Journal of Environmental Management 162 (2015) 306e325

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Journal of Environmental Management

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Review

Arsenic and uoride contaminated groundwaters: A review of current

technologies for contaminants removal
Sachin V. Jadhav a, Eugenio Bringas b, Ganapati D. Yadav a, *, Virendra K. Rathod a,
Inmaculada Ortiz b, Kumudini V. Marathe a
a
Department of Chemical Engineering, Institute of Chemical Technology, Nathalal Parekh Marg, Matunga, Mumbai, 400019, India
b
Department of Chemical and Biomolecular Engineering, Universidad de Cantabria, Avda, Los Castros s/n. 39005, Santander, Spain

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

Article history: Chronic contamination of groundwaters by both arsenic (As) and uoride (F) is frequently observed
Received 23 November 2014 around the world, which has severely affected millions of people. Fluoride and As are introduced into
Received in revised form groundwaters by several sources such as watererock interactions, anthropogenic activities, and
26 June 2015
groundwater recharge. Coexistence of these pollutants can have adverse effects due to synergistic and/or
Accepted 7 July 2015
antagonistic mechanisms leading to uncertain and complicated health effects, including cancer. Many
Available online 8 August 2015
developing countries are beset with the problem of F and As laden waters, with no affordable tech-
nologies to provide clean water supply. The technologies available for the simultaneous removal are akin
Keywords:
Fluoride
to chemical treatment, adsorption and membrane processes. However, the presence of competing ions
Arsenic such as phosphate, silicate, nitrate, chloride, carbonate, and sulfate affect the removal efciency. Highly
Membrane efcient, low-cost and sustainable technology which could be used by rural populations is of utmost
Adsorption importance for simultaneous removal of both pollutants. This can be realized by using readily available
Electrocoagulation low cost materials coupled with proper disposal units. Synthesis of inexpensive and highly selective
Ion exchange, Contaminant removal nanoadsorbents or nanofunctionalized membranes is required along with encapsulation units to isolate
the toxicant loaded materials to avoid their re-entry in aquifers. A vast number of reviews have been
published periodically on removal of As or F alone. However, there is a dearth of literature on the
simultaneous removal of both. This review critically analyzes this important issue and considers stra-
tegies for their removal and safe disposal.
2015 Elsevier Ltd. All rights reserved.

1. Introduction potable purposes by over 50% of the global population. Thus,

Water is not only an essential component for life but also a basic
building block to maintain quality of life. Water scarcity has already
revealed adverse effects on all populations in every continent. More
recently, UNICEF and WHO reports have conrmed that 748 million
people do not have adequate and safe water resource and over 2.5
billion people have access to meagre water supply. The WHO also
estimates that 1.8 billion people use faecally contaminated source
of drinking water (UNICEF/WHO, 2014). Groundwater is used for
Abbreviations: WHO, World Health Organization; USEPA, United States Envi-
ronmental Protection Act; CPC, chemical precipitation/coagulation; EC, electro-
coagulation; EF, electrocoagulation/otation; AD, adsorption; IE, ion exchange; MT,
membrane technology; RO, reverse osmosis; FO, forward osmosis; NF, nano-
ltration; ED, electrodialysis.
* Corresponding author.
E-mail addresses: gdyadav@yahoo.com, gd.yadav@ictmumbai.edu.in
(G.D. Yadav).
groundwater is sometimes described as the hidden sea. This is
indeed true to a greater extent in countries like India where local
supply to ~80% rural and ~50% urban dwellings is provided by
groundwater sources alone (Ayoob et al., 2008).
Presence of several naturally occurring, anthropogenic and in-
dustry generated ions such as uoride, arsenic, nitrate, sulfate, iron,
manganese, chloride, selenium, heavy metals, and radioactive
materials may greatly compromise water quality, leading to health
problems. The most signicant inorganic pollutants in groundwater
affecting human health at the global scale, according to the WHO,
are arsenic and uoride (Thompson et al., 2007). In this context,
uoride pollution of drinking water receives much less consider-
ation than arsenic.
1.1. Health effects of single and combined As and F
Fluoride is the only chemical in potable water that can cause

http://dx.doi.org/10.1016/j.jenvman.2015.07.020
0301-4797/ 2015 Elsevier Ltd. All rights reserved.
 S.V. Jadhav et al. / Journal of Environmental Management 162 (2015) 306e325
different health effects depending upon its concentration in dis-
solved form. A very small amount of uoride is benecial for bone
and teeth development and dental health. However, concentrations
higher than 1.5 mg/L are damaging to human health, causing dental
or skeletal uorosis (Miretzky and Cirelli, 2011). Children below 12
years are likely to be most exposed to uorosis as their body tissues
continue to grow during the formative age. Moreover, uorosis is
non-reversible and the disorder has no medical treatment. The
WHO permits a uoride concentration of 0.5e1 mg/L in drinking
water (WHO, 2011). Efuent limit of 4 mg/L for F from the waste-
water treatment facilities has been set by USEPA (Shen et al., 2003).
Fig. 1 depicts the statistics on population exposed to F contamina-
tion. Clearly, China and India are the most affected countries where
nearly 35 and 26 million, respectively, people are at uoride risk.
As for arsenic, As(V) (arsenate) and As(III) (arsenite) are the
most predominant valence states, which are found in aerobic sur-
face waters and anaerobic groundwaters, respectively. Between pH
4 and 10, major As(III) compound is charge neutral, whereas As(V)
species exists as charge negative. The occurrence of As in ground-
water poses even a greater danger than F hazards due to its extreme
toxicity at low concentration which goes undetected especially in
As(III) form (Camacho et al., 2011). Arsenic is well known for its
carcinogenicity in kidney, lung, liver, skin, and bladder. At high
concentrations, As causes gastrointestinal problems and arsen-
icosis, which arise mainly via consumption of water containing As
and its subsequent accumulation in the body (Sharma and Sohn,
2009; Villaescusa and Bollinger, 2008). Therefore, the WHO rec-
ommends As concentration of 10 mg/L as the upper permissible
limit in water (WHO, 2011). This limit is applicable in India, Japan
Taiwan, USA and Vietnam (Hug et al., 2008; Reddy and Roth, 2013)
while other countries like China, Bangladesh, and most of South
American nations have permitted a higher concentration of 50 mg/L
(Camacho et al., 2011; Chakraborti et al., 2010). A report prepared
by UNICEF consultant Ravenscroft (2007) estimates that natural As
pollution of groundwater and surface water affects more than 140
million people in at least 70 countries worldwide. A large popula-
tion of South Asia is exposed to As toxicity (Fig. 2).
When two different types of harmful contaminants are
Fig. 1. Estimated population exposed to F contamination in selected countries (
103) (CDC, 1993; Diaz-Barriga et al., 1997; Fewtrell et al., 2006). * no recent data available.
307
ingested, they may function independently or synergistically or
antagonistically to one another (Chouhan and Flora, 2010). While
the harmful effects of As and F individually have been widely
studied, the exposure to both together has received little atten-
tion. Rao and Tiwari (2006) reported that As and F in combina-
tion affect integrity of cells genetic material more than the
individual exposure. In animal studies for rats, co-exposure of As
and F even at low concentrations resulted in decreased comet tail
and detrimental effect on liver and kidney (Flora et al., 2009;
Mittal and Flora, 2006). Wang et al. (2007) reported that chil-
dren's growth and intelligence were severely inuenced by high
concentrations of As or F. Hence, it is important to remove these
toxicants from potable water. Despite the extreme seriousness of
the issue, very less data exist on the populations facing simul-
taneous toxicity of As and F.
This article analyzes the genesis of the combined presence of
geogenic uoride and arsenic in groundwater and drinking water as
well as the treatment methods for their removal. Also, it reviews
the effectiveness of several treatment methods when these two
contaminants are present together.
2. Occurrence of F and As in groundwaters
There is an evidence of the presence of uoride in different
latitudes such as south-east of Africa, United States, the Middle East
of Asia, South America, and Asian countries. However, China and
India are the worst affected countries (Fig. S-1, supplementary
information).
For past few decades, the areas with arid and semi-arid climates
are suffering from the scarcity of water due to the fact that the
uptake of groundwater is in far excess than water recharge as well
as excessive evaporation leading to decreased availability of water
(Jakariya et al., 2003, 2007). Since uoride primarily originates from
uoride rich rocks, concentrations of uoride are directly propor-
tional to the extent of leaching/dissolution of crystalline minerals
through watererock interactions. The sources of uoride in
groundwater through uoride-rich rocks are (i) urospar (CaF2)
from lime stones, sand stone, sedimentary rocks; (ii) cryolite
308 S.V. Jadhav et al. / Journal of Environmental Management 162 (2015) 306e325
Fig. 2. Estimated population exposed to As contamination in selected countries (
103) (Ravenscroft, 2007).
(Na3AlF6) from igneous rocks, granite; (iii) uorapatite (Ca5(PO4)3F)
from igneous rocks, metamorphic rocks, and (iv) sellaite (MgF2)
from bituminous dolomiteeanhydrite rock.
Arsenic occurs in the environment in several oxidation states as
stated earlier. Parsa and Shahidi (2010) stated that unusual large
proportions of As are present in potentially soluble forms. Studies
have shown that over exploitation of shallow (or main) aquifer has
been the source of many arsenic problems (Jakariya and
Bhattacharya, 2007). Fig. S-2 (supplementary information) shows
the identied regions of world having arsenic contamination of
groundwaters. Very high concentrations of As can be seen pre-
dominant in Mexico, USA, China, Bangladesh, Vietnam and
Pakistan. Recently, groundwaters in Japan and Korea were also
found to be contaminated with As (Ahn, 2012; Yoshizuka et al.,
2010). The major mechanism responsible for the As contamina-
tion in groundwater is desorption from iron oxides or hydroxides
from natural rocks and their reductive dissolution (Kim et al., 2012;
Li et al., 2012).
Fig. S-3 (supplementary information) shows the co-occurrence
of uoride and arsenic worldwide. Arsenic and F are found to co-
exist in groundwaters in China, Argentina, Mexico, and Pakistan
among other countries where As concentrations up to 5300 mg/L
and F up to 29 mg/L are noticed in the same groundwaters (Jing
et al., 2012). Recently, Australia, Japan, Korea, and Chile have also
been shown with elevated levels of As and F co-occurrence (Fig. S-3,
supplementary information) (Ahn, 2012; Chakraborti et al., 2011;
Fernandez-Turiel et al., 2005; Richards et al., 2009; Yoshizuka
et al., 2010). Table S-1 (supplementary information) presents
detailed information on As and F co-contamination in groundwa-
ters with respect to geographical location and lists key ndings of
various publications.
Arsenic is found to be frequently associated with uoride in
shallow aquifers around the world. A high concentration of As is
also found in semi-arid regions that contain oxidized groundwater
(Currell et al., 2011). The correlations between these two toxicants
are dissimilar as per redox potential (Kim et al., 2012). The Fe-
hydroxides adsorption capacity of F and As decreases with in-
crease in pH, releasing both components into groundwater indi-
cating that the Fe-(hydr)oxides play an important role for hosting
the co-contamination (Streat et al., 2008). High concentrations of
As (10e5300 mg/L) and F (51e7340 mg/L) are reported in shallow
groundwaters, indicating potential risk of arsenicosis and uorosis
in Chaco-Pampean plain of Argentina where As and F borne dis-
eases affect ~2e8 million people (Nicolli et al., 2012). The concur-
rent presence of As and F in groundwater is connected to volcanic
eruptions, geothermal currents and mining activities (Alarcon-
Herrera et al., 2013).
Selected data on As and F levels in waters from around the world
are presented in Table 1. Excessive rates of evaporation in arid and
semi-arid regions lead to generation of saline groundwaters and
alkaline pH, which are related to high concentrations of As and F in
groundwater (Nicolli et al., 2008a, 2008b). Presence of Na and
HCO 3 are also correlated with simultaneous presence of high
concentrations of As and F. On the other hand, studies in Yuncheng
Basin, northern China, have found a moderately positive correlation
between pH and As and F concentrations indicating that high pH
may favor desorption of F and As, while HCO 3 may act as a sorption
competitor (Currell et al., 2011). These authors also have found a
strong correlation between As and F, suggesting that the enrich-
ment of As and F is governed by a common mechanism and/or due
to a set of aquifer conditions.
The sediment geochemical data of 2046 samples from northern
Mexico were generated by Alarcon-Herrera et al. (2013). The region
is surrounded by large basins lled with alluvium, and dominated
by a large number of wells. A strong correlation between As and F
was observed in these localities where As has been reported in high
amounts indicating co-occurrences of As and F. Nicolli et al. (2008b)
have found a strong link between F and As concentration in deep
wells in Cordoba province, Argentina.
3. Methodologies for toxicant removal from groundwaters
3.1. Fluoride removal
Basically, deuoridation of water can be introduced at two
organizational levels; as household deuoridation, carried out by
individual households for their own water consumption, and as
community deuoridation, carried out at village, town, sub-urban
area levels. As it has been previously reported in the reviews of
Ayoob et al. (2008) and Mohapatra et al. (2009), many technologies
 S.V. Jadhav et al. / Journal of Environmental Management 162 (2015) 306e325 309

