Mineral Processing & Extractive Metall. Rev.

, 31: 224–235, 2010

Copyright # Taylor & Francis Group, LLC
ISSN: 0882-7508 print=1547-7401 online
DOI: 10.1080/08827508.2010.483380

COLUMN BIOLEACHING OF A LOW-GRADE SILICATE

ORE OF URANIUM

Abhilash1, K. D. Mehta1, V. Kumar1, B. D. Pandey1, and

P. K. Tamrakar2
1
MEF Division, National Metallurgical Laboratory (CSIR), Jamshedpur,
Jharkhand, India
2
CR&D Department, Uranium Corporation of India Limited, Jaduguda,
Jharkhand, India

The bioleaching of a low-grade Indian uraninite ore (triuranium octoxide, U3O8: 0.024%),
containing ferro-silicate and magnetite as the major phases, and hematite and pyrite in
minor amounts, has been reported. Experiments were carried out in laboratory scale column
reactors inoculated with enriched culture of Acidithiobacillus ferrooxidans isolated from the
source mine water. The pH effect on uranium recovery was examined with the same
amounts of ores in different columns. With the presence of 10.64% Fe in the ore as
ferro-silicate, the higher uranium biorecovery of 58.9% was observed with increase in cell
count from 6.4
107 to 9.7
108 cells/mL at pH 1.7 in 40 days as compared to the uranium
recovery of 56.8% at pH 1.9 with a corresponding value of 9.4
108 cells/mL for 2.5-kg ore
in the column. The dissolution of uranium under chemical leaching conditions, however,
recorded a lower value of 47.9% in 40 days at room temperature. Recoveries were similar
with 6-kg ore when column leaching was carried out at pH 1.7. The bioleaching of uranium
from the low-grade ore of Turamdih may be correlated with the iron(II) and iron(III)
concentrations, and redox potential values.

Keywords: Acidithiobacillus ferrooxidans, bioleaching, column, ferric ions, uranium

INTRODUCTION
Uranium is an important strategic metal often used for power generation. With
the increasing mismatch between demand and supply, efforts are made worldwide to
augment its production. As such, India’s uranium production accounts for 1% of the
world’s capacity (Beri 1989; Padmanabhan and Suri 2007) and, therefore, uranium
recovery from the low-grade ores gains importance for the country. The bioleaching
of uranium from such ores by Acidithiobacillus ferrooxidans (A. ferrooxidans), an
iron- and sulfur-oxidizing chemolithotroph, has often been considered (Silverman
and Lundgren 1959; Mathur and Dwivedy 1994; Dwivedy and Mathur 1995). The
role of ferric iron, an oxidizing agent in the bacterial leaching of sulfides, stems from
the presence of soluble iron species contributing to high Fe3þ=Fe2þ ratios and redox

Address correspondence to Dr. B. D. Pandey, National Metallurgical Laboratory, Jamshedpur

831007, Jharkhand, India. E-mail: bd_pandey@yahoo.co.uk, biometnml@gmail.com

224
 COLUMN BIOLEACHING OF URANIUM FROM SILICATE ORE 225

potential (Temple and Colmer 1951). At low pH (1.5–2.0), A. ferrooxidans (At. f)

follows direct and indirect leaching mechanism through either oxidation via attach-
ment on the surface or by the reaction of Fe3þ (Hansford and Vargas 2001; Sand
et al. 2001) with the sulfides.
In uranium solubilization through indirect mechanism (Tuovinen 1972; Guay,
Silver, and Troma 1977; McCready, Wadden, and Marchbank 1986), pyrite present
in the ore is oxidized by the bacteria as

2FeS2 þ 2H2 SO4 þ OAt:f

2 ¼ 2FeSO4 þ 2H2 O þ 4S0 ð1Þ

2FeSO4 þ H2 SO4 þ 1=2OAt:f

2 ¼ Fe2 ðSO4 Þ3 þ H2 O: ð2Þ

Sulfur formed is also oxidized to H2SO4 by A. ferrooxidans and ferric sulfate

acts as an oxidizing agent (Tuovinen and Hsu 1984; Tuovinen and Bhatti 1999;
Mathur et al. 2000) for converting insoluble uranium(IV) to the water-soluble
uranium(VI) sulfate:

