Trans. Nonferrous Met. Soc.

China 32(2022) 345−353

Nickel and aluminium recovery from spent reforming catalyst through

selective leaching, crystallization and precipitation

Naga Raju BATTI1,2, N. R. MANDRE2

1. Department of QC & SSP Audit, Projects & Development India Limited (Govt. of India U/T),
PDIL Bhawan, A-14, Sector-1, Noida, Gautam Buddh Nagar, U.P – 201301, India;
2. Department of Fuel, Minerals and Metallurgical Engineering,
Indian Institute of Technology (Indian School of Mines), Dhanbad, Jharkhand – 826004, India
Received 26 January 2021; accepted 3 September 2021

Abstract: An attempt has been made to investigate and optimize the recovery of Ni and Al through sulphuric acid
(3.0−5.5 mol/L) leaching under different operating conditions. From the leaching experiments, it was possible to extract
98.5% of NiO and 40.7% of Al2O3 under the conditions of 5.5 mol/L H2SO4, reaction time of 4 h, solid-to-liquid ratio
0.2 g/mL, temperature of 358 K, particle size <100 μm, 200−250 r/min with 5.0 g catalyst dosage. The leached liquor Al
was separated by selective crystallization using 1.4 mol/L KOH and Ni was separated by selective precipitation using
0.3 mol/L H2C2O4. From the studies, it is possible to recover around 97.9% of NiO having 98.3% purity, around 25% of
Al2O3 was also recovered as alum-(K) having 99% purity and 14.7% of Al2O3 as a salt of Al−K−C2O4−SO4. Sulphuric
acid was found to be a suitable leaching agent for selective leaching and it was also observed that alum-(K) can be
selectively crystallized from sulphate solutions. The study also indicated the effective extraction and recovery of nickel
and aluminium which were well supported by characterization studies using TG-DTA/DTG and XRD techniques.
Key words: spent catalyst; leaching; precipitation; crystallization; nickel; aluminium

source of Ni and other metals need to be recycled to

1 Introduction recover the metal values. Although different pyro-
based processes have been used earlier, recent
Reforming catalysts (NiO−CaO−Al2O3) are developments involve hydrometallurgical processes
used in ammonia and petroleum industries for the for their recovery. In this regard many reagents,
conversion of steam reformation reaction in the such as NaOH, H2SO4, NH3, (NH4)2SO4 and
primary reforming tubes and secondary reformer oxalic acid with H2O2 and Fe(NO3)2 have been
reactors. Most of these commercial catalysts consist employed for the extraction of nickel [6−8]. From
of 10%−20% NiO, dispersed in a refractory support the studies reported it may be seen that 73%−99%
material Al2O3 and promoted with alkaline earth of crucial metals were extracted using ammonia,
oxides such as CaO/MgO [1]. After periodical use, caustic and acid leaching and Na2CO3 [9].
these catalysts have to be discarded as spent CHAUDHARY et al [10] reported the extraction of
catalysts due to decrease in their conversion nickel (~73%) at 80 °C from a spent catalyst (17.7%
efficiency and mechanical strength. Generation of Ni) employing HCl leaching. From a study carried
huge quantity (150000−170000 t/a) of the spent out by AL-MANSI and ABDEL MONEM [11], it
hydro-processing catalysts is also reported in the was possible to obtain ~99% Ni extraction with
Refs. [2−5]. These spent catalysts being the rich 50% sulfuric acid at 100 °C in more than 5 h from a
Corresponding author: Naga Raju BATTI, E-mail: nrbatti@[Link]
DOI: 10.1016/S1003-6326(22)65799-6
1003-6326/© 2022 The Nonferrous Metals Society of China. Published by Elsevier Ltd & Science Press
346 Naga Raju BATTI, N. R. MANDRE/Trans. Nonferrous Met. Soc. China 32(2022) 345−353

