Rev Environ Sci Biotechnol (2014) 13:163–181

DOI 10.1007/s11157-013-9330-2

REVIEWS

A review on economically adsorbents on heavy metals

removal in water and wastewater
Ai Phing Lim • Ahmad Zaharin Aris

Published online: 29 November 2013

Ó Springer Science+Business Media Dordrecht 2013

Abstract Heavy metals contamination in water has factors such as pH, contact times, temperature, initial
been an issue to the environment and human health. concentration and modified materials were revised and
The persisting contamination level has been observed summarized in this review for further reference.
and concerned by the public due to continuous Comparisons of the adsorbent between the modified
deterioration of water quality. On the other hand, and natural products were also demonstrated to
conventional treatment system could not completely provide a clear understanding on the kinetic uptake
remove the toxic metals in the water, thus alternative of the selected adsorbents. Some of the natural
purification methods using inexpensive materials were adsorbents appeared as good heavy metal removal,
endeavor to improve the current treatment process. while some were not and require further modifications
Wide ranges of low cost adsorbents were used to and improvements to enhance the adsorption capacity.
remove heavy metal in aqueous solution and waste- SWOT analysis (strength, weakness, opportunities,
water. The low cost adsorbents were usually collected threat) was also performed on the low cost adsorbents
from agricultural waste, seafood waste, food waste, to identify the advantages of using low cost adsorbents
industrial by-product and soil. These adsorbents are and solve the weaknesses encountered by the utiliza-
readily available in a copious amount. Besides, the tion of low cost materials. This tool helps to determine
pretreatment are not complicated to be conducted on the potential quality of low cost materials in the
the raw products, which is economically sound for an application for water and wastewater treatment.
alternative treatment. The previous studies have
provided much evidence of low cost adsorbents’ Keywords Low cost  Adsorbents  Heavy
efficiency in removing metal ions from aqueous metals  Adsorption capacity  SWOT analysis
solution or wastewater. In this review, several low
cost adsorbents in the recent literature have been
studied. The maximum adsorption capacity, affecting 1 Introduction

The demand on water usage is high as the domestic

and industrial activities are increasing rapidly espe-
cially in the manufacturing sectors. However, on the
A. P. Lim  A. Z. Aris (&) other hand, the waste litters handling are not well
Environmental Forensics Research Centre, Faculty of
managed, and at the same time the amount of waste
Environmental Studies, Universiti Putra Malaysia, 43400,
UPM Serdang, Selangor, Malaysia being dumped are greatly increasing. This problem has
e-mail: [email protected] affected the water quality causing the water quality to

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deteriorate (UNESCAP 2000). Discharge effluent Conventional methods for treating wastewater were
from the industrial and agriculture activities are high long conducted to provide a better water quality and to
in volume that such heavy metals, including organic treat it before being released into the water bodies.
compounds and some effluents were drained without Among the conventional water treatment conducted
proper treatment, which directly affected the water were chemical precipitation, coagulation, flocculation,
quality (UNESCAP 1999). Surface water and ground- ion exchange, membrane filtration and activated
water were also affected by the nonpoint sources carbon (Bailey et al. 1999; Sud et al. 2008; Demirbas
pollutants contributed by agricultural activities, where 2008; Chiban et al. 2012; Dave et al. 2012). However,
the usage of chemical fertilizers leaches into ground- the conventional methods were rather expensive, as
water and runoff. The high demand on the agricultural higher cost was needed during the operation. More-
products led to the high utilization of fertilizer in order over, the conventional methods tend to have residuals
to yield a high number of productions (Dzikiewicz and incomplete removal of the pollutants posing
2000). It has been found that exposure to staggering another problem (Chiban et al. 2012). Recently,
level of heavy metal such as arsenic to humans lead to scientists have been studying on using inexpensive
arsenic poisoning (Reddy et al. 2013; Tandon et al. adsorbents to remove heavy metals in the water. The
2013; Vadahanambi et al. 2013). The arsenic pollution low cost adsorbents used to practice adsorption
in the West Bengal districts of India, which caught the activities were usually waste products from another
world concern, has affected so many people who are production like agriculture, industrial and food pro-
living within that area (Das et al. 1995). The inorganic duction, which can be obtained abundantly.
arsenic in drinking water had caused the people who The common removal or stabilizing agents used to
consumed the polluted drinking water to be suffered stabilize heavy metals based on the recent studies are
with health problem (Basu et al. 2001). agricultural waste, oyster shells, crab shells, kaolinite,
Many studies found that the natural surface water portland cement, fly ash, mussel shells, lime and Fe
and groundwater are contaminated by heavy metals nanoparticles (Lee et al. 1997; Yoon et al. 2003;
either due to anthropogenic sources or natural geo- Vijayaraghavan et al. 2004; Moon et al. 2008; Tang
logical reason (Sarmani 1989; Karadede and Unlu et al. 2011; Seco-Reigosa et al. 2012). The main
1999). Trace metals were found to be accumulated in component in some natural products is calcium
the aquatic life and these protein sources were then carbonate (CaCO3), which can be used to immobilize
entered the human’s bodies through food cycle (Basu the hazardous components of the heavy metals (Bothe
et al. 2001). The accumulation of Cu, Zn, Pb, Cd and and Brown 1999; Ismail et al. 2013). The agricultural
Hg in the pink shrimp are said to be due to the release waste products have the ability to remove the metals in
of industrial discharge into the river water according to aqueous solutions effectively (Ferro-Garcia et al.
Biney and Ameyibor (1992). 1988; Demirbas et al. 2002; Wu et al. 2013). Among
Many types of treatments have been introduced to the agricultural wastes, which were popularly used to
remove the toxic metals in the water ranging from the remove heavy metals were rice husk, palm fruit shell,
expensive chemical treatment to the low cost biosorp- fruit seed, nut shells, and fruit peels (Tan et al. 1993;
tion. The chemical treatment for wastewater required Saifuddin and Kumaran 2005; Johan et al. 2011; Lim
mixture of chemical compound to reduce the metals et al. 2012; Olu-owolabi et al. 2012; Omri and Benzina
pollutant, yet the removal could not achieve as 2013; Sugashini and Begum 2013). These adsorbents
expected in the guideline (Sanchez et al. 1999; Ismail were called as low cost based on the economic value,
et al. 2013). Some treatment methods developed such abundant supply and can be easily collected from the
as coagulation, flocculation, reverse osmosis, mem- industrial, agricultural and food-processing produc-
brane separation, ion-exchange, solar photo degrada- tion (Bailey et al. 1999; Jain et al. 2013). The low cost
tion and ozonation were conducted either to remove or adsorbents, which review in present paper, are shown
degrade the pollutants in wastewater to harmless form in Fig. 1.
(Pal et al. 2012; Lim and Aris 2013; Prieto-Rodrı́guez The purpose of this review is to provide potential
et al. 2013). The hazardous state of the toxic metals is low cost materials used in the recent studies and also to
changed into a stable and safe state so that the threat to compare the efficiency of various low cost materials in
human and the environment is reduced. removing the metals. This review can serve as

