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Procedia
Environmental
Procedia Environmental
Procedia Sciences
Environmental 8 (2011)
Sciences 13 1636–1642
(2012) 1609 – 1615
Sciences
www.elsevier.com/locate/procedia

The 18th Biennial Conference of International Society for Ecological Modelling

Remediation technology for the uranium contaminated

environment: a review
J. Lia, Y. Zhang a*
State Key Joint Laboratory of Environmental Simulation and Pollution Control, School of Environment, Beijing Normal University,

Xinjiekouwai Street No. 19,Beijing 100875, China

Abstract

Radioactive uranium mining and use is increasing with the development of human society, so the environment is
facing increasing radioactive contamination. The remediation technology for the uranium polluted environment is
divided into physical, chemical and biological categories. Physical methods are appropriate for small areas of water
contaminated by uranium; chemical methods have high efficiency and low cost to remove the uranium, but most are
still being in the experimental stage, needing to be popularized in a large scale; bioremediation methods including
phytoremediation and microbial remediation are appropriate for large areas of soil and water contaminated by low
concentrations of uranium. The methods have small disturbance to the environment and don’t produce secondary
pollution. In practical applications, integrated utilization of various remediation methods should be based on
environmental conditions in order to remove uranium from contaminated environments efficiently and thoroughly.
©
© 2011
2011 Published
Published by
by Elsevier
Elsevier B.V.
Ltd. Selection and/or peer-review under responsibility of School of
Environment, Beijing Normal University. Open access under CC BY-NC-ND license.
Keywords: Uranium pollution; Remediation; Physical methods; Chemical methods; Biological methods; Review

1. Introduction

Human demand for energy has been growing as a result of the continuous development of the world
society and its economy. As the traditional oil, coal and other non-renewable fossil fuels are gradually
consumed, the world is facing an unprecedented energy crisis. Development and use of nuclear energy is
one solution to this problem, but mining and processing of uranium mineral resources has also brought a
large area of U pollution. Depleted uranium (DU) which is the by-product of the extraction of 235U in

* Corresponding author. Tel.: +86 10-5880-7596; fax: +86 10-5880-7596.

E-mail address: zhangyanyxy@126.com.

1878-0296 © 2011 Published by Elsevier B.V. Selection and/or peer-review under responsibility of School of Environment, Beijing Normal University.
Open access under CC BY-NC-ND license. doi:10.1016/j.proenv.2012.01.153
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natural uranium has been used to manufacture DU weapons. In recent years, DU weapons have been used
in war frequently, leading to DU contaminated soil and water in combat areas. Uranium has a long half-
life and will remain long in the environment; therefore, there are long-term potential dangers to human
health. Finding a remedy for the uranium contaminated soil and water effectively and thoroughly, has
become a hot research topic. Remediation technologies can be divided into physical, chemical and
biological methods. Bioremediation is divided into plant and microorganism methods. Each method has
both advantages and disadvantages and the appropriate repair techniques should be based on the
environmental conditions.

2. Uranium contamination and damage

Uranium causes soil and water radioactive contamination mainly through mining uranium, nuclear
research, nuclear fuel, depleted uranium weapons, war and other means.
Because of its high density and low cost, DU is extensively used in the military, industrial and medical
fields. In the military, DU has been widely used to manufacture armor-piercing bombs, incendiary
devices and tank armor [1]. In the 1991 Gulf War, the United States used depleted uranium for the first
time. Later, it was used in the 1994-1995 Bosnia-Herzegovina war and the 1999 Kosovo war. Soldiers
who participated in combat missions have been suffering from chronic fatigue, muscle pain, insomnia,
dizziness, hair loss, trances and other strange diseases, known as the "Gulf War Syndrome" and "Balkan
Syndrome."
Uranium has biologically dynamic toxicity, metabolism toxicity and chemical toxicity, leading to
potential long-term harm to mammalian reproduction and development with reduced biological fertility,
abnormal and slow embryonic development [2].
Long large-scale U pollution may also bring ecological risks. For 30 years, there has been uranium
mining in the south-eastern part of Siberia, around which prairie soil U concentration is 600 times the
background value. Compared to the controlled area, on the U contaminated soil, community diversity of
Eupolyphaga is reduced, macroinvertebrate abundance and diversity is reduced 3-37 times, and the
concentration of U in beetle’s bodies was 2-41 times higher [3].