spent reforming catalyst. SAHU et al [12] achieved out selective leaching of Ni, Al and their separation
a high Ni leaching (~98%) with H2SO4 from a spent in the acidic medium. The results obtained from the
fertilizer catalyst (NiO−SiO2−Fe2O3−Al2O3). A investigation were supported by the detailed
combined acid (HNO3/H2SO4/HCl) leaching study characterization studies.
carried out by LAI et al [13], indicated a recovery
of 99% V and Ni, and ~90% Mo. In another study 2 Experimental
by LEE et al [14], it was possible to recover 98%
NiO with 100% purity by the precipitation and 2.1 Materials and chemicals
separation of Al with Na2CO3 solution at pH ~5.4 The spent reforming catalysts used in this
from a sulphuric acid-leached solution of spent study were collected from Rashtriya Chemicals and
Raney-nickel catalysts (NiO−Al2O3). NAZEMI Fertilizers (RCF), Thal Unit (Mumbai, India). These
et al [15,16] showed a leaching process to recover spent catalysts were dried at 393 K in a hot air oven
about 99% Ni by H2SO4. Nickel ammonium for 4 h to remove moisture, further ground in
sulphate could partly be precipitated by NH3 and central peripheral ball mill and screened through a
nickel in the supernatant was enriched using SX set of standard sieves to obtain the particle size
with D2EHPA. PARHI et al [17] proposed the <100 μm. During the study, analytical reagent grade
diffusion-controlled model to represent the leaching chemicals such as sulphuric acid (3.0−5.5 mol/L)
kinetics, and they have also reported that over for selective leaching, 1.4 mol/L potassium
99.9% Ni was leached using HCl at 50 °C from hydroxide for selective crystallization of alum-(K),
spent Ni−Al2O3 catalyst. SHEIK et al [18] and 0.3 mol/L oxalic acid for selective precipitation of
RAMOS-CANO et al [19] studied the dissolution nickel, 2% sodium hydroxide for neutralization of
kinetics of Ni from spent catalysts in 5 mol/L HNO3 effluent and distilled water for preparation of
at 90 °C with 90% conversion and in 50% nitric
reagent solutions were used throughout the process.
acid at 65 °C with 85% extraction of NiO.
ABDEL-AAL and RASHAD [20] studied nickel
2.2 Analysis
leaching kinetics on spent nickel catalysts
2.2.1 X-ray diffraction (powder/single crystal) and
(NiO−Al2O3) with 50% H2SO4 and extracted 94%
thermal analysis
NiO at 358 K. VALVERDE et al [21] studied the
The phase identification of metal oxides
isolation of elements (>98%) through solvent
present in spent reforming catalyst and recovered
extraction and precipitation from a sulphuric
material was determined by powder XRD (Model:
acid-leached solution of spent catalyst (NiMo/
X’pert Pro, Panalytical) equipped with a Cu target
Al2O3/CoMo) at 363 K. CHAUHAN et al [3],
(Cu Kα1 radiation, λ=1.540598 Å) operated at 45 kV.
VUYYURU et al [4], GOEL et al [22], and OZA
and PATEL [23] have shown more than 95% Ni The diffraction peaks assigned to NiO (JCPDS
recovery as NiSO4 or Ni(NO3)2 from spent nickel No. 01−072−1464) [22,26], Al2O3 (JCPDS
catalysts by EDTA leaching. MUZAYANHA No. 43−1484), CaO, NiAl2O4, CaAl2O4 [27], and
et al [24] studied Li−Ni−Al oxide material from deposited carbon [26]. The diffraction spectrogram
waste cathode via mixed metal hydroxide using obtained from the study is given in Fig. 1. Further,
strong acids as leaching agents and NaOH as a single-crystal XRD (SuperNova, Single source at
precipitant at pH 11−12. BATTI and MANDRE [25] offset/far, EosS2; radiation type Mo Kα and
investigated the spent methanation catalyst and wavelength is 0.71073) study was carried out to
recovered 99% NiO with 98.9% purity by selective identify the crystal phase present in the recovered
and oxidative leaching with HNO3; in the study, alum-(K), the thermal studies (thermogravimetry,
Fe (III) precipitated at pH~3.5 to 4.5 with an TG; differential thermal analysis, DTA; and
alkaline solution and Ni was selectively precipitated differential thermogravimetry, DTG) were carried
using oxalic acid. out using N2(g) purge and protective gas with
From a detailed literature survey, it may be the heating rate at 10 K/min in the TG-DTA/DTG
seen that there is a need to develop suitable instrument (Model: No-NetzschSta 449F3) to
leaching and separation of these minerals. Hence, in obtain compound information of recovered nickel
the present study, an attempt has been made to carry oxalate and alum-(K).
 Naga Raju BATTI, N. R. MANDRE/Trans. Nonferrous Met. Soc. China 32(2022) 345−353 347
separated. In the third stage, Ni was selectively
precipitated using 0.3 mol/L oxalic acid in an acidic
medium by stabilizing the rest of aluminium in the
aqueous state [30,31]. In the fourth stage, the rest of
aluminium, sulphate, potassium and excess oxalate
were recovered from the filtrate of nickel oxalate
precipitate by open-pan crystallization process by
maintaining the specific gravity of ~1.40.