2S0 þ 3O2 þ 2H2 OAt:f ¼ 2H2 SO4 ; ð3Þ

UO2 þ Fe2 ðSO4 Þ3 ¼ UO2 SO4 þ 2FeSO4 : ð4Þ

Leaching in columns, with or without the recirculation of the leach liquor,

simulates percolation and, hence, these conditions can be extrapolated to the
heap leaching (Lizama and Suzuki 1989; McCready and Goud 1990; Ahonen and
Tuovinen 1995). Garcia (1993) carried out bacterial leaching of uranium ore of
Figueira-PR, Brazil in column percolation experiments at semi-pilot scale and
reported 50% uranium extraction. Based on the series of experiments in columns
for bioleaching of uranium ores from the FE mine (Saelices el Chico, Spain) using
A. ferrooxidans, two kinetic models were developed (Muňoz et al. 1995). Bacterial
leaching of complex sulfide ore containing chalcopyrite, pentlandite, pyrite, pyrrho-
tite, and sphalerite mineral samples in bench-scale columns was also investigated
(Lizama and Suzuki 1989; Ahonen and Tuovinen 1995).
The column bioleaching experiment simulates the flow or, at least, one of
the possible paths of a liquid percolating through a mass of material by gravity
and the results are considered a precursor to the heap=dump leaching conditions.
The solid=liquid contact area, which is a function of particle size of the material,
is a major factor in determining the kinetics of the leaching reactions. The lixiviant
may also penetrate into the microfissures and micropores of the ore, thus reducing
the need for energy-consuming crushing and grinding operations (Kawatra, Eisele,
and Bagley 1989; Lima de Andrade 2006).
In our efforts on uranium extraction from a low-grade Indian uranium ore by
A. ferrooxidans (Abhilash et al. 2009), further investigations on the treatment of such
an ore in laboratory scale columns with continuous recirculation of leach liquor are
presented.
226 ABHILASH ET AL.

MATERIAL AND METHODS

Ore and Microorganism
The low-grade uranium ore containing 0.024–0.03% triuranium octoxide
(U3O8) was collected in the form of lumps from Turamdih mines, Jharkhand, India.
The ore was crushed, ground, and passed through a sieve of 75-mm size. Earlier,
bench-scale bioleaching experiments were carried out with this material (Abhilash
et al. 2009). A representative sample was prepared by coning and quartering for
chemical analysis of uranium and other metals. The chemical composition of the
ore sample was found to be 10.64% Fe; 0.093% Cu; 0.048% Ni; 0.056% Co; 47.4%
SiO2; 1.085% CaO; 0.383% TiO2; 0.168% S, and 15.5% Al2O3. X-ray diffraction
(XRD) analysis of the ore showed the presence of silica, alumina, and magnetite
as the major phases, while aluminium silicate, ferro-silicate, and hematite being
the minor phases. Uranium was present as uraninite (UO2) in the ore with
38–40% metal in the U(IV) state and rest as U(VI).
The ore was ground and separated into various sizes for column of 2.5 kg
(1–150 mm: 200 g, 5–1 mm: 2.0 kg, and 5–4 mm: 300 g). A very small amount of
(1% of the total load) fine size (<150 mm) ground ore was discarded. Whereas, only
two fractions, viz., 5–1 mm (4.0 kg) and 15–10 mm (2.0 kg) were present in the 6.0-kg
column experiment, a small amount (2%) of finer fractions (<1-mm size) was also
discarded.
The bacteria used in this work were isolated from the mine water of Turamdih
mines and were microbiologically characterized as motile, non-endospore-forming,
gram-negative, and straight, rod-shaped bacteria of about 0.5–1-mm length. These
strains were also microbiologically and biochemically characterized at National
Metallurgical Laboratory (NML). A. ferrooxidans was grown in 9-K medium
(Silverman and Lundgren 1959; Abhilash et al. 2009) containing FeSO4  7H2O:
44.8 g=L, (NH4)2SO4: 3.0 g=L, MgSO4  7H2O: 0.5 g=L, K2HPO4: 0.5 g=L, Ca(NO3)2:
0.01 g=L, and KCl: 0.1 g=L. The cultures of A. ferrooxidans were incubated in
500-mL Erlenmeyer flasks, each containing 200 mL of the medium and 10% (v=v)
inoculum, on a rotary shaker at 120 rpm at a constant temperature of 35 C. The
initial pH of the culture was adjusted to 1.7 using 10-N H2SO4. The pure and
sub-cultured isolates were maintained in the same medium under similar conditions.
The enriched cultures that were used in bioleaching experiments were adapted on 5%
(w=v) slurry of the ore at pH 2.0 and temperature of 35 C. The stock culture was
sub-cultured at 3-week intervals to keep it active and to maintain microbial cells
in exponential phase.