Table 1
Data on groundwaters containing As and F.

Parameter Geographical location

Zhijiliang, Inner Meoqui City, Kalalanwala and Un-known site, Kyushu, Japan Chihuahua, Geumsan Santiago del Estero
Mongolia, China Chihuahua, Kot Asadullah, India 16 sites Mexico County, Province, Argentina
Mexico Pakistan Korea
2 sites 2 depths Min. and
Max.

pH 7.57 7.2 7.4 8 7.55 7.2 2.8-8.5 7.17 5.78 8.68 6.4-9.3
Temperature,  C 13 e e 25 2 25 2 20.5 e 25 12 23 e
Arsenic, mg/L 1.10 0.134 0.075 0.235 0.06 0.13 0.01e3.23 0.435 e 113 0.01-15
Fluoride, mg/L 1.59 5.9 4.8 11 1.47 5 0.04e3.76 11.8 e 7.54 0.7-22
Sodium, mg/L 119 e e 630 273 e 1.1e1501 250 1.64 66.8 e
Carbonate, mg/L 10 121 126 857 410 e e e 8.64 239 e
Turbidity, NTU 311 1.4 1.1 e e 320 e 1 e e e
Hardness, mg/L 51.5 24.5 58.3 e e e e e e e e

Reference Zhang et al. Pinon- Farooqui et al. Devi et al. Yoshizuka et al. Nevarez et al. Ahn Bhattacharya et al.
Miramontes
et al.

Year 2003 2003 2007 2008 2010 2011 2012 2006

have been employed and are currently being used to carry out the F
removal from potable water such as ion exchange (Chubar, 2011),
adsorption (Bhatnagar et al., 2011; Gong et al., 2012a), coagulation
and electrocoagulation (Behbahani et al., 2011; Gong et al., 2012b),
and membrane processes (Richards et al., 2010). Each of these
technologies has its own merits and demerits. Fig. 3 presents a
typical initial concentration range treatable by a particular tech-
nology and its corresponding removal efciency. It can be seen that
chemical treatment is capable of treating very high concentrations
of F; since it cannot bring F concentration within WHO permissible
limit, it can be coupled with other technologies as a primary
treatment method (Islam and Patel, 2007). This approach offers
advantage of better life expectancy of secondary or tertiary treat-
ment due to reduced load.
3.1.1. Chemical precipitation/coagulation (CPC)
The roots of the deuoridation processes can be traced to the
early 1930's since when researchers from all around the world have
been trying to develop a sustainable cost effective technology to
reduce F concentrations in water. CSIR-NEERI in Nagpur, India,
developed the Nalgonda process for the deuoridation of drinking
water. The technique has been operated in a number of villages in
India as ll and draw type and hand-pump attached plants
(Meenakshi and Maheshwari, 2006).
Chemical precipitation technique involves addition of
aluminum salts along with lime to the F rich water followed by
occulation and sedimentation or ltration. In the rst step, lime
reacts with F impurities such as NaF, HF, etc. to form insoluble
calcium uoride.
Ca(OH)2 2F/CaF2 2OH (1)
Ca(OH)2 (aq) 2NaF (aq) / CaF2 (s) 2NaOH (aq) (2)
Essentially, in the second step, aluminum sulfate or aluminum
chloride or both together, is added. Aluminum salt acts as a