3 Results and discussion

3.1 Leaching and separation of minerals
3.1.1 Leaching
Leaching experiments were performed with
sulphuric acid in an isothermal reaction vessel. The
Fig. 1 XRD pattern of spent reforming nickel catalyst NiO and Al2O3 were leached and generated a
sulphate solution of Ni and Al according to
2.2.2 Chemical analysis Reactions (1) and (2).
Chemical analysis was done by using ED-XRF
(Energy Dispersive X-Ray Fluorescence, PAN NiO(s)+H2SO4(aq)+5H2O→NiSO4.6H2O(aq) (1)
analytical, Epsilon-1), atomic absorption Al2O3(s)+3H2SO4(aq)+15H2O→
spectrophotometer (AAS; Thermo Fisher, Model Al2(SO4)3·18H2O(aq) (2)
No. Pu9000) and EDTA complexometric methods From the experiments, it was observed that the
[25,28]. Sulphate was estimated by the gravimetric leaching of Ni and Al increased with an increase in
method with 5% BaCl2 solution [29]. Results of the the concentration of sulphuric acid (3.0−5.5 mol/L),
studies are given in Table 1. reaction time (1−4 h), temperature (333−358 K),
2.2.3 Experimental methods of leaching and and decreased with increasing solid-to-liquid ratio
recovery (0.20−0.58 g/mL); stirring speed was maintained at
Isothermal leaching experiments were carried 200−250 r/min. From the studies suitable leaching
out in a 500 mL round bottom flask fitted with a conditions can be obtained under the conditions of
reflux condenser which was dipped in an oil bath 5.5 mol/L H2SO4, 0.2 g/mL solid-to-liquid ratio,
placed on a magnetic stirrer; and it was connected stirring speed 200−250 r/min, particle size <100 μm
with an automatic temperature controller and at 358 K of temperature for 4 h of reaction time; the
indicator through resistance temperature detector results obtained are given in Tables 2−5. From the
(RTD) (accuracy ±1 K). The second end of RTD results, it was possible to extract 98.5% of NiO and
was immersed in an oil bath to measure the reaction 40.7% of Al2O3. It was also noted that the calcium
temperature. In this process, the fixed conditions was not found in the leached solution, which may
were as follows, i.e., spent catalyst particle size be attributed to the formation of acid-insoluble
<100 μm, stirring speed 200−250 r/min and catalyst gypsum [32].
dosage of 5.0 g. In the first stage, nickel and 3.1.2 Selective crystallization of alum-(K)
aluminium were leached with sulphuric acid On cooling the leached solution, salt
(3.0−5.5 mol/L). In the second stage, about 25% deposition was observed, which may be due to the
Al2O3 was selectively crystallized as alum-(K) high concentration of aluminium present in the
from leached solution using 1.4 mol/L KOH and solution [33]. Further, the solution was diluted

