Environmental Research 164 (2018) 288–301

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Environmental Research
journal homepage: www.elsevier.com/locate/envres

Review article

Selenium contamination, consequences and remediation techniques in water T

and soils: A review
⁎ ⁎
Yangzhuo Hea, Yujia Xianga, Yaoyu Zhoua, , Yuan Yanga, Jiachao Zhanga, , Hongli Huanga,
Cui Shanga, Lin Luoa, Jun Gaoa, Lin Tangb
a
College of Resources and Environment, Hunan Agricultural University, Changsha 410128, PR China
b
College of Environmental Science and Engineering, Hunan University, Changsha 410082, PR China

A R T I C LE I N FO A B S T R A C T

Keywords: Selenium (Se) contamination in surface and ground water in numerous river basins has become a critical pro-
Selenium blem worldwide in recent years. The exposure to Se, either direct consumption of Se or indirectly may be fatal to
Contamination the human health because of its toxicity. The review begins with an introduction of Se chemistry, distribution
Remediation and health threats, which are essential to the remediation techniques. Then, the review provides the recent and
common removal techniques for Se, including reduction techniques, phytoremediation, bioremediation, coa-
gulation-flocculation, electrocoagulation (EC), electrochemical methods, adsorption, coprecipitation, electro-
kinetics, membrance technology, and chemical precipitation. Removal techniques concentrate on the ad-
vantages, drawbacks and the recent achievements of each technique. The review also takes an overall
consideration of experimental conditions, comparison criteria and economic aspects.

1. Introduction et al., 2005). In global terms, Se can concentrate in sedimentary more

As is known to all, selenium (Se) is an essential micronutrient for the
creature and it is good for our health at low concentration. However,
excessive Se in the environment causes serious pollution in soil, at-
mosphere and water, and brings severe risk and damage to human
health (Sakamoto et al., 2012). Industrial and agricultural activities are
the dominant anthropogenic sources of Se pollution. Selenium absence
and toxicity lead to contamination in drinking water and in wastewater,
which is a latent threat for water systems (Santos et al., 2015b).
Therefore, in recent years, selenium contamination has attracted tre-
mendous interests and has been understood more and more deeply
around the world (Sakamoto et al., 2015) (Figs. 1 and 2).
Listing in the sixth main group in the periodic table of elements,
selenium is a crystalline “metalloid” and possesses similar chemical
properties with sulfur. Selenium can occur in environment as various
oxidation states such as: selenate (SeO42-, Se(VI)), (SeO32-, Se(IV), se-
lenide (Se2-)) and elemental (Se0). However, Se(IV) and Se(VI) present
in aqueous environment commonly. Besides, the Se(IV) is more toxic
than Se(VI) (Awual et al., 2015). Selenium is also widely scattered in
rock materials. It exists in various rocks due to its dispersive nature, but
its concentration usually less than 0.1 mg/kg. The abundance in the
Earth's crust is approximately 0.05–0.09 mg/kg, it is about 1/6000 and
1/50 of the respective abundances of sulfur and arsenic (Rodriguez
easily than igneous rocks (Rodriguez et al., 2005).
As we know that the chemical form of selenium influences its
toxicity greatly. In particular, inorganic and organic selenium com-
pounds have different toxicity profiles, with the latter being much less
toxic than the former (Mehdi et al., 2013). The standards of public
health for selenium should consider chemical form, because selenium
exists in drinking water almost entirely with inorganic form. On the
contrary, inorganic forms of selenium in foods are not generally found.
Selenium is detected throughout the world in many environmental
matrices including soil, air, plants, foods, and drinking waters. In
drinking waters, selenium is generally detected at relatively low con-
centrations (Mehdi et al., 2013). Subsequent investigations indicated
that high selenium exposure by drinking water was related to lower
blood glutathione peroxidase activity, suggesting an unexpected inverse
relation between enzymatic activity and selenium intake through
drinking water at these unusually high exposure levels (Lee and Jeong,
2012).
As recently reviewed (Vinceti et al., 2013a), in most countries or
regions (e.g., European Union, Australia, Japan, Canada, Thailand and
New Zealand, the United States Food and Drug Administration), the
upper limit of Se has been set to 10 μg/L, with the exception of Russia,
which has set a limit of 1 μg/L as selenium trioxide since 1970, the U.S.
Environmental Protection Agency, which has set a limit of 50 μg/L and

⁎
Corresponding authors.
E-mail addresses: zhouyy@hunau.edu.cn (Y. Zhou), jiachao.zhang@163.com (J. Zhang).

https://doi.org/10.1016/j.envres.2018.02.037
Received 12 December 2017; Received in revised form 4 February 2018; Accepted 26 February 2018
Available online 20 March 2018
0013-9351/ © 2018 Elsevier Inc. All rights reserved.
Y. He et al.
Fig. 1. Schematic diagram shows the transfer of selenium from environment to human beings through daily life. Intake of selenium by human beings causes several diseases.
the California Environmental Protection Agency, which has set a limit
of 30 μg/L. The provisional guideline for selenium of the World Health
Organization (WHO) in drinking water was set at 40 μg/L
(Organization, 2011). However, epidemiologic studies investigated that
the current commonly used limit of 10 μg/L for selenium in drinking
water applied in most countries or regions should be decreased, and the
standard should reduction to 1 μg/L suggested by Vinceti et al. in order
to decrease the risk of adverse health effects, including neoplasms and
endocrine and neurological diseases, due to long-term exposure
(Vinceti et al., 2013a). Thus, the prevention and treatment of selenium
pollution is a crucial project for the human being.
Here, the goals of this review are to compile and analyze the current
state of knowledge of the sources of selenium in the environment,
health hazards, and remediation of selenium contamination; and to
identify knowledge gaps and future research needs. The review is
structured into four topics: a) sources of selenium in the environment;
b) health hazards; c) remediation of selenium contamination; d)
knowledge gaps and research needs.
2. Sources of selenium in the environment
The main source of selenium in the environment (e.g., hydrosphere,
pedosphere, biosphere and atmosphere) includes natural and anthro-
pogenic sources. The natural source covers marls, gypsum, volcanic
eruptions, sea spray, volatilization/recycling via biotic cycling, the
weathering of selenium-containing rocks and soils, etc. (Fairweather-
Tait et al., 2011; Rodriguez et al., 2005). Anthropogenic sources include
mining, agriculture, coal combustion, insecticide production, oil re-
fining, photocells and glass manufacture (Santos et al., 2015a). Emis-
sion of selenium to soils annually from human activities outdistances
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Environmental Research 164 (2018) 288–301
those from all natural sources summarized. Table 1 shows the selenium
concentration of several countries/areas affected by selenium exposure.
2.1. Soil
In the worldwide, all the selenium concentration in soil typically
exists within the range from 0.01 to 2.0 mg/kg with a general average
of 0.4 mg/kg (Fairweather-Tait et al., 2011). The soils present a mass of
concentration (up to 1200 mg/kg) originated in seleniferous parent
materials, including sandstones, shales, slate, limestones and coal series
(Fairweather-Tait et al., 2011). The soil is the primary source of Se that
can be transported and accumulated in the leaves by the water stream
from solum. Vegetables rich in sulfur, for example, some Allium species
and Brassica, possess a higher capacity of accumulating Se since it can
replace S in the proteins. But this accumulation is still limited at low Se
concentrations in soil (De et al., 2014).
The selenium in the soil changes depending on the type, texture and
organic matter content of soils and rainfall amount. Selenium in soils is
mainly from the rocks erosion containing selenites and selenides which
are linked to sulfide minerals and with mass fractions less than 1 mg/kg
(Mehdi et al., 2013). Selenium has several forms such as ferric selenite
and selenate salts or its organic form. SeO32− and SeO42− appear fre-
quently in most soils. Its assimilation through the plant is impacted by
the physicochemical factors of the soil (e.g., pH and redox status), and
microbiological activity. The average concentration of selenium in soil
varies from 100 to 700 ppb. For clay soils, it is 800–2000 ppb, while in
tropical soils, it is 2000–4500 ppb (Hoet, 2013). Soil acidity decides the
assimilate rate of selenium in plants and crops. In general, acid soils
tend to release less selenium than alkaline ones. Selenite oxidizes in
alkaline soils and forms soluble selenate that can easily assimilate by
Y. He et al. Environmental Research 164 (2018) 288–301

Fig. 2. Schematic diagram is indicating various techniques used for selenium removal from soils and water. These techniques are discussed in detail in next text.

Table 1
Concentrations of selenium in environment of the countries/areas affected by excessive selenium.

Location (Countries) Selenium sources Selenium concentrations(average) References

USA Seleniferous soils up to 28 mg/kg (Bajaj et al., 2011).

