published paper-jr. clean soil air water

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Pham Thi Thuy1

Nguyen Viet Anh2

Bart van der Bruggen1

1Laboratory for Applied Physical

Chemistry and Environment

Technology, Department of Chemical

Engineering, K.U. Leuven, Belgium2Institute of Environmental Science

and Engineering, Hanoi University of

Civil Engineering, Hanoi, Viet Nam

Research Article

Evaluation of Two Low-CostHigh-Performance

Adsorbent Materials in the Waste-to-Product

Approach for the Removal of Pesticides from

Drinking Water

This study evaluates the performance of two low cost and high performance adsorption

materials, i.e., activated carbon produced from two natural waste products: Bamboo and

coconut shell, in the removal of three pesticides from drinking water sources. Due to the

fact that bamboo and coconut shell are abundant and inexpensive materials in many

parts of the world, they respond to the low-cost aspect. The adsorptioncapacities of two

local adsorbents have been compared with commercial activated carbon to explore their

potential to respond to the high quality aspect. Two pesticides were selected, namely

dieldrin and chlorpyrifos, because they are commonly used in agriculture activities, and

may remain in high concentrations in surface water used as drinking water sources. The

results indicate that the adsorption of pesticides on activated carbons is influenced by

physico-chemical properties of the activated carbon and the pesticides such as the

presence of an aromatic ring, and their molar mass. The activated carbon produced

from bamboo can be employed as low-cost and high performance adsorbent, alternative

to commercial activated carbon for the removal of pesticides during drinking water

production. The performance of activated carbon from bamboo was better due to its

relatively large macroporosity and planar surface. The effect of adsorbent and pesticide

characteristics on the performance was derived from batch experiments in which the

adsorption behavior was studied on the basis of Freundlich isotherms.

Keywords:Activated carbon; Adsorption; Biomass; Surface water

Received:April 27, 2011;revised:August 10, 2011;accepted:September 20, 2011

DOI: 10.1002/clen.201100209

1 Introduction

Because water is the basis of the development of any society, the

Millennium Development Goals (MDGs), set for 2015, include Target

10 of Goal 7, which aims to halve, by 2015, the proportion of people

without sustainable access to safe drinking water and basic sani-

tation [1]. Nevertheless, millions of people worldwide are suffering

from shortage of fresh and clean water. Causes of water supply

problems in urbanized regions (especially in developing countries),

as described by van der Bruggen et al. [2] are to be found in the high

rate of population growth, lack of economical resources, and suit-

able infrastructure. In addition, surface water resources nowadays

are becoming polluted with many toxic compounds because of

untreated or partially treated industrial effluents and agricultural

run-off, which are difficult to remove by conventional treatment

methods [3]. Pesticides, which have adverse effects on human health

at low concentrations and often remain in water for a long time[46],

are a group of such hazardous materials found in surface water

bodies as a result of agricultural wash out [7]. Standards for pesti-

cides in drinking water were sharpened following the introduction

of WHO drinking water standards 2006 [8]. The concentration of a

single pesticide in drinking water cannot exceed 0.1 mg/L while the

sum of all pesticide concentrations cannot exceed 0.5 and 13 mg/L

[9]. Consequently there is a need to intensify drinking water treat-

ment and additionally, special attention should be given to the

removal of organic compounds, including pesticides [10, 11].

Conventional drinking water treatment, which is widely applied in

water treatment plants, requires improvements because of the increas-

ingly poor quality of water sources in many parts of the world [10]. In

particular, water treatment plants in developing countries often make

use of basic technologies providing inadequate purification (e.g.,coagulationflocculation). Several methods are available for pesticides

removal such as photocatalytic degradation [12, 13], combined photo-

Fenton and biological oxidation [14, 15], advanced oxidation processes

[16], nanofiltration [17], ozonation [18, 19], and adsorption [2022].