Table 1 Chemical analysis of spent reforming catalyst by different methods (wt.%)

Ni Ca Al Fe Na Si P Cr Mg
XRF
8.94 1.18 44.68 0.24 0.51 0.43 0.25 0.03 0.16
Classical quantitative NiO CaO Al2O3 *LOI at 1173 K
method 11.8 1.7 84.5 0.14
* LOI: Loss on ignition
348 Naga Raju BATTI, N. R. MANDRE/Trans. Nonferrous Met. Soc. China 32(2022) 345−353
Table 2 Effect of acid concentration on leaching of NiO Table 5 Effect of solid-to-liquid ratio on leaching of NiO
and Al2O3 under conditions of particle size <100 μm, and Al2O3 under conditions of particle size <100 μm,
stirring speed 200−250 r/min, sample dosage 5.0 g, stirring speed 200−250 r/min, sample dosage 5.0 g,
temperature 358 K, time 4 h, and solid-to-liquid ratio temperature 358 K, time 4 h, and H2SO4 5.5 mol/L
0.2 g/mL
Solid-to-liquid Dissolution/%
Acid concentration/ Dissolution/%
ratio/(g·mL−1)
(mol·L−1) NiO Al2O3 NiO Al2O3
3.0 65.8 26.9 0.58 82.6 17.7
3.5 74.8 28.4 0.45 87.3 25.6
4.0 80.4 31.8 0.31 94.2 34.3
4.5 87.9 34.5
0.2 98.5 40.7
5.0 94.1 38.2
5.5 98.5 40.7
For selective crystallization of aluminium, the
pH of the solution (100 mL) was increased from
Table 3 Effect of temperature on leaching of NiO and ~1.5 to ~2.81 using 1.4 mol/L KOH (~10 mL) in a
Al2O3 under conditions of particle size <100 μm, stirring graduated open-pan with a stirring rate around
speed 200−250 r/min, sample dosage 5.0 g, time 4 h, 200 r/min [34]. The mixed solution was evaporated
H2SO4 5.5 mol/L, and solid-to-liquid ratio 0.2 g/mL and cooled for 24 h. Selective crystallization of
Dissolution/% alum-(K) was achieved by vaporizing ~27.3 vol.%
Temperature/K
NiO Al2O3 of 110 mL mixed solution and the results obtained
333 72.4 19.7 are given in Table 6. From this, it was possible to
338 77.9 23.1 recover 25% of Al2O3 as alum-(K) having 99%
343 83.4 26.8 purity. The formation of alum-(K) crystal is given
348 86.8 31.4 in Reaction (3) and the chemical analysis of
353 94.7 37.1
recovered alum-(K) is given in Table 7.
+
358 98.5 40.7 Al3+(aq)+2SO42–(aq)+K (aq)+12H2O(l)
KAl(SO4)2·12H2O(s) (3)
Table 4 Effect of reaction time on leaching of NiO and 3.1.3 Selective precipitation of nickel
Al2O3 under condition of particle size <100 μm, stirring After completion of the above tests, nickel was
speed 200−250 r/min, sample dosage 5.0 g, temperature selectively precipitated from Ni−Al filtrate by using
358 K, H2SO4 5.5 mol/L, and solid-to-liquid ratio 0.3 mol/L oxalic acid as a precipitant at different
0.2 g/mL stoichiometric concentrations of C2 O 42− to Ni. For
Dissolution/% this purpose, pH of the solution was maintained
Time/h
NiO Al2O3 at 1.50−2.0, in this pH range, Al has high
1 65.4 19.4 solubility and is independent of the concentration of
2 82.9 25.6
Table 6 Selective crystallization of alum-(K) from
3 93.5 33.7
leached Ni−Al−SO4 solution (~100 mL) using 1.4 mol/L
4 98.5 40.7 KOH (~10 mL) at pH ~2.81 by vaporization of 110 mL
mixed solution
using distilled water to prevent the deposition of Volume Al2O3 recovered as
unwanted salts and to promote the formation of a vaporized/vol.% alum-(K)/wt.%
homogeneous solution. The analysis of the solution 10 6
indicated 0.4% NiO (m/v), 1.4% Al2O3 (m/v), 15 12
pH~1.5 having a specific gravity of 1.07 at 305 K. 20 18
This indicated that, the concentration (m/v) of Al2O3
25 23
was higher than that of NiO (i.e. 1.4% Al2O3 >>0.4%
27.3 25
NiO and the ratio of Al2O3 to NiO ≥ 3.5).
 Naga Raju BATTI, N. R. MANDRE/Trans. Nonferrous Met. Soc. China 32(2022) 345−353 349
Table 7 Chemical analysis of recovered alum-(K) using and kept for 24 h without any disturbance to obtain
XRF (wt.%) crystals of Al compound. From this process, 14.7%
Ni Ca Al K S Si Fe P Al2O3 was recovered and the chemical analysis
0.01 0 5.32 7.96 13.41 0.07 0.01 0.13
results are given in Table 10.