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Low cost
Adsorbents

Fig. 1 Low-cost adsorbents reported in this review

examples for further studies on adsorption of heavy 2 Low cost adsorbents

metals using low cost products. Besides, the reviewed
low cost materials can include for the conventional 2.1 Nano zero-valent iron particles and minerals
wastewater treatments with a better economic aspect
and environmental sound method. Integration of ideas Recently, many studies have shown that arsenic can be
and knowledge upon the current technology can stabilized using agents such as cement kiln dust
provide a better wastewater treatment system and (CKD), New Zealand iron-sand, magnetite, activated
produce no secondary by-products of the treatment carbon, hematite, kaolinite, zeolite and natural pro-
activities. In this review, SWOT analysis was applied ducts like oyster shells (Jing et al. 2003; Singh and Pan
on the low cost adsorbent used in literature. SWOT 2006; Moon et al. 2008; Yadanaparthi et al. 2009; Ok
analysis of low cost adsorbent was applied to provide a et al. 2010; Kim et al. 2011; Moon et al. 2011; Panthi
perceived sight of an alternative water treatment and Wareham 2011).
method. Findings of SWOT for application of low cost pH plays an important role in affecting the adsorp-
adsorbents in removing heavy metals from water and tion rate, where the change of solution pH directly
wastewater also contribute a better understanding of contribute to the available sites of the adsorbents.
new water management and help in sustainable water Panthi and Wareham (2011) revealed that at pH 7,
management. New Zealand iron-sand has the maximum removal of

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4 mg/L As(III). At pH 3, 63.0 % of As(III) was being et al. 2009). The stabilized state of iron nano particles
adsorbed by the New Zealand iron-sand and at pH 11, also affects the reduction of the chromium in water and
the adsorption had reduces to 44 %. On the other hand, soil. Cr(VI) is effectively reduced to Cr(III) by using
adsorption for As(V) showed a good match in acidic the zero valent iron particles stabilized with carboxy-
pH, approximately 97.6 % of As(V) was eliminated in methyl cellulose, the harmful chromium form was
the pH range of 3.0–6.0 (Panthi and Wareham 2011). changed to a less toxic form by this reducing agent
The pH effects also occurred on the precipitation of with 90 % of 34 mg/L Cr(VI) being reduced in water,
arsenic on a calcium source (Bothe and Brown 1999). when the Fe dosage increased up to 0.12 g/L (Xu and
However, for the contact time between this adsorbents Zhao 2007). This study showed that the stabilized iron
and arsenic, it did not reach 100 % removal. For the nano particles had a better kinetic uptake for Cr(VI) as
first 24 h, only 77.3 % of 4 mg/L As(III) has removed compared to Cao and Zhang (2006) which used non
by this adsorbent, while for 4 mg/L of As(V) only scale iron particles (Xu and Zhao 2007). However, the
57.6 % has removed after the first 36 h (Panthi and carboxymethyl cellulose used as stabilizer for iron
Wareham 2011). Long contact times are required in nanoparticle is prone to decompose due to its organic
order to achieve more metals removal. structure, which can weaken the effectiveness of iron
According to Kim et al. (2011), a higher percentage nanoparticle in stabilizing Cr(VI) (Xu and Zhao 2007).
of arsenic was immobilized by nano-sized magnetite Magnetite is also one of the famous adsorbent for
coated with sodium dodecyl sulfate, follow by the heavy metal uptake. The magnetite reduced from
magnetite, zero valent iron and the nano-sized zero hematite by therma-mechanical reduction at 570 °C to
valent iron coated by sodium dodecyl sulfate. The powder mass of 25/1 for 15 h was observed to have a
surface coated on the nano-sized particle has made the better removal of Cr(VI) at pH 2 than the magnetite
mobility of magnetite to be effective in the arsenic reduced at 600 °C (Javadi et al. 2012). This is due to
contaminated soil where the magnetic component of the small crystalline particles generated in the longer
the magnetite has coated with negative charge of mechanical time. However, the removal percentages
sodium dodecyl sulfate to prevent aggregation in the of Cr(VI) by nanocrystalline magnetite were not high
soil particles (Kim et al. 2011). Aredes et al. (2012) at most only 40 % of removal for initial Cr(VI) of
studied that magnetite, goethite and laterite could 20 mg/L at pH 2 (Javadi et al. 2012). The adsorbents
remove 100 % of As(V) (5 ppm) in water while dosage needs to be increased in order to observe a
hematite only adsorbed 20 % As(V) due to saturation, higher removal percentage for this study because the
yet the hematite amount added to the arsenic solution increased of dosage can provide more binding surfaces
was only half of the amount of magnetite, goethite and for the metal ion (Singha and Das 2011).
laterite. Aredes et al. (2012) also conducted a simple Ultrafine Fe2O3 (a-Fe2O3) nanoparticles which was
household treatment test on 20 ppm of As(V) solution, proven by Tang et al. (2011) was able to remove
with just manual shaking of 100 ml As(V) and 5 g of As(III) and As(V) in a small amount. The As(III) with
laterite, the initial As(V) solution were reduced to concentration of 0.115 mg/L was totally removed by
1 ppm in 10 min, proving that natural iron material is 0.06 g/L Fe2O3 nanoparticles while for 0.095 mg/L of
a great source for easy and fast water treatment As(V) only 0.02 g/L of Fe2O3 nanoparticles (a-Fe2O3)
application. The zero-valent iron loaded with a high was required for 100 % removal (Tang et al. 2011).
amount of Fe with proportion of 95 % iron concretion, This study has also demonstrated on the commercial
2.5 % of carbon and 2.5 % of lime, and 90 % iron Fe2O3 powder, and the results revealed that the Fe2O3
concretion, 5 % of carbon and 5 % of lime have higher nanoparticles had two times higher removal percent-
removal of arsenic (500 ppm) which is about 99.95 age of As(III) and As(V) than the commercial Fe2O3
and 99.94 % of removal as compared to the zero- powder, which shows that the Fe2O3 nanoparticle has
valent iron loaded with lower Fe but substitute in other a great commercialize value (Tang et al. 2011). The a-
materials like carbon and lime with removal of Fe2O3 showed that modification can improve the
50.27 % only (Alshaebi et al. 2009). However, pH adsorption capacity of adsorbent in removing the
also constituted to the arsenic removal, low pH As(III) with the increased of surface areas for metal
remove higher amount of arsenic than high pH ions (Tang et al. 2011). Another study had enhanced
especially when the pH value is more than 7 (Alshaebi the Fe nanoparticle by coating SiO2 (Fe@SiO2) on the