Adsorption processes were studied intensively using a wide range

of adsorption materials and emerged as one of the most promising

techniques [23] due to their low investment cost, ease of operation,

and efficiency for the removal organic and inorganic micropollu-

tants including pesticides [2426]. Adsorption on activated carbon is

the most widespread technology used for purification of water

contaminated by pesticides [11]. Activated carbon is a very efficient

adsorbent for removing varieties of pesticides from drinking water

Correspondence: Dr. P. T. Thuy, Laboratory for Applied PhysicalChemistry and Environment Technology, Department of ChemicalEngineering, K.U. Leuven, W. de Croylaan 46, B-3001 Leuven, BelgiumE-mail:[email protected]

Abbreviations: ACBC, activated carbon made from bituminous coal;ACCS,activated carbon made from coconut shell; ACB,activated carbonmade from bamboo;SEM,scanning electron microscopy

Clean Soil, Air, Water 2011,00(0), 18 1

2011 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim www.clean-journal.com


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and wastewater due to its high surface area, porosity, and physico-

chemical characteristics [27]; however, its use is limited due to its

high cost and low selectivity. Recently, some agricultural waste

products, biomass, and various solidsubstances have been developed

as alternative cheap adsorbents to removal pesticides. Materials

investigated as adsorbents for pesticides include: charcoal from agro

waste [2830], straw [31, 32], date and olive stones [33], wood chips/

corn cob [32], lignocellulosic substrate from agro-industry [34], bark

[35], chestnut shells [36], watermelon peels [25], bagasse fly ash [37,

38], coal fly ash [39, 40], strawberry leave [41], tamarind fruit shell

[42], rice husk [43], andseaweed[44]. These low-cost materials have been

reported as inexpensive and effective adsorbents for removal of con-

taminants in water and wastewater treatment [45]. However, reported

low-cost adsorbents have cellulose, hemicellulose, lignin, waxes,

pectines, etc., as their constituents. The presence of waxes, pectines,

and other impurities adds to the hydrophobic character of

these adsorbents; furthermore, waxes and impurities also can use

surface area of the adsorbent, causing an overall decrease in the active

surface area and a negative effect to the efficiency of these adsorbents

[46]. The efficiency of low-cost adsorbents depends on the character-

istics and particle size of the adsorbent, and the characteristics andconcentrationof the adsorbate[45]. Therefore, unprocessed materials

mentioned above show a relatively poor removal of pollutants from

effluents compared to activated carbon [46]. Thus, unprocessed

materials appear not to be a good option particularly for safe drinking

water treatment. Activated carbon, produced from renewable and

cheap raw materials, can be considered as a low-cost and high per-

formance adsorbent. Moreover, the cost of biomaterials is negligible

when compared to the cost of commercial activated carbon [4749].

Bamboo is a large, woody-grasses member of the sub-family

Bambusoidae of the family Poaceae (Graminae) [50, 51].

Approximately 1500 commercial applications of bamboo have been

identified mostly in Asia [50, 51]. Bamboo is an abundant natural

resource in many countries in South-East Asia and elsewhere,

because it takes only a few months to grow up and has been

traditionally used to construct various living facilities, tools, and

handicraft [51, 52]. Bamboo also has been used as the structural

material for steps at construction sites in Viet Nam, China, India,

Malaysia, and other countries because of its properties such as

strong, tough, and low-cost material. The waste of bamboo can be

converted to a value-added product such as activated carbon [51, 53].

Coconut shell is themesocarpof coconut and a coconut consists of

3335% of shell [54]. Coconut is abundantly grown in South-East Asia,

e.g., in Viet Nam, about 180000 ha of land in the Mekong Delta and

the Central coast area is used for coconut plantation [55]. At present,

coconut shells are used as a domestic fuel, as fuel for coconut

processing, and also as a source of fiber for rope and mats [54, 56].

It is proposed to convert coconut shell into activated carbon to makebetter use of this cheap and abundant agricultural waste [54].

Conversion of coconut husk and bamboo to activated carbon will

serve a double purpose [54]. Firstly, unwanted agricultural waste and

industrial waste are converted to useful, value-added adsorbent and

secondly, theuse of agriculturaland industrial by-productsrepresents

a potential source of adsorbents, which will contribute to solving part

of the water and wastewater treatment problem [54]. Several studies

on removal of Cr(VI), nitratenitrogen, and cadmium(II) ions reported

effective adsorption capacity of coconut shell [57, 58] and bamboo

charcoal [59, 60]. Hence, the activated carbon based on coconut shell

and bamboo can be also employed as potential low-cost and high

performance adsorbent in the removal of pesticides.

