Dye and its Removal from aqueous solution by Adsorption: A review Mustafa T. Yagub, Tushar Kanti Sen, Sharmeen Afroze, H.M. Ang PII: DOI: Reference:
S0001-8686(14)00138-9 doi: 10.1016/j.cis.2014.04.002 CIS 1433
To appear in:
Advances in Colloid and Interface Science
Received date: Revised date: Accepted date:
4 August 2013 3 April 2014 4 April 2014
Please cite this article as: Yagub Mustafa T., Sen Tushar Kanti, Afroze Sharmeen, Ang HM, Dye and its Removal from aqueous solution by Adsorption: A review, Advances in Colloid and Interface Science (2014), doi: 10.1016/j.cis.2014.04.002
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ACCEPTED MANUSCRIPT Dye and its Removal from aqueous solution by Adsorption: A review Mustafa T. Yagub, Tushar Kanti Sen*, Sharmeen Afroze, H. M. Ang
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E-mail:
[email protected]
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GPO Box U1987, 6845 Bentley, WA, Australia
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Tel No : +61892669052
*Corresponding author
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Department of Chemical Engineering, Curtin University,
ACCEPTED MANUSCRIPT Contents 1.0 Introduction 1.1 classification of Dyes
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1.2 Toxicity effects of Dyes
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2.0 Present Treatment methods for Dye Removal
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3.0 Adsorption
3.1.1 3.1.2 3.1.3 3.1.4
Effect of solution pH Effect of initial dye concentration Effect of Temperature Effect of Amount of Adsorbent
3.2 Dye Adsorption Kinetic study
Application of Lagergren pseudo-first-order model on dye adsorption Application of Lagergren pseudo-second-order model on dye adsorption Application of Intraparticle Diffusion Model on dye adsorption
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3.2.1 3.2.2 3.2.3
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3.1 Factors Affecting Adsorption of Dye
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3.3 Applicability of various Adsorption Isotherm models on dye adsorption 3.3.1 Langmuir adsorption isotherm model to dye adsorption 3.3.2 Freundlich adsorption isotherm model to dye adsorption
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3.4 Various adsorbent in the removal of Dyes from aqueous phase 3.4.1 Activated Carbon 3.4.2 Low Cost Adsorbents for Dyes Removal 3.4.2.1 Agricultural Solid Wastes 3.4.2.2 Biomass solid waste based activated carbons adsorbent 3.4.2.3 Industrial By-Products 3.4.2.4 Inorganic Materials for Dye removal 3.4.2.4.1 Clay minerals 3.4.2.4.2 Siliceous materials 3.4.2.4.3 Zeolites 3.4.2.4.4 Metal Oxides 3.4.2.5 Biosorbents and Microbial Biomass
4.0 Conclusion 5.0 References
ACCEPTED MANUSCRIPT ABSTRACT In this review article the authors presented up to-date development on the application of adsorption in the removal of dyes from aqueous solution. This review article provides
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extensive literature information about dyes, its classification and toxicity, various treatment
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methods, dye adsorption and characteristics by various adsorbents. The one of the objective
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of this review article is to organize the scattered available information on various aspects on a wide range of potentially effective adsorbents in the removal of dyes. Therefore, an extensive list of various adsorbents such as natural materials, waste materials from industry, agricultural by-products, and biomass based activated carbon in the removal of various dyes
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has been compiled here. Dye bearing waste treatment by adsorption using low cost alternative adsorbent is a demanding area as it has double benefits i.e. water treatment and waste
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management. Further, activated carbon from biomass has the advantage of offering an effected low cost replacement for non-renewable coal based granular activated carbon provided that they have similar or better adsorption on efficiency. The effectiveness of
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various adsorbents under different physio-chemical process parameters and their comparative
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adsorption capacity towards dye adsorption has also been presented. This review paper also includes the factors affective adsorption of dye such as solution pH, initial dye concentration,
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adsorbent dosage, and temperature. The applicability of various adsorption kinetic models and isotherm models for dye removal by wide range of adsorbents also reported here. Conclusions have been drawn from the literature reviewed and few suggestions for future
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research are proposed.