Fig. 3. Fluoride removal performance of various technologies. Where, CPC-11 Reardon and Wang (2000); CPC AD-12 Islam and Patel (2007); EC EF-13 Zuo et al. (2008);
EC/EF-14 Bennajah et al. (2009); EC-15 Khatibikamal et al. (2010); AD-16 Cengeloglu et al. (2002); AD-17 Tripathy et al. (2006); AD-18 Tripathy and Raichur (2008); AD-
19 Thakre et al. (2010); AD-110 Ganvir and Das (2011); IE-111 Solangi et al. (2009); IE-112 Viswanathan and Meenakshi (2009); RO-113, NF-113 Kettunen and Keskitalo
(2000); RO-114, NF-114 Dolar et al. (2011); ED-115 Zeni et al. (2005); ED-116 Ergun et al. (2008).
310 S.V. Jadhav et al. / Journal of Environmental Management 162 (2015) 306e325
coagulant and is often being used for viable and effective F removal
from water. The basicity present in water with alum yields an
aluminum salt, [Al(OH)3], which is insoluble.
It has been reported that the pH of the contaminated water
increases up to 12; however, the best F removal is achieved be-
tween the pH range of 6e7 (Aoudj et al., 2012). The dose of alum is
typically around 20 fold the lime required. The uoride from
groundwater can be removed upto 96% from the initial concen-
tration of 109 mg/L using lime (Reardon and Wang, 2000). Similar
ndings on F removal by calcium salts have been conrmed by
Jadhav et al. (2014).
The Nalgonda technique has the advantages of low initial cost
and effectiveness. However, Nalgonda technique is not recom-
mended owing to high maintenance cost, unpleasant water taste,
requirement of large area for sludge drying, and a very high residual
aluminum (Liu et al., 2013). The residual aluminum in waters
ranges from 2.01 to 6.86 mg/L under different operating conditions.
Any amount over 0.2 mg/L of aluminum in drinking water can cause
serious health problems, including dementia (Shrivastava and Vani,
2009).
3.1.1.1. Electrocoagulation (EC) and electrocoagulation/otation (EF)
Passage of an electric current into an aqueous medium helps to
destabilize suspended, dissolved and emulsied impurities, and the
process is known as electrocoagulation (EC). During the past
decade, the use of electrocoagulation (EC) as well as electro-
coagulation/otation (EF) process is on the rise. It can be effectively
employed to treat oily wastewaters, dye and textile industry ef-
uents and removal of organic matter, heavy metals and uoride
(Hu et al., 2003, 2005). EC is advantageous since no impurities are
introduced and useful contents existing in raw water can be
retained during deuoridation.
Electrochemical cell (also known as electrolytic cell) is the
basis of electrocoagulation and electrootation techniques. An
electrocoagulation reactor typically consists of an electrolytic cell
with an anode and a cathode. Passage of the electric current leads
to the deterioration of the anode and cathode which may be made
of the same or different materials and which act as sacricial
electrodes (Mollah et al., 2001). It is reported that the following
three routes are adapted for the electrocoagulation/otation tech-
niques, namely, (i) electrode oxidation, (ii) generation of gas bub-
ble, (iii) otation and sedimentation of ocs (Emamjomeh and
Sivakumar, 2009).
Electrocoagulation deals with electrochemical production of
destabilization agents that lead to neutralization of electric charge
to remove pollutants. Charged particles coagulate together to make
a mass. Effective removal of pollutants by otation and sedimen-
tation is augmented by metal based coagulants having a similar
effect as the metal cations produced by anode. The key reactions are
as follows (Zuo et al., 2008):
Al / Al3 3e at the anode (3)
Al3 3H2O / Al(OH)3 3H (4)
Al(OH)3 xF / Al(OH)3xFx xOH (5)
2H2O 2e / H2 2OH at the cathode (6)
Evolution of hydrogen bubbles at the cathode improves the F
ion mass transfer rates and also leads to oating of the aluminum
complex (Al(OH)3xFx) ocs at the top of the electrocoagulation
system. Effective F removal can be achieved by isolating the
aluminum complex from the aqueous phase periodically. There-
fore, formation of aluminum complex [Al(OH)3xFx] results in the
deuoridation of the source waters. Developments during the
past decade have demonstrated that EC is an effective technique
for F removal in drinking waters and industrial wastewaters
(Abuzaid et al., 2002; Essadki et al., 2009; Han and Kwon, 2002;
Holt et al., 2002; Khatibikamal et al., 2010; Mameri et al., 2001).
It has been reported that by using EC, uoride concentrations
could be reduced to values lower than 1.5 mg/L from initial con-
centrations ranging from 10 to 20 mg/L (Bennajah et al., 2009).
Another advantage is that EC processes are characterized by lower
amount of sludge and absence of chemical handling. However,
electricity is required to operate the plant which increases its
operating cost.
3.1.2. Adsorption (AD)
Amongst other methods, adsorption (AD) is a conventional
technique which is widely used for deuoridation of water because
it is economical, robust, environmentally benign and efcient. New
advanced materials have been developed recently for effective and
cheap uoride removal from potable water. Many low cost adsor-
bents have also been employed for uoride removal like alumina,
red mud, clays, soils, activated carbon, calcite, brick powder, acti-
vated coconut-shell, activated kaolinites, oxides ores, modied
chitosan, bone char, and some other low cost materials (Mohapatra
et al., 2009).
A common mechanism by which the adsorption of F ions
occurs onto solid particles can be given by the following three
steps: (i) mass transfer of F ions to the external surface of
the adsorbent, (ii) F ion adsorption onto external particle surface,
and (iii) intra-particle diffusion of F ions from the exterior surface
and possible exchange with elements on the pore surface
inside particles (Fan et al., 2003). Activated alumina happens to
be one of the most popular and widely used solid adsorbents
for the deuoridation of potable water and many reports are
available on large-scale installations (Chauhan et al., 2007).
Alumina is popular amongst other adsorbents because it main-
tains its structural stability without shrinkage, swelling or
disintegration in water (Serbezov et al., 2011). Granules of acti-
vated alumina having a very high surface area of ~200e300 m2/g
possess a substantial number of active sites to facilitate adsorp-
tion. At rst, the acidication of alumina is carried out with HCl
as follows:
Alumina H2O HCl / Alumina HCl H2O (7)
( represents activated state)
The acidic alumina on contact with F ions displaces the Cl ions
and gets bonded to alumina.
AluminaHCl NaF / AluminaHF NaCl (8)
Further, regeneration is carried out by rst treating the adsor-
bent with alkaline solution followed by acid wash. A few reports
mention that F removal is due to ion-exchange as well as adsorp-
tion following both Freundlich and Langmuir isotherms (Bansiwal
et al., 2010; Ghorai and Pant, 2005).
Meenakshi and Maheshwari (2006) have reported the devel-
opment of domestic and hand-pump units with activated alumina
for deuoridation. The unit consists of ~20 L capacity bucket, tted
with a micro-lter at the bottom containing 5 kg of activated
alumina. Activated alumina coated with manganese dioxide was
found to reduce F concentration to 0.2 mg/L from 10 mg/L at pH 5.5
(Tripathy and Raichur, 2008). Magnesia-modied activated
alumina granules were also used successfully to reduce F from
drinking water with a maximum adsorption capacity of 10.12 mg/g
at F concentration of about 150 mg/L (Maliyekkal et al., 2008).
 S.V. Jadhav et al. / Journal of Environmental Management 162 (2015) 306e325
Biswas et al. (2009) characterized the synthetic hydrated iron (III)e
tin(IV) mixed oxide (HITMO) for F removal. It was found that the F
adsorption capacity decreased with increasing initial pH from 3.0 to
5.0, and it remained constant up to pH of 7.5. Also, the high bicar-
bonate content showed adverse effects on F removal by HITMO. It
was the pseudo-second order kinetics with multiple-stage which
dened rate-limiting step. The equilibrium data was best portrayed
by Langmuir isotherm model with adsorption capacity 10.50 mg/g
and adsorption energy ~9 kJ/mol. The uoride-rich material was
successfully regenerated up to 75% in desorption studies.
All in all, the choice of the adsorbent seems to be reliant on
factors such as the ability to adsorb from dilute solutions, pH,
removal duration, adsorbent stability, regeneration, and adsorption
capacity in the presence of competing ions, and the economics
(Mohapatra et al., 2009). The main disadvantage of the adsorption
process is that the adsorbent gets exhausted soon and considerable
time is required for regeneration. Moreover, regeneration steps
leads to secondary pollution because F containing aqueous solution
is discarded as a waste.
3.1.3. Ion exchange (IE)
Many reports have highlighted the efcacy of ion exchange with
other techniques (Onyango et al., 2005, 2006). Usually, ion ex-
change technique removes F by adsorption rather than exchanging
ions. The fundamental reason is that the uoride concentration is
comparably lower than other ions present in water. Cation ex-
change resins are more selective for F removal than anion exchange
resins (Meenakshi and Viswanathan, 2007). However, the
deuoridation capacity and selectivity for F is dependent on the
type of resin. The loading of metal ions inuences the uoride
removal drastically, owing to variations in their properties (Luo and
Inoue, 2004). Thus, it is difcult to maximize the deuoridation
capacity (DC) of ion exchange resins while simultaneously
enhancing the F selectivity.
Viswanathan and Meenakshi (2008) used a widely available ion
exchanger Indion FR 10 that has considerable F removal capabil-
ities. It was chemically altered with Ce3, Fe3, La3, and Zr4
species to understand their selectivity for deuoridation. The
maximum deuoridation capacity of all the modied resins was
measured around 0.5 mg/g. The authors pointed out that the
deuoridation was due to electrostatic adsorption and complexa-
tion. Recently, they have modied Indion FR 10 into Na and Al3
types by loading the metal ions in H type of resin (Viswanathan
and Meenakshi, 2009).
Chubar et al. (2005) obtained a new ion exchanger from double
hydrous oxide (Fe2O3$Al2O3$xH2O) by the solegel method from
easily available raw materials, which was used for adsorption of F,
Cl, Br, and BrO3 simultaneously. It was found that the pH effect of
F and Br was dependent on ion speciation. Sufcient capacity for
sorption of all these anions was in the pH range of 3e10. The F
adsorption of 88 mg/g was the highest among all species. Solangi
et al. (2009) modied anionic resin Amberlite XAD-4, in which
the amino group is introduced to the aromatic ring of the resin and
utilized effectively for F extraction. They found that the modied
resin was efcient particularly at pH 9 and was also effective in the
presence of other anions such as Br, NO   2
2 , NO3 , HCO3 and SO4 .
Subsequently, the authors modied Amberlite XAD-4 resin by
adding thio-urea binding sites into the aromatic rings (Solangi
et al., 2010). The modied resin had high efciency for F removal
from aqueous solution at a wide range of pH from 4 to 10. The resin
could be regenerated several times and used as an ion exchange
material in lters for F removal from potable water.
Ion exchange treatment has a great F removal potential (up to
95%). However, the resins are costly , thereby making the entire ion
exchange method expensive. Regenerating the resins is simple but
311
it generates a large volume of F loaded waste which again is a
problem.