Ireland Seleniferous soils up to 1200 mg/kg (Bajaj et al., 2011)
China Seleniferous soils up to 59 mg/kg (Bajaj et al., 2011)
California's San Joaquin Valley Drainage water of soils 75–1400 μg/L (Zelmanov and Semiat, 2013)
Japan Industrial wastewater ≤ 0.1 mg/L (Soda et al., 2011)
Amman Zarqa Basin (AZB), Jordan Lower aquifer 1.6–30 μg/L (13 μg/L) (Alkuisi and Abdelfattah, 2010)
Amman Zarqa Basin (AZB), Jordan Middle aquifer 1.5–742 μg/L (35 μg/L) (Alkuisi and Abdelfattah, 2010)
Amman Zarqa Basin (AZB), Jordan Upper aquifer 0.4–246 μg/L (9 μg/L) (Alkuisi and Abdelfattah, 2010)
Barwa, Jainpur Groundwater 341 μg/L (Bajaj et al., 2011).
Hisar Groundwater 3.2 μg/L (Bajaj et al., 2011)
Chandigarh Groundwater 0.9 μg/L (Bajaj et al., 2011)
Chennai, India Groundwater Se(IV)0.15–0.43 μg/L (Kumar and Riyazuddin, 2011).
Chennai, India Groundwater SSe(VI) 0.16–4.73 μg/L (Kumar and Riyazuddin, 2011)
Punjab, India Groundwater 669.5 g/L (Bajaj et al., 2011)
Punjab, India Soil 6.5 mg/kg (Bajaj et al., 2011)
Punjab, India Plants 3–670 mg/kg (Bajaj et al., 2011)

