used as the second step. The results
indicated that 2 mol/l H2SO4 (98% w/v), 5% H2O2, 25  C, 1/10 S/L
ratio and 200 rpm were founded as optimal conditions for Cu
25
extraction and extraction rate of Cu can reach approximately 100%.
For thiourea acid leaching process, 20 g/l of CS(NH2)2, 6 g/l of Fe3þ,
0.5 M H2SO4 were founded as optimal conditions for Au extraction
and extraction rate of Au exceeded 70%.
On the basis of leaching Au by acidic thiourea in the presence of
ferric iron, a modified hydrometallurgical technology was proposed
for selective recovery of Cu, Ag, Au and Pd from waste PCBs. Firstly,
through two consecutive sulfuric acid leaching steps in the pres-
ence of H2O2 as oxidizing agents, more than 99% of copper was
dissolved. The 2nd leaching step was acidic thiourea in the pres-
ence of ferric iron as oxidizing agent to leach the solid residue,
which 85.76% Au and 71.36% Ag was achieved. The leaching of Pd
and remained Au from the solid reside of 3rd leaching step was
performed in NaClOeHCleH2O2 leaching system, and then palla-
dium and gold were precipitated by sodium borohydride. 100% of
(2) Pd and Au of what was in the chloride leachate were precipitated by
using 2 g/l sodium borohydride (Behnamfard et al., 2013).
Thiocyanate is also an effective lixiviant for gold in acidic con-
ditions. The thiocyanate system has been considered to effectively
dissolve and recycle gold and silver from gold-bearing WEEE. One
important characteristic of the thiocyanate ion is that it can form
stable and soluble complexes of aurothiocyanate ðAuðSCNÞ 2 Þ, and
aurithiocyanate ðAuðSCNÞ 4 Þ (Li et al., 2012b). The equations of re-
actions are as follows:
2SCN þ Au ¼ AuðSCNÞ
2 þe