3.1.4. Membrane technology (MT)
In recent years, membrane-based techniques have got a lot of
attention due to their performance and reliability in operation for
the removal of F from groundwater. At present, nanoltration (NF),
reverse osmosis (RO), and electro-dialysis (ED) are the most pop-
ular membrane processes for F removal.
3.1.4.1. Reverse osmosis (RO) and nanoltration (NF)
In membrane ltration, the water containing high concentration
of pollutants is passed through a semipermeable membrane. The
membrane discards atoms on the criteria of size and electric charge.
The pollutants are removed from the water and collected at
retentate side; whereas, clean water is recovered through
permeate. In RO, pressure greater than the natural osmotic pressure
is applied to the concentrated side of the membrane. Kettunen and
Keskitalo (2000) evaluated the performance of a low energy RO
membrane with a NF membrane. A membrane ltration plant of
16e25 m3/h capacity was constructed in Laitila, Finland, to control
F and Al concentration in drinking water. The comparative removal
was above 95 and 76% for F and Al, respectively and RO needed
~1.6 bar excess feed pressure than that used in NF. Sehn (2008)
studied a large scale RO plant in southern Finland for three years.
The system was operated at a pressure of 6e11 atm and tempera-
ture range of 5e11  C, which was until recently possible only with
NF membrane. This resulted in low power requirements and the
plant was operated at 80% recovery without using a scaling inhib-
itor. Richards et al. (2011) used four commercial NF/RO membranes
in Australian groundwaters. Their investigations showed the in-
uence of solar irradiance levels on retention of F, Mg, NO3, K and
Na where convection/diffusion predominated the retention. About
85% of all solutes were retained during solar irradiance conditions.
Nanoltration (NF) is a relatively new process in contrast to RO,
ultraltration (UF) and microltration (MF), and it is emerging as a
practically functional technology in treating industrial wastewa-
ters. Nanoltration is characterized by attributes between reverse
osmosis (RO) and ultraltration (UF). Regardless of the similarity in
operation with RO, NF is operated at a comparatively lower pres-
sure yielding identical permeate ux even at lesser pressure. NF
removes less than 60% of the monovalent ions as opposed to 90% by
RO membranes. RO can completely demineralize water with very
low or practically no selectivity for monovalent ions but it suffers
from high operating pressure, low permeate ux and high energy
requirements (Alarcon-Herrera et al., 2013). In particular, fractional
deuoridation can be attained by altering the operating variables of
the NF process; while simultaneously keeping the required F con-
tent in the water.
Two of the popular NF membranes, NF90 and NF400, were used
to practically remove F from groundwaters (Tahaikt et al., 2007).
The quality of water achieved by the NF400 membrane was found
to be satisfactory especially for lower F content. For higher F con-
tent, a double pass was required to reduce it to an acceptable level.
Further, these authors calculated the economics of a 100 m3/h NF
plant corresponding to a recovery rate of 84%, F removal of 97.8%
and pressure of 10 bar (Elazhar et al., 2009). The capital cost was
estimated to be 748,000 V with operating cost of 0.212 V per m3.
Hu and Dickson (2006) investigated performance of negatively-
charged commercial thin-lm composite (TFC) nanoltration
membranes. They conrmed that higher pressures exhibit sub-
stantial positive effect on F removal along with increase in the ux.
Malaisamy et al. (2011) modied a commercially available NF
membrane by layer-by-layer assembly of alternating poly-
electrolyte thin lms in order to promote removal and selectivity
312 S.V. Jadhav et al. / Journal of Environmental Management 162 (2015) 306e325
towards monovalent ions, particularly F and Cl. Polystyrene sulfo-
nate (PSS) was the anionic polyelectrolyte and polydiallyldimethyl
ammonium chloride (PDADMAC) was the cationic polyelectrolyte.
Thin (0.5e8.5 mm) PDADMAC/PSS bilayers were deposited on the
substrate membrane. The F ion removal increased from 40% (un-
modied) to 70% (8-bilayer modied). These authors found that the
selectivity for Cl over F was 2.7 times for an 8-bilayer modied
membrane compared to 1 for unmodied membrane.
3.1.4.2. Electrodialysis (ED)
Electrodialysis is another emerging technique for removing
ionic compounds from aqueous media using ion exchange mem-
branes in which the applied electric eld acts as a driving force and
is responsible for separation of contaminants. The application of
electric current between two electrodes results in passage of cat-
ions to the cathode and anions to the anode through the negatively
charged cation exchange membrane and positively charged anion
exchange membrane, respectively. The end result is the increased
and decreased concentration of cations and anions in alternate
partitions. The global trend is shifting towards electrodialysis as an
alternate technique for deuoridation primarily because of its
simplicity and ability to overcome the shortcomings of the chem-
ical processes.
Zeni et al. (2005) examined two ion-exchange membranes,
namely, selenium AMP anionic membrane and photo-polymeric
anionic membrane (MZA) for electrodialysis. The AMP mem-
brane removed 69% and 97% F when the applied current density
was 0.1 and 0.7 A/dm2, respectively whereas the MZA membrane
removed 40% F without pretreatments. Ergun et al. (2008) reported
that electrodialysis is the best method for F removal wherein anion
exchange membrane SB-6407 was used and found that increasing
current density and feed concentration at pH 6 was the most
effective. The presence of Cl and SO4 ions in the feed decreased the
F removal efciency. The F ion concentration could be brought
down by 96% (0.8 mg/L), which is below the prescribed limit by
WHO. Sahli et al. (2007) also suggested that electrodialysis gives
better performance for the removal of Cl and F from brackish water.
The combination of adsorption and electrodialysis appears to be a
cost-effective and better method to remove F ions from brackish
groundwater.
The most predominant advantages offered by membrane pro-
cesses are: very high removal capacity (up to 98%), one step puri-
cation and disinfection, and no chemical usage. However, it is not
entirely appropriate as it removes all ions from the water. A remi-
neralization process is required after the treatment as some min-
erals are essential and must be present in potable water. Moreover,
it is costly due to high initial membrane cost and operating cost.
Also, disposal of concentrated F sludge which is produced at
retentate side can be a major problem.
3.2. Arsenic removal
The most commonly used As removal methods are also essen-
tially the same as those for F removal, namely, chemical treatment,
adsorption onto sorptive media, co-precipitation and adsorption
onto coagulated ocs, ion exchange resin and membrane processes.
Rahman et al. (2014) discuss a different approach from the con-
ventional methods and advocate utilizing exclusively bio-
organisms for As reduction. An assessment of the removal ef-
ciency of each of these can be seen in Fig. 4 along with the initial As
concentration. Fig. 4 suggests that the overall treatable As con-
centration ranges from 50 to 1000 mg/L. However, some researchers
have successfully treated very high initial concentrations of As
(5000e3,00,000 mg/L) (An et al., 2011; Robins et al., 2005; Song
et al., 2006).
3.2.1. Chemical precipitation/coagulation (CPC)
Arsenic can be removed most commonly by precipitation as
ferric arsenate, calcium arsenate or arsenic sulde. The ideal
operating pH for calcium generated precipitation is 10.5. Though
the reported attainable As concentration is 10 mg/L, usually the
concentrations below 1 mg/L are challenging to accomplish
(Robins, 2006). Additionally, As(III) removal during coagulation is
considerably less effective than As(V) under otherwise similar
conditions and pre-oxidation is required by using an oxidizing
agent such as Cl2, NaOCl, or H2O2 to convert As(III) to As(V). It is also
evident that As precipitation with ferric salts is more efcient than
alum (Mohan and Pittman, 2007). Ferric salts are added to As
contaminated water to form ferric arsenate (Holl, 2010):
Fe3 AsO4
3 /FeAsO4 s (9)
The efcacy of aluminum-based coagulation was examined with
reference to variable forms and As concentrations in three potable
water treatment plants in New Zealand (Gregor, 2001). Soluble
As(V), in general, was transformed to particulate As(V) by adsorp-
tion during fast mixing, and eventually was removed by clarica-
tion along with natural As. The soluble As(III) was oxidized during
nal chlorination, to soluble As(V). Baskan and Pala (2010)
conclusively stated that aluminum sulfate is a very efcient coag-
ulant at optimum pH of 6e8. The As removal efciency was found
to be higher than 85%. Song et al. (2006) studied coagulation with
Fe3 and coarse calcite, followed by normal ltration to achieve
over 99% removal of As from a high-As water in mine drainage
(5 mg/L As). However, ltration was essential after precipitation. In
the absence of ltration, the As reduction was only ~30%, but with
0.1 or 1.0 mm lter, the reduction exceeded 96% (Litter et al., 2010).
The Stevens Institute of Technology introduced a two buckets
technology. The setup consists of a mixing bucket (of iron sulfate
and calcium hypochloride) and a ocs separation bucket to achieve
sedimentation and ltration. The institute claimed to reduce As
content to less than 0.05 mg/L in 80e95% cases (Akter and Ali,
2011). The Bangladesh Council of Scientic and Industrial
Research (BCSIR) has introduced As removal technology by using
coagulation process followed by sand ltration involving ll and
draw type units. The Bucket Treatment Unit (BTU) also uses two
buckets of 20 L capacity and is based on the methods of coagulation,
co-precipitation and adsorption processes (Ahmed, 2001). It can
remove As in nearly 2e3 h by this method. This technology is
simple with low installation cost and only common chemicals are
used such as aluminum sulfate and potassium permanganate.
Moreover, it is possible to easily apply this technology to huge
water volumes to serve large communities.
On the other hand, like F, As can also be separated by electro-
coagulation method. The mechanism of electrocoagulation is was
already presented in section 3.1.1.1. Here the process can oxidize
more harmful and not so easily removable As(III) to less harmful
and easy to remove As(V) by virtue of electric current. Wan et al.
(2011) carried out batch experiments using iron electrode to eval-
uate the effect of various parameters on As removal. Faster removal
of As(V) was achieved as compared to As(III) with over 99.9% overall
As removal efciency. The authors also pointed out that the As
removal was inuenced by the presence of phosphate, while sulfate
and silica did not show any signicant effect. Studies by Kobya et al.
(2011) have shown the effectiveness of electrocoagulation by
lowering the As level to less than 10 mg/L. Arsenic removal was
observed to be slightly better in case of Al electrode (95.7%) as
compared to Fe electrode (93.5%). The calculated operational cost
for Fe and Al electrodes was 0.020 V per m3 and 0.017 V per m3,
respectively. Similar results for the As removal have been reported
elsewhere (Balasubramanian et al., 2009; Kumar and Goel, 2010).
 S.V. Jadhav et al. / Journal of Environmental Management 162 (2015) 306e325 313

