Journal of Cleaner Production 228 (2019) 1e7

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Journal of Cleaner Production

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

Surfactant-assistant atmospheric acid leaching of laterite ore for the

improvement of leaching efficiency of nickel and cobalt
Peiyu Zhang a, Linquan Sun a, Hairui Wang b, Jiwei Cui a, Jingcheng Hao a, *
a
School of Chemistry and Chemical Engineering, Shandong University, Jinan, Shandong 250100, China
b
Shandong Environmental Protection Industry Group Co., LTD, Jinan, Shandong 250000, China

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

Article history: Atmospheric acid leaching has attracted great attention from scientists due to the mild leaching con-
Received 29 December 2018 ditions. However, the leaching efficiency of nickel is lower than that using high pressure acid leaching.
Received in revised form Herein, we report the use of a surfactant (e.g., stearyltrimethyl ammonium chloride, STAC) to improve
20 March 2019
the leaching efficiency of Ni. The effects of surfactant type, ore-surfactant ratio, leaching temperature,
Accepted 23 April 2019
Available online 24 April 2019
and leaching duration on the leaching ratio of Ni were investigated. The use of STAC resulted in the high
efficiency for Ni leaching at 100
C with an ore-surfactant ratio of 15 and leaching duration of 8 h. The
leaching efficiencies of Ni and Co were significantly higher than that of atmospheric acid leaching. The
Keywords:
Atmospheric acid leaching
surface tension and viscosity of the leaching solution, and the zeta potential of the leached residue were
Surfactant analyzed to investigate the mechanism of the leaching process. The changes of interfacial properties
Ni improved ionic diffusion and decreased metal adsorption, which further lead to the increasing of
Laterite ore leaching efficiency.
© 2019 Elsevier Ltd. All rights reserved.

1. Introduction
Acid leaching is one of the hydrometallurgical methods for Ni
extraction from laterite ores, which includes high pressure acid
leaching (HPAL), heap leaching (HL), and atmospheric acid leaching
(AL) (Ma et al., 2017; MacCarthy et al., 2014; Oxley et al., 2016).
Although these processes have been used in industrial scale, the
related disadvantages restrict the development of the processes or
increase the cost of the production. For example, nickel and cobalt
can be selectively leached from laterite ore in the HPAL process,
nevertheless, the severe leaching conditions (250
C, 4e5 MPa),
high cost of equipment, and easy-forming fouling lead to high cost
€
and interrupted operation (Onal and Topkaya, 2014). HL is used to
leach valuable metals by spraying acid at the top of the ore heap,
whose operation measures are simple (Nosrati et al., 2014; Quaicoe
et al., 2013, 2014; Quast et al., 2013). However, the acid consump-
tion is even higher than that of HPAL, and the high concentration of
Fe ions in the leaching solution make the post treatment process
complexed. AL is operated under the boiling point of lixiviants and
atmospheric pressure, which leads to a low leaching kinetics (Fan
* Corresponding author.
E-mail address: jhao@sdu.edu.cn (J. Hao).
and Gerson, 2013; MacCarthy et al., 2015a, b). The long leaching
duration and high leaching ratio of Fe restrict the utilization of this
process.
The low leaching efficiency may be caused by the adsorption of
Ni and low mineral dissolving rate. To improve the mineral dis-
solving rate of AL, some attempts, such as adding of reducing
agents, changing the method of heating, and pretreating laterite
ore, have been reported (Bobicki et al., 2014; Che et al., 2010; Luo
et al., 2015). For example, Senanayake et al. used SO2 and Cu(II)
as reducing agents to promote the leaching of valuable metals and
decrease the leaching time (Senanayake et al., 2015). Sulfites were
also added to strengthen the leaching and decrease the polution of
SO2 (Basturkcu and Acarkan, 2016). Pinto et al. utilized microwave
to heat the leaching suspension for volumetric heating and fast
processing (Pinto and Soares, 2013). To liberate the minerals and
expose Ni, alkalis or mechanical activation were used to pretreat
laterite ores (Basturkcu et al., 2017; Wang et al., 2013, 2014).
Therefore, the use of appropriate agents or changing reaction
conditions could increase the leaching ratio of Ni and decrease the
leaching duration. However, seldom researches focused on the
decreasing of adsorption to increase the leaching ratio Ni.