(5)
4SCN þ Au ¼ AuðSCNÞ
4 þ e 
In sulfuric acid solutions with ferric as oxidizing agent, thiocy-
anate presents and gold dissolves according to reaction:
Au þ 2SCN þ Fe3þ ¼ AuðSCNÞ
2 þ Fe
2þ
(6)
The mechanism of dissolution of gold by ferric-thiocyanate so-
lution was considered as an auto-reduction process, namely, ferric
was spontaneously reduced to ferrous while oxidizing SCN. This
oxidation was considered through forming several intermediate
species, in particular (SCN)3 and (SCN)2, which acted both as ox-
idants and as complex for gold (Li et al., 2012c, d, e).
Followed by above studies, the leaching of gold has been studied
by the combining method of thioureaethiocyanate, using ferric
sulfate as oxidant (Yang et al., 2011). The gold leaching was higher
than either ferric-thiocyanate or ferric-thiourea solutions respec-
tively. The explanation was that the synergistic effect was attrib-
(3) uted to the formation of a mixed ligand complex Au(SC
[NH2]2)2SCN.
Recently, some organic acids are introduced as environment-
friendly leaching reagents. For example, citric acid and hydrogen
peroxide, DL-malic acid or other extraction agents as leaching re-
agents were introduced to leach cobalt and lithium from lithium-
ion batteries (LIBs) (Jha et al., 2013; Li et al., 2010a, b). Extraction
agent as PC-88A, D2EHPA, and Cyanex 272 were used to separate
(4)
and purify the metals (Chen et al., 2011; Dorella and Mansur, 2007;
Swain et al., 2006, 2007; Xu et al., 2008). Separation of base and
precious metals from WEEE using environment-friendly, low cor-
rosive leaching reagents, such as NH3$H2O/KI for Pd, Pt (Dawson
and Kelsall, 2007), and (NH4)2S2O3/CuSO4/NH4OH/O3-Cl for Ag,
Au was also widely investigated (Oh et al., 2003; Vinals et al., 2006;
Vinh Hung et al., 2014; Zhang and Zhang, 2013). Supplementary
data Table S1 summarizes main processes and reactions of modi-
fied hydrometallurgical technologies to recycle precious metals Au.
4.3. Biometallurgical technology
Biometallurgical process is well used in mineral processing as an
alternative technology for recovering metals from very low-grade
26 L. Zhang, Z. Xu / Journal of Cleaner Production 127 (2016) 19e36
ores and concentrates (Watling, 2006). However, most of applica-
tions of the biometallurgy for recovering WEEE are still in a labo-
ratory scale. There are two main fields of biometallurgy for recovery
of metals, namely bioleaching and biosorption.
Bioleaching is technically feasible by the use of bacteria-assisted
reaction to extract base metals such as Cu, Ni, Zn, Cr and precious
metals from WEEE such as Au, Ag in current results of laboratory
scale. For bioleaching, acidophilic group of bacteria plays an
important role in bioleaching of heavy metals such as Acid-
ithiobacillus ferrooxidans, Acidithiobacillus thiooxidans, Leptospir-
illum ferrooxidans, and Sulfolobus sp (Debaraj and Rhee, 2010; Liang
et al., 2010; Panda et al., 2015). For example, Wang et al. (2009) used
bioleaching processes to mobilize metals from waste PCBs. The
bacteria A. ferrooxidans and A. thiooxidans were grown and accli-
mated in waste PCBs and then used as bioleaching bacteria to sol-
ubilize metals. The results demonstrated that all the percentages of
Cu, Pb, and Zn solubilized into the leaching solution from PCBs. The
concentration of PCBs should be controlled under the range from
7.8 to 19.5 g/l. Under 7.8 g/l of the concentration of PCBs, the
dissolution rates of Cu are 99.0%, 74.9%, 99.9% at 0.5e1.0 mm of
sieve fraction at 9 d of leaching time by the pure culture of
A. ferrooxidans, the pure culture of A. thiooxidans, and mixed culture
of A. ferrooxidans and A. thiooxidans, respectively. Similar studies
also showed the leaching content of Cu increased when the amount
of the ferrous ion increased in the solution up to 7 g/l with A. fer-
rooxidans (Yang et al., 2009, 2014). Karwowska et al. (2014) evalu-
ated the possibility of bioleaching Zn, Cu, Pb, Ni, Cd and Cr from
waste PCBs by using a culture of sulfur-oxidizing bacteria and a
mixed culture of biosurfactant-producing bacteria and sulfur-
oxidizing bacteria. The results showed that 48% Zn and 93% Cd were
dissolved in both media. For Ni and Cu, a better effect was obtained
in the acidic medium with a removal rate of 48.5% and 53%
respectively. Pb was removed with very low effectiveness (below
0.5%).
Biosorption process is a physico-chemical and metabolism-
independent process resulting in the removal of substances from
solution by biological materials (Gadd, 2009). The properties of
certain types of inactive or dead microbial biomass materials also
allow them to bind and concentrate metal ions from industrial ef-
fluents and aqueous solutions. Biosorbents are prepared from
different microorganisms including bacteria, fungi, algae, actino-
mycetes, yeasts and some biowaste materials on precious metal