290
Y. He et al.
plants. In acid soils, conversely, selenite is often associated with iron
hydroxides, making it highly fixed by the soil (Stadlober et al., 2001).
2.2. Waters
Recently, new data from both human and laboratory studies on the
toxicity about organic and inorganic selenium make people reassess the
safety of selenium in drinking water timely and redesign the adequacy
of present regulatory standards (Vinceti et al., 2009). The selenium
toxicity in drinking water has caused debate since the 1970s. The
maximum permissible limit suggested by the WHO in drinking water is
10 ppb, while USEPA sets the limit at 50 ppb as well. A background
document recommended a guideline value of 40 μg/L for drinking
water (Toft, 2003), and this value became a part of the update of the
WHO guidelines for drinking water quality in 2011 (Organization,
2011). In some areas, the selenium content in well water or more
generally in underground waters used for human consumption may
reach 10–20 μg/L, with some concentrations in the hundreds of μg/L
(Emmanuelle et al., 2012). Mineral waters generally contain selenium
at levels of a few ng/L. Drinking water is not generally regarded as a
nutritional source of the element (Vinceti et al., 2013b).
2.3. Plants
In some countries like China and Egypt, Se deficiency in the diet
becomes a widespread problem. To solve this problem, researchers
employ Se compounds to boost the Se content in the edible parts of
crops, through foliar sprays or basic application of fertilizers (Feng
et al., 2013). Plants easily take up and assimilate Se through sulfur (S)
transporters and biochemical pathways, and can volatilize methylated
Se as well. Plants can be employed both to provide dietary Se in the
areas of Se deficiency, and to eliminate Se pollution from seleniferous
areas (Pilonsmits and Quinn, 2010). Concentrations of selenium in
plants are associated with surrounding selenium levels in the soils. In-
corporation and redistribution of selenium by the roots occurs rapidly,
however, it is dependent on the physiological conditions and plant
species. In most situations, 85% of selenate and 70% of selenite are
discovered in the aerial tissues (Wadgaonkar et al., 2018). The standard
content of selenium in forages ranges from 0.1 to 0.5 ppm. The risk of
livestock poisoning is high and exceeds 5 ppm (Ma et al., 2017).
2.4. Air
The major sources of emission of selenium in air derived from
burning coal and oil. The content of selenium is generally low in sur-
rounding air. The atmosphere occupies a significant status in the bio-
geochemical cycling of selenium because it can affect the transport and
transformation (Huang et al., 2012). The existence of selenium is as-
sociated with human activities such as burning of fossil fuels and in-
cineration of garbage, paper and tires (Marcocci et al., 2011; Soda et al.,
2011). It is also related to natural activities like forest fires, soil erosion
and volcanism. selenium dioxide and selenide are unstable in air, yet
dimethyl selenide is stable. Hydrogen selenide is oxidized into H2O and
selenium (Mehdi et al., 2013). In humid conditions selenium dioxide
takes transformation into selenious acid.
2.5. Food
The primary food offering selenium in the diet is cereals and bread,
eggs, fish, meat, and milk/dairy products. Besides, some Brazil nuts also
are a prominently rich source, with concentrations of selenium ranging
from 0.03 to 512 mg/kg fresh weight (Broadley, 2011; Silva et al.,
2017). The selenium content in the homologous soils usually decides
the selenium content of vegetables and grains. Vegetables like peas,
beans, turnips, potatoes, cucumbers, beets, carrots and tomatoes in-
clude 6 mg/g of selenium as a maximum, though when grown in
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Environmental Research 164 (2018) 288–301
seleniferous soil. Vegetables like asparagus and onion can accumulate
as much as 17 μg/g of selenium in such soils. Garlic and brassicas such
as cabbage, mustard and broccoli tend to accumulate selenium effec-
tively as well. In general, fruits include only a small number of sele-
nium. Similarly, the diet of these animals decides the selenium content
of foods eaten by animals (Mehdi et al., 2013).
3. Health hazard and interactions with heavy metals
3.1. Health hazard
Selenium plays a significant role as an antioxidant in humans.
Considering its importance for humans, the suggested dietary intake for
Se is 55 and 30 μg/d for healthy adults in the US and Europe, and
50–250 μg/d for adults in China by Chinese Nutrition Society. The se-
lenium recommended daily intake of the CSS (Council of Health) in
Belgium ranges from 60 μg/day for women to 70 μg/day for men (from
14 years). This recommendation is increased in to 65 μg for pregnant
women and 75 μg during lactation. The European Food Safety Authority
(EFSA) 2006 guidelines sets the tolerable upper intake (UL: Tolerable
Upper Intake Level) to 300 μg/day for adults. For children, the UL is
60 μg/day (children aged 1–3 years) to 250 μg/day (children aged
15–17 years) (Sun et al., 2014; Mehdi et al., 2013).
Selenium as a vital component of selenoproteins occupies a sig-
nificant status in many biological functions, like the formation of
thyroid hormones, antioxidant defense, DNA synthesis, fertility and
reproduction. Selenium is capable of being switched in the organism
into various metabolites. Such as methylselenol, plays an important
part in cancer prevention. Selenium also has a role in muscle function
through improving endurance and recovery and relieving the ageing
process, besides vitamin E (Mehdi et al., 2013). The trace element se-
lenium occupies a beneficial status in human health for many years
owing to different low-molecular-weight compounds and its existence
within 25 selenoproteins in the amino acid selenocysteine. Though
many selenoproteins maintain functionally uncharacterized, some of
their general functions contain redox homeostasis, thyroid hormone
metabolism and redox regulation of intracellular signaling. Pathologi-
cally, decreasing expression of selenoproteins has been associated with
the congenital muscle disease directly known as thyroid-hormone me-
tabolism defects and with selenoprotein N (SEPN)-related myopathy
(Papp et al., 2010).
There is a relatively narrow range between selenium intakes that
result in toxicity or deficiency. However, levels of dietary exposure at
which selenium becomes toxic and selenosis develops are difficult to
establish, because toxicity is affected by the form in which selenium is
available in the food supply, and probably also by combination with
other dietary components and, possibly interactions with genotype
(Fairweather-Tait et al., 2011).
It is well known that selenium supplementation or higher selenium
status has antiviral effects, which is important for successful reprodu-
cing of male and female, and lower the risk of autoimmune thyroid
disease. But excess selenium can result in cancer through generates
reactive oxygen species (ROS), which is closely connected with carci-
nogenesis. Some studies also indicate high selenium concentration are
positively associated with diabetes in humans, and tend to drive tu-
morigenesis by elevating TR1 expression (Sun et al., 2014). Besides a
close relation with carcinogenesis, selenium is related to development
of chronic degenerative diseases such as cardiovascular disease and
amyotrophic lateral sclerosis (Vinceti et al., 2009). In addition, sele-
nium tends to trigger neurodegenerative effect, further induces amyo-
trophic lateral sclerosis (Chen et al., 2010; Vinceti et al., 2013b). Se-
lenium is a neurotoxin, with inorganic selenium appearing to be about
40 times more neurotoxic than organic selenium (Vinceti et al., 2013a).
However, the selenium toxicity depends not only on its concentration
and speciation, but also on other components that accompanied with it.
These components can also induce significant effects on the target
Y. He et al.
Table 2
Examples of applications of various analytical methods for selenium species determination in different samples.
Sample Species
Grape pomace The total selenium
Food (fish, beef, chicken, milk, rice, wheat flour, The total selenium
egg)
Food (pepper, ginger, wheat flour, red lentil, The total selenium
traditional soup, corn flour, cornstarch, and
garlic)
Rats Selenoprotein and Se-containing
proteins separation
Nuts SeMet, SeCys, selenite and
selenite
Fish, oyster SeCys2, TMSe, SeMet, Se(IV), Se
(VI)
Soil (from Brazil) Se(IV)
Soil (from Brazil) The total selenium
organism because of antagonistic or synergistic effects, spanning 2 or 3
orders of magnitude generally for inorganic selenium species (Sharma
et al., 2017).
Some diseases and disorders related to selenium deficiency are well
known in humans and animals. Low selenium status has been related to
increased risk of mortality, weak immune function, and cognitive de-
cline. In humans, selenium deficiency can trigger peripheral myopathy,
necrotizing cardiomyopathy, decreased muscle tone and conduction
disturbances, hair thinning, opacification of the nails and anemia. The
relative risk of cancer was higher in individuals with low plasma sele-
nium concentrations (< 115 ng/mL) (Fairweather-Tait et al., 2011).
Cardiomyopathy in children was reported in China. It is known as Ke-
shan disease and was attributed to the selenium deficiency (Koyama
et al., 2013; Mehdi et al., 2013). In animals, selenium deficiency is
fairly common. Manifestations of selenium deficiency are different in
the young and the adult animals. The first organs affected by selenium
deficiency are the liver, the heart and the skeletal muscle. In young
animals, the most prevalent disorder resulted by selenium deficiency is
white muscle disease, which is rare and discreet in adults (Sordillo,
2013). In sheep, wool is the most sensitive to selenium production
deficiency. In dairy cows, a decrease in the fat content of milk is ob-
served (Mehdi et al., 2013). However, for most animals, consumption of
plant species with a Se content of 0.1–0.3 mg/kg is acceptable, while
the minimum nutritional concentration for animals is about
0.05–0.1 mg Se/kg in dry feed, and the minimum in grass is 0.1 mg/kg,
animals become selenosis because of ingesting plants containing several
thousand mg Se/kg dry weight (Rodriguez et al., 2005). The main signs
of selenium toxicity are musculoskeletal disorders such as stiff gait and
lameness. For aquatic organisms, some fish such as largemouth bass and
pumpkinseed showed sensitivity in water contained selenium, while
fathead minnow, common carp, eastern mosquitofish (Gambusia hol-
brooki), and black bullhead are on the contrary. It is reported that some
algae have tremendous tolerance for selenium. For example, algae can
bioconcentrate selenium with a greater extent than any other trophic
level. Chlorophytes typically accumulated the least selenium, whereas
prymnesiophytes, prasinophytes and dinoflagellates had the greatest
enrichments (Janz et al., 2010). Different species have differential
sensitivity to selenium.
3.2. Interactions with heavy metals
The issue of both negative, null and positive interactions between Se
and heavy metals is worth discussing. For example, both field and la-
boratory studies have observed the antagonistic effects of selenium on
Hg in fish (Burger and Gochfeld, 2012; Huang et al., 2013). Previous
studies showed that selenium tends to reduce MeHg bioavailability (so
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Environmental Research 164 (2018) 288–301
Analytical methods References
Flow injection-electrothermal atomic absorption (Martínez et al., 2018)
spectrometry (FI-ETAAS)
Flow injection-hydride generation atomic absorption (Sigrist et al., 2012)
spectrometry (FI-HGAAS)
Vortex-assisted ionic liquid-based microextraction (Bağda and Tüzen, 2017)
(VA-IL-DLLME)
Sodium dodecyl sulfate polyacrylamide gel (Pedrero and Madrid, 2009)
electrophoresis (SDS-PAGE)
Capillary electrophoresis (CE)-ICP-MS (Kannamkumarath et al., 2005)
HPLC-ICP-MS (Cabañero et al., 2005)
Ultrasound-assisted alkaline extraction and hydride (Schneider et al., 2016)
generation atomic absorption spectrometry (HG AAS)
High-resolution continuum source graphite tube (Schneider et al., 2016)
atomic absorption spectrometry (HR-CS GF AAS)
decrease assimilation) or increase the MeHg elimination, resulting in an
overall reduction of MeHg bioaccumulation (Miklavčič et al., 2013;
Wang and Wang, 2017). In addition, Se also can form well association
with Hg, in the bloodstream, selenite reacts also with Hg2+ to form a
species with a core of HgSe and GS-moieties ligated on the surface in
the form (HgSe)100(GS)5. This Se-protein is actively involved in a de-
toxification mechanism for Hg (Roman et al., 2014).
The antagonistic effect of selenium on arsenic toxicity has been
gradually accepted by the public. In recent years, more in vitro research
indicated that Se can alleviate arsenic toxicity through genotoxicity,
modifying cytotoxicity and oxidative stress (Chitta et al., 2013; Selvaraj
et al., 2012). Many have investigated the toxicological and metabolic
interactions between As and Se, most of which focus on their antag-
onistic effects. However, previous study pointed out that Se metabolites
(trimethylselenium ion and dimethyl selenide) can enhance arsenic
toxicity. Recently, some investigators reported that there is synergistic
effect between As and Se toxicity through mutually inhibiting each
other's metabolites. Later on, Song et al. provided new evidence to
support the opinion that Se can accelerate arsenic toxicity (Song et al.,
2010).
In theory, many metal cations can form insoluble colloids or com-
plexe with selenide, but only silver (Ag) has been demonstrated to ac-
cumulate in mammalian cells in this way. In contrast, Se is generally
associated to a decreased bioaccumulation of cadmium and arsenic, so
excretion mediated by conjugation of these elements with organic Se-
species may be gathered as the favored route (Roman et al., 2014).
4. Remediation of Selenium contamination
Selenium is a significant element in plant and animal nutrition. The
beneficial effects of selenium on human health are strongly dependent
on its chemical form and concentration, the isolation and accurate
characterization and quantification of selenium species is still a chal-
lenge (Pedrero and Madrid, 2009), Table 2 shows several analytical
methods for selenium species determination in different samples. Pre-
vious study reported that selenium doses at 100–200 μg/d inhibit ge-
netic damage and cancer development in human subjects; however, at
400 μg/d, selenium probably induces cancer (Sun et al., 2014). Ex-
ceeding the upper limit level may result in selenosis (Gorai, 2003). The
symptoms contain gastrointestinal disorders, hair loss, garlic odour on
the breath, neurological damage, sloughing of nails, fatigue, irritability,
and monstrous deformities. Extreme cases of selenosis may lead to
pulmonary edema, cirrhosis of the liver and death (Pérez-Corona et al.,
1997). Selenium is known to be mutagenic and teratogenic. Toxicity of
selenium in the aquatic food chain and its anthropogenic and natural
sources were well introduced previously (Hamilton, 2004). The
Y. He et al.
recognition that low concentrations of selenium in drinking water
brings out serious health effects, therefore, the removal methods of
selenium is more and more important. Some presently available tech-
nologies, such as oxidation, phytoremediation, coagulation–floccula-
tion, adsorption and so on will be discussed as follows.
4.1. Selenium removal by reduction techniques
Nanoscale zero-valent iron (nZVI) is one of the most widely applied
nanomaterials for the treatment and remediation of soil, groundwater