Table 10 XRF analysis of recovered crystals of

oxalic acid [34,35]. From the Ref. [36], these aluminium, sulphate, potassium and excess oxalate
aqueous Al ions were noticed to have solubility obtained from filtrate of nickel oxalate (wt.%)
–
properties similar to hydroxo aluminate [Al(OH)4 ] Ni Ca Al K S Si Fe Mg Cl
ions formed in the Bayers alkaline leaching of 0 0.04 9.61 6.98 11.24 0.01 0.01 0.03 0.08
alumina. Nickel precipitation was carried out at 1:1,
1.5:1 and 2:1 of oxalate to metal stoichiometry 3.2 Characterization of recovered materials
with oxalic acid by maintaining a stirring speed 3.2.1 Thermogravimetric studies of nickel oxalate
of 200−250 r/min, temperature range from Characterization of the recovered nickel
303 to 343 K and reaction time of 1−1.5 h oxalate was carried out by TG-DTA/DTG and the
(Reaction (4)) [31,35]. From the tests, it was found results are given in Fig. 2. From the figure, it may
that 2:1 of oxalate to nickel at 333 K for 1 h, 99.4% be seen that the mass loss observed up to 383.1 K
nickel was stoichiometry precipitated with high and 523.9 K is attributed to the moisture loss and
settling rate and the results obtained are given in removal of water of crystallization, respectively.
Table 8. The precipitate was dried at 383 K for 4 h, The endothermic peak found at 514.8 K with a
then decomposed into nickel oxide at 873 K mass loss of 18.3% is a close approach with the
(Reaction (5)). From the study, it was found that theoretical value of 19.7%, which may be attributed
about 97.9% NiO was recovered with 98.3% purity. to dehydration of hydrated nickel oxalate
Chemical analysis of recovered nickel oxide is (Reaction (6)).
given in Table 9.
NiC2O4·2H2O(s)→NiC2O4(s)+2H2O(g) (6)
NiSO4+H2C2O4·2H2O→
In the second stage, mass losses of 39.6% and
NiC2O4·2H2O+H2SO4 (4)
33.3% of residue were observed between 523.9 and
NiC2O4·2H2O→NiO+2CO2+2H2O (5) 662.2 K with an endothermic peak at 642.6 K
corresponding to the decomposition of dehydrated
Table 8 Selective precipitation and recovery of nickel
nickel oxalate (Reaction (7)) [37]. On further
oxide from Ni−Al−SO4 solution obtained from filtrate of
heating around 1023.5 K, the residue mass was
recovered alum-(K) using 0.3 mol/L oxalic acid at
gained and remained constant at 41.1% which
different oxalate-to-nickel stoichiometric ratios at 333 K
for 1 h is nearer to the theoretical value of 40%
(Reaction (8)) [27,31,38].
Stoichiometric ratio of oxalate to Ni NiO recovery/%
NiC2O4(s)→Ni(s)+2CO2(g) (7)
1:1 39.7
1.5:1 63.8
Ni(s)+CO2(g)→NiO(s)+CO(g) (8)