Fig. 4. Arsenic removal performance of various technologies. Where, CPC-21 Baskan and Pala (2010); CPC-22 Oehmen et al. (2011); EC-23 Wan et al. (2011); EC-24 Kobya
et al. (2011) AD-25 Tubic et al. (2010); AD-26 Chatterjee (2007); AD-27 Maji et al. (2008); AD-28 Amin et al. (2006); AD-29 Rahman et al. (2004); AD-210 Kundu et al.
(2004); IE-211 Anirudhan et al. (2007); IE-212 Barakat and Shah (2013); IE-213 Urbano et al. (2012); IE RO-214 Oehmen et al. (2011); RO-215 Teychene et al. (2013); FO-
216 Mondal et al. (2014); NF-217 Floch and Hideg (2004); NF-218 Saitua et al. (2005); NF-219 Harisha et al. (2010). Note: Some treatment methods with greater removal are
not shown in the gure due to their very high initial concentration range between 5000 and 300000 mg As/L (An et al., 2011; Robins et al., 2005; Song et al., 2006).

Coagulation can remove up to 99% of the As (Choong et al.,
2007). Working at pH 3e4 reduces sludge generation. However,
the quantity of iron required for equivalent As removal also in-
creases (Camacho et al., 2011). By using this technique, a relatively
large volume of As laden sludge is formed, which is normally
disposed of to landlls, which is a probable source of further
contamination (Litter et al., 2010).
3.2.2. Adsorption (AD)
As per USEPA classication, activated alumina, and in turn
adsorption, is amongst the best available technologies for As
removal in potable water (Dambies, 2005). Activated carbon has
also been extensively studied for the removal of As and F in water.
Arsenic adsorption by activated carbon is explored in detail by a
number of researchers (Chuang et al., 2005; Gu et al., 2005). Ac-
cording to the review published by Giles et al. (2011) the main
adsorbents of choice for As removal are Al2O3, Al(OH)3, carbon, FeO,
Fe2O3, modied iron oxides, SiO2, layered double hydroxides (LDH),
and organic polymers either as adsorbents per se or as supports. A
broad overview of adsorbents for As removal from drinking water
has also been published by Yadanaparthi et al. (2009).
Hydrous metal oxide particles are useful for adsorption and
form the hydroxyl groups in aqueous solutions leading to proteo-
lytic reactions. The surface of such particles is at pH values below
the zero charge point and the surface gets protonated and thus
adsorbs anions. This can be expressed as (Holl, 2010),
> Me  OH H / > Me  OH
2 (10)