biosorption. Au(III) was successfully recovered as metallic gold
nanoparticles using dead biomass of the brown alga Fucus ves-
iculosus by the study of Mata et al. (2009). The results indicated that
the brown alga F. vesiculosus can recover and reduce Au(III) to Au(0).
The greatest gold uptakes were obtained at initial pH values be-
tween 4 and 9, with an optimum at pH 7. The marine alga
Sargassum natans and the fungal cells of Aspergillus niger, Mucor
rouxii and Rhizopus arrihus were also found to take up precious
metals like gold (Das, 2010). Tasdelen et al. (2009) investigated
recovery of gold from synthetically prepared diluted gold-bearing
solutions of 50 ppm using DEAE-cellulose, a common biopolymer
derivative. The results demonstrated that gold can be effectively
recovered using excessive amounts of DEAE-cellulose (at DEAE-
cellulose/Au weight ratios of 400 and above) and recovery rate of
gold was found to be over 99%. Table 5 lists some recycled efficiency
of base and precious metals by bioleaching and biosorption.
4.4. Electrochemical technology
Electrochemical process is promising technology and offers
unique method to recover base and precious metals from WEEE
due to high environmental compatibility, high energy efficiency
and minimal chemical usage. Some researchers reported this
technology to recover metals from WEEE.
Kim et al. (2011b) developed a process of electro-generated
chlorine to carry out the leaching of metals from waste PCBs. The
technology of electro-generated chlorine has the advantage of
leaching precious metals because of acquiring high oxidation po-
tential (Kim et al., 2011b). Fig. 6a shows the schematic diagram of
separate reactors consisted of an electrolytic cell for chlorine gen-
eration. Two cathodes and anodes were used and hydrochloric acid
was poured into the leaching reactor. Anode reaction can be rep-
resented by the following equation:
2Cl ¼ Cl2 ðelectrode surfaceÞ þ 2e (7)
And the dissolution of gold reaction as:
Au þ Cl þ 3=2Cl2 ðaqÞ ¼ AuCl
4 ðaqÞ DG298 K
¼ 27:04 kcal=mol (8)
Au þ 3=2HClO þ 3=2Hþ þ 5=2Cl ¼ AuCl
4 þ 3=2H2 O DG298 K
¼ 33:29 kcal=mol
They found that the content of leaching of gold was increased
with increasing of temperature and initial concentration of chlo-
rine, and was favorable even at low concentration of acid. But the
leaching of copper was different, that is, leaching increased with
increasing of concentration of acid and decreasing of temperature.
In total leaching process, 97% copper was dissolved and the re-
covery rate of gold was 93% in the separate reactor. A combined
reactor (Fig. 6b) with simultaneous Cl2 generation and metal
leaching which can circulate and reuse chloride ion without addi-
tional supplementation, was compared with the separate reactor
for the recovery effect of metals (Kim et al., 2011a). It was observed
that the leaching rate of Cu increased with increase in current
density, temperature and time in both reactors. The dissolution of
Cu was about 20% and 25% in the combined and separate reactor
respectively with the copper leaching rate gradually diminished.
This result may be attributed to the surface area of copper forming
CuCl(s) with increasing of leaching time. And the leaching effi-
ciency of copper was lower in the combined reactor than that of the
separate reactor due to the change of electrode reactions.
Similarly, a mediated electrochemical oxidation was proposed to
recover copper and separate a rich gold residue from waste PCBs
(Fogarasi et al., 2013, 2014). The process was also carried out by
employing two different types of reactors coupled in series, ac-
cording to the experimental setup from Fig. 6c. One was a leaching
reactor with a perforated rotating drum to dissolve base metals,
and the other one was a divided electrochemical reactor for the
regeneration of the leaching solution with the parallel electro-
winning of copper. In the experiment, the electrolyte with 0.3 mol/l
HCl and different concentrations of FeCl3 was prepared with waste
PCBs. Cu in electrolytes HCl and mediators FeCl3 can be generated
through electrochemical reaction. And Fe3þ can regenerate through
the anodic oxidation. The electrochemical reactors connected in
series can allow the simultaneous generation of Fe3þ and dissolu-
tion of metals without supplementation of the leaching agent. The
process was evaluated through the dissolution efficiency, current
efficiency and specific energy consumptions. A 99.04 wt.% high
purity Cu at a current efficiency of 63.84% was gained at a leaching
of laboratory scale, and specific energy consumption of 1.75 kW h/
kg cooper. Electro-oxidation leaching copper in sulfuric acid solu-
tion was also studied for metal powders from waste PCBs (Ping
et al., 2009). The experiment tried to recover base metal copper
by leaching process using H2SO4, NaCl, CuSO4 and the air. In the
 L. Zhang, Z. Xu / Journal of Cleaner Production 127 (2016) 19e36 27