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surface, this Fe@SiO2 successfully removed 100 % of also is another interesting method to enhance the metal
70 mg/L Cr(VI) in 180 min (Li et al. 2012a). The SiO2 uptake ability. The clay coated with iron oxide showed
coated on the Fe nanoparticles restrained the jumble a great removal of Pb(II) than the natural clay and
up of Fe particles and providing the Cr(VI) the ability natural sand (Eisazadeh et al. 2013). The pH of metal
to adsorb on the surface easily. The factors of solution influences the removal efficiency of clay type.
preparing Fe@SiO2 indeed are crucial as the speed In Zhao et al. (2013), the Cr(VI) were highly removed
injection of boron hydride and amount of tetraethyl- in pH 2 because slight amount of natural components
orthosilicate (TEOS) affect the Cr(VI) removal ability such as Al2O3 and Fe2O3 from the Akadama clay had
of Fe@SiO2 (Li et al. 2012a; Ponder et al. 2000). leached out to bind with Cr(VI). This phenomenon
was also observed by Helios-Rybicka and Wójcik
2.2 Calcium carbonate and seafood waste (2012) where the iron oxide and manganese oxide
were found to leach out from the kaolinite and
Calcium carbonate and seafood waste were used to immobilized the toxic metals. Combined of two types
remove heavy metal due to the precipitation occur of adsorbents were done by El-Eswed et al. (2012) and
between the metal ions and carbonate from the Yousef et al. (2009), using kaolinite and zeolite tuff to
adsorbents (Patterson et al. 1977; Sdiri and Higashi remove multiple ions. The removal performance of
2012). The cement kiln dust, which contains calcium kaolinite-zeolite tuff was successfully greater than the
carbonate, is one of the examples that were used in alone material (El-Eswed et al. 2012).
stabilizing harmful state of arsenic (Moon et al. 2008, The uses of natural products from seafood are very
Woolard et al. 1999). The cement kiln dust with popular in the recent researches as they can be easily
mixture of kaolinite showed potential removal of As obtained, cheap and the products can be recycled
(III)and As(V) in the soil but the As(III) and As(V) in instead of being waste products. Many studies found
the mixture of cement kiln and montmorillonite are that metal ions can be reduced by using natural oyster,
higher than the concentration in kaolinite after 1 and crab and mollusk shells as its adsorbent (Lee et al.
7-day treatment (Moon et al. 2008). This showed that 1997; Rahman et al. 2008; Moon et al. 2011; Du et al.
the clay type also played a role in the stabilizing the 2012; Ismail et al. 2013). The natural oyster shell
heavy metals as the kaolinite is a 1:1 type clay where could reduced 72 % of 4,779 mg/kg of arsenic in the
the cation exchange is low and the arsenic anion can mine tailing after 28 days of treatment with 30 %
effectively removed from the soil. Positively charged natural oyster shell weight to the sample; for the
kaolinites and other clay type are greatly suitable for calcined oyster shell at 25 % weight, it effectively
anionic species of metals adsorption (Matusik and reduced 99 % of arsenic with the same contact period
Bajda 2013). This clay type adsorbent can be used for of 28 days (Moon et al. 2011; Seco-Reigosa et al.
removal of metals in aqueous solution. In Jiang et al. 2012). Best arsenic reduction results is shown by using
(2013), the 2:1 type clay used to adsorbed Cd(II) ions the calcined oyster shell with the Portland cement
were also found to contain large amount of calcium treatment, which surpassed its natural product, and its
and other negative charge minerals, which influenced combination with cement kiln dust achieved 95 %
the metal ions adsorption. The calcium content reduction of arsenic in 7 days period because of the pH
increased the pH, strongly decreased the mobility of and calcium contents in its combination with Portland
metal ions such as Cd(II) ions in soil and water cement (Moon et al. 2011). The natural products need
(Gerritse 1996). to be enhanced or modified with other products in
Modifications on the natural clays were conducted order to boost the reduction ability on the heavy
in several studies to improve the metals adsorption metals, where the increase of available calcium on the
efficiency. Djukic0 et al. (2013) discovered the adsorbents will improve the kinetic uptake of the
removal efficiency of Serbian natural clay improved heavy metals (Seco-Reigosa et al. 2012; Vieira et al.
after undergo milling process. The Cd(II) and Ni(II) 2012). Besides, the calcined oyster shells and natural
ions were reduced up to 87 % from the initial of 9.45 oyster shells also achieved a different heavy metals
and 10.2 mg/L, respectively, due to the increased of reduction (Liu et al. 2009; Ok et al. 2010). The natural
surface area and the increased of exchangeable cation oyster shells are consisting mainly CaCO3, which is in
capacity (Djukic0 et al. 2013). Surface coating clay the non-reactive form, while the calcined oyster shells