The crystalline structure, surface roughness, and other factors
usually results in some minerals being not neutral (Carlson and
Kawatra, 2013). Thus, electrostatic interaction may result in the

https://doi.org/10.1016/j.jclepro.2019.04.305
0959-6526/© 2019 Elsevier Ltd. All rights reserved.
2 P. Zhang et al. / Journal of Cleaner Production 228 (2019) 1e7
adsorption of Ni by the leached residue (Uddin et al., 2012). Another
cation could be added into the leaching solution to decrease the
adsorption of Ni by competitive adsorption (Vocciante et al., 2018;
Coelho et al., 2016). Surfactants are a type of molecules that consists
of both hydrophilic and hydrophobic groups, which have been used
in chemical cleaning products, medicine, and flotation. Surfactants
are used to separate concentrate and gangue in beneficiation by the
different of electrostatic forces between the three materials
(Filippov et al., 2014). Therefore, we hypothesized that the loss of Ni
could be decreased by adding surfactant during acid leaching. Be-
sides, the presence of surfactants could change the physiochemical
properties of surface and interface, which may further change the
mass transfer. Thus, common surfactants were chosen as the ad-
ditives to decrease the cost of the process.
In this work, surfactants were added to sulfuric acid during at-
mospheric acid leaching for increasing the leaching efficiency of Ni.
The effects of surfactant to ore ratio, temperature, and leaching
time on the leaching of Ni were investigated. To identify the
leaching mechanism, the zeta potential of the leaching residues and
surface tension of leaching solution were analyzed. The positive
zeta potential of leaching residues decreased the adsorption of Ni
on the surface of particles, and the low surface tension of leaching
solution improved the diffusion of lixiviant.
2. Experimental
2.1. Materials
Laterite ore used in this study was obtained from Philippine
laterite deposit. Dodecyl trimethyl ammonium chloride (DTAC),
tetradecyl trimethyl ammonium chloride (TTAC), cetyltrimethyl
ammonium chloride (CTAC),stearyltrimethyl ammonium chloride
(STAC), dodecyl dimethyl benzyl ammonium chloride (DDTAC)
were purchased from Shanghai Macklin Biochemical Co., Ltd. Hy-
drochloric acid was purchased from LaiyangKangde Chemical Plant.
All these reagents were analytical grade and were used without
further purification. Sulfuric acid was purchased from Laiyang
Economic and Technological Development Zone Fine Chemical
Plant and was of guaranteed reagent.
2.2. Apparatus
Element analysis was implemented by using atomic absorption
spectrophotometry (AAS, TAS-990, Beijing Purkinje General In-
strument Co., Ltd.). The phase compositions of laterite ore were
analyzed by X-ray diffractometer (XRD, D8 ADVANCE, Bruker). The
zeta potentials of laterite ore and leached residues were measured
by dynamic light scattering (NanoZS, Malvern). The surface tension
was analyzed by automatic interface tensiometer (Beijing Time Top
Technology Co., Ltd.). The viscosity of lixiviant was detected by
rotor viscometer (DV-II þ Pro, Brookfield).
2.3. Experimental procedure
The ore was ground with an average size of 74 mm with a pul-
verizer before blending. The powder of laterite ore was dried in an
oven at 60
C overnight. A certain amount of surfactant (according
to the ore-surfactant ratio) and 8% sulfuric acid were mixed before
they were agitated with dried laterite ore in 50 mL centrifuge tubes.
The rotational speeds of magnetons were set at 1200 rpm to insure
the slurries suspended uniformly. The centrifuge tubes were placed
in an oil bath with a thermostat to control the temperature of the
slurries. After the reaction, the tubes were centrifuged (3e30ks,
SIGMA) to separate pregnant solutions with residues. Then, the
pregnant solutions were diluted to certain concentrations for
analyzing the leaching ratio of valuable metals by using AAS. The
leaching solutions were also sampled to analyze the surface tension
and viscosity. The residues were dried in the oven before they were
used in the phases’ analysis and the zeta potential measurements.