Table 5
Recovery of base and precious metals by bioleaching and biosorption (Das, 2010; Ghosh et al., 2015).

Microorganisms Recovery rate (%)

Bioleaching Thiobacillus thiooxidans þ T. ferrooxidans Cu, Ni, Al, Zn >90%

Aspergillus niger Cu, Sn 65%
Penicillium simplicissimum Al, Ni, Pb, Zn >95%
Acidithiobacillus ferrooxidans Cu 81.6%
Acidiphilium acidophilum (ATCC 27807) Cu 3.6%, Ni 86% Zn 40.8%
Sulfobacillus thermosulfidooxidans þ acidophilic heterotroph (AlTSB) Ni 81%, Cu 89%, Al 79%, Zn 83%
Chromobacterium violaceum Au 68.5%
A. ferrooxidans Cu 99%
A. ferrooxidans Cu 99%
A. ferrooxidans þ A. thiooxidans genera Acidithiobacillus and Gallionella Cu 96.8%, Al 88.2%, Zn 91.6%
Sulfobacillus thermosulfidooxidans þ Thermoplasma acidophilum Cu 95%
Acidithiobacillus thiooxidans Cu 98%

Adsorbents Max of adsorption quantity (mmol/g)

Biosorption Algae
Fucus vesiculosus Au, 0.35
Dealginated seaweed waste Au, 0.4
Chlorella vulgaris Au, 0.5
Sargassum natanss Au, 2.1
Chlorella vulgaris Au, 0.5
Fungi
C. cladosporioides strain 1 Au, 0.4
C. cladosporioides strain 2 Au, 0.5
Fomitopsis carnea Au, 0.48
Cladosporium cladosporioides Au, 0.5
Aspergillus niger Au, 1
Rhizopus arrhizus Au, 0.8
Bacteria
Streptomyces erythraeus Au, 0.03
Desulfovibrio desulfuricans Pd 1.2, Pt 0.32
Desulfovibrio fructosivorans Pd 1.0, Pt 0.17
Others
Chemically modified chitosan Au 3.4
Bisthiourea derivative of resins Au 3.63
Thiourea derivative of chitosan Pt 2.0
Chitosan derivatives Pt 3.2, Pd 3.5