Apparatus and Procedure

Figure 1 shows the schematic diagram of the laboratory-scale column reactor
set-up. The experiments were carried out in a column that was fabricated from
0.2-cm thick Plexiglass. The height of the column was 75 cm with an internal diam-
eter of 6.5 cm. A high-density support rubber cork with 10-mm hole was placed in
the bottom of the column. The column was fed with the bacterial solution using a
peristaltic pump at the rate of 3 L=h for 2.5 kg and 4 L=h for 6.0-kg column. The
solution was aerated for 5 min everyday in the morning to ensure oxygen availability
 COLUMN BIOLEACHING OF URANIUM FROM SILICATE ORE 227

Figure 1 Schematic diagram of laboratory scale column reactor set-up (2.5 kg).

for the culture, which was then sprayed on the top surface of the column charge
using a simple garden-type sprinkler head. The leach solution was passed through
the ore sample by gravity and recirculated through a side loop with a peristaltic
pump. The solution level was maintained at a sufficient height (1.5 cm from the bot-
tom) to provide a seal, forcing the air upwards through the column charge with the
coarser size particles at the bottom. No flow of air from bottom was made and oxy-
gen availability was maintained for bacterial activity with air associated with voids in
the packed bed. In the leaching experiments, the column comprised 2.5 kg of sized
ore material and 10 L of medium solution without ferrous sulfate that contained
10% (v=v) inoculum, with resultant bacterial population of 6.4
107 cells=mL. In
another set, the column comprised 6.0 kg of sized ore and 25 L of medium solution
containing 10% (v=v) inoculum without ferrous sulfate with the bacterial density of
6.5
106 cells=mL. Feed and spent solutions were sampled and analyzed to deter-
mine the metal concentrations and computing the metal dissolution. Experiments
were conducted at room temperature and the pH of the feed was maintained at
1.7, unless stated otherwise. One set of experiments was also carried out to test
the bioleaching of uranium in a large-scale column comprising 80-kg ore.
228 ABHILASH ET AL.

Analysis
Uranium and total iron concentrations in the bioleached solutions were mea-
sured by Flourimeter (FL-6224ATM) and Atomic Absorption Spectrometer
(GBCTM-980 T), respectively. The solid residues were air-dried and samples were
taken for chemical analysis and XRD studies. Cell count was determined in a
Petroff-HauserTM counter of 0.1-mm depth and 0.0025-mm2 area using LeicaTM bio-
logical microscope (
1000). The Fe2þ concentration was analyzed by titration
against K2Cr2O7. The pH of the leach solution was maintained at alternate days.
The pH of the culture suspension and uranium extractive solution was monitored
at room temperature with a pH meter (ToshniwalTM, Model CL 54). Redox poten-
tial (ESCE) was measured against saturated calomel electrode (SCE) and reported as
such. For all the experiments, chemical grade reagents and raw water were used,
except for the preparation of indicators, for which deionized water was used.

RESULTS AND DISCUSSION

Column Leaching at 2.5-kg Scale
The uranium biorecovery from Turamdih ore was found to be fairly high
(98%) in shake flask experiments at pH 1.7, as reported elsewhere (Abhilash
et al. 2009). The recovery was slightly lower at pH 1.9 under similar conditions in
shake flask experiments. On the basis of these observations, the effect of pH (1.7
and 1.9) on uranium recovery was examined with equal load of the ore in the col-
umns (1–150 mm: 200 g at the top; 5–1 mm: 2.0 kg in the middle, and 5–4 mm:
300 g at the bottom). The three columns used may be designated as (i) control leach-
ing at pH 1.7, (ii) bioleaching at pH 1.7, and (iii) bioleaching at pH 1.9. The leaching
rate was studied in detail with most particles (80%) in the size range 5–1 mm. The
leaching of uranium showed increasing trend, yielding 58.9% biorecovery in 40 days
with corresponding increase in bacterial count from 6.4
107 to 9.7
108 cells=mL
at pH 1.7 (Figure 2); the recovery being 56.8% in 30 days with bacterial population
of 6.1
108 cells=mL. The uranium biorecovery was found to be 56.8% in 40 days
and 52.9% in 30 days at pH 1.9 (Figure 3) with almost similar bacterial population
(9.9
108 cells=mL) as that observed at pH 1.7. The dissolution of uranium in
column under chemical leaching conditions (control experiment) recorded a lower
value of 47.9% in 40 days at room temperature with 2.5-kg ore (Figure 4). The
pH increased over first 30 days, which was evident from the consumption of acid
(286 mL of 10 N H2SO4) to control the pH at 1.7 with the proton attack of pyrite
according to Equations 1 and 2. The extraction rate increased quite rapidly at pH
1.7, where formation of hydronium jarosite ðH3 OÞFe3þ 3 ðSO4 Þ2 ðOHÞ6 Þ precipitate,
as indicated by XRD analysis, was observed, but not in very substantial amount.
The increased amount of jarosite precipitate formation at pH 1.9 could limit the rate
of uranium solubilization by hindering the diffusion of soluble reactants, such as
ferric sulfate, through the product layer. The bacterial growth may be controlled
by the nutrients and the amount of ferrous ions in the medium. The bacterial counts
reported in the text are based on free-swimming bacteria only and no attempt was
made to determine bacterial densities either qualitatively or quantitatively on
mineral surfaces.
 COLUMN BIOLEACHING OF URANIUM FROM SILICATE ORE 229