3. Remediation methods for uranium contamination

3.1 Physical methods

For small areas of water contaminated by uranium, coagulation, precipitation, evaporation, extraction,
and membrane separation technologies are used to eliminate most U from the water [4]. Adsorption has a
high removal efficiency, but costs are also higher. The coagulation process can be done simply and
cheaply, but the standard effluent concentration is hard to reach, so there is a need for follow-up treatment.
Combined with adsorption, coagulation can remove 99% of U. The extraction process can remove
effluent U concentrations of less than 0.05mg / l, but it will produce a lot of waste and needs for further
research trials. Reverse osmosis water is good, but because of the high cost, it is difficult to have a large-
scale application. The evaporation method is simple and effective, the removal rate is high, but there are
high costs and sludge needs that must be dealt with.
The adsorbent used in adsorption is resin, activated carbon, activated silica, titanium adsorbent, and so
on. Chen used synthetic hydroxyapatite to remove U from waste water and studied the impact factors of
hydroxyapatite adsorption of uranium [5]. The results showed that 95% of uranium can be adsorbed by
hydroxyapatite. Temperature, pH, adsorbent dosage and adsorption time will affect their adsorption. After
60minutes, the adsorption will achieve balance. Removal rate has positive correlation with adsorbent
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dosage and the adsorbed time. Acidic to neutral media is conducive to the adsorption of uranium. To
study the mechanism of apatite removing U (VI) is to evaluate the technical feasibility of apatite-based
permeable reactive barriers. In the batch absorption experiments of U (VI) and synthetic hydroxyapatite,
99.5% of the dissolved U can be disposed of in the equivalent range of U (VI) and total phosphorus in the
suspension, so that the U concentration in solution is less than <0.05 μM. In the U (VI) concentration
range of ≤ 4700 ppm, analysis of the reaction products of U (VI) and hydroxyapatite by X-ray absorption
spectroscopy and X-ray diffraction showed that there is no U (VI) phosphate, hydroxide and carbonate
salt [6]. In the development of repairing groundwater containing U (VI) by permeable reactive barrier
technology, the study provides the basis for evaluating the mechanism of the apatite adsorbing the U (VI).
Membrane separation has great potential development as a treatment technology. A study that
extracted uranium (Ⅵ) from wastewater with a hollow fiber membrane device showed that: when the pH
of aqueous phase was greater than 2, pH had less impact on the rate; when the pH is less than 2, the
extraction rate increased significantly as the pH increased; when the organic phase concentration is less
than 0.01mol/L, the extraction rate increased with the rise in the concentration of HDEHP; when the
concentration was more than 0.01mol / L, change of the concentration in the organic phase had little
effect on the extraction rate [7]. The HDEHP-kerosene membrane extraction rate could be enhanced by
increasing the extraction time and the water flow rate; the flow rate of the organic phase and temperature
affected the membrane extraction rate less.
The traditional approach is inadequate: large amounts of slurry are produced; there is a need to do
follow-up treatment; and it is not suitable for large-scale sewage treatment. When the amount of water
and ions is small and the aqueous solution is acidic, priority can be given to the use of coagulation,
extraction, adsorption and membrane separation technologies.
Synthetic resin can effectively remove uranium-contaminated groundwater. Batch experiments and
field column tests conducted at the comprehensive test site of the U.S. Department of Energy in Oak
Ridge, Tennessee showed that: when comparing strong base anion exchange resin with metal chelating
resins, the former was more efficient for eliminating U from the near-neutral pH (6.5), high pH (8), and
low nitrate content groundwater, the latter could clear more U from groundwater with acidic pH (5) and
high nitrate [8]. These batch tests showed that Dowex1-x8, and Purolite A-520E anion exchange resin
was more effective than metal chelating resins in removing U from artificial groundwater with pH (8) and
a low nitrate content. However, in groundwater of acidic pH (5) and high nitrate levels, metal chelating
resin Diphonix and Chelex-100 anion have removed more uranium than the exchange resin has. This
study helps to better understand the selective sorption kinetics of removing U from the groundwater of
different nitrate content and different pH values with different ion-exchange resins.

3.2 Chemical methods

German scientist Chicgoua Noubactep proposed that zero-valent iron (ZVI) be used to remove U from
contaminated water. He studied the potential role of FeS2 and MnO2 as a zero-valent iron material to
remove U from water, putting forward the concept that coprecipitation between U and iron corrosion
products is the first mechanism of U removal [9]. Caroline J. Evans removed uranium from waste water
containing phosphates by the photochemical method; the removal rate reached 98% by the 6th hour in the
solution of pH (2). Chemical methods of removing the U contamination has high efficiency and low cost,
but are only at an experimental stage at present. They need large-scale applications.