leaching system, chloride ion was taken as complex agent, and
Cu2þ, air were taken as oxidants. The result showed that the
leaching rate of copper can reach 100%. Oishi et al. (2008) improved
this process. The impurities in the solution were removed by sol-
vent extraction using LIX 26, and the purified Cu(I) solution was
electro-won in a diaphragm cell.
Electrorecycling is a technology which utilizes minimal chemi-
cal input to dissolve and recover metals on a cathode for further
processing (Lister et al., 2014). The advantage of this process is that
use a single electrochemical cell to maximize energy efficiency. A
diagram of the electrorecycling system is shown in Fig. 6d. The
electrorecycling process generated oxidizing agents at anode to
dissolve metals from the scrap matrix meantime dissolved metals
were reduced at the cathode. The electrochemical cell configured a
trough with the cathode solution. EepH diagrams and the data of
metal dissolution were presented for anticipated conditions in the
electrorecycling system. In their work, two stages of electro-
recycling were proposed. Firstly Cu, Sn, Ag and magnet materials
using Fe3þ were dissolved in sulfate and then Pd and Au were
dissolved using Cl2 in a HCl solution. Over 95% Cu and Ag were
recovered, but the recovery rate of Au and Pd was low.
4.5. Supercritical technology
In recent years, supercritical technology is introduced as an
environment-friendly method to decompose organic polymers and
recycle metals due to its special properties, such as low viscosities,
high mass transport coefficient, high diffusivity, and high solubility
for organics (Matsumoto and Oshima, 2014; Xiu et al., 2015; Zhu
et al., 2012).
Li and Xu (2015) applied supercritical water (SCW, Tc ¼ 374  C,
Pc ¼ 22.1 MPa) to decompose brominated epoxy resin (BER) from
waste memory module and environmental friendly recover metals.
Fig. 7a shows the schematic diagram of the semibatch-type reactor.
Experiments were carried under external-catalyst-free with tem-
peratures 350e550  C, pressures 25e40 MPa, and reaction times
120e360 min in a semibatch-type reactor. The results showed that
BER could be quickly and efficiently decomposed under SCW con-
dition, and the recovery rate of metal reached 99.80%. The mech-
anism was possibly free radical reaction.
Supercritical methanol (SCM, Tc ¼ 240  C, Pc ¼ 8.09 MPa) to
simultaneously recover polymers and metals from waste PCBs was
conducted by Xiu and Zhang (2010). Their study focused on the
characteristics of both oils and solid products obtained from the
SCM treated waste PCBs. Fig. 7b shows the schematic diagram of
the chemical recovery process from waste PCBs using supercritical
methanol. The waste PCBs were put into the reactor with methanol
of appropriate volume. After SCM reaction, the liquidesolid
mixture in products was filtered by a membrane filter with pore
size 1.0 m. High concentrations of Cu (34%), Fe (7.9%), Sn (7.9%), Pb
(6.3%) and Zn (2.6%) were found in most of the solid products when
waste PCBs were concentrated effectively after SCM treatment. A
rotary evaporator was used to recover the solvent methanol, and
then the oil and gas products were also recovered. Besides super-
critical methanol, other supercritical fluids were also employed for
the recycling of waste PCBs. Sanyal et al. (2013) used supercritical
28 L. Zhang, Z. Xu / Journal of Cleaner Production 127 (2016) 19e36
Fig. 6. Schematic diagram of (a) separate reactor consisted of an electrolytic cell for chlorine generation; (b) combined reactor consisted of an electrolytic cell for chlorine gen-
eration; (c) a mediated electrochemical oxidation; (d) electro-recycling system (Fogarasi et al., 2014; Kim et al., 2011a, b; Lister et al., 2014).
CO2 as solvent with an additional small amount of water to recover
copper foil, glass fiber and polymer in waste PCB.
A technology of supercritical water oxidation (SCWO) combined
with electrokinetic (EK) process was developed to recover metals
(Xiu et al., 2013, 2015; Xiu and Zhang, 2009a, b). In the process, the
PCBs were pretreated in supercritical water, and then subjected to
EK process (Fig. 7c, d). Xiu et al. used this technology to recover Cu,
Pb (Xiu and Zhang, 2009b) and to prepare Cu2O nanoparticles (Xiu
and Zhang, 2012) from waste PCBs. In the SCWO treatment exper-
iments, the sample and distilled water were employed, and
hydrogen peroxide (H2O2, 30 wt.%) was used as the source of ox-
ygen. The EK process relied upon an electric field with 20 ml of
1 mol/l HCl solutions added to the SCWO-treated waste PCBs. The
metal ions or ionic complexes were formed and migrated to the
cathode or anode. Experimental results showed that supercritical
water oxidation (SCWO) process was strong enough to decompose
the organic compounds of waste PCBs, and XRD spectra indicated
that copper and lead were oxidized to CuO, Cu2O and PbO2. In the
EK process, Cu and Pb can form complexes with Cl and the com-
plexes can be positively charged, negatively charged or uncharged
(MeClþ, MeCl2 (aq), MeCl3 and MeCl2 4 ). The recovery percentages
of copper and lead under optimum SCWO þ EK treatment condi-
tions were around 84.2% and 89.4% respectively.
Highly uniform and monodisperse Cu2O nanoparticles were
gained successfully from waste PCBs in EK process. The average size
of Cu2O nanoparticles decreased from 49.5 to 18.2 nm when current
density increased from 10 to 20 mA/cm2, and the size uniformity of
nanoparticles was improved significantly at a higher current den-
sity. Up to 90 wt.% of Cu in waste PCBs could be recovered as Cu2O
nanoparticles under optimized condition.
4.6. Vacuum metallurgical technology
In recent years, vacuum metallurgical technology has been
applied to recover metals from WEEE because of no waste water
pollution. The separation of metals is based on the difference of
vapor pressure of these metal elements at the same temperature
(as shown in Fig. 8a). Under the guidance of separation crite-
rion, different metals can be successfully separated and recycled
from several waste PCBs. Vacuum distillation of metals is
considered to need to experience four crucial processes, namely,
heat transfer, evaporation, mass transfer and condensation.
Volatile metals in interior of the melt spread to the surface and
arrive at the boundary layer. The temperature and pressure of
volatile metals is Tv and Pv. And then the metals begin to
evaporate. They are condensed at condensation wall, which the
temperature and pressure of volatile metals decrease to Tk and
Pk. Fig. 8b shows the process of metal from volatilization to
condensation. In the process, the rates of volatile metals can be
described different mathematics model (Bird et al., 2002; Li
et al., 2013).
Zhan and Xu (2008, 2009, 2011, 2012) carried out a series of studies
on recycling metals fromwaste PCBs by vacuum separation, using the
self-made vacuum furnace (as shown in Fig. 9a). The study indicated
that Cd can be evaporated preferentially, and subsequently Zn can be
separated as a result of their huge vapor pressure gaps. Mixed metal
particlesofZn,Cddirectsublimatedbysolidstateandsurfaceoxidation
film can hamper this evaporation process. The separation of Pb was
more difficult because the PbeBi alloy was formed with a low vapor
pressure.AndPbwasalsofoundinthesoldersofwastePCBsduetoform
of PbeSn alloy.
 L. Zhang, Z. Xu / Journal of Cleaner Production 127 (2016) 19e36 29

Fig. 7. Schematic diagram of (a) semibatch-type SCW reactor; (b) SCM recovery process; (c, d) SCW combined with EK process (Li and Xu, 2015; Xiu and Zhang, 2009b, 2010, 2012).