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changed the ordinary state of the natural oyster shell eggshell as the calcinations enhanced the adsorption of
into CaO, which is the reactive form (Yoon et al. 2003; metal, but for Pb(II), natural eggshell was preferable in
Ok et al. 2010). The surfaces of the modified shells removing it from the wastewater due to the present of
were also improved with more porous and available its soluble species (Park et al. 2007). The Cd and Cr
site for adsorption of heavy metal ions (Liu et al. were suitable in higher pH value uptake for these
2009). Study had shown that the calcined oyster shells adsorbents than the Pb, which favored slightly lower
had better stabilization of Cd and Pb in the soil than the pH (Park et al. 2007). Park et al. (2007) also conducted
unmodified oyster shells due to the quicklime, which removal of Cd(II), Cr(VI) and Pb(II) in real wastewa-
changes the soil pH (Ok et al. 2010). This same ter by using the calcined eggshell which showed a
adsorbent is applicable in the contaminated metal great potential for application in the industrial waste-
solution. water since the metals could effectively reduce and the
In Tudor et al. (2006), clam, oyster, and lobster acidic wastewater has also shifted to neutral condition.
shells were used to carry out metal adsorption on Efficiency of natural hen and duck eggshells were
10,000 mg/L of Pb(II) and Cd(II), respectively with compared with the boiled hen and duck egg shells in
comparison of adsorption capacity of using limestone removing lead (2.365 mg/L) in the battery wastewater
and chitosan. The clam, oyster and lobster shells had by Arunlertaree et al. (2007). This study focused on
the best uptake capacity for Pb with[99.9 % after 1, 5 the optimum pH, contact time and adsorbent dosages
and 326 h; while for Cd, only clam shell had the best obtained from the experiment, showed the ability of
removal capacity which is [99.9 % after 24 and egg shells in removing 100 % of lead in real waste-
168 h. This is due to the larger adsorption surface of water (Arunlertaree et al. 2007). In fact, the natural
lobster and oyster shell (Tudor et al. 2006; Du et al. duck shells had shown to have higher adsorption
2012). However, shells and chitosan appeared to be capacity, which is 1.643 mg/g, compared to the
effective in removing Hg in the water due to the natural hen egg shells, which is 1.457 mg/g. This
organic constituent on the lobster shells surface and can be explained by the volume of pores on natural
the chitosan enable Hg to bind with the organic duck egg shells which were more and higher with level
compound (Tudor et al. 2006). of protein fibers than natural hen egg shell (Arunl-
ertaree et al. 2007). The protein fibers were not broken
2.3 Egg shells down in its natural state, making it held lead ions better
than the boiled egg shells in acidic condition (Arunl-
In recent times, carbonated shells from food industries ertaree et al. 2007). Both Park et al. (2007) and
have been commonly used in many studies to perform Arunlertaree et al. (2007) proved that eggshells are
metal ions adsorption due to its abundances after food very suitable for battery wastewater treatment with
processing (Ahmad et al. 2012; Wang et al. 2013). high removal efficiency; natural characteristics of
Eggshells are one of the examples of carbonate shells eggshells can act as pH adjuster, which makes this
used for metal removal. The natural chicken eggshells adsorbent, has budgetary and environmental friendly
were used to remove 96.43 % of 7 mg/L of Fe(III) in values.
the aqueous solution with the optimum temperature of
20 °C and dosage of 2.5 g/L with control pH 6 2.4 Chitosan
(Yeddou and Bensmaili 2007).
pH has always been the control factors for adsorp- Chitosan is well known for having the ability to
tion of heavy metals, depending on the metal, certain remove heavy metals in the water based on the
metals prefer more neutral pH and higher pH for previous study (Bailey et al. 1999; Saifuddin and
effective removal to occur because of the negatively Kumaran 2005; Pontoni and Fabbricino 2012). Cu(II)
charged surface which promote more adsorption to with initial concentration of 200 ppm was found to
take place; while anionic metals prefer lower pH for bind effectively with the chitosan with its small ionic
better adsorption between adsorbents in aqueous diameter of 70 pm, which demonstrated 99.25 % of
solution (Kadimpati et al. 2012; Suteu et al. 2012). Cu(II) removal in aqueous solutions (Uzun and Güzel
The calcined eggshells showed fast removal of 3 mg/L 2000). In contrast, Mn was found to be the least being
of Cd and Cr, respectively, as compared to the natural removed among Fe, Ni and Cu due to its bigger ionic

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diameters and its stable complex which only form and solution temperature of 25 °C compared to the
hydroxide and carbonate in alkaline condition (Uzun acid treated coconut shell and chitosan coated coconut
and Güzel 2000; Choi et al. 2007). because the coconut shell treated with acid and coated
In the recent studies, chitosan is often combined with chitosan has the most surface areas for Zn(II) to
and modified with other adsorbents to promote its attach on (Amuda et al. 2007). The adsorption
effectiveness. Chitosan coated acid beads were able to capacities of the modified coconut shells were also
reduced 65 % of 20 mg/L Cr(VI) at pH 1–92 % well represented by the Langmuir and Freundlich
removal at pH 5 (Nomanbhay and Palanisamy 2005). isotherm (Amuda et al. 2007).
Chromium and arsenic are pH dependent metals, the Adsorption of heavy metals on the natural product
changes of the pH will directly affect the adsorption has also successfully removed the heavy metals from
performance (Nomanbhay and Palanisamy 2005, contaminated water. Coconuts coir activated carbon
Singha and Das, 2011). Adsorbent dosage also influ- was used in Chaudhuri and Azizan (2011) to remove
enced the adsorption activities, 86 % of 20 mg/L of the Cr(VI) in the aqueous solution. The contact time,
Cr(VI) was removed by 13.5 g/L of chitosan coated adsorbent dosage and pH factors affected the adsorp-
acid beads, 64 % removal of Cr(VI) with 18 g/L of tion of Cr(VI), Cu(II) and Cd(II) by the coconut coir
chitosan coated beads, and 52 % Cr(VI) removal by activated carbon (Chaudhuri et al. 2010; Chaudhuri
24 g/L of commercial activated carbon (Nomanbhay and Azizan 2011). The Cr(VI) with 20 mg/L of
and Palanisamy 2005). The optimum agitation speed concentration was removed 100 % with the 8 g/L of
enables homogeneous surface binding to occur at the coconut coir activated carbon and the optimum
maximum condition (Nomanbhay and Palanisamy adsorption occurred between pH 1–2 as the H? in
2005; Bhuvaneshwari et al. 2012). the solution alter the adsorbents’ surface charges
(Chaudhuri and Azizan 2011). pH always influence
the adsorbent’s metal uptake, as such Cr(VI) ions are
3 Agricultural waste preferable to be removed in acidic condition (Aliabadi
et al. 2006). The coconut coir activated carbon have
3.1 Coconut husk also shown a better adsorption capacity compared to
the commercial activated carbon and its adsorption of
Coconut husks are waste product of coconuts and it is Cu(II) and Cd(II) which fits well in Langmuir isotherm
usually available in abundance in the tropical coun- (Chaudhuri et al. 2010). This study showed that
tries. The high tannin in the coconut husk makes it a coconut coir activated carbon is another good alter-
good metal adsorbent (Abdulrasaq and Basiru 2010). native for removing heavy metals in water.
pH of the working solutions gave a significant
influence in the adsorption process because 50 mg/L 3.2 Rice husk
Fe(III), 50 mg/L Cu(II) and 10 mg/L Pb(II) were
removed best in pH 5, where the removal capacities Rice is one of the main food sources in some countries,
were almost 90 % and precipitation can be avoided. and it has been growing largely especially in South
The adsorption of Fe(III) and Cu(II) using coconut East Asia countries. The waste produced from the rice
husk also obeyed the Freundlich isotherm with R2 packaging has been chosen as one of the popular low
value equal to 1, implicating the adsorption of Fe(III) cost adsorbent to remove heavy metals in water
and Cu(II) occurred due to the chemical bonding; because of its highly available amount from the
while the Pb(II) showed better adsorption in Langmuir production. The utilization the by-product of rice such
isotherm. The three metals also well described in the as rice husk will positively contribute to economic
second-order kinetic which illustrated the occurrence yield (Chakraborty et al. 2011).
of chemisorptions (Abdulrasaq and Basiru 2010). In Rehman et al. (2011), the ordinary rice husk was
Modified coconut husk is proven to have a better modified with polyaniline for a better adsorption
adsorption of heavy metal. The coconut shell treated performance. From all the observed factors, pH,
with acid and coated with chitosan has the best contact time, agitation speed, temperature, it was
removal performance for 25 mg/L zinc with 93 % found that the polyaniline/rice husk showed the highest
removal at pH 6, 30 g/L of adsorbent, 3 h contact time removal of Cd(II) which were 93.08 % (20 min),