3.3 Biological methods

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Some studies showed that micro-organisms (bacteria and fungi), plants can change the extracellular
binding sites and the pH by biological activity, changing the form and bioavailability of U, so it can
reduce or increase the transfer of U to the food chain, which may be used as the repair of the environment
polluted by U [10,11].

3.3.1 Application of microbiological methods in repairing uranium pollution

Pseudomonas MGF-48, a gram-negative, motile, oxidase negative, catalase positive, yellow pigmented
bacterium, isolated from electroplating effluent, has been found to accumulate uranium with high
efficiency. This bacterium can rapidly absorb uranium ranging from 50 to 200 mg/l and the amount
increases in direct proportion to the concentration. The largest amount of uranium uptake was 174 mg per
gram dry weight bacterial biomass, observed to occur in a stationary phase. Uptake was determined by
flow injection analysis; maximum uranium accumulation was obtained at pH 6.5, with 86% of the
uranium being removed within 5 minutes of incubation. Release of uranium bound to the cells was
accomplished by the addition of a sodium carbonate and EDTA solution (0.1 M). The solution was
reusable, serving as a biosorbent. Cells immobilized in polyacrylamide gel yielded 90% uranium removal.
Pseudomonas MGF-48 showed excellent efficiency in biosorbing uranium both when immobilized and as
free cells. Compared to other reports of uranium enrichment, we concluded that Pseudomonas MGF-48
shows excellent potential for bioremediation of uranium-polluted aqueous effluents [12].
Environmental Remediation Sciences Program (ERSP) Field Research Center at Oak Ridge, TN
(ORFRC) contains up to 135 microM uranium as U(VI) [13]. Using in suit bio-stimulation can lower U
(VI) concentrations. By dosing ethanol to the groundwater to stimulate the growth of denitrification
bacteria, ferric iron-reducing bacteria and sulfate-reducing bacteria two days per week, these bacteria can
restore the U (VI) to U (IV) and fixate uranium. After two years, the dissolved uranium concentration
would reach a lower level in groundwater. After adding sulfite to remove dissolved oxygen, U (VI)
concentration was reduced to the drinking water concentration limits (<30 μg/L or 0.126 μmol/L). Under
anaerobic conditions, even without dosing ethanol, the U concentrations can be maintained at a low level.
However, when sulfite additions stopped and the dissolved oxygen entered the injection well, after 60
days, the U (VI) concentration increased less than 0.13μM to 2.0μM in the vicinity of the injection wells
and the U (VI) concentration was basically unchanged far away from the water injection well. By dosing
ethanol within 36h, Fe (III), sulfate, U (VI) was restored again. After two years of continuous ethanol
dosing, U (IV) accounted for 60% -80% of the total U in the sediment samples. The repair works was
completed after 1260 days with the U concentrations below 0.1μM in the multi-level sampling wells. In
the sampling wells, U (VI) levels were low because the ground water and sediment contain microbial
communities restoring the U (VI), including the Desulfovibrio genus Bacillus and Geothrix Bacillus
which was restoring Fe (III).

3.3.2 Application of phytoremediation methods in repairing uranium pollution

Phytoremediation technology is widely used to repair large areas of low concentration of uranium-
contaminated soil, with the advantages of economic viability, effectiveness, no secondary pollution, and
relatively small disturbance to the environment. Phytoremediation is a pollution control technology for
removing pollutants from the environment by plant and microbial systems based on a plant being able to
excessively accumulate one or more chemical elements. The objects of phytoremediation are heavy
metals, organic or radioactive contaminated soil and water. Studies have shown that the plant can purify
the soil and water contaminants by rhizosphere filtration, absorption, stability, degradation, volatilization
and so on.
U has not yet been found to be nutrients for the plant, but the roots of sunflower, Indian mustard and
other plants will absorb a large number of U, and some plants will transport U to their aerial parts [14].
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There are reports about repairing contaminated water by the filtering action of plant roots. Dushenkov
removed uranium from water using sunflowers, the root concentration factor of which is 30000;
wastewater on site was treated in the pilot-scale, uranium concentrations ultimately reached the water
quality control standards of the U.S. Environmental Protection Agency [15]. Sunflower is considered the
first choice to treat U polluted water because of its bio-volume. There are experiments shown that celery,
water purslane, small duckweed, and willow moss have shown enrichment for U in water [16]. The
enrichment factor of small duckweed is 2.87 × 103, 1.567 × 103 respectively in the still water and running
water.
There has been additional researches in foreign countries to carry out repairing uranium contaminated
soil by phytoremediation. The United States, Japan, the Czech Republic and other countries used Indian
mustard, cabbage, tumbleweed, reeds, and sunflowers to absorb and accumulate U in the soil [17-21].
Tumbleweed will absorb a large amount of DU before flowering; Huang used acetic acid, citric acid,
malic acid to improve the bioavailability of uranium in soil. Result showed that citric acid was the best. It
enhanced the enrichment of U from less than 5mg/kg to 5000mg/kg for the Indian mustard and Chinese
cabbage growing in soil containing U 750mg / kg. In China, Xia Chuanqing developed ten kinds of plants
in soil containing U 100 mg/kg, and measured uranium content of the aerial parts and roots of plants after
harvesting in 55 d,. The results showed that for vegetables and selected mustard of the ten plants tested,
the uranium content of the aerial parts is higher than that of the roots. Aerial parts have a higher
extraction of uranium, suitable for phytoremediation as uranium hyperaccumulators [22]. Differences of
the accumulation of U in soil for spinach, cabbage, amaranth in winter were also studied, showing that
spinach has more patience and U enrichment capability [23].
There are many factors affecting phytoremediation efficiency. Soil properties such as pH, water
content, soil texture, organic matter content can affect plant growth conditions and the bioavailability of
uranium. Soil conditioner can effectively increase the bioavailability of uranium, and promote plant
uptake of uranium [15]; soil microorganisms such as fungi can form symbiotic associations with plant
roots, combining microbial remediation and phytoremediation technology, so it can effectively repair the
uranium polluted environment [24].