and hazardous waste (Ling et al., 2015). It is being employed for the
detoxification commonly of a broad range of pollutants like haloge-
nated hydrocarbons, nitroaromatic compounds, azo dyes, antibiotics,
flame retardants, perchlorate, hexavalent chromium, heavy radio-
nuclides and metal ions (Liu et al., 2017a; Raychoudhury et al., 2014;
Tang and Lo, 2013). Increasing research shows that nZVI can treat and
remove selenium effectively.
Zhou et al. proved that chemical reduction of Se(IV) to Se(0) is the
main Se(IV)-nZVI reaction mechanism. Se(IV) is separated from water
via nZVI by chemical reduction to Se(II) and Se(0), as well as en-
capsulation in the nanoparticles (Zhou et al., 2016b). The reduction and
sequestration mechanisms can account for the rapid removal of Se(IV)
and large capacity for selenium encapsulation fully. It is also suggested
that defects on the nZVI particle shell markedly facilitate the spread of
selenium and enhance the capacity of nZVI for selenium sequestration
(Ling et al., 2015; Zhou et al., 2016c). In addition, results indicate that
STEM-XEDS method is a valuable tool used for visualizing solid phase
reactions, in particular powerful for mapping inorganic elements like
heavy metals in a single nanoparticle near atomic resolution (Tang
et al., 2016).
4.2. Phytoremediation
Phytoremediation as a green biotechnology is effective to remove Se
from contaminated environments, mainly including phytoextraction
and phytovolatilization (Wu et al., 2015). Se contamination because of
industrial activities has attracted increasing concerns. It has been re-
ported that phytoremediation is an effective and feasible approach to
get rid of Se from Se-contaminated environment. Plants that can ac-
cumulate and tolerate moderately elevated Se levels (up to 1000 mg Se/
kg DW) are called Se accumulators. True Se hyperaccumulator species,
from the genera Stanleya, Astragalus, Xylorhiza and Oonopsis, can ac-
cumulate 1000– 15,000 mg Se/kg DW (0.1–1.5% Se) without any
toxicity symptoms (El Mehdawi and Pilon-Smits, 2012). In recent years,
a kind of arsenic (As) hyperaccumulator Pteris vittata L. (Chinese Brake
fern) was discovered to be a Se accumulator (Wu et al., 2015). The Se
accumulation mechanism was determined by focusing on antioxidant
responses of the plant to six levels of selenite (0, 1, 2, 5, 10, and 20 mg/
L). The results indicated that Chinese Brake fern accumulated much Se
without any visible toxic symptoms and important decrease in its bio-
mass. However, the root absorbed more Se than the fronds. The highest
selenium concentration in roots and fronds respectively was 1.536 mg/
kg and 242 mg/kg, demonstrating a typical accumulation character to
Se (Feng and Wei, 2012). Addition of 2 mg/L Se decreased, yet ≥ 5 mg/
L Se boosted the production of malondialdehyde (MDA), showing an
antioxidant role of Se at low dosages. The enzymes of peroxidase
(POD), ascorbate peroxidase (APX) and catalase (CAT) contributed
their anti-oxidative performance only under low dosages of Se, for in-
stance, their activities enhanced at Se levels ≤ 5 mg/L and activities
decreased at Se levels > 5 mg/L. The enzyme activity of glutathione
reductase (GR) and concentration of glutathione (GSH) were stimulated
by ≥ 5 mg/L Se. Superoxide dismutase (SOD) activity was also in-
creased by 20 mg/L Se (Feng and Wei, 2012). The results indicate that
GR, GSH and SOD were likely responsible for, however, enzymes of
POD, APX, and CAT play limited roles in accumulation of selenium in
Chinese Brake fern.
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Environmental Research 164 (2018) 288–301
To sum up, Chinese Brake fern is able to assimilate a large number
of selenium under hydroponic condition which can be used to eliminate
Se possibly from Se-contaminated water. Further researches must be
carried out to assess its remediation efficiency and the impact factors of
Se removal (Feng and Wei, 2012).
4.3. Bioremediation
Microbial selenium (Se) bioremediation is on basis of conversion of
toxic, water soluble Se oxyanions to elemental, water insoluble Se.
Formed Se of biogenic element is of nanometer size, hindering
straightforward separation from the aqueous phase (Buchs et al., 2013).
Selenium is an element of concern especially when released to the
environment by anthropogenic activity. Biofilms, or communities of
microorganisms, occupy significant status in biotransforming elements
into less toxic chemical forms (Fu et al., 2014). Yang et al. employed
novel tools to characterise the destiny of oxyanions (selenite or selenite)
in multi-species biofilms inoculated from an origin receiving coal
mining effluent. Confocal laser scanning microscopy (CLSM) showed a
distinct biofilm morphology at increased oxyanion concentrations
(Yang et al., 2011). Selenium K near-edge X-ray absorption spectro-
scopy (XAS) demonstrated biofilm biotransformation of oxyanions and
extended X-ray absorption fine structure (EXAFS) showed elemental
selenium as a product. Micro X-ray fluorescence imaging combined
with the CLSM revealed highly localized decreased selenium species in
the biofilm. Isolation and partial 16S rRNA gene sequencing indicated
four principle bacterial genera were responsible. Biofilms is able to both
detoxify and sequester selenium, playing critical parts in the fate and
effects in aquatic environments (Yang et al., 2011).
Alishewanella sp. WH16-1 isolated from mining soil is a facultative
anaerobic bacterium. Under aerobic conditions, this bacterium reduces
selenite efficiently. A flavoprotein with 37% amino acid identity to the
E. coli chromate reductase ChrR was identified from genome (named
CsrF). Gene mutation and complementation along with the hetero-
logous expression revealed the capacity of CsrF to reduce selenite in
vivo. The purified CsrF was yellow and indicated an absorption spectra
similar to FMN. In vitro, CsrF catalyzes the Se(IV) reduction using the
NAD(P)H as cofactors with optimal condition of temperature of
30–37 °C and pH 7.0. Using Nicotinamide Adenine Dinucleotide
Phosphate (NADPH) as the electron donor, the Km for the Se(IV) re-
duction was 204.1 ± 27.91 μmol/L (Xia et al., 2018). Site-directed
mutagenesis indicated that Arg13 and Gly113 were of crucial im-
portance for the reduction of Se(IV). The products of the reduction of Se
(IV) was Se(0). For all we know, CsrF is a well-characterized and novel
bacterial aerobic selenite reductase (Xia et al., 2018).
Up to now, some bacterial species have been found to can reduce Se
(IV) to Se(0), and the process is a detoxification reaction (Nancharaiah
and Lens, 2015). The bacterial Se(IV) reduction may occur both en-
zymatically and non-enzymatically. The non-enzymatic reduction che-
mical compounds include siderophore, H2S and glutathione
(Nancharaiah and Lens, 2015). In anaerobic bacteria, enzymatic re-
duction of Se(IV) usually appears as reduction during respiration.
Currently, fumarate reductase (Li et al., 2014), nitrite reductase
(Demoll-Decker and Macy, 1993), hydrogenase I (Yanke et al., 1995),
arsenate reductase (Afkar et al., 2003) and sulfite reductase (Harrison
et al., 1984) have been reported to can reduce Se(IV). Se(IV) or other
substrates such as nitrite, sulfite, arsenate and fumarate play the part of
terminal electron receptor for these enzymes (Zhou et al., 2014).
Thioredoxin reductase (Hunter, 2014a), NADH: flavin oxidoreductase
(Hunter, 2014b) and glutathione reductase were reported to serve as
aerobic selenite reductases in aerobic conditions. However, they are
still not been well studied in vivo and also lack of enough proofs in
vitro. Besides, the products of selenite reduction are able to form SeNPs
in some bacteria (Lampis et al., 2016; Li et al., 2014; Tan et al., 2016;
Zheng et al., 2014).
Y. He et al.
4.4. Coagulation-flocculation
Selenium is a kind of contaminants needed to be stipulated in
drinking water treatment, but little information has been collected up
to now regarding Se removal by coagulation. Hu et al. reported that the
performance of removing Se by coagulation has been evaluated as re-
gards the dependence on Se species, water pH, interfering ions, and
coagulant type (Hu et al., 2015). They found that Fe-based coagulants
were much more efficient than the Al-based coagulants in Se removal.
The removal of selenite (Se(IV)) by coagulation was much more pro-
minent than that of selenate (Se(VI)) (Adio et al., 2017). With an FC
dosage of over 0.4 mM Fe/L, Se(IV) removal efficiency of over 98%
could be achieved when the initial concentration of Se(IV) was 250 μg/
L (Hu et al., 2015; Staicu et al., 2015c). For Al-based coagulants (AlCl3
(AC) and the polyaluminum chloride (PACl)) the efficiency of Se re-
moval was correlated with the content of Al13 species positively during
the coagulation process. Adsorption onto hydroxide flocs was the most
positive coagulation mechanism for removal of Se and precipitation
also played specific parts at low dosage, in particular for Se(IV) removal
and with Fe coagulant (Staicu et al., 2015b). High coagulant dosage and
weakly acidic pH can increase the formation of hydroxide flocs having
more positive adsorption sites and high zeta potential, and so favored
Se removal. These findings are significant to understand the mechan-
isms and efficiency of Se removal by coagulation (Adio et al., 2017).
In addition, Hu et al. (2015) found that Fe-based coagulant was
much more efficient than Al-based coagulants. The removal of se(IV)
could be more easily than Se(VI) by coagulation. The results showed
that the coagulation with iron salt is an effective technique for Se(IV)
removal. The negative influence on Se(IV) removal among the four
oxyanions tested followed the order: PO43- > SiO32- > CO32- > SO42-.
Pre-reduction of Se(VI) to Se(IV) appears to be necessary to achieve
effective removal of Se. Besides, some coagulant aids, chitosan for ex-
ample, is possible to have the potential to increase Se(VI) removal by
coagulation (Hu et al., 2015).
4.5. Electrocoagulation (EC)
Colloidal elemental selenium (Se(0)) adversely influences mem-
brane separation processes and aquatic ecosystems. As a solution to this
issue, Staicu et al. researched for the removal potential of Se(0) the first
time by electrocoagulation process. Colloidal Se(0) was produced by a
kind of Pseudomonas fluorescens and indicated limited gravitational
settling. The best Se(0) turbidity removal (97%) was obtained by using
iron electrodes at 200 mA. Aluminum electrodes got rid of 96% of
colloidal Se(0) only at higher current intensity (300 mA). In the con-
dition of the best Se(0) removal efficiency, electrocoagulation with
using Fe electrode removed 93% of Se concentration, but with Al
electrodes the Se removal efficiency only reached 54% (Staicu et al.,
2015a). Because the Al flocs were the less compact nature, the Se-Al
sediment was treble more voluminous than the Se-Fe sediment. The
toxicity characteristic leaching procedure (TCLP) test indicated the Fe-
Se sediment released Se under the regulatory level (1 mg/L). However,
the concentration of Se leached from the Al-Se sediment was higher
than the limit by about 20 times (Malakootian et al., 2011; Sharrad
et al., 2012). This might be attributed to the mineralogical nature of the
sediments. Electron scanning micrographs indicated Fe-Se sediments
with a reticular structure, but the Al-Se sediments lacked an organized
structure (Malakootian et al., 2011). Overall, the results obtained de-
monstrated that the Fe electrodes as soluble anode in electrocoagula-
tion forms a better option than Al electrodes with regard to the elec-
trochemical sedimentation of colloidal Se(0) (Staicu et al., 2015a).
4.6. Electrochemical methods
Selenium, mainly selenite and selenate, can be transformed into Se
(0) by several techniques including abiotic reduction by green rust,
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Environmental Research 164 (2018) 288–301
biological reduction, photocatalysts, and zero-valent iron (ZVI)
(Chakraborty et al., 2010; Gonzalez et al., 2010; Olegario et al., 2010;
Yoon et al., 2011). The reduction reduced the actual risk of exposure to
selenium due to non-mobility. Among these reduction techniques, ZVI
has received more attention as it can be applied in permeable reactive
barriers of Se for in situ remediation in groundwater. But the reduction
of Se relies heavily on the surface characteristics of iron as well as
dissolved oxygen concentration in groundwater. Surface coating by iron
oxide significantly reduces the reactivity, and ZVI does not make a
transformation of Se under limited concentrations of dissolved oxygen
(Yoon et al., 2011). Recently, electrochemical methods have been used
for transforming contaminants as well as overcoming the uncontrolled
reactivity of ZVI. In an electrochemical system of using iron anode,
oxidation of iron anode stops formation of oxygen and water oxidation.
It produces ferric ions and ferrous resulting in the formation of ferric
hydroxides and ferrous in a mixed cell (Ciblak et al., 2012). Electro-
chemical reduction of selenate (selenate to Se(0) or selenite) and oxi-
dation of ferrous or ferrous hydroxide can occur as follows (Baek et al.,
2013):
SeO42 − + 2e− + 3H+ → HSe32 − + H2 0 E0 = 1.060 V (1)
HSeO3− + 4e− + 5H+ → Se0 + 3H2 O E0 = 0.903 V (2)
Fe2 + → Fe3 + + e− E0 = −0.771 V (3)
Fe(OH)2 + OH− → Fe(OH)3 + e−E0 = 0.54 V (4)
The oxidation of ferrous to ferric (Eq. (3)) might not be coupled with
the reduction of selenate or selenite (Eq. (1) or Eq. (2)) based on the
standard reduction potential. Electrochemical removal of selenate by
iron anode has been investigated (Baek et al., 2013). The removal of
selenate exists in solution, possibly because of the formation of ferrous
hydroxide precipitates. The selenite reduced from selenate was might
decreased to Se(II) or Se(0), non-extractable precipitates by ferrous
hydroxide. The reduction rate of selenate boosts with increasing the
applied current and with reducing the initial concentration of selenate.
The number of the ferrous hydroxide, reducing agent, is proportional to
the applied current (Yang et al., 2015; Zhang et al., 2014b). The redox
potential and pH vary for different background electrolytes, but sele-
nate was removed from the solution just at different rates. The ferrous
irons would be oxidized to ferric forms due to the existence of dissolved
oxygen. The partial oxidation of ferrous could reduce the amount of
ferrous hydroxide slightly, a reducing agent of selenite (Zhang et al.,
2014b). This electrochemical system is able to be applied to both oxic
and anoxic system to remove selenate. There is a study has demon-
strated that electrochemical system is effective to reduce and remove
selenate from water environment such as groundwater or mining areas
(Baek et al., 2013).
4.7. Adsorption
Various techniques have been applied for selenium removal: ad-
sorption, lime softening, coagulation/filtration, anion exchange, re-
verse osmosis, electrodialysis and distillation, among which the ad-
sorption technique holds the advantages of removal economy, simple
process and efficiency. Adsorption method has been known to be ef-
fective in removing heavy metal cations and metalloid anions (Fu et al.,
2014; Zhou et al., 2016c). As presented in Table 3, it can be seen that
adsorption technique has been successfully used for selenium re-
mediation.
4.7.1. Activated alumina
Nanocrystalline metal oxide impregnated chitosan beads (MICB)
were developed with nanocrystalline aluminum oxide (n-Al2O3) suc-
cessfully to form n-Al2O3 impregnated chitosan beads (AICB) (Yamani
et al., 2014). AICB can adsorb inorganic aqueous selenite and selenate
simultaneously more effectively than chitosan or n-Al2O3 alone. For
Y. He et al. Environmental Research 164 (2018) 288–301