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97.5 % (30 °C),and 94.45 % (100 rpm) as compare to (Wantala et al. 2012). pH also influenced the adsorp-
the ordinary polyaniline and polyaniline/saw dust tion of As(V) where As(V) was highly adsorbed in the
which have lower removal percentage (Rehman et al. acidic form (Wantala et al. 2012). Wantala et al. (2012)
2011). The polyaniline/rice husk and polyaniline/saw also suggested that rice husk MCM-41 loaded with iron
dust also fits better in Langmuir isotherm, while simple to be used on the real contaminated groundwater and
polyaniline is well represented by Freundlich. This regenerate the used adsorbent, while for the exhausted
showed that the adsorption occurred on the monolayer adsorbent need to be placed in a well-aerated sand filter
of the polyaniline/rice husk and polyaniline/saw dust to prevent the toxic leachability.
while for the simple polyaniline, the adsorption The rice husk activated with higher temperature
occurred on the heterogeneous surface (Rehman et al. imposed a higher yield of heavy metals because the
2011). Besides, the modified rice husk used throughout pores on the surface increased which improves
this study can be reused after regeneration of the adsorption efficiency (Yahaya et al. 2010; Tseng
adsorbents by using nitric acid (Rehman et al. 2011). et al. 2006). The different activation times and
Rice husk was also being modified in Johan et al. temperatures gave a significant effect on the rice husk
(2011) by incinerating the rice husk with a microwave activation ash which would affect the removal amount
incinerator at 500 and 800 °C to turn it into ashes of the heavy metals. Yahaya et al. (2010) studied that
form. The removal of Cu(II) was affected by the pH, the most favorable of activation time and temperature
the removal capacity increased when the pH increased for rice husk activation ash to remove 50 mg/L of
accordingly. The rice husk ash produced from 800 °C Cu(II) were at 737 °C and 1.82 h with the removal of
has revealed a better adsorption of Cu(II) with 71.4 % 11.7 % of Cu(II).
of 10 mg/L Cu(II) removal at pH 5 while for the rice
husk incinerated in 500 °C, its removal capacity was
66 % (Johan et al. 2011). This can be explained when 3.3 Palm fruit
the structure of rice husk incinerated in 800 °C has
exposed with more pores as compared to rice husk Palm oil plantations are one of the most lucrative
incinerated in 500 °C. This has allowed the adsorption agricultural activities in Malaysia. Tones of palm oil
to occur on the surface of the ash. The Freundlich and products from palm fruits were produced every
isotherm and pseudo kinetic second order also well year. This massive industry has also generated agri-
represent these adsorbents as the adsorption happened cultural waste from the beneficial production (Saifud-
in the multilayer of the ashes (Johan et al. 2011). din and Kumaran 2005). In Ideriah et al. (2012), the
In order to have an effective adsorption, rice husk removal of Cr by palm fruit fiber biomass at pH
was also treated both chemically and physically to between 4 and 10 was very low, while Pb was removed
improve its uptake performance. The activated rice 100 % at pH 10 and Cu was removed 100 % at pH 10
husk treated with KOH and K2CO3 had proven that the and 12. However, the maximum adsorption of Pb by
adsorption capacity was 441.52 mg/g, which is higher okra waste was optimized at pH 5 (Hashem 2007).
compared to the other absorbent such as bamboo, This showed that Pb is pH dependent but at the same
cotton stalk, pine wood powder, coffee ground, and time depends on the adsorption materials, which are
durian peel (Foo and Hameed 2011). This is due to used to remove heavy metals in aqueous solution
increased of BET surface area, external surface area (Hashem 2007; Ideriah et al. 2012). Issabayeva et al.
and pore size, which influenced the adsorption process (2010) has shown that Cu(II) is a pH-dependent
(Foo and Hameed 2011). because the Cu(II) at pH 3 was not effectively
Rice husk MCM-41 loaded on with Fe also found to removed as compared to pH 5, Cu(II) was highly
be a great adsorbent for 3 mg/L As(V) and 4.5 mg/L adsorbed by the palm shell activated carbon. The palm
As(III). The Fe content prepared by Wet Impregnated shell was observed to have better adsorption with
Technique (WIT) showed lower adsorption value than single Cu(II) than with Cu(II) in complexing agents
the Fe content prepared by Direct Hydrothermal which were the malonic acid and the boric acid where
Technique (DHT) (Wantala et al. 2012). However, the concentration of Cu(II) with the presence of these
with the increased of Fe in DHT, the adsorption of complexing agents was higher than the single Cu(II) in
As(V) was lower due to the insufficient surface area the aqueous solution (Issabayeva et al. 2010).