The purpose of this work is not only to use a low-cost method, but

also to evaluate the high-performance adsorption capacity of coco-

nut shell and bamboo based activated carbon to remove pesticides

during drinking water production. Due to thefact that coconut shell

and bamboo are abundant and inexpensive materials, they respond

to the low-cost aspect. They will be compared with the adsorption

performance of commercial activated carbon, which is a high-per-

formance adsorbent to explore their potential to respond to the

high quality aspect. Two pesticides were selected, namely dieldrin

and chlorpyrifos, because they are commonly used in agriculture

activities, and may remain in high concentrations in surface water

used as drinking water sources.

2 Materials and methods

2.1 Materials

2.1.1 Activated carbon

The granulated activated carbons were selected from different raw

materials: Activated carbon made from bituminous coal (ACBC)

(Desotec Activated carbon Co., Belgium); activatedcarbon madefrom

bamboo (ACB) (Ha Bac Activated Carbon Co., Hoa Binh, Viet Nam),

and activated carbon made from coconut shell ((ACCS); Tra Bac

Activated Carbon Co., Ben Tre, Viet Nam). The commercial activated

carbon, made from bituminous coal, was used as a reference in

comparison with the two local activated carbons. Bamboo and coco-

nut shell were obtained from local traditional bamboo handicraft

villages and coconut processing factories in Viet Nam as waste after

producing goods. The preparation method of bamboo and coconut

shell activated carbon was physical activation. Raw materials were

cut into pieces (13cm), dried in an oven at 75 8C for three days,

crushed and screened to a particle size of 14 mm. Raw materials

were first carbonization under a flow of nitrogen gas at 6008

C f o r 2 h .The resulting chars were secondarily activated under flow of vapor

steam to the range of 80010008C for 2 h. Finally, the materials were

washed and cooled to room temperature by nitrogen. For better

understanding the surface properties, characterization of all the

adsorbents were examined using scanning electron microscopy

(SEM). A Philips XL 30 FEG SEM has been used to study surface

morphology of the adsorbents at 10 keV.

Before the batch experiments, the carbon was washed with dis-

tilled water to make sure that fines and impurities in carbon were

removed, oven dried at 1108C for 6 h and stored in plastic containers

for further use.

These activated carbons were analyzed for molasses number and

Methylene Blue number by using CEFIC standards [61], and iodine

number by using ASTM D4607-94 [62].

2.1.2 Pesticides

Two pesticides commonly used in agriculture activities, which may

remain in high concentrations in surface water sources, were

selected: dieldrin and chlorpyrifos. Dieldrin and chlorpyrifos has

been commonly used in agriculture for control of soil insects and

plant pests in rice, coffee and maize which are the main crops and

their products are also main source of income for a lot of farmers in

South-East Asia [63]. The pesticides (Pestanal) were purchased from

Riedelde Haen (SigmaAldrich, Bornem, Belgium). The formulas and

some properties of pesticides in this study are shown in Tab. 1.

2 P. T. Thuy et al. Clean Soil, Air, Water 2011,00(0), 18



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obtained with backscattered electrons clearly shows an irregulardistribution of the inorganic particles on the surface carbon piece.

This irregular distribution was mainly due to the anisotropic struc-

ture of bamboo. The SEM image of ACCS (see Fig. 3) proves that the

surface of ACCS contains well-developed pores. Many large pores

with a honey comb shape were clearly observed on the surface. The

ACCS was mesoporous with relatively large and plane surface area

[54]. The SEM images show that all three activated carbons had high

well-developed pores in surface, which shows a potential possibility

for pesticides to be adsorbed [66].

3.2 Removal efficiency in distilled water and river

waterThe removal efficiency of pesticides using selected activated carbons

using 100 mg activated carbons in distilled water and river water is

shown in Tab. 3.