3.4 Combined method of physical, chemical and biological

Prior studies have shown that bacterium are able to use organic compounds as electron donors,
removing U from contaminated groundwater by reducing the soluble U (VI) to relatively insoluble U (IV).
Studies were conducted to determine whether electrodes might serve as an alternative electron donor for
U(VI) reduction by a pure culture of Geobacter sulfurreducens and microorganisms in uranium-
contaminated sediments [25]. U (VI) can be removed from the solution rapidly in the absence of cells,
when Electrodes poised at −500 mV (vs a Ag/AgCl reference). Once the balance voltage disappears, all
the U (VI) comes back to the solution, indicating that the electrode hasn’t reduced the U (VI). If there are
Terrabacter on the electrode, U (VI) will not return to solution, unless the electrode is exposed to oxygen.
This phenomenon indicates that the existence of bacteria on the electrode can reduce U (VI) to a stable U
(IV) in deposition until being re-oxidated by the oxygen. If the electrodes are placed in the U
contaminated sediments below the surface, U (VI) can be removed from groundwater and collected. If the
electrodes are placed in the flow columns filled with sediment, U (VI) can be removed easily from the
groundwater. 87% of U can be collected from the electrode surface. These results indicate that
microorganisms can reduce U (VI) with electrons from the electrode. It is possible to remove and collect
U from contaminated groundwater using equilibrium electrodes.
Column experiments done by Zhou showed that: coordination system sulfate-reducing bacteria and
zero valent iron can effectively remove the radioactive from waste water containing uranium [26].
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Removal rates of U (Ⅵ) and sulfate were 99.4% and 86.2% respectively. Wastewater was treated up to
near-neutral pH. Sulfate-reducing bacteria remove electronic U (Ⅵ) and sulfate by providing electrons.

4.Conclusion

Transforming U into a harmless form is a way forward in the uranium pollution abatement. It could
temporarily retard the spread of uranium and toxic effects on organisms. But when the conditions of the
external environment change, such as pH values decreasing and oxidative environment substituting for
restore environment, the U (Ⅳ) may be re-oxidated to the U (Ⅵ). Therefore, the most fundamental U
pollution control measure is removing U from the environment completely. We should combine physical,
chemical and biological methods based on on-site environmental factors in order to remove U from the
contaminated environment efficiently and thoroughly.

Acknowledgements

This work was supported by the National Natural Science Foundation of China (no. 41171068 and
40701004), the Program for Changjiang Scholars and Innovative Research Team in University (no.
IRT0809), the Special Funds of State Key Joint Laboratory of Environment simulation and pollution
control (10Z02ESPCN), and the Fundamental Research Funds for the Central Universities.