Fig. 8. (a) Migration process of the metals from the melt; (b) relationship between the saturation pressure and temperature of metals.

Vacuum metallurgy can also be used to get metal nanoparticles.
Synthesis of bismuth nanoparticles was systematically investigated
following mechanism of aerosol nucleation, condensation and
coagulation. Fig. 9b shows a schematic of the jet aerosol flow
condenser unit. Bismuth vapor was produced in an externally
heated tube flow condenser containing a crucible with the Bi melt.
Transport of the vapor in an argon carrier gas jet was followed by
rapid quenching with second argon streams (in a diluter) and by
particle collection on a filter. The results showed that rapid
quenching of the Bi-vapor flow produced particles with narrow size
distribution. In contrast, counter flow quenching resulted in early
particle formation and broad particle residence time distributions
producing particles with a wide size distribution. Bismuth nano-
particles were synthesized through this process, which average
diameter was about 12e37 nm (Wegner et al., 2002). On the basis
of Karsten Wegner's study, Xing and Zhang (2011) investigated a
novel process for lead nanopowder synthesis from the waste
cathode ray-tube funnel glass.
30 L. Zhang, Z. Xu / Journal of Cleaner Production 127 (2016) 19e36
Fig. 9. Schematic illustration of (a) vacuum distillation recovery system; (b) aerosol flow condenser with its Inconel pipe; (c) vacuum-chlorinated separation system; (d) vacuum
pyrolysis process (Ma et al., 2012; Xing and Zhang, 2011; Zhan and Xu, 2009; Zhou and Qiu, 2010).
Lin and Qiu (2011) tried to use the vacuum reduction technology to
recover Pb in waste lead storage battery. They recovered Pb from two
parts: metallic grids and lead pastes. The results showed that Pb could
be satisfactorily recycled. Similarly, the vacuum reduction technology
also was used to recover Pb (about 20e30% PbO) (Me ar et al., 2006) in
cathode-ray tubes (CRTs). Chen et al. (2009) studied lead recovery
efficiency, optimizing of this process and the evaluation of environ-
mental safety of the product. A reaction equation was shown:
PbO þ C ¼ PbðgÞ þ COðgÞ
DGT ¼ 289; 427  481:88T þ 2RT ln pð328  885  CÞ
The experimental condition was that temperatures were
600e1000  C, vacuum pressures were 10e10,000 Pa, carbon adding
amounts were 0e9%, and holding times were 0.5e6 h, respectively.
Lead, with a purity of 99.3%, was successfully separated and
recovered. The test of Toxicity Characteristic Leaching Procedure
(TCLP) indicated that lead from the foam glass leached at optimum
conditions was below the regulated value. Besides, the waste
NieCd batteries recycling were also investigated (Huang et al.,
2009b, 2010).
For the recovery of rare and precious metals from WEEE, He
et al. (2014) adopted coke powder as the reducing agent to get
metallic indium from discard liquid crystal display (LCD) panels.
In2O3 can be reduced to metallic indium under high temperature
condition with reducing atmosphere. The reactions can be
expressed by follows the equation:
In2 O3 þ 3C ¼ 2InðsÞ þ 3COðgÞ
The experiment for the recovery of indium from waste LCD
power showed that the best parameters were confirmed as 1223 K
and 1 Pa with 30 wt.% carbon addition for 30 min and the recovery
rate of indium could reach to 90 wt.%. On the basis of vacuum
carbon-reduction, an efficient rough vacuum-chlorinated separa-
tion method was proposed for the recovery of indium from waste
LCD panels. NH4Cl was used as the chlorinating agent. Fig. 9c shows
the schematic illustration of the vacuum-chlorinated separation.
The results indicated that the reaction condition of vacuum-
chlorinated metallurgy was easier than the reaction of vacuum
carbon-reduction. The reactions can be expressed by follows the
equation:
(9)
In2 O3 þ 6HCl ¼ 2InCl3 þ 3H2 OðgÞ (11)
The weight ratio of NH4Cl to glass powder and the optimum
particle size were confirmed as 1:2 and less than 0.13 mm, at 400  C
respectively. Indium chloride was successfully recovered from the
waste LCD panels using this method. The recovery rate of indium
and the purity of indium chloride were 98.02 and 99.50% respec-
tively (Ma et al., 2012).
Pyrolysis technology can be considered as an alternative tech-
nology of recycling WEEE in recent years. Pyrolysis can remove
non-metallic materials from WEEE, and then metals can be recov-
ered (Alston et al., 2011; Hall and Williams, 2006). Zhou and Qiu
(2010) and Zhou et al. (2011) have introduced two-step vacuum
pyrolysis processes to recycle metals from waste PCBs. One process
was to separate the solder of the waste PCBs firstly, which was
molten in the heated diesel oil and separated by centrifugal sepa-
ration; and then use vacuum pyrolysis to recover the waste PCBs
(10)
without solder. The other process pyrolyzed the waste PCBs under
vacuum condition firstly; and then the obtained pyrolysis residue
was heated under vacuum to recover the solder by centrifugal
 L. Zhang, Z. Xu / Journal of Cleaner Production 127 (2016) 19e36
separation. The vacuum pyrolysis was carried out on the self-made
equipment, as shown in Fig. 9d. The equipment consisted of elec-
tromotor, reactor, rotating drum, temperature controlled furnace,
cold trap, vacuum pump, etc. The rotating drum was designed
especially to recover solder from waste PCBs. In pyrolysis process,
the solder of waste PCBs was separated and recovered when the
temperature range was 400e600  C, the rotational speed was
maintained at 1000 rpm, and the rotating drum was rotated for
10 min. The recovered solder can be reused directly. The pyrolysis
residues containing other metals, glass fibers and other inorganic
materials still need further treatment.
4.7. Other novel technologies
Some new technologies such as ultrasound technology
(Fengchun et al., 2009), mechanochemical technology (Chen et al.,
2010), and combination with pyrometallurgy and hydrometallurgy
technology (Havlik et al., 2010, 2011) also have been tried to recycle
metals from WEEE.
The technology of ultrasound was applied in recycling metals.
Recover the copper and iron from waste PCBs sludge by ultrasoni-
cally assisted acid leaching. The ultrasonically assisted leaching
experiment device is shown in Fig. 10a. Sample was pretreated
firstly, which was put into a beaker with water and 30% of H2O2, and
stirred at a speed of 300 rpm for 60 min at room temperature
(25  C). Lime was put into sample and then the slurry was filtered.
The solution of pH was adjusted to below 1.5. The result demon-
strated that this method can effectively separate copper from iron,
which the leaching rates of copper and iron were enhanced with
Fig. 10. Schematic illustration of (a) ultrasonically assisted leaching technology; (b) mechanochemical technology; (c) molten salts leaching technology; (d) combined pyro-
hydrometallurgical technology (Flandinet et al., 2012; Havlik et al., 2011; Tan and Li, 2015; Xie et al., 2009).
31
increasing of ultrasound energy were reached at 93.76% and 2.07%
respectively (Huang et al., 2011; Xie et al., 2009).
The mechanochemical method can make technically feasible the
recycling of metals from some specific wastes, such as CRTs funnel
glass. Tan and Li (2015) provided a systematic review of the utilization
of mechanochemistry in metal recycling the wastes from the effect of
mechanochemical methods to discuss the physicochemical changes,
reactions occurred during these processes, and analyze its mecha-
nisms (as shown in Fig. 10b). Mechanochemical technology can be
used as a means of pretreatment, and then hydrometallurgical
technology to recycle metals. Through this way, the recovery rate of
metal was significantly higher than ordinary hydrometallurgy.
Molten salt oxidation (MSO) technology to recover metals in
waste PCBs has been proposed and this method was efficient for
recovering a copper-rich metallic fraction (Flandinet et al., 2012).
Molten salts and specifically molten KOHeNaOH eutectic was used
to dissolve glasses, oxides and plastics in waste PCBs without
oxidizing the most valuable metals. The molten salt was selected a
mixture of hydroxides, specifically NaOHeKOH, with eutectic