3. Results and discussion
3.1. Element and phase analysis
The main components of laterite ore are listed in Table 1. The
contents of Ni and Co in the laterite ore were 1.14% and 0.09%. The
contents of Fe2O3, MgO, and SiO2 were 21.57%, 27.83%, and 30.12%,
respectively, which indicated that the laterite ore was saprolitic
laterite ore. According to the XRD spectra showed the main phase of
the ore (Fig. 1a), the laterite is mainly consisted of clinochrysotile,
goethite, and quartz, which further indicated that this laterite was a
typical saprolitic laterite ore. The crystallinity of the phase is weak,
which may be caused by the weathering and leaching of laterite
ore. After acid leaching with or without STAC, the peak intensity of
the XRD spectrum decreased, which indicates the decomposing of
the laterite ore. Since Ni and Co existed in goethite and clinochry-
sotileby adsorption and lattice replacing, the disintegration of
laterite ore improved the leaching of valuable metals. Fig. 1a also
shows that clinochrysotile decomposed more easily than goethite.
3.2. Zeta potential analysis
As mentioned above, electrostatic adsorption is one of the main
reasons that result in the loss of Ni. The zeta potential suggests the
surface charge of particle, which affects the adsorption of metal
ions on particle. Thus, the leaching ratio of Ni may increase by
controlling the zeta potential of particles. The zeta potentials of
laterite ore in water were 9.0 mV and 9.8 mV after 0.5 and 6 h of
agitation, respectively (Table 2). The negative surface charges may
be caused by the defects of the crystals. Positively charged ions (e.g.,
Ni2þ and Co2þ) can be absorbed by laterite ore (Maiti et al., 2007),
which may lead to the low leaching ratio. The zeta potential of
laterite ore in water with STAC (water system) were 32.0 and
33.6 mV after 0.5 and 6 h of stirring, respectively (Table 2), which
indicated that STAC could be adsorbed on the surface of laterite ore.
The main force of this process is electrostatic and hydrophobic
interactions. The zeta potential reversed and the potential process
is showed in Fig. 1b. In traditional system, the zeta potential of
leached residue was negative. However, it was higher than the zeta
potential of ores, which indicated the adsorption of metal ions on
the surface during leaching. As the results above, the zeta potential
of particles could be controlled by adding cation surfactants. The
zeta potential of leached residue may also be changed by adding
cation surfactant. Thus, DTAC, TTAC, CTAC, STAC, DDTAC were used
as adding reagents to leach laterite ore by atmospheric sulfuric acid
leaching. As can be seen from Fig. 1c, the zeta potentials of leached
residues are higher than the leached residue of traditional system.
Besides, the zeta potential increased as the increase of the chain
length, which may be caused by the stronger hydrophobic in-
teractions of longer chain surfactants. The zeta potential of the
leached residue based on DTAC was about 2.2 mV, which may
result in the adsorption of Ni on the surface of the residue.
To investigate the changing of zeta potential during the whole
Table 1
The main components of laterite ore.
Element Ni Co Fe2O3 MgO SiO2 Al2O3
Content (wt.%) 1.14 0.09 21.57 27.83 30.12 1.22
 P. Zhang et al. / Journal of Cleaner Production 228 (2019) 1e7
Fig. 1. XRD of laterite ore and leached residue (a), zeta potential of particles in different system (b), effect of surfactant on the zeta potential of the leached residues (c), the effect of
leaching time on the zeta potential of the leached residues (d).
Table 2
Zeta potential (mV) of laterite ore in water and water solution of STAC.
Time (h) water STAC water solution
0.5 9.0 32.0
6 9.8 33.6
leaching process, further experiments based on STAC system were
determined (Fig. 1d) because of the highest zeta potential. The zeta
potential of the residue after 0.5 h leaching using sulfuric acid with
STAC was 13.5 mV, which was higher than that in the traditional
system. This indicated that STAC adsorbed on the particles quickly
and decreased the adsorption of Ni at the beginning of leaching.
The values of the potential were positive during the whole leaching
process, which suggested that surfactant may decrease the
adsorption of Ni during the process. In contrast, the zeta potential
of the residue after 0.5 h leaching using sulfuric acid was 1.0 mV.
The values of potential were negative during the whole traditional
leaching process, which were lower than that in the STAC system.
This indicated that zeta potential of particles could be changed by
adding STAC. Thus, the positive potential of particles in STAC system
may result in the higher leaching ratio of Ni than that of traditional
system. The leaching ratio of Ni based on other surfactants (except
DTAC system) may also be larger than traditional system because of
3
the positive zeta potential.