Table 3
Main characteristics of other adsorbents reviewed.

Adsorbents Advantages Efficiency Assessment

AICB AICB can adsorb inorganic aqueous selenite For coexisting systems of selenite and selenate, AICB is In order to hold consistent removal in more realistic
and selenate simultaneously more potentially the most robust option. systems, it will be necessary for a pre-treatment process
effectively than chitosan or n-Al2O3 alone. to manage sulfate as indicated for other adsorbents
performed for selenium adsorption in aqueous systems.
Activated A kind of multifunctional sorbent Activated carbons are capable of decreasing the It offers an attractive option for use of removing Se in
carbons Cost-effective emission of majority of the pollutants to acceptable flue gases as it has proved to have favorable retention
limits. characteristics for mercury species in gaseous phase.
Y2(OH)5Cl Be reusable and have high efficient At the low concentration region, Y2(OH)5Cl 1.5H2O It is a promising and emerging material for efficient
1.5H2O removal capability can almost remove selenium completely from aqueous removal of selenate and selenite and other anionic
Be emerging material solution. environmental pollutants.
MGO Be reusable and efficient The removal percentage for selenate (80%) and The MGO composite has prominent removal capability
Indicate efficient and high binding capacity selenite (> 99.9%) with MGO dosage 1 g/L and initial of selenite and selenite in water with significant
for Se(VI) and Se(IV) concentration of selenium of 300 ppb within a few potential practical applications in removing selenium
seconds. from wastewater.
NanoFe Cost-effective and efficient This technique achieved concentration of residual This method enables the recovery of the adsorbent
Be reusable selenium less than 0.01 ppm, being acceptable by through producing concentrated selenium solution that
water quality regulations and at lowest 95–98% could be treated further to obtain selenium-containing
regeneration efficiency of selenium with the proposed crystals when recovering the cleaning solution.
adsorbent.