Figure 2 Change in uranium biorecovery with cell count at pH 1.7 using 2.5-kg ore with adapted enriched
culture of A. ferrooxidans.

Rise in uranium bio-dissolution with time at pH 1.7 and 1.9 may be correlated
with the generation of ferric ions to the tune of 1.77 g=L and 1.73 g=L, respectively,
as given in Figures 5 and 6 through bacterial oxidation of Fe(II), which supplemen-
ted bacterial growth as well. The increasing bacterial population (Figures 2 and 3)
and consequently Fe(III) concentration has resulted in steady increase in metal
recovery beyond 10 days of leaching. There was a slight decrease in total iron level
in spite of some amount of hydronium jarosite precipitation, which was partially
compensated by the contribution of iron dissolution through chemical leaching of

Figure 3 Change in uranium biorecovery with cell count at pH 1.9 using 2.5-kg ore with adapted enriched
culture of A. ferrooxidans.
230 ABHILASH ET AL.

Figure 4 Uranium recovery in control leaching at pH 1.7 using 2.5-kg ore.

magnetite present in the ore. The presence of 0.35 g=L Fe(II) at the end of the control
leaching indicated the low rate of consumption of the ferric ion that was generated
by aerial oxidation in acidic environment. This may be correlated with the lower ura-
nium leaching (Figure 4).
The variation in redox potential in control and bioleaching columns at pH 1.7
and 1.9 is shown in Figure 7. It is apparent that the role of A. ferrooxidans, as given
in Figure 2, led to the rise in Fe(III) concentration (Figures 5 and 6), and conse-
quently the redox potential from 540 mV to 665 mV gave rise to higher metal recov-
ery in bioleaching at pH 1.7. The lower uranium dissolution may be associated with
the lower value of redox potential (564 mV) in control leaching in 40 days of leach-
ing. The redox potential during the same period was found to be 623 mV for the

Figure 5 Variation of Fe2þ, Fe3þ, and total iron [Fe(T)] concentration in column bioleaching at pH 1.7.
 COLUMN BIOLEACHING OF URANIUM FROM SILICATE ORE 231

Figure 6 Variation of Fe2þ, Fe3þ, and total iron [Fe(T)] concentration in column bioleaching at pH 1.9.

bioleaching at pH 1.9. The higher value of redox potential attained in bioleaching

and involvement of Fe(III) in the dissolution process may thus be attributed to
the indirect leaching mechanism for uranium recovery.
The lower uranium recovery (56.8%) in column leaching at pH 1.7 as compared
to 98% uranium leaching in shake flask experiments in 30 days may be the result of
the mode of contact of the lixiviant with the ore particles and granulometry of par-
ticles. The finer size (<75 mm) of the ore, submerged in the lixiviant during shake
flask experiment, facilitated higher uranium dissolution than that observed in
column with lixiviant trickling of coarser particles down the bed.

Figure 7 Variation of redox potential in 2.5-kg column in control and bioleaching.