In STAC system, the zeta potential was positive. However, the
value was smaller than that of water system. The reason why the
zeta potential of the residue in STAC system was lower than that in
water system may be because of the following point. The reason
may be the competitive adsorption between STAC and cations
(Fig. 1b), which led less STAC to be adsorbed on the surface of
residue. The hydrophobic interaction between STAC was weaker,
and less cationic groups were exposed compared with that in the
water system. Thus, the competitive adsorption made the zeta
potential in STAC system lower than that in the water system. More
important, the presence of competitive between STAC and cations
may decrease the loss of Ni. Thus, different kinds of surfactants
were used as additives during leaching to confirm that leaching
ratio of Ni could be increased.
3.3. The effect of surfactant types on the leaching ratio of Ni
The Ni leaching ratios based on different surfactants is showed
in Fig. 2a. The Ni leaching ratios of surfactants systems (except
DTAC system) were higher than that of traditional system. The
leaching ratio of Ni was 64.9% after 6 h of leaching in 8 wt% sulfuric
acid, and with a liquid-solid ratio (v/w) of 10 at 90
C. Whereas, the
leaching ratio of Ni was 70.1%, 65.3%, 79.0%, 72.1% at ore-surfactant
4 P. Zhang et al. / Journal of Cleaner Production 228 (2019) 1e7
Fig. 2. Effect of surfactant types on the leaching ratio of Ni (a), effect of ore-surfactant ratio on the leaching ratio of Ni (b).
of 10 under the same condition for TTAC, CTAC, STAC, and DDTAC
systems, respectively. The Ni leaching was 38.6% when DTAC was
added into the lixiviant, this may be caused by the increase of the
lixiviant viscosity. The results confirmed that the leaching ratio of
Ni could be changed by adding surfactants. In DTAC system, the
unchanged zeta potential was one of the main reasons that result in
the lower leaching ratio of Ni compared with traditional system. In
contrast, the high zeta potential decreased adsorption and
improved the leaching ratio of Ni in other systems. Thus, STAC was
selected as adding reagent in the following experiments because of
the highest leaching ratio.
3.4. The effect of ore-surfactant ratio on the leaching ratio of Ni
Fig. 2b shows the changes of the leaching ratio of Ni with the
increase of ore-surfactant ratio at the temperature of 90
C, leach-
ing duration of 6 h, and liquid-solid ratio of 10 (v/w). The leaching
of Ni increased from 74.8% to 79.1% as the ore-surfactant ratio
increasing from 1 to 5, and it remained constant as the ratio
increased to 15. However, when the ore-surfactant ratio increased
from 15 to 30, the Ni leaching decreased from 79.3% to 71.7%. Few
amount of STAC changes the zeta potential of ore surface and im-
proves the diffusion ions, which may promote the increase the
leaching ratio of Ni. However, excessive STAC may cause a pykno-
morphic adsorbed layer and viscous lixiviant, which restrict the
diffusion of ions. Considering the leaching ratio of Ni and the cost of
the process, the optimal ore-surfactant ratio was chosen as 15 and
was used in the following experiments.
3.5. The effect of temperature on the leaching ratio of valuable
metals
The Ni leaching of the two systems shows distinct leaching
regular patterns (Fig. 3a). The leaching ratio of Ni in the STAC sys-
tem is higher than that of the sulfuric acid system when the tem-
perature is between 60
C and 90
C. Fig. 3a shows that the Ni
leaching ratio based on STAC did not change significantly when the
leaching temperature was increased from 60
C to 70
C, and
increased rapidly at higher temperatures. For example, the leaching
ratios of Ni were 67.5% and 87.5% at 80 and 100
C, respectively. The
Ni leaching of traditional leaching system increased much more
slowly when the leaching temperature was changed at the same
conditions.
For the leaching of different metals, Co was leached more easily
compared with Ni. Fig. 3b shows that the Co leaching ratio of
traditional leaching system was more than 74.9% when the laterite
ore was leached at 60
C, and increased to 83.7% at 90
C after 6 h of
leaching. Fig. 3b also shows that the existing of STAC during at-
mospheric acid leaching improved the leaching ratio of Co. The
leaching ratio of Co increased by 8.3% when STAC was added into
the leaching lixiviant at 60
C. More than 91.3% of Co could be
leached at 90
C, and the Co leaching ratio of the STAC system is
7.6% higher than that of the traditional system at 90
C. Fig. 3a and b
demonstrate that the leaching ratio of Co was also higher than that
of Ni in the STAC system. Since the approximately equal solubility
products of the two metals hydroxides (Yavuz et al., 2003), the low
concentration of Co in the leaching solution may result in the easy
leaching of Co.