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Rev Environ Sci Biotechnol (2014) 13:163–181 171

3.4 Nut shell Cu(II), Pb(II) and Zn(II) as compared to chestnut

pretreated with acid formaldehyde, which causes the
Recently, agriculture wastes have been very popular swelling of the adsorbent surface (Vázquez et al. 2009;
among the other low cost bioadsorbents since the cost 2012). 100 mg/L of Cd(II) was removed faster by
is inexpensive and the amounts can be easily collected using the chestnut shell pretreated with NaOH in
in a large volume. Modified cashew nuts showed a comparison with Zn(II), Cu(II) and Pb(II) (Vázquez
great potential in removing Cu(II), Cd(II), Zn(II) and et al. 2012). This is due to the negatively charged
Ni(II) with the maximum adsorption capacity of surface of the pretreated chestnut shell, which attracts
406.6, 436.7, 455.7 and 456.3 mg/g based on Lang- adsorption to occur. Pb(II) and Cd(II) were pH
muir isotherm (Kumar et al. 2012). Several factors dependent metals, as the pH changes from 2 to 4, the
such as pH, temperature, initial concentration, and higher amount of 20 mg/L of Pb(II) and 20 mg/L of
contact time affect the adsorption kinetics. The best Cd(II) were being adsorbed by walnut shells with the
pH value for maximum adsorption of modified cashew removal of[90 % for Pb(II) and almost 90 % removal
nuts were pH 5 with 100 % removal for 100 mg/L of for Cd(II) (Almasi et al. 2012).
Cu(II), as for the optimum temperature was 30 °C Modified base-washed peanuts shells with citric
while for the initial concentration, the lower metal acid demonstrated a better removal ability of Cd(II),
concentrations achieved the highest adsorption com- Cu(II), Pb(II), Ni(II) and Zn(II) than some of the
pare to the high initial concentration due to the commercial resins such as Duolite GT-73 and car-
saturation state of the absorbents (Kumar et al. 2012). boxymethyl cellulose (Chamarthy et al. 2001). While
The castor seed hull showed to have almost five for mixed metal ion solution of Cd(II), Zn(II), and
times adsorption capacity than the activated carbon in Cr(III) in Cimino et al. (2000), Cr(VI) is found to be
comparison with the same fix contact time (300 min) removed most compare to the other two metals. This
and initial concentrations (5, 10, 20, and 30 ppm) (Sen study contributed that agricultural waste can be an
et al. 2010). The uptake of Cd(II) in the aqueous alternative to remove metals in a cheaper cost with
solution by the castor seed hull were influenced by the relatively simple modifications.
pH where the adsorption at acidic state was lower and
as the pH increased, the adsorption capacity improved 3.5 Fruit bagasse
due to the negative-charged surface which attracted
the Cd(II) (Sen et al. 2010). pH also influenced the Fruit bagasse is the fibrous residue from the extraction
uptake of Cr(VI) by using cornelian cherry, apricot of the fruit juice. It is normally abundant from the food
stone and almond shells where the removal capacity industries after massive of food and beverage produc-
for 105 mg/L of Cr(VI) was 99.99 % with the tion or packaging (Chakraborty et al. 2012). Studies
optimum pH of 1 (Demirbas et al. 2004). have found that fruit bagasse contained high amount of
Comparison between the effectiveness of peanut hydroxyl and phenolic functional groups, have the
hull carbon (PHC) and granular activated carbon ability in reducing heavy metals in water (Villaescusa
(GAC) in removing Cu(II) had been conducted by et al. 2004; Farinella et al. 2007; 2008; Chakraborty
Periasamy and Namasivayam (1996), showed that et al. 2012). Grape bagasse from the wine production
PHC performed a better recovery of Cu(II) in aqueous showed potential in removing cadmium and lead with
solution and wastewater. This study revealed that the adsorption capacity of 0.479 and 0.204 mmol/g esti-
PHC was able to remove 95 % of 20 mg/L of Cu(II) mated from Langmuir isotherm (Farinella et al. 2007).
with 0.9 g/L of carbon concentration while GAC Sugar cane treated with sulphuric acid and sugar
needed 13 g/L of carbon concentration. PHC also used cane activated carbon were used to remove Cd(II)
2.5 times shorter period to remove Cu(II) (10, 15 and (Krishnan and Anirudhan 2003). Sugar cane treated
20 mg/L) compared to GAC (Periasamy and Namas- with 8.9 % of sulphuric acid had maximum adsorption
ivayam 1996). This study had proven that agricultural of 98.8 % of 50 mg/dm3 Cd(II) while for sugar cane
waste is a time effective and economic-wise activated carbon, 56.8 % of 50 mg/dm3 Cd(II) were
absorbent. removed at pH 6 with (Krishnan and Anirudhan 2003).
The chestnut shell pretreated with 4 % of NaOH The pH affected the surface of the bagasse adsorbents
were found to be more efficient in removing Cd(II), by changing it to have negative charges and caused the

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172 Rev Environ Sci Biotechnol (2014) 13:163–181