References

[1] A. Bleise, P.R. Danesi, W. Burkart. Properties, use and health effects of depleted uranium (DU): a general overview.
Journal of Environmental Radioactivity 2003;64:93-112.
[2] Jose L. Domingo.Reproductive and developmental toxicity of natural and depleted uranium:a review. Reproductive
Toxicology 2001;15:603-609.
[3] Gongalsky K B. Impact of pollution caused by uranium production on soil macrofauna. Environmental Monitoring and
Assessment 2003;89:197-219.
[4]Tang ZJ, Zhang P, Zuo SQ. Technology research of treatment for uranium waste water of low concentration. Industry water
and waste 2003;4:9-12. (in Chinese)
[5]Chen CM, Zeng GM, Tang C. Research of hydroxyapatite Adsorption to uranium wastewater. Metal Mine 2009;5:135-137.
(in Chinese)
[6] Fuller CC, Bargar JR, Davis JA, etal. Mechanisms of uranium interactions with hydroxyapatite: implications for groundwater
remediation. Environ. Sci. Technol 2002;36:158-165.
[7] Sun XB, Du HF, Zhou ZM. Research of hollow fiber membrane device for processing wastewater containing uranium (Ⅵ).
Evironmental Science of ShangHai 2000;19:475-477. (in Chinese)
[8] D.H.Philiips, B.Gu, D.B.Watson, etal. Uranium removal from contaminated groundwater by synthetic resins. Water
Research 2008;42:260-268.
[9] Chicgoua Noubactep, Günther Meinrath , Broder J. Merkel. Investigating the Mechanism of Uranium Removal by
Zerovalent Iron. Environmental Chemistry 2005;2:235-242.
[10] Dushenkov S. Trends in phytoremediation of radionuclides. Plant and Soil 2003; 249: 167 -175.
[11] Kalin M,Wheeler W N,Meinrath G. The removal of uranium from mining wasterwater using algal/microbial biomass.
Journal of environment Radioactivity 2004;78:151-177.
[12] Malekzadeh F, Farazmand A, Ghafourian H, etal. Uranium accumulation by a bacterium isolated from electroplating
effluent. World journal of microbiology and biotechnology 2002;18:295-300.
1642 J. Li and Y. et
J. Li Zhang / Procedia
al./ Procedia Environmental
Environmental Sciences
Sciences 13 (2012)
8 (2011) 1609 – 1615
1636–1642 1615

[13] Wu WM, Carley J, Luo J, etal. In Situ Bioreduction of Uranium (VI) to Submicromolar Levels and Reoxidation by
Dissolved Oxygen. Environ. Sci. Technol 2007;41:5716-5723.
[14] Yao J, Ma Y, He H. The potential applications for phytoremediation in controlling radioactive uranium pollution in the
uranium mining. Environment of Sichuan 2010;29:48-51. (in Chinese)
[15] Dushenkov S, Vasudev D, Kapulnik Y, etal. Removal of uranium from water using terrestrial plants. Environ. Sci. Technol
1997b;31:3468-3474.
[16] Pratas Joao, Nelson Rodrigues, Carlos Paulo. Uranium accumulator plants from the center of the Portugal-their potential to
phytoremediation. Merkel B J.Uranium in the environment:mining impact and consequences. Berlin Spring-Verlag Press 2006:477-
482.
[17] Dana Ulmer-Scholle. Tumbleweeds good for uranium clear up.Ann Caims. Geological Society of America 116th Annual
Meeting. Denver 2004:120-125.
[18] Huang J W, Blaylock M J, Kapulnik Y, etal. Phytoremediation of uranium contaminate soils: role of organic acids in
triggering uranium hyperaccumulation in plants. Environ. Sci. Technol 1998;32:2004-2008.
[19] Shahandeh H, Hossner L R. Role of soil properties in phytoaccumulation of uranium. Water,Air,and Soil Pollution
2002;141:165-180.
[20] Chang PC, Kyoung-Wong Kim, Satoshi Yoshida, etal. Uranium accumulation of crop plants enhanced by citric acid.
Environmental Geochemistry and Health 2005;27:529-538.
[21]Venek T. Radiophytoremediation from laboratory to field application. 17th WCSS[C]. Thailand 2002;8:502.
[22]Tang L, Bai Y, Deng C. Restoration of uranium-contaminated soil hyperaccumulator and accumulation characteristics of
the screening. Nuclear technology 2009;32:136-140. (in Chinese)
[23]Xu J, Gong YB, Zhang QC. Differences of patience and uranium uptake and accumulation of uranium in soil for three
plants. Chemical Research and Application 2009;21:322-326. (in Chinese)
[24] Chen BD, Chen MM, Bai R. The potential role of Arbuscular mycorrhizal in controlling uranium contamination in the
environment. Evironmental Science 2011;32:809-815. (in Chinese)
[25]Gregory KB, Lovley DR. Remediation and recovery of uranium from contaminated subsurface environments with
electrodes. Environ. Sci. Technol. 2005;39: 8943-8947.
[26]Zhou QY, Tan KX, Zeng S. Co-processing waste water containing uranium by sulfate-reducing bacteria and zero valent
iron. Atomic Energy Science and Technology 2009;43:808-812. (in Chinese)