Fig. 3c illustrates that the Fe leaching ratio of traditional leach-
ing system increased from 24.6% to 33.5% as the leaching temper-
ature increased from 60
C to 100
C. However, Fe expressed a
different leaching behavior compared with that of Ni and Co when
STAC was added into the lixiviant. The leaching ratio of Fe based on
STAC was lower than the Fe leaching of traditional system. The
former decreased to 17.5% when laterite ore was leached with STAC
at 60
C. Although, the Fe leaching increased as the temperature
increased, it still remained lower than that of the traditional sys-
tem. Therefore, the presence of STAC improved the leaching
selectivity of Ni and Co. The selectivity is better at lower temper-
atures because of the lower concentration of Fe in the leaching
solution. However, the leaching ratio of valuable metals was also
low. In consequence, 100
C was chosen as the optimal leaching
temperature.
3.6. The effect of leaching duration on the leaching ratio of metals
Fig. 4a indicates that the leaching behaviors of Ni in the two
systems were different while changing the leaching times. The
leaching ratio of Ni increased from 55.4% to 63.2% as the leaching
duration varied from 0.5 to 5 h when laterite ore was leached with
sulfuric acid, and decreased to 56.6% after 8 h of leaching. This may
be a consequence of the adsorption of Ni by leached residue. The
leaching ratio of Ni in STAC system was 51.5% at the beginning of the
process, which was comparable with the traditional system. Even
though the Ni leaching of the STAC system exceeded the Ni leaching
of traditional system after 2 h, it quickly increased from 62.7% to
 P. Zhang et al. / Journal of Cleaner Production 228 (2019) 1e7
Fig. 3. The effect of temperature on the leaching ratio of Ni (a), the leaching ratio of Co (b), and the leaching ratio of Fe (c).
Fig. 4. The effect of leaching time on the leaching ratio of Ni(a), the leaching ratio of Co (b), and the leaching ratio of Fe (c).
79.3% from 4 to 6 h, and reached 84.0% after 8 h of leaching. The
kinetics was different in the first 4 h and the latter, which showed
different kinetics with atmospheric acid leaching. This may be due
to the presence of STAC in the lixiviant.
The Co leaching ratio of traditional leaching system did not
change significantly during the 8 h of leaching (Fig. 4b). The
leaching ratio of Co in the STAC system was 75.5% at the leaching
duration of 0.5 h, which is lower than that of the traditional system.
However, it increased to 83.2% and exceeded the traditional system
when the laterite ore was leached at 1 h. The Co leaching in the
STAC system reached the plateau after 5 h. The slow leaching ki-
netics of the STAC system in the first 0.5 h may also be caused by the
presence of STAC.
The leaching ratio of Fe in the traditional leaching system
increased from 21.5% to 34.5% as the leaching duration increased
from 0.5 h to 8 h (Fig. 4c). It was greater than Fe leaching in the STAC
system. The latter increased from 18.0% to 33.8% in the same time
range. The presence of STAC may cause the leaching ratio of Fe to
decrease. The reason may be caused by the adsorption of Fe com-
plex (e.g. FeCl
4 ) on the surface of particles, which formed by the
anion of STAC and leached Fe3þ. The selectivity of valuable metals
was improved due to the increase of valuable metal leaching and
the decrease of Fe leaching. After a systematic consideration, the
optimal leaching duration was determined to be 8 h.
3.7. Effect of surfactant on the leaching process
The surfactants may also change the physiochemical properties
of the leaching solution, which may also affect the leaching ratio.
Thus, the viscosity and surface tension of leaching solutions were
detected.
The high viscosity has a detrimental effect on the mass transfer.