adsorption of Cd(II) to increase after treated with 5.1 Strength of low cost adsorbents
higher percentage of sulphuric acid (Krishnan and
Anirudhan 2003). ‘‘Low cost’’ by the words itself has explained the
financial meaning of inexpensive and affordable. The
strengths of low cost adsorbents based on SWOT
4 Bone charcoal analysis are cheap in term of cost, abundant amount in
the environment and easily obtain, as most of the
Bone charcoals were usually retrieved from the animal adsorbents are waste products. The low cost materials
bone, and calcinations are conducted to change the used to perform heavy metals adsorption in this paper
original morphology of the bone for further utilization. are basically the waste or by-products of manufactur-
The bone charcoal, which has the properties of carbon ing and food industries. One of the examples is mollusk
and calcium carbonate (CaCO3), is capable to remove shell, which can be easily obtained from either the food
heavy metals like Cu(II) and Zn(II) and also some industries or collect from the coastal area (Moon et al.
organic compounds (Wilson et al. 2003). Dahbi et al. 2011; Seco-Reigosa et al. 2012; Suteu et al. 2012).
(2002) has reported using bone charcoal from bovine to These products will become waste after either being
remove Cr(III) in wastewater where the removal of consumed by humans and cause odor and aesthetic
Cr(III) involved the reaction between the calcium in the problem if these wastes are not well-managed (Ok et al.
bone charcoal. The study revealed that the use of camel 2010; Seco-Reigosa et al. 2012; Suteu et al. 2012). By
bone charcoal in removing Hg(II) is due to the ion- using these materials to conduct heavy metals removal,
exchange of mineral component on the bone charcoal, will help to solve the pollution problem, furthermore,
such as calcium and phosphate components (Hassan less cost is needed to pre-treat the materials before the
et al. 2008). pH also influenced the metal removal adsorption activities (Moon et al. 2011; Ok et al. 2010).
activities where the pH range affects the adsorption Besides, the by-product from agricultural production
characteristics of the activated carbon. The Cr(VI) like rice husk, rice bran, rice straw, palm oil husk, nut
amount adsorbed by the activated carbon apricot stone shell, apricot stone, fruit baggasses, sugar cane bagg-
decreased when the pH increased, Cr(VI) is preferably ases and coconut husk are also easily available as these
to be adsorbed in an acidic condition (pH 1) with the are the wastes from the agricultural production (Cha-
removal capacity of 99.99 %; while for cadmium, marthy et al. 2001; Chang et al. 2012; Demirbas et al.
cobalt, Cr(III), nikel and lead, the amount adsorbed by 2004; Farinella et al. 2007; Ferro-Garcia et al. 1988;
activated apricot stone increased with higher pH Hashem 2007; Ideriah et al. 2012; Johan et al. 2011;
(Demirbas et al. 2004; Kobya et al. 2005). The pH of Kakalanga et al. 2012; Kobya et al. 2005; Krishnan and
the aqueous solution is directly affecting the metals Anirudhan 2003; Rehman et al. 2011). These products
adsorption activities for the pH dependent metals. are so abundance as they are generated from the daily
food production. Moreover, these products have a great
ability in removing heavy metals in water and no
5 Gap and future perspectives on low cost secondary product or sludge is generated. This ability
adsorbents has made these adsorbents bonus in water treatment
system. Besides, some studies have also conduct
The usage of low cost adsorbents has introduced a new regeneration of the used adsorbents which also make
alternative for water treatment system, and it also the low cost adsorbents can be reused again, making
brings more opportunities in producing a better way of these materials a new alternative for water management
management. The future perspectives of low cost (Rehman et al. 2011; Bhuvaneshwari et al. 2012). At the
adsorbent can be determined by SWOT analysis where same time, regeneration of the used adsorbents pro-
the strength, weakness, opportunities and threats of motes sustainability water treatment products.
low cost adsorbents can be identified. The weakness
and threats should be identified and changed to 5.2 Opportunities of low cost adsorbents
strength and opportunities to provide sustainable
products in removing heavy metals in water (Praveena SWOT analysis also focuses on the opportunities of
and Aris 2009). low cost adsorbents in water treatment system. The

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Rev Environ Sci Biotechnol (2014) 13:163–181 173

Table 1 Summary of SWOT analysis for low cost adsorbents

Strengths Weaknesses

Cheap and inexpensive materials (Bailey et al. 1999; Gupta and Suhas 2009; Usually the adsorbents are not in readily form
Kurniawan et al. 2006)
By-products from agricultural and industrial activities (Chamarthy et al. 2001; Pre-treatment and pre-washing processes are needed
Chang et al. 2012; Demirbas et al. 2004; Farinella et al. 2007; Ferro-Garcia (Tudor et al. 2006)
et al. 1988; Hashem 2007; Ideriah et al. 2012; Johan et al. 2011; Kakalanga
et al. 2012; Kobya et al. 2005; Krishnan and Anirudhan 2003; Rehman et al.
2011)
Abundant in the environment (Chang et al. 2012; Kurniawan et al. 2006) Some materials do not appear to be good adsorbents
in natural form (Moon et al. 2011)
High ability in removing heavy metal from water (Saravanane et al. 2001; Some adsorbents are only suitable for certain metal
Zahra 2012) ions (Ahmad et al. 2012)
Opportunities Threats

Costs for water treatment system can be reduced (Patil 2012) May cause insufficient of adsorbents due to the high
demand in dosage
Long hour of contact period can be reduced (Periasamy and Extra chemical costs may be needed for pH adjusting to
Namasivayam 1996) provide suitable condition for optimum adsorption to
Modification and enhancement of low cost adsorbents can turn into occur
marketable products
Improvement and potential replacement for the conventional water
management system (Gupta and Suhas 2009; Patil 2012)

studies on low cost adsorbents have reported for cost enhancements are needed to change the original state
and time-efficient, this can be used to replace the to reactive form for a better adsorption result (Liu et al.
expensive and time-consuming treatment methods 2010b; Park et al. 2007; Quintela et al. 2012). Besides,
(Arunlertaree et al. 2007; Champagne and Li 2009). some adsorbents in small amount or too much dosage
The low cost adsorbents can be pre-treated or modified cannot remove metal ions in water due to the
to improve the current efficiency in order to produce a insufficient binding surfaces and aggregation (Yeddou
marketable product for the water management system and Bensmaili 2007). Some adsorbents are particu-
and the manufacturing industries (Hsien and Liu larly effective on selected metal ions while failed on
2012). Besides, the low cost adsorbents are environ- the other metal ions (Ahmad et al. 2012). Enhance-
mentally friendly product, making it a better choice for ment and modification can be done in order to produce
water management (Kırbıyık et al. 2012). The oper- better adsorbents for metal ions uptake (Chamarthy
ational cost can be reduced with the addition of et al. 2001; Liu et al. 2012).
adsorbents to the traditional water treatment system
(Martinez-Juarez et al. 2012). 5.4 Threat of low cost adsorbents

5.3 Weakness of low cost adsorbents The over-explored of low cost adsorbents is the threat
toward low cost adsorbents. When the low cost
The weakness of low cost adsorbents has pointed out adsorbents are being widely used, the demand will
by SWOT analysis, as the low cost adsorbents are be higher than the supply. This will also caused
usually not readily available. The low cost adsorbents problem to the industries due to the insufficient supply.
usually present as raw materials (Liu et al. 2009). Besides, some metal ions are pH dependent and it will
Cleaning and pre-treatments are needed in order to cause the treatment system to use more chemical to
eliminate the residue of contaminants on the surface of adjust the suitable pH for the adsorbents. Desorption
the low cost adsorbents (Hadi 2012; Liu et al. 2009). of metal ions can be done in order to regenerate the
Some low cost materials do not appear to be good adsorbents for the further usage (Bhuvaneshwari et al.
adsorbents in its natural form, modification and 2012; Grover et al. 2012; Hsien and Liu 2012). By this