integrity, adsorption capability was also compared to n-TiO2, an ex-
tensive research adsorbent for Se, and n-TiO2 impregnated chitosan
beads (TICB). For the selenite system, n-Al2O3 as the main active ad-
sorbent was responsible for removal because chitosan has a low affinity
for selenite (Larraya et al., 1994). However, for selenate, chitosan was
the main active adsorbent. For coexisting systems of selenite and sele-
nate, AICB is potentially the most robust option because it kept the most
consistent performance in spite of fractionation of the selenium species
(Pyrzyńska et al., 1998; Su et al., 2008). Equilibrium isotherms and
Kinetic studies were completed and effectively modeled using Langmuir
adsorption theory and pseudo-second order kinetics, making it the first
comprehensive systematic research of AICB and neat n-Al2O3 for sele-
nium adsorption. Because of changes in the adsorbent surfaces charge,
pH observably influenced adsorption. Increasing pH coincided with
decreasing adsorbent performance, beginning at about pH 6.5–7.0 for
AICB. The tendency in performance because of the effect of pH showed
that selenate binds to the amine group into chitosan, as recommended
by other studies. Furthermore, increasing background sulfate con-
centration was discovered to influence adsorption efficacy negatively
for both selenite, and more importantly, because of their similar
structures, selenite, as sulfate is familiar to compete with selenium
oxyanions. The results show that, in order to hold consistent removal in
more realistic systems, it will be necessary for a pre-treatment process
to manage sulfate as indicated for other adsorbents performed for se-
lenium adsorption in aqueous systems (Yamani et al., 2014).
4.7.2. Activated carbons
The emission of possible toxic compounds of selenium exists in flue
gases origin from coal combustion and gasification processes has re-
sulted in the requirement for gas cleaning systems capable of decreasing
their content (Jiang et al., 2015). Selenium are listed in the toxic air
metals addressed input the 1990 Clean Air Act Amendments (CAAA).
One of the anthropogenic sources of emissions of the element is Coal-
fired plants for electricity generation (López-Antón et al., 2007; Zhou
et al., 2016a).
Selenium concentrations in coal generally range between 0.2 and
1.4 μg/g, and its mode of occurrence vary for different coals. Generally,
selenium is found in iron and sulfur minerals or linked to pyrite, but
may also be organically related in low rank coals (Jiang et al., 2015;
López-Antón et al., 2007). Upon coal combustion, much of this element
gets away from the coal matrix and distributes between the vapour and
particulate phases in diverse proportions, depending on factors like the
particulate control devices, the operating conditions and design of the
combustion facility and the initial concentration in the parent coal.
Commonly, selenium remains mainly in gas phase. Selenium as one of
the most volatile trace elements in coal, is second only to the mercury
and the halide species. Though selenium also has distribution between
the vapour and condensed forms, an important portion of this element
escapes into the atmospheric environment in the form of vapour. Se-
lenium is able to exist in the flue gas in different chemical forms de-
pending on the flue gas composition and temperature (Dobrowolski and
Otto, 2013).
The retention of trace compounds origin from flue gases caused by
coal combustion and gasification making use of solid sorbents have
been published according to several researches. These sorbents have
been primarily used in two ways; (i) by passing the flue gases through a
fluidised bed or fixed of sorbent and (ii) by injecting directly of the
sorbent as a powder. Several solid materials, like fly ashes, metal oxide
mixtures, specially hydrated lime (Ca(OH)2) and clay minerals have
been tried out as sorbents for retaining selenium compound in gases
from coal combustion and gasification (Dobrowolski and Otto, 2013).
In majority of these works, chemisorption is regarded as one of the
probable retention mechanisms. Because of the existence of multiple
trace elements in flue gases, recent efforts of the study community have
been directed to develop a multifunctional sorbent capable of de-
creasing the emission of majority of the pollutants to acceptable limits.
Activated carbon as a multifunctional sorbent offers an attractive op-
tion for use as it has proved to have favorable retention characteristics
for mercury species in gaseous phase (López-Antón et al., 2007; Wu
et al., 2016; Zhou et al., 2017a, 2017b).
4.7.3. Other adsorbents
Selenium has drawn public attention because of its sharply toxic
characteristic at raised dosage and the long-range radiotoxicity of 79Se.
The contents of selenium in agricultural runoff, drinking water and
industrial wastewater have to be limited to 40 μg/L as the maximum
concentration. The selenium was uptake use a well-defined cationic
layered rare earth hydroxide structurally, Y2(OH)5Cl 1.5H2O. The
desorption, selectivity, isotherms and sorption kinetics of selenate and
selenite on Y2(OH)5Cl 1.5H2O were investigated systematically at pH 7
and 8.5 using a batch method (Qin et al., 2017). The maximum sorption
capacities of selenate and selenite are 124 and 207 mg/g, respectively,
both standing for the new records among inorganic sorbents. At the low
concentration region, Y2(OH)5Cl 1.5H2O can almost remove selenium
completely from aqueous solution even in the existence of competitive
anions like NO3-, Cl-, CO32-, SO42-, and HPO42-. The consequent con-
centration of selenium is less than 10 μg/L, which meet the strictest
standard well for the drinking water. After desorption, Y2(OH)5Cl

295
Y. He et al.
1.5H2O could be reused to get rid of selenate and selenite. The con-
sequences showed in this work make a confirmation that cationic
layered rare earth hydroxide is a promising and emerging material for
efficient removal of selenate and selenite and other anionic environ-
mental pollutants (Zhu et al., 2017).
Most conventional adsorbents, such as clay, silica gel, molecular
sieve, activated carbon, activated aluminum oxide and ferric oxyhydr-
oxide, have good defined adsorption capacity of Se(IV), however,
showing very weak performances in Se(VI) removal (Twidwell, 2011).
Se(IV) have a formation of an inner-sphere adsorption on ferric oxy-
hydroxides, yet Se(VI) is adsorbed in an outer-sphere adsorption
manner normally, being much weaker than the inner-sphere adsorp-
tion, resulting in less effective Se(VI) removal using common ad-
sorbents. Therefore, there is an urgent requirement to develop reusable
and efficient adsorbent materials to remove the water-borne selenium
with high removal capacity. Hydrophilic monolayer Graphene Oxide
(GO) and graphene have drawn much attention in recent years and
demonstrate promising performance to remove heavy metal ions (Jiang
et al., 2017; Kemp et al., 2013), radionuclide (Romanchuk et al., 2013),
anions (Chandra et al., 2010), oil spill-ups (Iqbal and Abdala, 2013),
organic contaminations (Liu et al., 2012), and microbial community
(Ahmed and Rodrigues, 2013).
In addition, iron oxides, such as goethite, hematite and magnetite,
have been known to be effective for selenite removal. the development
of a novel adsorbent materials for selenium removal have been stimu-
lated by the interesting surface properties of GO and iron oxide through
functionalizing the GO sheets with the magnetic iron oxide nano-
particles (Zhou et al., 2016a).
The MGO composites indicate efficient and high binding capacity
for Se(VI) and Se(IV), with removal percentage for selenate (80%) and
selenite (> 99.9%) with MGO dosage 1 g L−1 and initial concentration
of selenium of 300 ppb within a few seconds. Acidic pH boosts the
adsorption of Selenium ions on MGO as well as the removal percentage
of Se(VI) enhances to > 95% at pH 2.0 (Fu et al., 2014). Therefore, the
MGO composite has prominent removal capability of selenite and se-
lenite in water with significant potential practical applications in get-
ting rid of selenium from wastewater (Yang et al., 2011).
There is a research relates to an adsorption technique process for
treating a fluid containing selenium contaminants (Se4+ and Se6+) for
remove the fluid of the contaminant and grow a process for recovering
the adsorbent material. The method for this purification process was
made by using iron (Fe3+) oxide/hydroxide nanoparticles sol (NanoFe)
serve as an adsorbent (Liu et al., 2017b). The technique provides a cost-
effective and efficient method for selenium removal from water. A
strong effect was indicated of iron (Fe3+) oxide/hydroxide nano-
particles-based concentration and the level of pH of polluted water on
removal efficiency (Zelmanov and Semiat, 2013). The exceptional ad-
sorption characteristics of synthesized NanoFe adsorbent are demon-
strated. This technique achieved concentration of residual selenium less
than 0.01 ppm, being acceptable by water quality regulations and at
lowest 95–98% regeneration efficiency of selenium with the proposed
adsorbent (Zelmanov and Semiat, 2013; Zhou et al., 2017c). The ad-
sorption capacity of selenium on the iron(III) oxide particles at the
equilibrium concentration of 0.01 mg/L as Se is approximately one
order of magnitude higher than the values reported in the literature in
the solution. This method enables the recovery of the adsorbent
through producing concentrated selenium solution that could be
treated further to obtain selenium-containing crystals when recovering
the cleaning solution (Zelmanov and Semiat, 2013; Zhou et al., 2017c).
4.8. Coprecipitation
Several techniques can be used to decrease the selenium level in
solutions such as adsorption, ion-exchange, bioremediation, and co-
precipitation (Bleiman and Mishael, 2010; Gezer et al., 2011;
Nishimura et al., 2007; Opiso et al., 2009). Although ion-exchange
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Environmental Research 164 (2018) 288–301
resins is able to be available for the selective separation of Se(VI)or Se
(IV), an increasing concentration of competitive ions, like sulfate, sig-
nificantly reduces adsorption capability during for the ion-exchange
separation (Bleiman and Mishael, 2010; Nishimura et al., 2007). Re-
tention by adsorption on mineral surface is unstable in the long run as
well, because changes in the surrounding environment can release the
adsorbed ions back into water (Opiso et al., 2009).
Therefore, this study surveyed the immobilization of a trace element
in the mineral during crystal growth, a process called as coprecipita-
tion, to develop effective removal techniques of Se(VI) and Se(IV) from
a polluted solution (Tokunaga and Takahashi, 2017). The advantages of
the method are short treatment time, low cost, simplicity, and able to
preserve substituent ions in crystal lattice for a long time, making it
work as engineered barriers to retain various ions, including Se(VI) and
Se(IV). Previous study has been conducted to design and optimize
techniques using barite (BaSO4) for the purpose and analyzed their
efficiencies in incorporating Se(VI) and Se(IV) (Tokunaga et al., 2013a).
Barite is a common phase in numerous geological environments and can
be used to get rid of toxic and/or radioactive elements from con-
taminated waters. Barite as a sequestering phase shows following
characteristics: (i) incorporation of many elements owing to the large
ionic radii of substituted ions (Ba2+: 1.68 Å; SO42-: 1.48 Å), (ii) ex-
tremely low solubility (Prieto, 2013) (ca. Ksp = 10–9.98 at 25 °C,
1 atm), (iii) high density compared with other minerals (4.5 g/cm3),
and it is an advantage for rapid sedimentation during the coprecipita-
tion process, and (iv) high crystal stability at wide ranges of Eh, pH,
temperature, and pressure conditions (Bosbach et al., 2010;
Klinkenberg et al., 2014; Nishimura et al., 2007; Prieto et al., 2016;
Rosenberg et al., 2011a, 2011b; Tokunaga et al., 2016, 2013a, 2013b;
Widanagamage et al., 2014; Zhang et al., 2014a). Therefore, barite
works as a sequestering phase for the toxic and/or radioactive elements
removal from polluted solutions. For example, barite serves as an ideal
host mineral for Ra2+ in brine or fresh water due to the high stability
and larger incorporation of Ra2+ compared with other minerals
(Bosbach et al., 2010; Klinkenberg et al., 2014; Rosenberg et al., 2011a,
2011b).
4.9. Electrokinetics
Electrokinetic (EK) remediation is a method that already had proven
its effectiveness, especially in contaminated fine-grain soils (Mahmoodi
et al., 2013; Wang et al., 2010). A study reported that three phenomena
occurs during electrokinesis are electrophoresis, electromigration and
electro-osmosis. This technique uses a low-level direct current as
“cleaning agent”, several transport mechanisms (electrophoresis, elec-
tromigration and electroosmosis) and electrochemical reactions (elec-
trodeposition and electrolysis) are induced. The migration of non-ionic
pore fluids through electro-osmosis as well as the ionic migration of
dissolved ions happens towards the electrodes when a direct electrical
field is used across a wet mass of contaminated soil (Tabelin et al.,
2017). This method has certain advantages over the conventional
techniques: (1) it is efficient at low permeability soil and it is difficult to
treat through using other methods; (2) it is probable to set-up in situ for
sites which are impossible to excavate, like residential areas and
railway soil and (3) it can get rid of organic and inorganic pollutants
from soil simultaneously. The electro-remediation is seen as the most
effective in treating the near saturated, clay soils polluted with metals,
due to its removal is 490% (Suzuki et al., 2013). There are studies re-
ported that in sub-surface the electromigration rate rely on the density
of water current, ionic mobility, soil pore, grain size, total ionic con-
centration and concentration of contaminant. In turn, it is dominated by
advection and it is generated by electroosmotic flow and externally
used hydraulic gradients, the diffusion of acid front to the cathode as
well as the migration of anions and cations to the respective electrodes
(Singh et al., 2015).
Y. He et al. Environmental Research 164 (2018) 288–301