2:01 99.4

Table 9 Chemical analysis of recovered nickel oxide

using XRF (wt.%)
Ni Ca Al K Fe S Cr Mg
77.24 0.01 0.11 0.33 0.11 0.13 0.02 0.12

3.1.4 Crystallization of aluminium, sulphate,

potassium and excess oxalate
Further, nickel-free Al filtrate (NiO<0.02×10−6,
pH ~1.5) was concentrated in the open-pan
crystallization process under quiescent conditions Fig. 2 TG-DTA/DTG curves of recovered nickel oxalate
350 Naga Raju BATTI, N. R. MANDRE/Trans. Nonferrous Met. Soc. China 32(2022) 345−353
3.2.2 X-ray diffraction studies of recovered nickel
oxide
Apart from the above studies, characterization
was also carried out by using XRD test and the
result is given in Fig. 3. The diffraction peaks
found with high intensity indicated bunsenite (NiO)
phase [27,35], the low-intensity peaks indicated
alum-(K) [39,40] and t-spinel (NiAl2O4) [26], it was
also observed that, the absence of diffraction lines
correspond to Al2O3 [35] and CaO [26]. The XRD
pattern of recovered NiO is well-indexed to JCPDS.
Here it may be observed that the above results
supported the ED-XRF and TG-DTA/DTG studies
for the effective separation and recovery of NiO Fig. 4 TG-DTA/DTG curves of recovered potassium
from the spent reforming catalyst. alum

KAl(SO4)2·12H2O→12H2O(g)+KAl(SO4)2 (9)

2KAl(SO4)2→Al2(SO4)3+K2SO4 (10)

2KAl(SO4)2→K2SO4+Al2O3+3SO2(g)+3/2O2(g) (11)

3.2.4 X-ray diffraction studies of recovered

alum-(K)
From the single crystal XRD study of
recovered alum, axes angle (θ) and cell length/axes
are well indexed to the standard cubic lattice
parameters of alum-(K) (Table 11) [40,41]. This
indicates that the XRD results support the ED-XRF
and TG-DTA/DTG studies for the effective
Fig. 3 X-ray diffraction pattern of recovered nickel oxide recovery and purity of alum-(K).

3.2.3 Thermogravimetric studies of recovered

Table 11 Unit cell parameters of recovered alum-(K)
alum-(K)
using single-crystal XRD
The results of the thermogravimetric studies
Experimental parameter Standard parameter
carried out on recovered alum-(K) are given in
Fig. 4. From the figure it may be seen that a mass Axes Axes
Cell length/Å Cell length/Å
angle/(°) angle/(°)
loss of 43.2% in the temperature range from 344.1
(Ti) to 525.1 K (Tf) with peak temperature at 12.1649 (a) 90.0 (α) 12.1640 (a) 90.0 (α)
402.2 K has a close agreement with the theoretical 12.1649 (b) 90.0 (β) 12.1640 (a) 90.0 (β)
value of 45.6%, which indicates the loss of water of
12.1649 (c) 90.0 (γ) 12.1640 (a) 90.0 (γ)
crystallization (Reaction (9)). Further, in the second
stage, mass loss of 20.2% and residue of 35.9% Volume = 1800.2 Å3 Volume = 1799.82 Å3
were found in the temperature range from 973.1 (Ti) * alum-(K) = Potassium aluminum sulphate [KAl(SO4)2·12H2O]
to 1170.8 K (Tf) with a peak temperature at 1066.8
K, which may be attributed to the release of gases From the studies carried out, a schematic
due to decomposition of KAl(SO4)2 [37]. The process flow diagram developed for the leaching
endothermic peaks of DTA curve at 404.6, and recovery of nickel and aluminium from spent
504.7 and 1069 K correspond to Reactions (9)−(11) reforming catalyst composed of NiO−CaO−Al2O3 is
respectively, as shown in Fig. 4. given in Fig. 5.
 Naga Raju BATTI, N. R. MANDRE/Trans. Nonferrous Met. Soc. China 32(2022) 345−353 351