composition (Tmelting ¼ 170  C). The experimental setup, as shown
in Fig. 10c, consisted of a stainless steel cell and gas inlet through by
pure argon and iron melting-pot. Crushed waste PCBs samples
were placed in an iron melting pot containing the salt. Non-metallic
components, such as fiberglass, epoxy resin were dissolved in the
molten KOHeNaOH eutectic at 300  C. The metallic fraction which
contained copper and all the precious metals, was recovered with
no dissolution or melting phenomena.
A combined pyro-hydrometallurgical method to treat the prin-
ted circuit boards from used computers was studied for copper and
32 L. Zhang, Z. Xu / Journal of Cleaner Production 127 (2016) 19e36
tin extraction. The samples after thermally pretreated were leached
in the solution of 1 mol/l HCl at 80  C. Fig. 10d is the apparatus for
thermal treatment and the leaching apparatus. The results showed
that the significant increase trend of the copper extraction for
burned samples compared with unburned samples. After burning
process, metallic copper changed into the copper oxides. The cop-
per oxides were well leached in the hydrochloric acid, and this is
the reason why the cooper was leached out from burned samples.
Unlike copper, after burning, SnO2 can be formed and was mini-
mally leached in HCl. Hence, the leaching had not too much
changed before and after burning process (Havlik et al., 2010, 2011).
5. Environmental and practical defects of advanced
technologies
As described in Section 4, all of these methods and technologies
have been improved and upgraded on the basis of traditional
methods.
Pyrometallurgy can recycle some base metals such as Cu, Pb, Zn,
etc., and these metals can be gained with high purity through
smelting, refining process. Advanced pyrometallurgical technology
firstly adds the mechanicalephysical pretreatment of WEEE. In
addition, it pays great attention to the treatment of waste gas
during metals smelting and refining processes. However, although
pyrometallurgy has been improved furthest, some pollution prob-
lems are still inevitable. For example, atmosphere pollution resul-
ted from fine particles PM2.5 and PM10 or the release of some toxic
gas, such as dioxins and furans should be considered. Moreover, the
equipments are expensive, consume a vast amount of energy, and
not suit for small and medium-sized enterprises. Moreover, the
equipments are expensive, consume a vast amount of energy, and
not are suitable for small and medium-sized enterprises. More
importantly, the pyrometallurgical technology has limitations in
recycling the single metal from rare and precious metals.
Some modified hydrometallurgical technologies, such as mild
extracting technology, electrochemical technology are designed
with the main purpose to solve the problem of the single metal
recycling, and it has good performance in terms of recovery ratio
and purity. However, there are still some defects and shortages to
be improved. Take non-cyanide leaching methods to recover
precious and valuable metals for example. Most of non-cyanide
lixiviants are low cost and environment-friendly, but has low
chemical stability with low metal recovery. In addition, for thiourea
leaching, an above 90% recovery rate can be gained in a short
leaching time, yet the thiourea consumption would be too high and
very expensive compared to cyanide lixiviant. Biometallurgy has
too many limitations: Certain microorganism treats specific metal;
and the kinds and content of recycling metal by biometallurgy also
are limited. Electrochemical technology is an environment-friendly
technology, but the sludge generating through this process is
hazardous waste. Disposing of sludge is complicated and difficult.
For supercritical technology, although it can effectively decompose
organic substances from WEEE, remaining metals mixture still
need to be further separated through hydrometallurgical technol-
ogy or other technologies. In addition, generated liquid phase and
gas through supercritical process also have a negative impact on
environment to a certain extent. For example, liquid phase contains
a significant number of phosphated compounds and phenol
derivatives.
The environmental and economic benefits of vacuum metal-
lurgical technology for recycling WEEE have been validated. In
some industrial practices, gas flow can be effectively controlled and
no waste water discharge or dust emission occurs. This technology
is an environment-friendly and promising method for recycling
metals from WEEE. However, it still needs to be improved for
further promotion. On the one hand, vacuum metallurgical tech-
nology has obvious advantages for low boiling point, high satura-
tion vapor pressure base metals separation, such as Zn, Pb, and Cd.
On the other hand, the separation effect for rare and precious
metals which have low saturated vapor pressure such as Au, Ag
through vacuum distillation method is not perfect. In addition,
whether it can meet the industrial standard for metal purity after
the separation should be investigated. There are also some theo-
retical issues waiting for further research before its industrial
application, according to the review of Zhan and Xu (2014). Table 6
shows the status of these technologies of recycling metals from
WEEE.
In fact, almost all efforts from new technologies aim to achieve
better cost-effectiveness, environmental promotion and sustain-
ability. With the continuous improvement and development of
recycling technologies, the researchers have begun to focus on new
technologies which have small harm to the environment and hu-
man. As a result, some combinative recycling technologies should
be put forward to improve recycling of the metals from WEEE.
6. Perspectives on recycling technologies
6.1. Recycling technologies aspect
After a decade of effort, the recycling technologies for metals
from WEEE have gained obvious improvement. However, it is no
deny that current technologies still have some challenges for
further promotion. For example, these new and novel recycling
processes for metals are relatively single and dispersed. They are
difficult to independently and efficiently separating metals from
WEEE.
There are three considerations that ought to be noticed and
ensured for the future recycling technology innovation: (1) Tech-
nologies in the future should be prepared to face commercializa-
tion, and suit for small and medium-sized enterprises in terms of
investment or equipment; Further research should focus on the
development of pilot scale tests to generate operational and cost
data with the ultimate aim of commercialization; (2) Single tech-
nology cannot solve all the problems because WEEE is a compli-
cated system. So, recycling technologies would be more varied, and
technology should be integrated according to the physical and
chemical properties of all kinds of WEEE; (3) Future technologies
should own high separation efficiency, recovery rate and greater
sustainability.
6.2. Environmental protection aspect
As reviewed above, developed and modified technologies can
successfully recover base metals, such as Cu, Pb, Zn, Cd and precious
metals, such as Au, Ag. Advanced recycling methods and technol-
ogies also have been improved and upgraded comparing with
traditional methods in aspect of environmental protection. How-
ever, some methods still have negative effects on the environment.
There are three considerations that ought to be noticed and
ensured for the future recycling technology innovation: (1) Well-
designed pretreatments like removing plastics, papers, irons, etc.
are necessary. For example, a mechanicalephysical technology as
the means of pretreatment is a must procedure to separate the
metal and non-metal, in order to avoid the generation of toxic gases
such as PCDD/Fs and residues resulting from non-metals in WEEE;
(2) Enterprise or government should advocate the use of “green”
reagent in recycling processes/technologies to reduce pollution of
waste water; (3) Comprehensive resource utilization as far as
possible for both metals and non-metals in WEEE should be the
target in recycling processes/technologies.
 L. Zhang, Z. Xu / Journal of Cleaner Production 127 (2016) 19e36 33