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 Table 2 Summary of adsorption capacity/removal efficiency at equilibrium for the adsorbents conducted in the previous studies
174

Types of materials Adsorption capacity (mg/g)/removal efficiency (%) References

As(III) As(V) Cr(VI) Cu(II) Cd(II) Zn(II) Ni(II) Pb(II) Co(II) Mn(II) Fe(III)

123
Coconut shell 20.0 mg/g Alaerts et al. (1989)
Coconut shell 6.0 mg/g Selomulya et al. (1999)
Dust coal 4.4 mg/g
Hazelnut shell 177.0 mg/g Cimino et al. (2000)
Resin-supported 28 mg/g, 90 % Ponder et al. (2000)
ferragel
Bituminuous coal 44.4 mg/g Hamadi et al. (2001)
Sawdust 1.9 mg/g
Petroleum pitch 23.7 mg/g Park et al. (2003)
Bone charcoal 27 ± 1.3 mg/g 24.5 ± 3.0 mg/g Wilson et al. (2003)
Almond shell 20.0 mg/g Demirbas et al. (2004)
Apricot shell 21.0 mg/g
Hazelnut shell 170.0 mg/g Kobya (2004)
Hevea brasiliensis 44.1 mg/g Karthikeyan et al.
sawdust (2005)
Terminalia arjuna nuts 28.4 mg/g Mohanty et al. (2005)
Palm shell charcoal 154 mg/g Saifuddin and Kumaran
coated with chitosan (2005)
Pine leaves (pH 2, 99 % Aliabadi et al. (2006)
15 mg/g Cr(VI)
Nano scale zero valent 1.75 mg/g, 24–38 % Cao and Zhang (2006)
iron
Chitosan-coated acid 60.41 mg/g Amuda et al. (2007)
treated coconut shell
carbon
Chitosan-coated 50.93 mg/g
coconut shell carbon
Acid treated coconut 45.14 mg/g
shell carbon
Natural hen egg shell 1.457 mg/g Arunlertaree et al.
(2007)
Boiled hen egg shell 1.092 mg/g
Natural duck egg shell 1.643 mg/g
Boiled duck egg shell 1.236 mg/g
Fly ash(pH 8.5, 92.20 % Sharma et al. (2007)
1.5 mg/L Mn)
Rev Environ Sci Biotechnol (2014) 13:163–181
 Table 2 continued
Types of materials Adsorption capacity (mg/g)/removal efficiency (%) References

As(III) As(V) Cr(VI) Cu(II) Cd(II) Zn(II) Ni(II) Pb(II) Co(II) Mn(II) Fe(III)

Sodium carboxymethyl 255 mg/g, 90 % Xu and Zhao (2007)

cellulosestabilized Fe
nanoparticles
Scrap iron 19 mg/g, 25 % Gheju et al. (2008)
Zerovalent iron 180 mg/g, 98 % Li et al. (2008)
nanoparticles
Manganese-Coated Sand 90 % Lee et al. (2009)
(pH 9)
Manganese-Coated Sand 100 %
(Birm commercial sand)
(pH9)
Rev Environ Sci Biotechnol (2014) 13:163–181

Coconut husk 92 % ± 2.8 94 % ± 3.2 94 % ± 1.4 Abdulrasaq and Basiru

(2010)
Nano-scale Fe0 particles 181 mg/g Li et al. (2010a), (b)
supported on a PAA/
PVDF membrane
Entrapment of nanoscale 98.40 % Liu et al. (2010a)
zero-valent iron in
chitosan beads
Palm shell 12.6 mg/g Owlad et al. (2010)
Granular activated carbon 1.385 mg/g Sen et al. (2010)
Castor seed hull 6.983 mg/g
Bituminuous coal 27.8 mg/g Chaudhuri and Azizan
(2011)
Coconut coir 38.5 mg/g
MicrowaveIncinerated 3.279 mg/g Johan et al. (2011)
Rice Husk Ash (500 °C)
MicrowaveIncinerated 3.479 mg/g
Rice Husk Ash (800 °C)
Polyaniline 0.165 mg/g Rehman et al. (2011)
Polyaniline/saw dust 4.739 mg/g
Polyaniline/rice husk 5.128 mg/g
Fly ash-based geopolymer 183.605 mg/g Al-Zboon et al. (2011)
(35 °C, pH 4)
Silica fume supported-Fe0 88 % Li et al. (2011)
nanoparticles
175

123
 Table 2 continued
176

Types of materials Adsorption capacity (mg/g)/removal efficiency (%) References

As(III) As(V) Cr(VI) Cu(II) Cd(II) Zn(II) Ni(II) Pb(II) Co(II) Mn(II) Fe(III)

123
New Zealand Iron sand 97.60 % Panthi and Wareham
(2011)
Ultrafine Fe2O3 100 % Tang et al. (2011)
nanoparticles
Nano hydroxyapatite 98 % Asgari et al. (2012)
(n-HAp) (pH7)
Phanerochaete 84.20 % Chen et al. (2012)
chrysosporium
loaded with
nitrogen-doped TiO2
nanoparticles
Jojoba oil (20 mg/L 95 % 98 % El Kinawy et al. (2012)
Cu, Pb)
Banana peel (5 mg/L 85 % Hossain et al. (2012)
Cu)
Banana peel (10 mg/L 88 %
Cu)
Modified cashew nut 406.6 mg/g 436.7 mg/g 455.7 mg/g 456.3 mg/g Kumar et al. (2012)
shell
Fe@SiO2 467 mg/g, 64.18 % Li et al. (2012a)
Spent grain (pH9) 92.63 % Li et al. (2012b)
Activated carbon 28.67 mg/g 45.44 mg/g Moreno-Pirajan and
orange peel Giraldo (2012)
Duckweed (pH6, 89 % Singh et al. (2012)
20 mg/L Pb,
10 days)
Fe loaded on rice husk 156 mg/g 1,111 mg/g Wantala et al. (2012)
RH-MCM-41
Rev Environ Sci Biotechnol (2014) 13:163–181
Rev Environ Sci Biotechnol (2014) 13:163–181 177

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