The percentage of pesticides removal was found to decrease with

increase of the initial concentration of pesticides, and to decrease

with a decrease in the amount of activated carbon dosages in dis-

tilled water and river water. This is also what should be expected

based on adsorption theory [64]. In most cases, the percentage

removal of pesticides in distilled water was higher than in river

water confirms that the substances present in river water (e.g.,

natural organic matters) interact with the adsorbents and decrease

the adsorbents surface areas available for adsorption [6]. In accor-

dance with the results given in Tab. 3, the removal efficiency of lowinitial pesticidesconcentration (1mg/L) is nearlythe same in distilled

water and river water. This indicates that at low initial concen-

tration, the surface area and the availability of adsorption sites were

relative high in adsorbents. At low initial concentration of two

pesticides in river water and distilled water, the removal efficiency

of the two local activated carbons studied were found to be nearly

equal to ACBC. This confirms that the structure of the pores of the

twolocalactivated carbonsis well suitedfor adsorption of pesticides,

similar to commercial activated carbon.

The removal efficiency of dieldrin was higher than of chlorpyrifos

in distilledwaterand river water.The structureof thepesticide plays

an important role for the adsorption capacity [65]. Thus, the higher

adsorption capacity observed for dieldrin in most cases is probably

due to the absence of an aromatic ring of chlorpyrifos. The branched

substituent of aromatic ring of chlorpyrifos causes the rate and

extent of adsorption of this pesticide to be the highest by providing

hydrophobicity to the structure [65].

The removal of pesticides by ACCS (from 68.6 to 90.5% with chlor-

pyrifos and 71.1 to 92.1% with dieldrin in distilled water) is the

lowest, followed by ACB (from 71 to 93.1% with chlorpyrifos and

76 to 94% with dieldrin in distilled water) and the highest for ACBC

(from 74.5 to 93.9% with chlorpyrifos and 79.5 to 94.1% with dieldrin

in distilled water. The two local activated carbons have a good

adsorption capacity for pesticides, as is clearly from the results with

distilled water; they were evidently found to have adsorption

capacity almost equal to commercial activated carbon, especially

Figure 2. SEM image of bamboo activated carbon (Magnification: 2000). Figure 3. SEM image of coconut shell activated carbon (Magnification:2000).

Table 3.The removal efficiency of pesticides using 100 mg selected activated carbons in distilled water and river water

Conc. (mg/L) ACBC ACB ACCS

Chlorpyrifos Dieldrin Chlorpyrifos Dieldrin Chlorpyrifos Dieldrin

DW RW DW RW DW RW DW RW DW RW DW RW

1 93.9 93.2 94.1 94.1 93.1 92.5 94.0 93.0 90.5 89.0 92.1 91.110 80.6 77.7 87.9 85.4 85.1 79.5 84.7 83.7 79.2 71.5 81.6 72.6100 74.5 68.6 79.5 74.6 71.0 66.1 76.0 71.2 68.6 64.3 71.1 69.5

ACBC, activated carbon from bituminous coal; ACB, activated carbon from bamboo; ACCS, activated carbon from coconut shell; Conc.,concentration; DW, distilled water; RW, river water.




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in the low concentration range. Hence, two local activated carbons

could be used as low costhigh performance adsorbents as alter-

natives to commercial activated carbonfor the removal of pesticides.

In particular, ACB shows better adsorption capacity than ACCS and

almost equal to ACBC.

3.3 Adsorption isotherms

Adsorption isotherms were determined to quantify the interaction

between solute and the activated carbons, critical in optimizing the

purification process. Two isotherm models (Langmuir and

Freundlich) were employed to understand of the equilibrium data

and conclude on adsorption mechanisms. The linear form of the

Langmuir [66, 67] model is:

Ce

qe

Ce

qm

1

Kaqm(3)

where Ce (mg/L) is the equilibrium concentration, qe (mg/g) the

amount of pesticides adsorbed at equilibrium, qm(mg/g) the adsorp-tion for a complete monolayer, Ka (L/mg) is the adsorption equi-

librium constant. When Ce/qe is plotted against Ce and the data

are regressed linearly, qm and Ka constants are calculated from

the slope and the intercept. The linear form of the Freundlich [65,

68] isotherm is:

ln qe lnKF 1

n

ln Ce (4)

The constantKF (mg/g (L/mg)1/n) is related to theadsorption capacity

of activated carbons; and 1/nis related to the surface heterogeneity.