Table 4
Summary on the different remediation techniques for selenium.

Treatment methods Mechanism Advantages Comments

Reduction techniques Chemical reduction of Se(IV) to Se(0)
Phytoremediation Phytoextraction and phytovolatilization
Bioremediation On basis of conversion of toxic, water soluble Se
oxyanions to elemental, water insoluble Se.
Coagulation- High coagulant dosage and weakly acidic pH can
flocculation increase the formation of hydroxide flocs having
more positive adsorption sites and high zeta
potential, and so favored Se removal.
Electrocoagulation (EC) Iron (Fe) and aluminum (Al) sacrificial electrodes
were used in a batch reactor under galvanostatic
conditions.
Electrochemical Electrochemical removal of selenate by using iron
methods anode.
Coprecipitation The trace element was immobilized in the mineral
during crystal growth.
Electrokinetics The technique uses a low-level direct current as
“cleaning agent”, several transport mechanisms
(electrophoresis, electromigration and
electroosmosis) and electrochemical reactions
(electrodeposition and electrolysis) are induced.
Membrance technology Both lab-scale and full-scale membranes were
prepared at first by coating PVDF membranes with
the PAA, then, followed by ion exchange of ferrous
ions and after reduction to zero-valent iron
nanoparticles.
Chemical precipitation Using sulfide ions to precipitate selenium.
Defects on the nZVI particle shell markedly
facilitate the spread of selenium and enhance
the capacity of nZVI for selenium
sequestration.
Chinese Brake fern (a Se accumulator) can
accumulate much Se without any visible toxic
symptoms and important decrease in its
biomass.
Biofilms can both detoxify and sequester
selenium.
Many microorganisms can reduce selenite
efficiently.
Adsorption onto hydroxide flocs was the most
positive coagulation mechanism for removal
of Se and precipitation also played specific
parts at low dosage.
The best Se(0) turbidity removal can reach
97% by using iron electrodes at 200 mA.
ZVI can be applied in permeable reactive
barriers of Se for in situ remediation in
groundwater and reduce the actual risk of
exposure to selenium due to non-mobility.
The methods are short treatment time, low
cost, simplicity, and able to preserve
substituent ions in crystal lattice for a long
time.
It is efficient at low permeability soil.
It is probable to set-up in situ for sites which
are impossible to excavate, like residential
areas and railway soil.
It can get rid of organic and inorganic
pollutants from soil simultaneously.
The membrane prevents particle aggregation
and dissolution.
Selenious ions can be precipitated from weak
acidic solutions effectively using sodium
sulfide.
In the region of complete precipitation, the
selenium and sulfur atoms form a solid
solution.
Increasing research shows that nZVI can treat
and remove selenium effectively.
Phytoremediation is an effective and feasible
approach to get rid of Se from Se-contaminated
environment.
Phytoremediation is an effective and feasible
approach to get rid of Se from Se-contaminated
environment.
Biofilms, or communities of microorganisms,
occupy significant status in biotransforming
elements into less toxic chemical forms.
Se(IV) removal efficiency of over 98% could be
achieved.
Fe-based coagulants were much more efficient
than the Al-based coagulants in Se removal.
The use of Fe electrodes as soluble anode in
electrocoagulation constitutes a better option
than Al electrodes for the electrochemical
sedimentation of colloidal Se(0).
This electrochemical system can be applied to
both oxic and anoxic system to remove selenite
and effective to reduce and remove selenate from
water environment.
Barite serves as an ideal host mineral for Ra2+ in
brine or fresh water due to the high stability and
larger incorporation of Ra2+ compared with
other minerals.
The electro-remediation is seen as the most
effective in treating the near saturated, clay soils
polluted with metals.
Integration of the nanofiltration (NF) and iron-
functionalized membranes achieves the selenium
concentration below 10 µg/L.
Selenious ions can be precipitated from weak
acidic solutions effectively using sodium sulfide.
In the region of complete precipitation, the
selenium and sulfur atoms form a solid solution.