> Me  OH
2 An / > Me  OH2 An (11)
where, Me trivalent metal atom on surface and Ane anions.
A nano-sized Fe(OH)3 (~5 nm) offers a relatively large surface
area (200e500 m2/g), which is particularly useful for adsorbing a
variety of anions and cations from waters (Gilbert et al., 2009;
Pinney et al., 2009; Yavuz et al., 2006). As(V) adsorption is
strongly dependent on hydrous Fe(III) oxide concentration and pH,
whereas As(III) adsorption is independent of pH (Ranjan et al.,
2003). Adsorption of As(III) and As(V) onto activated alumina
revealed that the best As(III) and As(V) removal can be carried out
at pH 6.1 and 5.2, respectively (Lin and Wu, 2001). Robins et al.
(2005) investigated the characteristics of Fe(III) and Al(III) hy-
droxides in removing As(III) and As(V) from solution. Fe(OH)3 was
better than Al(OH)3 in adsorbing As(V). When Fe(OH)3 was used to
remove As(III) and As(V), with 10-fold ratio of Fe(III) to As, the re-
sidual concentration of As dropped from 10 mg/L to 0.2 mg/L at pH
between 6 and 7.5. A comparative study was preformed over the
performance of polyaluminum chloride, aluminum sulfate and
ferric chloride for the removal of As from groundwater (60.5 mg As/
L) (Tubic et al., 2010). Chlorine was utilized as the oxidizing agent
leading to the formation of insoluble hydroxides at pH 7. Despite
the fact that excess ferric chloride was required, the freshly
precipitated hydroxides were able to reduce the As levels to less
than 10 mg/L. Reddy (2007, 2011) reported development of a novel
adsorbent cupric oxide (CuO) which was free from limitations of pH
or redox potential modication for As removal and its performance
was excellent in the company of competing anions. Additionally,
CuO can be regenerated, by leaching with NaOH solution for reuse.
The effectiveness of CuO particles was established over a range of
pH from 7.11 to 8.95 wherein competing anions such as sulfate
(1.3e735 mg/L), phosphate (0.05e3.06 mg/L) and silica
(1e54.5 mg/L) were present (Reddy and Roth, 2013).
On the other hand, several lowecost natural adsorbents are
found to be equally effective as the aforementioned adsorbents.
The As(V) removal efciency by using chitosan showed values
varied from 40 to 96.8%, depending upon: (i) tested temperature;
(ii) polymer characteristics, and (iii) water composition (Pontoni
and Fabbricino, 2012). Another low cost material, laterite soil
reduced ~98% of As from initial 0.33 mg/L from groundwaters
within 30 min (Maji et al., 2008). Amin et al. (2006) also have
reported complete removal of both As(III) and As(V) by using rice
husk columns. The conditions were: 100 mg As/L, 6 g rice husk,
6.7 and 1.7 ml/min ow rate at pH of 6.5 and 6.0, respectively. A
review presented by Malik et al. (2009) exclusively lists a number
of low cost materials for As removal which could be benecial for
314 S.V. Jadhav et al. / Journal of Environmental Management 162 (2015) 306e325
developing countries.
The presence of natural organic matter in water has also been
reported to delay the adsorption equilibrium and limits the degree
of As(III) and As(V) adsorption (Grafe et al., 2001; Redman et al.,
2002). Also, in many cases, the aggressive potential of the toxi-
cants reduces after binding to humic substances (Perminova et al.,
2006). Redman et al. (2002) studied the effect of natural organic
matter on the adsorption of As onto hematite. Four organic sub-
stances were seen to form aqueous complexes with As(V) and
As(III). The extent of complexation varied with the organic matter
origin and increased as the cationic metal (mainly Fe) content
increased. In addition, organic matter showed active redox
behavior towards As species. This indicates that the presence of
organic matter may greatly inuence redox as well as complexation
speciation of As. Similar reports about humic substances have been
published elsewhere (Blinova et al., 2007; Perminova et al., 2007;
Zhilin et al., 2004). The presence of amine groups in organic mat-
ter play signicant role due to their protonation at denite pH
values (Saada et al., 2003; Sorkina et al., 2014). As(V) sorption onto
different forms of kaolinite and two kaolinites coated with humic
acids was carried out by Saada et al. (2003). The humic acid coat-
ings inuenced As sorption, signifying that adsorption rst
occurred on the humic acid sites fully followed by the remaining on
kaolinite sites. Studies on zero-valent iron by Mak et al. (2009)
suggested that, although the formation of Fe-humate complex in
water delays the As(V) adsorption, As removal effectiveness re-
mains practically unaffected in calcium and bicarbonate environ-
ment once enough CaCO3 particles are formed.
Sono Arsenic lter and Kanchan Arsenic lter are currently in
use in Bangladesh and Nepal (Giles et al., 2011). The Sono lter is
regarded as the best of 15 technologies to remove As (Chatterjee,
2007; Khan et al., 2000; Hussam and Munir, 2007). It can reduce
As concentration from 1100 mg/L to below the WHO permissible
limit.
3.2.3. Ion exchange (IE)
The application of synthetic ion exchange resins can remove As
species very effectively from drinking water described as by USEPA
(An et al., 2011). The extensive reviews summarize the performance
of anion exchange resins, macro reticular resins and cation ex-
change resins such as Cu(II), Ce(IV), Fe(III), Y(III), La(III), Zr(IV)
(Dambies, 2005; Mohan and Pittman, 2007). The order of exchange
capacity for the most strongebase resins is given below:
HCrO 4
   and crossow velocity had no effect on As removal (Saitua et al.,
(maximum) > CrO2 2 2
4 > ClO4 > SeO4 > SO4 > NO3 > Br > (HPO4 ,
2
2 2 2    4 4
HAsO4 , SeO3 , CO3 ) > CN > NO2 > Cl > (H2PO , H2AsO ,
HCO3) > OH > CH3COO > F
For As removal, strongly basic ion exchange resins, particularly
in the chloride form, have been recommended by EPA (Holl, 2010):
   
R  NCH3 3 Cl H2 AsO
4 /R  NCH3 3 H2 AsO
4
Cl
(12)
where, R matrix phase.
Choong et al. (2007) proposed a mechanism of As elimination.
The ion exchange resins are normally loaded with chloride ions in a
vessel/bed called as exchange sites and the As-laden water is own
downward through the vessel where ion exchange takes place. The
exhausted resin is regenerated by using aqueous NaCl. However,
 
competing ions such as SO2 4 , NO3 , and F affect the ion exchange
capacity (Baciocchi et al., 2005; Litter et al., 2010; Sharma and Sohn,
2009).
An et al. (2011) showed nearly complete As removal within 1 h,
by employing a new starchebridged magnetite nanoparticles. A
recent work carried out on the As removal from Camarones River
water, North Chile demonstrated very good results (Urbano et al.,
2012). The river water contained sulfate (154 mg/L), chloride
(541 mg/L), boron (15.68 mg/L), chromium (<0.05 mg/L), and total
dissolved solids (1650 mg/L) most of which are known to interfere
with As exchange. Water insoluble polymereclay nanocomposite
resin (using N-methyl-d-glucamine ligand groups) displayed
retention higher than 98% in laboratory studies but decreased to
75% in real water samples. Thirunavukkarasu et al. (2002) reported
the removal capacities of the three As sorption media in the
following order: Amberlite IR-120 (max) > iron oxide-coated
sand > manganese greensand.
Resin Tech's strongly basic hybrid anion-exchange resin called
as TECH RESINTECH ASM-10-HP is a specically prepared sorbent
to remove As amid competing ions (Mohan and Pittman, 2007).
Several commercial organizations have introduced new tailored
anionic exchangers to achieve As content below 10 mg/L which
include resins of Dow Chem, Rohm and Haas, Purolite, Bayer.
As(V) removal is achieved effectively by ion exchange method,
with less than 1 mg/L of As in the efuent, while As(III), being un-
charged, is not eliminated, and a prior oxidation step is required
(Litter et al., 2010; Ravenscroft et al., 2009).
3.2.4. Membrane technology (MT)
Membrane technologies, especially RO, have proven reliable for
As removal. RO is probably the best practiced technology which can
completely purify water and meet the strict water legislations. Both
lab and pilot-scale experiments have shown more than 95% As(V)
and 74% As(III) removal efciencies achieved by RO (Holl, 2010;
Katsoyiannis and Zouboulis, 2006). Membrane processes get rid
of As through ltration, electric repulsion, and adsorption of As
containing compounds. The mechanism of membrane ltration
was mentioned earlier in Section 3.1.4.
The distinction between the removal of As(III) and As(V) was
explored by Seidel et al. (2001) with the help of polysulfone thin-
lm NF membrane (BQ01). It was observed that elimination of
As(V) was much higher than that of As(III). Only less than 30% of
As(III) was removed in contrast to 60e90% of As(V) removal. Floch
and Hideg (2004) used pilot scale ZW-1000 (Zenon) membrane
module, with 0.02 mm pore size, for As removal from waters and the
pilot plant could remove As below 10 mg/L from an initial As con-
centrations up to 300 mg/L. Another study on the NF operating
conditions found that the transmembrane pressure, temperature
2005). These results were supported further by Shih (2005). The
studies by Harisha et al. (2010) also conrm the aforesaid NF
ndings on high As removal (99.80%).
Recently, a different approach was applied by Oehmen et al.
(2011) for As elimination from drinking water where a hybrid rig
based on ion exchange membraneecoagulation was used. The nal
As concentration was reduced to 0.3 mg/L from an initial concen-
tration of 53.4 mg/L with 99.43% removal efciency. The hybrid
membrane-coagulation system also proved to be better than con-
ventional coagulation/ltration process where nal As concentra-
tion was reduced to at 3 mg/L from an initial concentration of 57 mg/
L. Electrodialysis has similar efciency as RO which is used pri-
marily in treating water with high TDS. Electrodialysis with rever-
sion of polarity of the electrodes (EDR) is an improvement of ED
with minimum scaling (Litter et al., 2010; Ravenscroft et al., 2009).
4. Simultaneous removal of As and F
The technologies that allow the simultaneous removal of As and
F are essentially similar to the individual removal using adsorption
 S.V. Jadhav et al. / Journal of Environmental Management 162 (2015) 306e325
(Jing et al., 2012; Li et al., 2011), membrane ltration (Padilla and
Saitua, 2010; Nevarez et al., 2011) and coagulation (Pinon-
Miramontes et al., 2003; Ingallinella et al., 2011) and adsorption
on various low cost materials (Devi et al., 2008). However, each of
them presents several benets and shortcomings. Table 2 presents
the consolidated information of the recent research work carried
out by various researchers on the above mentioned technologies
for simultaneous removal of As and F with their merits and de-
merits. Fig. 5 compares the simultaneous As and F removal
performance.
4.1. Chemical precipitation/coagulation (CPC)
As discussed earlier, chemical precipitation involves addition of
cake alum and/or ferric chloride in the water body. Pinon-
Miramontes et al. (2003) evaluated the combined use of cake
alum and a polymeric anionic occulent (PAF) for the removal of As
and F from drinking water from two wells at Meoqui City, Mexico.
As and F concentrations were reduced up to 99 and 77%, respec-
tively at US$ 0.38 per m3 of treated water at the optimal pH 7.1. The
authors found that the efcacy of F removal was dependent on the
cake alum quantity used and pH adjustment was needed, whereas
As removal had no effect of pH. Further studies have found that
efcient removal of F and As can be achieved using pre-
chlorination, aluminum sulfate and a cationic polyelectrolyte as
coagulant in precipitation (Ingallinella et al., 2011).
ArCISeUNR process was developed and applied to groundwater
in Argentina, where the As and F concentrations vary between 100
and 150 mg/L and 1.7e2.5 mg/L, respectively (Ingallinella, 2008).
The system consisted of a coagulationeadsorption process, using
polyaluminum chloride (PAC) as a coagulant with an initial pH
adjustment and two ltration stages. Further, the process was
modied with F and As concentrations ranging from 2.4 to 3.2 mg/L
and 60e90 mg/L, respectively (Ingallinella et al., 2011). The As and F
removal efciency was up to 85 and 55%, respectively.
It has been shown that electrochemical processes are an
attractive alternative to the conventional methods. A primary
mechanism of coagulation and electrocoagulation was explained in
sections 3.1.1 and 3.2.1. Vasudevan et al. (2011) studied the effect of
various coexisting ions on the removal F using electrocoagulation.
The solutions with F concentration of 5e20 mg/L were treated with
As(V) (0e5.0 mg/L) as a competing ion. Electrocoagulation removed
F to the extent of 93, 85.3, 77, 69 and 35% in the presence of As(V)
concentrations of 0, 0.5, 1, 3 and 5 mg/L, respectively. The authors
attributed the reduction in F removal to the preferential adsorption
of As(V) ions over F ions with increase in the As(V) concentration.
The presence of carbonate, phosphate and silicate also reduced the
F removal efciency.
Zhao et al. (2011) designed an integrated electro-oxidation and
electrocoagulation system to simultaneously remove As(III) and F
ions from water. By utilizing one Fe plate piece and three parts of Al
plate electrodes, which reduced As(III) to less than 10 mg/L
compared to its initial level of 1 mg/L and F 1 mg/L when its initial
concentration was 4.5 mg/L. Rise in the pH of the solution led to
increase in the As(III) removal efciency with best removal at 6e7
pH. When Fe plate was employed as anode in the electro-
coagulation process, As(V) was effectively removed from water
because of the co-operation between Fe and As ions (Ratna Kumar
et al., 2006). Arsenic and F co-removal by coagulation/precipitation
is summarized in Table 2.
4.2. Adsorption (AD)
Adsorption technique is more popular due its simplicity, better
efciency at high levels of total solids and suitability for household
315
and small community schemes. Extensive research has been car-
ried out using various adsorbents for individual as well as simul-
taneous removal of As an F. Adsorbents used for the simultaneous
removal of F and As are activated alumina (Li et al., 2011), activated
carbon (Jing et al., 2012), layered double hydroxides (Dadwhal et al.,
2011; Delorme et al., 2007), ferric hydroxides (Streat et al., 2008),
goethite (Tang et al., 2010), FeeCe oxides (Zhang et al., 2010),
inorganic ion exchange adsorbents (Chubar, 2011), volcanic ash
(Chen et al., 2011), FeeAl doped polymers (Kumar et al., 2011),
modied cellulose (Tian et al., 2011), and low cost materials such as
goethite coated sand, hematite coated sand and bone and cow char
(Brunson and Sabatini, 2009; Mlilo et al., 2010).
Activated alumina has proved to be one of the best adsorbents
for the As and F removal. Mechanism of adsorption has been dis-
cussed earlier in sections 3.1.2 and 3.2.2. However, the use of this
sorbent is limited by its strong dependence on solution pH and
coexisting ions (Liu et al., 2013). To encounter these shortcomings,
mesoporous alumina and calcium-doped alumina were synthe-
sized (Li et al., 2011). Excellent F and As removal capacities were
obtained by using these materials reducing As(V) concentration
from 100 mg/L to 1 mg/L (99% removal). The highest F removal ob-
tained was 450 mg/g while 1 g of mesoporous alumina was effec-
tive to treat 200 L of As water at pH 7.0. Comparatively, activated
alumina has removal capacity of ~9.0 mg As/g and 7.6 mg F/g (Ku
and Chiou, 2002; Lin and Wu, 2001). Jing et al. (2012) developed
a composite adsorbent with titania and lanthania supported on
granular activated carbon (TLAC) to effectively remove As(V) and F.
Arsenic and F removal was found to be more than 80 and 35%,
respectively. On the other hand, Al- and Fe-doped, activated micro
(~0.8 mm) and nano (~100 nm) sized porous adsorbents showed
signicant removal of F (~100 mg/g) and As(V) (~40 mg/g) ions
(Kumar et al., 2011). Delorme et al. (2007) evaluated mixed oxides
synthesized from the mild thermal treatment of quintinite
(Mg4Al2(OH)12CO3$H2O) for the removal of F, As(V) from water.
100% As and 80% F removal efciency was obtained from initial
concentrations of 16 mg/L and 10 mg/L for As and F, respectively.
However, CO3 addition led to 90 and 20% of the entrapped F and As
being released in the solution conrming that the presence of CO3
ions can signicantly affect the removal efciency of mixed oxides.
This is in agreement with numerous reports that analyzed the
presence of competing ions such as phosphate, silicate, nitrate,
chlorides, carbonates, and sulfates. Detailed information on several
other adsorbent studies are summarized in Table 2. The presence of
humic acid also affects As and F adsorption on various adsorbents
(Dadwhal et al., 2011; Guan et al., 2012; Jimenez-Nunez et al., 2012;
Wei et al., 2011). In fact, the coexistence of As and F too affects the
individual removal (Chen et al., 2010, 2011; Zhang et al., 2010).
In order to develop simple and cost effective processes to serve
on the community level, several low cost materials have been
evaluated and found to be equally effective in F and/or As removal
(Brunson and Sabatini, 2009; Mlilo et al., 2010). Fish bone char and
cow bone char were used for treating water with high concentra-
tions of As and F (Brunson and Sabatini, 2009). Fish bone char was
better in removal of F and As simultaneously with minimal
competition; F was removed more efciently than As. Further, the
use of sh bone char is a practical solution for F removal in poor
countries where rural populations cannot meet the expense of
membranes and electricity. Mlilo et al. (2010) have reported that F,
As(III) and As(V) adsorption capacity was higher in bone char than
in goethite coated sand and hematite coated sand.
4.3. Membrane technology (MT)
Membranes have well-proven their use in various processes
especially in desalination, membrane distillation and membrane
Table 2