When lnqe is plotted against lnCe and thedata are analyzed by linear

regression, 1/n and KFconstants can be determined from the slope

and intercept [65, 68].The parameters of Langmuir and Freundlich equations for the

adsorption capacity of two pesticides onto the three activated car-

bons obtained as described above are given in Tab. 4. The isotherms

obtained using these parameters are presented in Figs. 4 and 5 for

chlorpyrifos and dieldrin, respectively, together with experimental

data points [65].

The Freundlich equation had the correlation coefficients (R) always

>0.95, which shows the suitability of experimental isotherm data. This

result demonstrates the formation of multilayer coverage of pesticide

molecule at the outer surface of the three activated carbons [66].

The value ofKFdetermines the adsorption capacity of a adsorbent

at equilibrium concentration in a solution [11]. A higher KF value

corresponds to a higher adsorption capacity. According to the KF

values listed in Tab. 4, the adsorption capacities of the pesticides

studied are higher fordieldrin than for chlorpyrifos. Because adsorp-

tion of pesticides depends on their physico-chemical properties [6], a

more hydrophobic compound has a higher adsorption capacity and

thus a higher removal efficiency [6]. Similarly, substances with highmolecular weight have a tendency to be adsorbed more strongly

than chemical compounds with low molecular weight [11]. This was

confirmed in our experiments, the pesticides examined can be

ordered accordancewith the increasingmolecular weight as follows:

Dieldrin> chlorpyrifos.

TheKFvalues of the two local activated carbons are lower than for

ACBC. Comparing the pesticide removal efficiency of the two local

activated carbons, ACB is observed to possess a higher adsorption

Table 4.The Freundlich and Langmuir parameters of adsorption isotherm

Parameter ACBC ACB ACCS

Chlorpyrifos Dieldrin Chlorpyrifos Dieldrin Chlorpyrifos Dieldrin

Freudlich isothermKF(mg/g (L/mg)

1/n) 34.61 44.80 35.60 37.63 26.50 30.701/n 0.69 0.69 0.68 0.71 0.72 0.71Correlation coefficient (R) 0.96 0.96 0.97 0.95 0.96 0.95Langmuir isothermQm(mg/g) 872.67 909.80 588.23 597.67 500.00 543.6Ka(L/mg) 0.06 0.09 0.07 0.05 0.04 0.06Correlation coefficient (R) 0.85 0.86 0.86 0.85 0.86 0.87RL 0.62 0.53 0.59 0.66 0.71 0.62

ACBC, activated carbon from bituminous coal; ACB, activated carbon from bamboo; ACCS, activated carbon from coconut shell.

Figure 4.Freundlich isotherm for the removal of (a) dieldrin and (b) chlor-pyrifos by adsorption on three activated carbons.

Clean Soil, Air, Water 2011,00(0), 18 Evaluation of Two Low-CostHigh-Performance 5



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capacity than ACCS. Firstly, this might be dueto compatibility of size

between the pesticide molecules and the pores of the ACB. Secondly,

due to the irregular distribution of the inorganic particles on the

surface carbon piece, the ACB could adsorb better the multilayer

coverage of pesticide molecules at the outer surface of the activated

carbons than ACCS, which was macroporous with relatively large

andplanesurface area. Thirdly, thehigher fraction of mesoporesand

macropores of ACB compare to ACCS also acquires a reasonable

surface area of adsorbing the multilayer coverage of pesticide mol-

ecules. Hence, among the two local activated carbons, ACB is pre-

ferred as a low-cost, high performance adsorption material.

The slope (1/n) value in Freundlichs equation allows for assessing

the adsorption intensity of a given substance from water phase of

adsorbent [11]. The value of 1/nis known as the heterogeneous factor

and ranges between 0 and 1 [65]; the more heterogeneous the sur-

face, thecloser 1/n isto 0 [69]. The slope (1/n) values for twopesticidesin ACBC, ACB, and ACCS were


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