4.10. Membrance technology solved by integration of the nanofiltration (NF) and iron-functionalized
membranes, and concentration of selenium below 10 µg/L was
The remediation of toxic metals from water environment with high achieved (Gui et al., 2015).
concentrations of salt has been a rising area for membrane separation.
Cost-effective nanomaterials like iron and iron oxide nanoparticles have
4.11. Chemical precipitation
been used in reductive and oxidative degradation of toxic organics
widely. Similar procedures are able to be used for redox transforma-
Sulfur dioxide is used in industry commonly to precipitate and get
tions of the metal species (e.g., metal oxyanions to the elemental
rid of selenious ions from aqueous solution. The literature showed that
metal), and/or adsorption of species on surface of iron oxide (Ilgen
when coping with hot and relatively concentrated hydrochloric or
et al., 2017). In this research, iron-functionalized membranes were
sulfuric (> 1 g/L of soluble Se) acid solutions (above 80 °C and pH
developed for reduction as well as adsorption of selenium from the coal-
below 1.0), full selenium reduction to elemental state exists very ra-
fired power plant scrubber water. Iron-functionalized membranes have
pidly (Geoffroy and Demopoulos, 2011). However, when working with
certain advantages over iron suspension because the membrane pre-
Se(IV) of lower concentration dissolved in room temperature solutions,
vents particle aggregation and dissolution. Both lab-scale and full-scale
like those encountered in the zinc industry, the decrease of Se(IV) with
membranes were prepared at first by coating polyvinylidene fluoride
SO2 gets too slow to be of practical interest. As mentioned earlier
(PVDF) membranes with the polyacrylic acid (PAA), then, followed by
several other reagents have been discovered to reduce selenious ions to
ion exchange of ferrous ions and after reduction to zero-valent iron
elemental state. Sodium dithionite is one of those that has found in-
nanoparticles. Water permeability of membranes reduced as the percent
dustrial application as described otherwhere albeit with its own
PAA functionalization boosted, and the highest ion exchange capacity
drawbacks, like high cost, relatively poor efficiency and subsequent
was acquired at 20% PAA with the highly pH responsive pores. High
redissolution of the selenium (Mishra et al., 2011). There is a work
concentrations of chloride and sulfate in scrubber water reduced the
describe that the removal of selenium(IV) by sodium sulfide. The pre-
reaction rate of selenium reduction, however, this was indicated to be
cipitation of selenium using sulfide ions is not a new system because it

297
Y. He et al.
has been mentioned almost two centuries ago initially. In spite of this
long history, its chemistry remains poorly understood and away from
being optimized, especially as far it focuses its use in industrial effluent
treatment.
Selenious ions are able to be precipitated from weak acidic solutions
effectively using sodium sulfide. Below a pH of about 7.0 and the sul-
fide/selenium molar ratio of 1.7–11, after 10 min at ambient tem-
perature the precipitation reaction goes to only 0.005 mg/L completely
of soluble selenium remaining in solution. If the pH was allowed to go
up between 7.0 and 9.5 the selenium precipitation was incomplete
while pH above 9.5 the solution became dark red and was determined
to contain the colloidal selenium (Geoffroy and Demopoulos, 2011;
Mishra et al., 2011). The latter transforms to crystalline selenium ag-
gregates on acidification (terminal pH < 7.0). The reaction involved
oxidation of sulfide and reduction of selenium to their respective ele-
mental states. In the region of complete precipitation :1.7 < S/Se <
11 and 1.7 < pH < 7.0, the selenium and sulfur atoms form a solid
solution seemingly consisting of sulfur–selenium ring molecules which
have the SenS8-n formula, with n = 2.5–3.0. Elevation of pH above 7.0
results in a breakdown of the SenS8-n solid solution structure and forms
the individual elemental and selenium colloidal particles. The sele-
nium–sulfur solid solution phase was discovered to be stable
(< 0.005 mg/L Se) extremely when subjected to more than 60-day
leachability test at pH 7.0. Secondary sulfur formation occurs following
the precipitation of SenS8-n by the decomposition of the excess sulfide
(Geoffroy and Demopoulos, 2011).
5. Conclusion and knowledge gaps
A considerable amount of selenium contaminated wastewater is
generated. Therefore, the only effective option to decrease health ha-
zard for human is the treatment of selenium contamination. To achieve
this goal, various methods are being applied. Table 4 provides an
overview of main features of these treatment processes. However, some
of those have certain flaws. Thus, for curb environmental pollution
better, new methods with the options of new hybrid technologies are
required urgently. Among those techniques, adsorption is seemed to be
more effective for remediation of selenium contamination. However,
further study is required to develop more suitable and efficient tech-
niques without drawbacks. Below the knowledge gaps, we need to ex-
plore constantly. It is noted that there exist some aspects require at-
tentions and make the efforts, while additional gaps not included
hereinafter also need research.
Gap1: Coagulation, ion exchange, electrocoagulation, biological and
chemical reduction and so on are methods of removal selenium that
have been used currently. These approaches are able to remove sele-
nium to below 5 µg/L in optimal conditions (Hasan and Ranjan, 2010).
However, incomplete technologies and expensive processing methods
have restricted development of selenium contamination remediation.
When large areas of soils are polluted, traditional treatments of metal
contamination in soils are extremely expensive. According to USDA and
NRCS, treatments, including washing process, the use of solidification
agents, and high-temperature treatments can be performed either in
situ or ex situ, however, they are prohibitively expensive. Thus, cost is a
prominent problem we need to solve at present.
Gap2: Biosorption has obtained important credibility during recent
decades because it is a low-cost domestic technique for remediating, has
excellent performances, and is also eco-friendly in nature, which pro-
mises to be an excellent method to remove selenium from water. While
literature survey suggested that most of studies on the selenium sorp-
tion have been confined to batch equilibrium studies, the possible
reason for the restriction is mainly because of the unavailability of bulk
quantity of biomass, and batch operations apply in the laboratory study
easily, but less convenient for field applications (Hasan et al., 2010).
Moreover, there still exists a great challenge in developing low-cost
biosorbents for removal of selenium with high uptake efficiency (Hasan
298
Environmental Research 164 (2018) 288–301
and Ranjan, 2010).
Gap3: Phytoremediation is an effective technology for selenium
removal, the selection of plant species that are crucial in selenium ac-
cumulation is of primary significance. However, the uses of Se-accu-
mulating plants are restricted because of their slow growth and un-
defined growth requirements and low biomass (Esringü and Turan,
2012). Some plants, however, called selenium hyperaccumulators,
discovered in Se-rich areas of the USA can accumulate selenium no less
than 0.5% of their dry weight (Zhang et al., 2007). Over 400 species of
plants have been showed to be the hyperaccumulators of elements like
Ni, Cd, Co, and Se (Raskin and Ensley, 2000). In spite of their high
capacity to accumulate selenium, the hyperaccumulator plants so far
have not been used for phytoremediation due to their generally slow
growth rates.
Gap4: The process of removing selenium in various ways has certain
flaws such as their by-products might be a further potential source for
secondary selenium pollution. Besides, the use of toxic chemicals, and
sludge generation severely limit their wide application (Bleiman and
Mishael, 2010; Hu et al., 2006; Sharma et al., 2009; Tan et al., 2003).
Gap5: In adsorption, the focus of considerable research has recently
shifted to n-Fe2O3 because of the concentration of adsorption sites and
the higher surface area (Yamani et al., 2014). The primary flaw of n-
Fe2O3 is difficult to synthesize a uniform material for which perfor-
mance is able to be predicted accurately because the morphological
characteristics and crystalline of each synthesis are dependent on the
method used highly (Carbajal-Franco et al., 2013). Furthermore, a
comprehensive study for selenium and the varieties of forms of n-Fe2O3
has not to be completed yet as the field is in its infancy (Ritter et al.,
2013).
Gap6: To protect ecological and human health within a context of
ecosystem sustainability is a primary goal of environmental manage-
ment (Burger et al., 2012). There maybe is no chemical contaminant for
which there are more contradictions about ecological risks in aquatic
environments than selenium. The adverse effect on policy is indicated
by huge differences in regulations among jurisdictions and environ-
ments. In Europe, selenium is not considered an ecological threat. It is
not listed in chemicals of concern in the European Commission's Dan-
gerous Substance Directive. Nor is it among the 41 chemicals for which
Environmental Quality Standards are applicable (Förstner, 2007). Al-
though revisions are being proposed, U.S. selenium guidelines for
marine waters allow a maximum concentration of 300 µg/L and a
continuous concentration of 71 µg/L (Luoma and Presser, 2009). In
contrast, Canada's marine and freshwater guidelines are 2 µg/L and the
EPA's freshwater criterion is 5 µg/L (Luoma and Presser, 2009). Redu-
cing such disparities and internationally harmonizing management of
ecological risks from selenium is significant. The costs of managing
selenium risks may increase where regulations are not based on con-
vincing scientific evidence (Li et al., 2010). There is also a possibility
that selenium problem will grow in future years with the exploitation of
coal and similar fossil fuels, mining of phosphate ore, and irrigation in
semiarid regions. Thus, it is significant to establish a globally consistent
regulatory approach to selenium.
Acknowledgments
The study was financially supported by the National Natural Science
Foundation of China (51709103), the National Program for Support of
Top-Notch Young Professionals of China (2012), the Program for New
Century Excellent Talents in University from the Ministry of Education
of China (NCET-11-0129), Project of Science and Technology of Hunan
Province (2015WK3016 and 2016WK2010).
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