Table 6
Status of all kinds of technologies of recycling metals from WEEE (Akcil et al., 2015; Cui and Zhang, 2008; Hadi et al., 2015; Tan and Li, 2015; Zhan and Xu, 2014).

Recycling technology State of recovery Species and effect of recovery metals Advantages of environmental Disadvantages of
metals and technological aspect environmental and
technological aspect

Pyrometallurgical technology
Mild extracting technology
Biometallurgical Technology
Electrochemical technology
Supercritical technology
Vacuum metallurgical technology
Other metallurgical technologies
(ultrasonical, mechanochemical
technology, etc.)
Pure solid metals Almost all metals; high recovery rate Totally-commercial; owing Vast cost of investment; fine
some dust chamber and particles pollution; consuming
exhaust gas treatment plant a vast number of energy;
difficult to recovery of precious
metals
Solution Almost all metals; recovery rate Low toxicity; simple and easy High cost of some reagent;
related to the reagents and accessibility; relative low some reagents could result in
reaction condition environment damage waste water pollution; semi-
commercial
Solution Only for a few specific metals; Environment-friendly; low cost High selectivity of metals (only
considerable recovery rate of investment for a few specific metals, such as
for Cu, Zn, Au, etc. Cu, Zn, Au); no industrialization
Pure solid metals Only for specific metals; High recovery efficiency; low Waste water and residue
high recovery rate cost of investment; mature pollution; low
technology industrialization;
Solid mixture Almost all metals; high High recovery efficiency; low Failure to recycle single metal;
of metals recovery rate cost of investment; low waste oil and waste gas
environment damage pollution; low industrialization
Solid single metal Only for high vapor pressure metals; Environment-friendly; short Relative high cost of
high recovery rate technological process investment; low
industrialization; immature
technology
Solid mixture Need to combined with other Environment-friendly; low cost Failure to recycle single metal;
of metals/solution technologies to recycle metals of investment no industrialization

7. Conclusions
On the one hand, the WEEE can cause serious environmental
problems if not be treated properly. On the other hand, WEEE
contains considerable quantities of metal resources. Therefore,
developing the novel technologies to recycle the metals from WEEE
is of great significance from both economy and environment per-
spectives. Current status of recovery technologies for metals from
WEEE is summarized and discussed in detail in this review.
Based on traditional recycling technologies of WEEE, pyromet-
allurgical technology and hydrometallurgical technology have been
significantly improved in recent years. Some modified and mild
extracting technologies, such as leaching process of chlorinate,
ammoniaeammonium and non-cyanide lixiviants can effectively
recycled metals from WEEE in aspect of recovery ratio and envi-
ronmental protection. The leaching rate of base metal Cu from
WEEE can reach 98%. In the non-cyanide leaching precious metals
Au systems, thiourea, thiocyanate and combining method of
thiourea-thiocyanate can form stable and soluble complexes of
AuðSC½NH2 2 Þþ 2
2 , Au(SCN) , Au(SC[NH2]2)2SCN, etc. to extract Au
and extraction rate of Au exceeded 70%. In addition, some novel and
new technologies, such as supercritical technology, vacuum
metallurgical technology, ultrasound technology, etc. were put
forward in past decade and had also obtained quite satisfactory
results in terms of recycling base and precious metals from WEEE.
For example, exceeding 80% Cu in PCBs can be recycled by super-
critical technology. Vacuum metallurgical technology can success-
fully separate Cu, Pb, Zn, etc. metals in PCBs.

E-scrape
(Cu, Fe, Al, Au, Ag,
Mechanical and physical technology Metals separation technology of past
Magnetic
In, Y, Eu ) Metals (Fe, Co,
Metals (Fe, Co, Ni )
Eddying separation Ni, Cu, Al, Au,
Automatic Ag, Y, Eu ) Precious Metals
Nonmagnetic Incineration
dismantling Magnetic (Au, Ag, Pt etc)
Metals (Cu, Al,
separation
Au, Ag, Y, Eu ) Heavy metals
Corona electrostatic Nonmetals Dissipated metals
separation rare earth metals Acid leaching
process
Multistiage crushing

Metals separation technology of now and future

Pyrometallurgy
Mind extracting technology
Precious Metals
(Au, Ag, Pt etc)
Vacuum-metallurgy
Heavy metals
Dissipated metals
rare earth metals
Electrometallugy
Supercritical technology

Others Technologies
(Biological, Physical, etc)

Fig. 11. A schematic flow sheet showing an integrated recycling technology to recycle the metals from WEEE.
34 L. Zhang, Z. Xu / Journal of Cleaner Production 127 (2016) 19e36
Although many endeavors about development of recycling
technologies have been attempted, yet until now there is still a
huge room to achieve the environment-friendly and sustainable
recycling for metals. Single technology still has some limitations
and can't solve all problems because WEEE is a complex system.
Some combined and integrated technologies have begun to be put
forward. For example, mechanochemical technology can be used as
a means of pretreatment, before hydrometallurgical technology
being used to recycle metals (Tan and Li, 2015). Combination of
physical processing and selective leaching was used to extract Cu in
WEEE (Silvas et al., 2015). Hence, in the future, some combined and
integrated technologies should be applied to recover metals from
WEEE. We can predict that future technologies are more efficient,
low cost, environment-friendly, and combined with various tech-
nologies, such as physical, chemical, biological, and so on. Just as
shown in the flow chart of Fig. 11, an integrated recycling tech-
nology will be presented to recycle metals. The recycling technol-
ogies of metals from WEEE, meeting the requirements of
environmental protection and social needs, will be realized in the
near future.
Acknowledgments
This work was supported by the National Natural Science
Foundation of China (51534005, 51278293 and 51178262).
Appendix A. Supplementary data
Supplementary data related to this article can be found at http://
dx.doi.org/10.1016/j.jclepro.2016.04.004.
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