316
Potential treatment methods for the simultaneous removal of As and F.

Technology Investigators and level of Type of water, raw materials/ Maximum removal capacity, Reference Merits Demerits Cost
development composition, geographical origin optimal/affecting parameters

Coagulation  Combination of cake alum and  Groundwater  F removal 99% Pinon-Miramontes et al.  Low cost  As/F laden sludge Lowa
polymeric anionic occulent  Composition: Well 1:  As removal 77% (2003)  Simple to use generation
(PAF) F 5.9 mg/L; As 0.139 mg/L ;  Optimal pH 7  Well proven  Unpleasant water
 Pilot plant lab scale research Well 2: F 4.8 mg/L;  Readily available taste
As 0.075 mg/L chemicals  Residual aluminum
 Meoqui City, Chihuahua,
Mexico
 ArCIS-UNR process  Groundwater  F removal 50e55% Ingallinella et al. (2011)
optimization  Composition: F 2.4e3.2 mg/L  As removal 75e85%
 Polyaluminum chloride As 60e90 mg/L
 Pilot plant
 Direct current  Synthetic water  F removal 91.5e93% Vasudevan et al. (2011)
electrocoagulation processes  Composition:  F removal (For As(V)

S.V. Jadhav et al. / Journal of Environmental Management 162 (2015) 306e325

 Aluminum alloy as electrodes F 5e20 mg/L
 Lab scale research As(V) 0e5 mg/L
 integrated electro-oxidation  Synthetic water
and electrocoagulation (hybrid  Composition: F 4.5 mg/L
DSA-Fe-Al electrode) As 1 mg/L
 Current density mA/cm2
 Duration 40 min
Adsorption  Adsorbent prepared through  Synthetic water
the cross-linking reaction of  Composition: F 10 mg/L,
PANF by hydrazine hydrate PO3 30 mg/L As(V) 38 mg/L
and functionalized reaction of (Separately treated) Mixed
hydrazine-modied ber in ions, F 5 mg/L, PO3 50 mg/
mixture of sulfur powder and L, and As(V) 34.23 mg/L
ethylenediamine treated in another run
 Lab scale research  Flow rate 2.5e3.5 ml/min
 CeeFe adsorbent  Groundwater
 Lab scale research  Composition: As(V) 1.1 mg/L
F 1.59 mg/L
 Zhijiliang Village, Inner
Mongolia, China
 Granular activated carbon-  Synthetic water
based iron-containing adsor-  Composition: As 105 mg/L  Max As adsorption (prepared
bents (As-GAC) and 1031 mg/L 90.0 mg solid
 Lab scale research per 30.0 ml solution
 pH 4.7
 Duration 24hr
 Synthetic water
concentrations of 0, 0.5, 1, 3
and 5 mg/L) 93, 85.3, 77, 69
and 35%, respectively.
 F removal 81% Zhao et al. (2011)
 As(V) removal 98%
 Optimal pH 5e7
 As(V) adsorption 97.9% at pH Ruixia et al. (2002)  Low to medium cost  pH sensitive Low to medium
3.5 to 7  Simple to use  Considerable
 F adsorption 90.4% at pH 3  Efcient adsorbent
 PO3 adsorption > 99% at pH 3  Commercially available regeneration time
to 5.5 sorbents  Needs standby process
 In mixed ions F, As(V) and PO3  Can handle high levels of during regeneration
adsorption was ~50, 85 and solids  Exhausted adsorbent
90% respectively disposal problem
 Equilibrium was reached  Competing ions reduce
within 5 min for all the efciency
experiments
 Phosphate seriously affected Zhang et al. (2003)
removal of As(V) while F did
not compete with As(V) even
at F/As molar ratio as high as
30, suggesting that adsorption
sites for As(V) and F were
different
 Mean As(V) adsorption
capacity 16 mg/g at pH 3-7
 Max As(V) adsorption
capacity 8.3 mg/g at pH 5.5
 As removal > 98% Gu et al. (2005)
by NaCl oxidation) 6572 mg/g
 Presence of P and SiO
signicantly decreased As(V)
removal at pH > 8.5
 Effects of Cl, and F were
minimal
 F removal 80% Delorme et al. (2007)
 Mixed oxides obtained from  Composition:
the moderate thermal F 10 mg/L As(V) 16 mg/L  NO3 removal 15%
treatment of quintinite NO3 100 mg/L
 Lab scale research
 Three types of granular ferric  Synthetic water
hydroxide materials  Composition:
 Lab scale research As(V) 0.0133 mmol/L
F 0.0133 mmol/L
P 0.0133 mmol/L
 pH 4e8
 Cow and sh bone char  Synthetic water
 Lab scale research  Composition: F 10 mg/L
As(V) 0.250 mg/L
 Magnetite-type adsorbent  Groundwater
 Lab scale research/Field  Composition:
sample testing As 0.01e3.23 mg/L F 0.04
e3.76 mg/L B 0.1e33.9 mg/L
 16 sites, Kyushu, Japan
 Ceramic adsorbent prepared  Synthetic water As(V) 10  As(V) adsorption
with a mixture of akadama and 20 mg/L (kinetic studies)
mud, wheat starch, and Fe2O3 As(V) 5, 10, 20, 50, 65, 80,
 Lab scale research and 100 mg/L, respectively
(isotherm studies)
 Bone char, goethite coated  Synthetic water
sand (G-IOCS) and hematite  Composition: F 1e200 mg/L
coated sand (H-IOCS) with or without As (0.25 mg/
 Lab scale research L) As 0.1e2.5 mg/L with or
without F (10 mg/L)
 Goethite  Synthetic water
 Lab scale research  Composition:
F 5.1e25.1 mg/L
As(V) 2.51e10.12 mg/L
 As(V) removal 100%
 CO3 addition resulted
in trapped ion leaching (90% F
and 20% As released)
 F adsorption Streat et al. (2008)
capacity 1.8 mmol/g
 As(V) adsorption
capacity 0.9e1 mmol/g
 Phosphate adsorption
capacity 0.65e0.75 mmol/g
 Being not a triprotic acid, F did
not compete for same sites
with As
 As(V) showed no Brunson and Sabatini
signicant competition for F (2009)
 F adsorption
capacity 3.94 0.15 mg/g
S.V. Jadhav et al. / Journal of Environmental Management 162 (2015) 306e325
 As(V) adsorption
capacity 4.41 0.23 mg/g
 Bone char showed greater
capacity to remove F than As
 Reduction of As concentration Yoshizuka et al. (2010)
to less than 0.01 mg/L was
obtained up to bed
volume 200
 Remarks:
 The focus was only on As; no
mention on F removal
Chen et al. (2010)
capacity (Langmuir
isotherm) 4.19 mg/g
 Complex multilayer As(V)
adsorption was observed on
ceramic material
 Presence of P and F affected
As(V) adsorption
 F and As(III) and As(V) Mlilo et al. (2010)
adsorption capacity was
higher in bone char than in
G-IOCS and H-IOCS
 F removal was not affected by
the presence of
environmentally signicant
As(III) and As(V)
concentrations
 F competes with As(V) for
adsorption onto bone char
 F adsorption Tang et al. (2010)
capacity 0.191e0.518 mg/g
 As(V) adsorption
capacity 0.247e0.941 mg/g
 F and As adsorption was seen
strongly dependent on
contact time, pH, and surface
loading
(continued on next page)
317
Table 2 (continued )
Technology Investigators and level of Type of water, raw materials/ Maximum removal capacity,
development composition, geographical origin optimal/affecting parameters
 FeeCe oxide  Synthetic water
 Lab scale research  Composition:
As(V) 13.3 mmol/L Series of
molar ratios of As to P (1:0.1,
1:1, and 1:10) and As to F (1:1,
1:10, and 1:100)
 pH 5.0 0.2
 Adsorption on layered double  Power plant efuent data from
hydroxides greater Los Angeles, USA used
 Lab scale research to simulate water
 Composition: As 0.02 mg/L
F 1 mg/L NO3 5 mg/L
Cl 100 mg/L CO3 5 mg/L
SO4 100 mg/L HPO4 1 mg/L
 pH 8
 Inorganic ion exchangers  Synthetic water
developed based on double
hydrous oxides of Mg and Al
 Lab scale research
 Adsorption on  Synthetic water and surface
ferric-impregnated water
volcanic ash  Composition: As z 1 mg/L
 Lab scale research F 0.2e0.5 mg/L
 Lake Kasumigaura, Japan
 Fe and Al doped micro and  Synthetic water
nano-polymeric beads  Composition:
 Lab scale research F 10e100 mg/L As 1
e50 mg/L (Separately treated)
 Mesoporous alumina and  Synthetic water
calcium-doped alumina  Composition: F 2e1000 mg/
 Lab scale research L As 100e200 mg/L
(Separately treated)
318
Reference Merits Demerits Cost
 F and As(V) adsorption onto
goethite obeyed pseudo
second-order rate law
 As(V) showed much stronger
afnity for goethite than F
 P strongly inhibited adsorption Zhang et al. (2010)
of As(V) at the low-binding-
energy sites
 Coexistence of F, only
inuenced total adsorption
capacity of As(V) at high
simultaneous F concentrations
 As(V) and P were mainly
adsorbed through the
S.V. Jadhav et al. / Journal of Environmental Management 162 (2015) 306e325
substitution of Fe surface
active sites
 F was mainly adsorbed
through substitution of Ce
surface active sites on FeeCe
surface
 Effect on As adsorption Dadwhal et al. (2011)
F < NO3 < Cl < CO3 < SO4 < P
 Presence of F greatly affected
adsorption equilibrium
constant in As adsorption
 As adsorption
capacity 3.6 mg/g
 F adsorption
capacity 34.9 mg/g
 Very fast kinetics of arsenate Chubar (2011)
adsorption was observed
 As(V) adsorption
capacity 220 mg/g
 As(III) adsorption
capacity 30e35 mg/g
 Fluoride, bromate, bromide,
selenate, borate, etc. compete
for adsorption sites
 As(V) adsorption Chen et al. (2011)
capacity (Langmuir
isotherm) 6.13 mg/g
 Existence of multivalence
metallic cations improved
As(V) adsorption
 Competing anions (F and P)
affected As(V) adsorption
 F adsorption Kumar et al. (2011)
capacity 100 mg/g
 As adsorption
capacity 40 mg/g
 F adsorption Li et al. (2011)
capacity 450 mg/g
 As(V) adsorption
capacity 19.8 mg/g

 N-methylglucamine
immobilized onto cross-linked 
chitosan beads
 Lab scale research
 Cellulose-g-PDMAEMA
adsorbent prepared by
modifying surface of native
cellulose bers with poly (N,N-
dimethyl aminoethyl
methacrylate)
 Composite adsorbent with 
titanium and lanthanum
oxides impregnated on  Groundwater
granular activated carbon
 Lab scale research
 Nickel and magnesium
hydrotalcite-like compounds
(NiAlHT, MgAlHT)
 Lab scale research
Membrane  Combination of solar energy
ltration and NF/RO (PV-membrane)
 Pilot plant
 Nanoltration
 Pilot plant
 Solar (photovoltaic) powered 
UFeNF/RO system
 Lab scale research
 Synthetic water
Composition: As(V) 0
e150 mg/L F 0e1 mM
 Synthetic water
 Composition:
F 1.8e12.8 mg/L
As 0.05e8.9 mg/L
Synthetic water and  As removal > 80%
groundwater
Composition:
As(III) 0.73 mg/L
As(V) 0.69 mg/L F 2.01 mg/
L TOC 7.5 mg/L
 pH 8.0
 TLAC 1 g/L
 Shanxi Province, China
 Synthetic water
 Composition: F 5 mg/L 5 ml
of one of the following
solutions: Cl 20 mg/L,
SO4 35 mg/L or
As(V) 2 mg/L to 50 mg of
each hydrotalcite-like
compound
 Speed 200 rpm
 Groundwater
 Composition:
F z 10 mg/L As z 5e6 mg/L  Mg rejection 99%
Mg z 150 mg/L  Pine Hill
Station and Ti Tree Farm,
Australia
 Synthetic water
 Composition As(V) 180 mg/L  F rejection 89%
F 5 mg/L HCO3 84 mg/L
 pH 8
 Pressure 7 bar
Groundwater
 Composition: F 1.1 and
0.464 mg/L As 0.005 and
0.003 mg/L TDS 5700 and
1080 mg/L
 Pine Hill and Ti Tree, Australia  F rejection ~98.5% on BW30
 As(III) adsorption
capacity 5 mg/g
 Adsorption was highly pH Wei et al. (2011)
dependent
 As(V) adsorption
capacity 69.28 mg/g at pH 5
 Effects of competitive anions:
SO4 >> P >> F
 F adsorption capacity 1.5 Tian et al. (2011)
e7.5 mg/g
 As(III) adsorption
capacity 0.06e7.8 mg/g
 As(V) adsorption
capacity 0.05e8.7 mg/g
 Adsorption capacities
calculated from Langmuir and
Freundlich equations were
S.V. Jadhav et al. / Journal of Environmental Management 162 (2015) 306e325
both in the order of
As(V) >> As(III) > F
Jing et al. (2012)
 F removal > 35%
 The interference of other Jimenez-Nunez et al. (2012)
anions in the sorption kinetic
of F ions by NiAlHT and
MgAlHT was: SO4 > As(V) > Cl
 F rejection  88% Richards et al. (2009)  Highly efcient  High initial cost High
 As rejection 78%  No chemicals required  High operating cost
 Does not inuence water  High water rejection
taste and color  Brine disposal
 Ability to completely problem
purify water  Need of after
 As(V) rejection 93% Padilla and Saitua (2010) treatment re-
mineralization
 HCO3 rejection 85%
 More than 85% overall Richards et al. (2011)
rejection
 As rejection ~64e79% on
BW30, TFC-S, ESPA4, and
NF90 membranes
membrane
 Rejection of arsenic was
independent of pH from
3 to 11
(continued on next page)
319
 320 S.V. Jadhav et al. / Journal of Environmental Management 162 (2015) 306e325

reactors. As described earlier, although there are several reports

on F as well as As removal from synthetic aqueous solutions by
employing RO and NF processes with high removal efciencies,

Very high
only a few reports have dealt with natural groundwater (Nevarez
Cost

Low
et al., 2011). A widely known separation mechanism has already
been described in section 3.1.4.
A series of experiments were performed in Central Australia to
evaluate elemental retention with four different membrane
modules (BW30, ESPA4, NF90, and TFC-S) at different pH values
ranging from 3 to 11 (Richards et al., 2009). A pilot plant using
solar energy and a two-staged membrane process consisting of UF
Demerits

followed by NF/RO was developed for water purication. The

average removal of F and As was found to be nearly 88 and 78%,
respectively, on NF90 membrane. Moreover, F and As removal was
observed to be independent of pH. Average retention of As was 79,
65, and 75% for the BW30, TFC-S, and ESPA4 membranes,
respectively. It has been suggested that variations in retention
based on membrane type were likely due to membrane charac-
teristics. Further, the same membranes were used in another study
for photovoltaic powered UFeNF/RO system in real water treat-
Merits

ment to conrm the results (Richards et al., 2011). A recent study

on forward osmosis (FO) has demonstrated promising results
(~95%) for As(V) removal in presence of F (Mondal et al., 2014). A
Yarlagadda et al. (2011)

pre-oxidation of As(III) was necessary for efcient As removal at

 As rejection 17.80e25.40% Nevarez et al. (2011)

pH 7. Also, a two pass FO-RO system was proven to be more

Devi et al. (2008)

sustainable than a two pass RO system.