232 ABHILASH ET AL.

Column Leaching at 6.0-kg Scale

For column studies packed with 6.0-kg ore (15–10 mm: 2 kg at the bottom and
5–1 mm: 4 kg in the middle) using enriched culture of A. ferrooxidans at pH 1.7 and
room temperature, a flow rate of 4 L=h was maintained. Experiments were conduc-
ted for 30 days to compare the trend of results with that of 2.5-kg column. The data
presented in Figure 8 showed the uranium extraction and cell count values attained
in solution as a function of time. The uranium biorecovery of 53.6% was achieved
with a rise in bacterial population from 6.5
106 to 2.1
108 cells=mL in 30 days.
The redox potential varied from 512 mV to 719 mV with the exponential rise in bac-
terial population. It was interesting to note that 38% uranium recovery in 5 days of
bioleaching in 6.0-kg column (Figure 8) was achieved as compared to 16–18% ura-
nium dissolution in 2.5-kg column at pH 1.7 (Figure 2). This illustrated that the cell
concentration reached the phase of maximum growth rate in shorter time in the
6.0-kg column and accumulation of toxic material could have later on caused the
decreased ferric ion formation, which subsequently led to steady increase in uranium
recoveries till 30th day. The role of granulometry (particle size) of the ore is evident
from the uranium recovery of 57% in 2.5-kg column at pH 1.7 as against 53.6% in
6.0-kg column in 30 days leaching. The presence of larger amount (33% of the load)
of coarser particles (15–10-mm size) in 6.0-kg column may apparently be responsible
for slightly lower uranium dissolution.
The change in the concentration of ferrous ion with bacterial population with
time as a function for the test run is shown in Figure 9. The oxidation rate of ura-
nium increased when soluble ferric iron concentration in the leach solution was high
due to biological activity. The decline in Fe(II) concentration from 2.3 g=L to 0.7 g=L
was duly represented by the increase in ferric ions into the solution with the involve-
ment of bacteria. The active bacterial cells (6.1
106=mL) multiplied to a level of
2.1
108 cells=mL, while raising the Fe(III) concentration from 0.5 g=L to 1.9 g=L.

Figure 8 Biorecovery of uranium and change in cell count in column leaching with 6.0-kg ore at pH 1.7
using adapted enriched culture of A. ferrooxidans.
 COLUMN BIOLEACHING OF URANIUM FROM SILICATE ORE 233

Figure 9 Change in redox potential with respect to Fe(II) and Fe(III) concentration (g=L) in column
leaching at pH 1.7 using 6.0-kg ore with adapted enriched culture of A. ferrooxidans.

Similar to the 2.5-kg column experiment, the total iron decreased only marginally
even with some amount of hydronium jarosite formation. The increase in uranium
biorecovery with the duration of leaching was again reflected by the convincing
higher Fe(III)=Fe(II) ratio raising the redox potential from 512 mV to 719 mV in
30 days.
Column bioleaching was also carried out on 80-kg scale, which reported an
appreciable biorecovery of uranium (70%) at pH 1.7 in 60 days against a control
recovery of 55%. The uranium biorecovery of 60% in 40 days was almost similar
to that obtained (59%) in laboratory column experiment. The details of the
80-kg experiments are not included in this paper.

CONCLUSIONS
On the basis of the findings of the above investigations, the following conclu-
sions have been drawn:

1. Enriched culture of mesophilic iron oxidizing bacterium, A. ferrooxidans isolated

from the mine water of Turamdih mines may be effectively used for bioleaching
of uranium from the low-grade uraninite ore in laboratory-scale columns.
2. The solubilization of uranium from the ores is a chemical process involving the
reaction of ferric ions as a key component. The relationship between metal dissol-
ution, Fe (II) and Fe (III), and redox potential in the solution suggests that
uranium recovery is accompanied by indirect leaching mechanism.
3. The bioleaching activity of the bacteria is not adversely affected by increasing the
load with marginal change in the particle size. The experiment conducted in a
6-kg column shows uranium biorecovery of 53.6% with a rise in redox potential
from 512 mV to 719 mV in 30 days. The increase in cell count of A. ferrooxidans
234 ABHILASH ET AL.

from 6.5
106 to 2.1
108 cells=mL in 30 days may be correlated with the oxi-
dation of Fe (II) to Fe (III), which improves the uranium recovery. For 2.5-kg
laboratory column, 58.9% uranium biorecovery is recorded in 40 days at pH
1.7 as against 56.8% at pH 1.9 with maximum ESCE values of 665 mV and
623 mV, respectively. The control experiment yields a lower uranium recovery
(47.9%) in 40 days at pH 1.7. The experiment conducted in a large-scale column
validates the uranium bio-dissolution data obtained in the laboratory column.

ACKNOWLEDGMENTS
Authors wish to acknowledge the financial support received from the Council
of Scientific and Industrial Research, New Delhi through network project. Thanks
are also due to Prof. S. P. Mehrotra, Director, NML, Jamshedpur for giving
permission to publish this paper.

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