Fig. 5 Process flow diagram for recovery of nickel and aluminium from spent catalyst

(3) The aluminium, sulphate, potassium and

4 Conclusions excess oxalates present in the final filtrate
were effectively recovered by the open-pan
(1) Sulphuric acid was found to be a suitable crystallization process.
leaching agent for selective extraction of nickel and (4) From the studies, it was possible to recover
aluminium from a material composed of about 98.5% NiO and 40.7% Al2O3; about 97.9%
NiO−Al2O3−CaO. This may be attributed to the NiO was recovered with 98.3% purity, 25% Al2O3
formation of acid-insoluble gypsum, soluble nickel was recovered as alum-(K) with 99% purity
and aluminium sulphates. and 14.7% Al2O3 was recovered as a salt of
(2) Aluminium was selectively crystallized at Al−K−C2O4−SO4 with less than 1% of Ca, Ni, Fe
pH ~2.8 as alum-(K). During the process, Ni has and Mg impurities.
remained in the aqueous state due to the high (5) Recovered NiC2O4·2H2O, NiO and
concentration and low solubility of alum-(K) than alum-(K) were well characterized with TG-DTA/
nickel sulphate. Nickel was selectively precipitated DTG and XRD studies. The study also indicated the
and separated as NiC2O4·2H2O from the filtrate of effective extraction, separation and recovery of
alum-(K). nickel and aluminium, which created the
352 Naga Raju BATTI, N. R. MANDRE/Trans. Nonferrous Met. Soc. China 32(2022) 345−353
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通过选择性浸出、结晶和沉积回收废重整催化剂中的镍和铝
Naga Raju BATTI1,2, N. R. MANDRE2
1. Department of QC & SSP Audit, Projects & Development India Limited (Govt. of India U/T),
PDIL Bhawan, A-14, Sector-1, Noida, Gautam Buddh Nagar, U.P – 201301, India;
2. Department of Fuel, Minerals and Metallurgical Engineering,
Indian Institute of Technology (Indian School of Mines), Dhanbad, Jharkhand – 826004, India

摘 要：研究和优化不同工艺条件下硫酸(3.0~5.5 mol/L)浸出回收 Ni 和 Al 的工艺。浸出实验表明，在 H2SO4 浓

度 5.5 mol/L、反应时间 4 h、固液比 0.2 g/mL、温度 358 K、粒径<100 μm、搅拌速度 200~250 r/min、催化剂用量
5.0 g 的条件下，可提取 98.5%的 NiO 和 40.7%的 Al2O3。浸出液中的 Al 用 1.4 mol/L KOH 选择性结晶分离，Ni
用 0.3 mol/L H2C2O4 选择性沉淀分离。此法可回收约 97.9%的 NiO，纯度达 98.3%；约 25%的 Al2O3 以明矾(纯度
为 99%)形式回收，14.7%的 Al2O3 以 Al−K−C2O4−SO4 盐的形式回收。研究结果表明，硫酸是一种合适的选择性浸
出溶剂，而且可以从硫酸盐溶液中选择性结晶出明矾。TG-DTA/DTG 和 XRD 表征研究证明，本工艺可以有效地
提取和回收镍和铝。
关键词：废催化剂；浸出；沉积；结晶；镍；铝
(Edited by Xiang-qun LI)