A pilot scale NF plant was operated to evaluate performance on
Reference

simultaneous removal of As, F and HCO3 from a synthetic water

solution laden with 180 mg As(V)/L, 5 mg F/L and 84 mg HCO3/L
(Padilla and Saitua, 2010). At 7e8 bar, the removal of As and F was
e10,000 mg/L As and U 10  As, F and U reduction ~96.5
matter present in groundwater
(solar irradiance between 0.2

affected by ionic and organic

and 1.0 kW/m2) inuenced F

93 and 89%, respectively. However, reducing the pressure to 2 bar

membranes was found to be
 F rejection 14.29e27.14%

20 ppm (>99% rejection of

composition, geographical origin optimal/affecting parameters
Maximum removal capacity,

reduced the removal efciency to 91.6 and 73.3% for As and F,

concentrations less than

respectively. These ndings are in consonance with the so-called

 As removal 93.07%
F 11.8 mg/L As 0.435 mg/L  As and F removal by

 F removal 85.60%

dilution effect; at higher pressures, the permeate water ux

 Energy variations

Synthetic water and brackish  Dissolved solids

increases more than the salt ux (Seidel et al., 2001). Therefore,

(0.009 mg/L)

the salt concentration in permeate is reduced due to increased

(0.72 mg/L)
rejection

removal. Further, by reducing the pressure, the convection is low

e99.9%
salts)

and consequently, the diffusive contribution becomes signicant.

Similar ndings have been reported by other workers as listed in
Table 2.
Brackish water composition:

An interesting investigation carried out on nanocomposite

F 5 mg/L As 0.13 mg/L
Unknown source, Probably
Type of water, raw materials/

e400 mg/L F 1e30 mg/L

membranes suggested that As and F removal can be inuenced by

Dissolved solids 1000

ionic and organic matter content in groundwater (Nevarez et al.,

The cited literature does not give actual costs and hence this is relative.
Chihuahua, Mexico

2011). Nanocomposite membranes synthesized from propio-

Drinking water

nated lignin (such as Kraft, Organosolv and Hydrolytic) and cel-

Composition:

Composition:
Groundwater

lulose triacetate (CTA), removed 17.80e25.40% As and

pH 7.17

14.29e27.14% F. Membrane effectiveness was also inuenced by

water
India

The bold text represents the country of groundwater source.

suspended solids (Meenakshi et al., 2004).

There are several RO plants operating in Argentina and Mexico









for F and As removal. Regardless of their high separation efciency,

 Filtration on home-made lter
tion method from propionated
lignin and cellulose triacetate
vapor-induced phase separa-

RO systems suffer from considerable water loss (35e65%) due to

 Direct contact membrane
distillation (DCMD) using

the discharge of concentrated retentate stream which should be

membranes prepared by
 Nanocomposite (NF/RO)

polytetrauoroethylene
Investigators and level of

treated before being discharged. However, there are no means to

ltration/Distillation

 Lab scale pilot plant

polypropylene and

treat or safely dispose the rejected brine. Moreover, poor com-

 Lab scale research

munities cannot afford the high running cost (Ingallinella et al.,

membranes

2011).
 Membrane
 Pilot plant
development

 Filtration

media

4.4. Other technologies

Table 2 (continued )

In a quest to develop appropriate technology for the concurrent

elimination of As and F, a limited number of researchers have
Technology

made out of the box efforts to see the opportunities. Devi et al.
(2008) carried out removal of F and As by modied home-made
Others

lter media for potable water. The system consisted of two

a

metal tanks, each with 30 cm diameter and 100 cm height, tted

 S.V. Jadhav et al. / Journal of Environmental Management 162 (2015) 306e325 321

with 1.25 cm outlet pipe, a drain valve and an outlet tap. One tank
was lled with 10 cm stone at bottom (pebbles); 8 cm lter gravel
consisting of two layers of different sizes of 4 cm deep each (particle
size ranges 0.8e1.5 mm) and a layer at the top of 40 cm deep lter
sand (size of 0.2e0.8 mm). The second tank was also lled similarly
except that a 10 cm crushed brick (particle size ranging from 0.25 to
0.5 mm) was added to operate the experiments in batches for 2, 4,
6, 8, 10 and 12 h. The initial concentrations of F and As were kept at
5 mg/L and 0.13 mg/L, respectively during the experiment. This
simple set-up was effective to remove F and As nearly by 86 and
93%, respectively.
Yarlagadda et al. (2011) used a different approach of direct
contact membrane distillation process for the recovery of potable
water from As, U and F contaminated groundwaters. Polypropylene
and polytetrauoroethylene membranes were evaluated with
synthetic brackish water composition: As and U: 10e400 mg/L; F:
1e30 mg/L; and salts: 1000e10,000 mg/L. The results showed more
than 99% removal of salts along with As, F and U removal in the
range of 96.5e99.9%.
5. Disposal of trapped/separated As and F
Although a lot of work has taken place to remove As and F in
isolation or together from a mosaic of ions, the real worry is two-
fold: how to dispose of the concentrate or retentate and how to
stop its recycle back into the groundwaters. Communities using any
of the low-cost technologies to make their local potable water
supply free of As and F, also need to be provided with low-cost and
effective means of dealing with the loaded and exhausted adsor-
bents or concentrated brines. There is no worthwhile technology
available except the disposal of concentrated streams in sea.
The foregoing discussion illustrated that successful treatment of
water containing high dissolved solids (TDS) can be carried out by
using activated alumina (AA). Conversely, the presence of
competing ions (sulfates, nitrates, selenium, chlorides, etc.) may
seriously affect the adsorption rates. Nearly 5e10% loss of absorp-
tive sites for every run should be considered as a benchmark while
separating As(V) with activated alumina. This is due to high
selectivity of activated alumina towards As(V) resulting in regen-
eration problems.
Pre-oxidation step is required to convert As(III) to As(V) for
practical removal of As(III). Strong dependency on pH limits the
applicability of adsorption. Moreover, regeneration steps result in
secondary pollution which is also applicable to ion exchange;
although in the case of ion exchange resins, high cost of resins is
always associated with high removal (~95%) performance for As
and F (Mohan and Pittman, 2007; Solangi et al., 2009). Fluoride,
sulfate, nitrate, selenium and phosphate are competitive species
with arsenic affecting the duration of adsorption. Improved
removal along with the reduction in regeneration cycle can be
achieved by passing of water through a series of columns. Ion ex-
change beds are susceptible to clogging due to the presence of
suspended solids and pretreatment is recommended which
otherwise escalates the equipment and operating cost (Shah,
2008).
More than 95% As and F removal is achieved by RO along with
complete purication and disinfection when the operating pressure
is ideal (Dolar et al., 2011; Oehmen et al., 2011). For instance, Fig. 5
demonstrates that RO and NF are the most useful technologies in As
and F removal. Literature reports illustrate that electrodialysis
reversal can eliminate 80% of the pollutants (Litter et al., 2010;
Ravenscroft et al., 2009). However, the release of brine is also of
great concern. Moreover, these membranes suffer from 35 to 65%
water loss at retentate side which should be treated before being
discharged. Although membrane distillation has shown promising
co-removal potential, it turns out to be the most expensive tech-
nique for As and F removal (Fig. 5). Fig. 5 also shows that co-
presence of As and F results in nearly 15e20% reduction in
removal efciency of any treatment method. Therefore, consider-
ation must also be given to this issue while synthesizing and/or
selecting the treatment route. On the other hand, although cost
effective, the precipitation scheme for F removal leaves toxic re-
sidual aluminum complex in drinking water.
The synthesis of nanosized adsorbents and encapsulation
technologies to isolate loaded adsorbents and dispose them as
landll or for burial will be highly useful. Synthesis of highly

Fig. 5. Simultaneous uoride and arsenic removal performance of various technologies. Where, CPC-31 Pinon-Miramontes et al. (2003); CPC-32 Ingallinella et al. (2011); EC-
33 Zhao et al. (2011); AD-34 Ruixia et al. (2002); AD-35 Jing et al. (2012); AD-36 Brunson and Sabatini (2009); RO/NF-37 Richards et al. (2009); RO/NF-38 Richards et al.
(2011); RO/NF-39 Padilla and Saitua (2010); RO/NF-310 Nevarez et al. (2011); Other-311 Devi et al. (2008); Other-312 Yarlagadda et al. (2011). Note: A special note of
Delorme et al. (2007) should be taken as this is not shown in gure due to drawing constraints. The authors obtained 100% As and 80% F removal from initial concentrations 16 mg
As/L and 10 mg F/L.
322 S.V. Jadhav et al. / Journal of Environmental Management 162 (2015) 306e325
selective nanomaterials for membranes could be used for both As
and F removal. Activated alumina treatment is pH dependent and
hence treatment of water with mineral acids will be required. This,
however, needs further research, particularly sustainable means of
contaminants laden sorbents. Rice husk, bone char, red mud, coal,
sand, and some other low cost materials available in large quanti-
ties, possibly can be used as adsorbents. Developing a technology
based on these materials could prove to be a practical solution in
developing markets. For example, some researchers have got
excellent As (93%) and F (86%) co-removal on relatively inexpensive
home-made lter media by combining sand and crushed bricks
(Devi et al., 2008).
6. Conclusions
The literature analysis on As and F removal leads to the
following conclusions:
1. The technologies available for the simultaneous removal of As
and F are divided broadly into three, namely, coagulation,
adsorption and membrane processes. The process with very
high efciency for the removal of individual contaminants is not
necessarily suitable for the simultaneous removal of both As and
F.
2. At present, the most capable treatment method for As and F
removal is the RO and NF with the marginal reduction in per-
formance in the company of competing ions. However, high
xed cost associated with the membrane plants is a major
setback for rural populations. Apart from the operating costs,
the rural masses face another set of problems in terms of limited
(or irregular) electricity supply for water pumping, washing of
fouled membrane and scraping.
3. The sorption materials seldom make it to the practical utility
despite of their proven high efciency of As and F removal. The
problem with the adsorbents is the competing ions and their
afnity for the same adsorption sites. The presence of organic
matter has a profound effect on adsorption in terms of delaying
the adsorption equilibrium.
4. Extensive research is required for the development and imple-
mentation of a low-cost, sustainable and hybrid technology
which can overcome the drawbacks of the individual process for
the simultaneous removal of As and F.
5. There is no meaningful knowledge available for the disposal of
removed As and/or F from groundwaters. Innovative encapsu-
lation methods to isolate As and F loaded materials for nal
permanent disposal or burial without any risk of further
contamination may provide an effective solution, but they are
yet to be developed.
Conicts of interest
The authors declare no conict of interest.
Acknowledgments
This work is part of the project sponsored by the EU e India New
Indigo Project of Spain (I. Ortiz), India (G.D. Yadav) and Finland (R.
Keiski). Financial support from the Spanish Ministry of Economy
and Competitiveness through the projects CTQ2008-00690,
CTQ2012-31639 and INDIGO-DST1-017 Govt. of India is gratefully
acknowledged.
Appendix A. Supplementary data
Supplementary data related to this article can be found at http://
dx.doi.org/10.1016/j.jenvman.2015.07.020.
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