5
Thus, the viscosities of leaching solutions were investigated by a
rotor viscometer to determine the effect of viscosity on the leaching
ratio of valuable metals (Fig. 5a and b). Firstly, the viscosities of the
leaching solutions with different surfactants were detected. The
viscosities were almost the same after 8 h leaching, which indicated
that the type of the surfactants has little effect on the mass transfer
(Fig. 5a). Then, the effect of leaching time on the viscosity was
determined based on STAC system (Fig. 5b). At the beginning of the
leaching, the viscosity of the atmospheric acid leaching solution
was 1.40 cp, which was lower than that of the STAC leaching so-
lution. The higher viscosity of the leaching solution led to the
slower mass transfer, and made the leaching ratio of Ni lower
compared with the traditional leaching process. The viscosity of the
atmospheric acid leaching solution increased quickly, and was
similar to that of the STAC system after 2 h of leaching. The viscosity
of the solution is no longer the main factor that influences the
leaching ratio of valuable metals.
The surface tension affects the wettability of leaching solution,
which further affects the diffusion of ions. To analyze the effect of
surfactant type on surface tension, it was investigated by an auto-
matic surface tensiometer. The surface tension based on DTAC was
46.0 mN/m, which indicated the poor wettability of the leaching
solution (Fig. 5c). However, the leaching solutions based on STAC
and DDBAC showed good wettability because of the low surface
tension. The low surface tension of STAC and DDBAC systems was
one reason that the leaching ratio of Ni was higher than traditional
and DTAC systems. To further analyze the effect of surfactant on the
leaching ratio, the surface tension was detected at different leaching
time based on traditional system and STAC system. The surface
tension was 63.1 mN/m after 0.5 h of leaching with sulfuric acid and
increased due to the increase of the metal sulfate in the leaching
solution (Fig. 5d) (Tuckermann, 2007). The high surface tension of
6 P. Zhang et al. / Journal of Cleaner Production 228 (2019) 1e7
Fig. 5. The effect of surfactant on the viscosity (a) and surface tension (c) of the leaching solutions, the effect of leaching time on the viscosity (b) and surface tension (d) of the
leaching solutions.
the leaching solution may lead to the decrease of wettability of
lixiviant on the particles surface and prevent the lixiviant to enter
the cracks of particles, which may be one reason causing the low
leaching rate of valuable metals. Because the presence of STAC, the
surface tension of the STAC system was lower than that of the
traditional system during the whole leaching processes. The low
surface tension improved the wettability of lixiviant, and promoted
the leaching of valuable metals. At the beginning of the leaching, the
viscosity was the main factors which affected the leaching ratio of
Ni; however, the surface tension became to be the main factor after
about 1 h of leaching. Thus, the leaching kinetics of valuable metals
based on STAC showed two stages because of the presence of STAC.
The improvement of Ni and Co leaching may be due to the
following factors. Firstly, the surface tension of the STAC leaching
solution is lower compared with that of the traditional leaching
solution. The lower surface tension can promote the lixiviant to
enter the crevices of the granule, which may be beneficial for mass
transfer. Secondly, the surfactant can enter into the cracks of the ore
particles like a wedge, and liberate the particles to small granules.
Compared with larger particles, the smaller ones have larger spe-
cific surface areas, which is beneficial for the reaction. Lastly, the
competitive adsorption between surfactant and valuable metals
decrease the adsorption of Ni and Co, and thus improve the
leaching ratio. Therefore, after 2 h of leaching, the leaching ratio of
Ni and Co exceeds that of the traditional leaching system (Fig. 4a).
4. Conclusion
The addition of surfactants into lixiviant can improve the
leaching ratio of Ni and Co. STAC showed a better stimulation on the
leaching ratio compared with other surfactants. Our experiments
indicate that ore-surfactant ratio of 15, leaching temperature of
100
C, and leaching time of 8 h are the optimal conditions for
leaching of Ni and Co. The viscosity is the peripheral element
affecting the leaching ratio. The surface tension of the leaching
solution in STAC system was lower than that in the traditional
leaching system, which was beneficial for the entry of the lixiviant
to the internal of the particles. The zeta potential of the leached
residue reversed because of the existing of STAC, which can
decrease the adsorption of valuable metals. Therefore, the use of
appropriate surfactants in the leaching process is promising to
improve the leaching ratio for valuable metals in the practical ap-
plications. Overall, the leaching ratio of Ni and Co increased when
STAC was added into the lixiviant.
Acknowledge
This work was financially supported by the National Natural
 P. Zhang et al. / Journal of Cleaner Production 228 (2019) 1e7
Science Foundation of China (Grant No. 51704175), and the
Fundamental Research Funds of Shandong University (Grant No.
2016GN011).
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