Keywords: Adsorption characteristics; Dye removal; Low cost adsorbents; Activated carbon
ACCEPTED MANUSCRIPT 1.0 Introduction Dyes are basically chemical compounds that can connect themselves to surfaces or fabrics to
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impart colour. The majority of dyes are complex organic molecules and are required being
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resistant to many things such as the action of detergents. Synthetic dyes are widely used in many fields of advanced technology, e.g., in various kinds of the textile industry [1] , paper
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[2], leather tanning [3], food processing, plastics, cosmetics, rubber, printing and dye manufacturing industries [4-6]. Synthetic dyes are also employed in ground water tracing [7], for the determination of specific surface area of activated sludge [8], sewage [9] and
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wastewater treatment [10], etc. Their discharges into hydrosphere possess a significant source of pollution due to their recalcitrance nature. This will give undesirable colour to the water
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body which will reduce sunlight penetration and resisting photochemical and biological attack to the aquatic life [11]. Till data, more than 100,000 commercial dyes are known with an annual production of over 7 x105 tonnes/year [12]. The total dye consumption in textile
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industry worldwide is more than 10,000 tonnes/year and approximately 100 tonnes/year of
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dyes are discharged into water streams [13]. Basically exact data on the amount of dyes discharged from various processes in the environment are unknown. However, the release of
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essential amounts of synthetic dyes to the environment has posed challenges to environmental scientists. Various methods such as adsorption, coagulation, advanced oxidation, membrane separation, etc. are used in the removal of dyes from wastewater [14]. Adsorption is one of the most effective processes of advanced wastewater treatment which industries employ to
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reduce hazardous inorganic/organic present in the effluent [15]. Many textile industries use commercial activated carbon for the treatment of dye waste. The current research is focused on the need to alternative to commercial activated carbon as the cost effective, but potential adsorbent. Many researchers have reported the feasibility of using various low cost adsorbents derived from natural materials, industrial solid wastes, agricultural by-products and biosorbents as precursors [16]. The lignin cellulosic biomass behave as good effective adsorbents [16]. Different physical or chemical treatment was applied to the raw biomass adsorbents for improving their adsorption capacity which were also reported by investigators [16]. The present state of art on the application of adsorption in the removal of dyes from aqueous solution is presented in this paper. The main goal of this review article is to provide up-todate development on the application of commercial activated carbon and various sustainable
ACCEPTED MANUSCRIPT low cost alternative adsorbents such as agricultural solid waste, industrial solid waste, agricultural by-products, and biomass based cost effective activated carbon, and various natural materials in the removal of dyes from aqueous phase. This review article also
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critically analyse the effectiveness of various adsorbents under different physiochemical
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process parameters and their comparative adsorption capacity is also presented. A compilation of relevant published data with respect to adsorption kinetics, isotherm models,
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thermodynamics and adsorption capacity under various process conditions along with important findings are presented here. Although there are couple of review articles such as low cost adsorbents for the removal of organic pollutants from wastewater by Ali et al [17];
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cationic and anionic dye adsorption by agricultural solid wastes by Salleh et al [18]; nonconventional low-cost adsorbents for dye removal by Crini [19]; decolourization of dye
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wastewaters by biosorbents by Srinivasan & Viraraghavan [20]; biodegradation of synthetic dyes by Ali [21]; and adsorption of methylene blue on low-cost adsorbents by Rafatullah et al [22], but all are dealing with specific system only and also not relatively presented up-to-date
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information. Therefore, this present review article was undertaken in order to provide more
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comprehensive up-to-date and critical review information on the adsorption of various dyes from aqueous solution by wide range of adsorbents. The new aspect of this review article is
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to cover up-to-date research results presentation on various dyes adsorption and its adsorptive effectiveness in the removal of various dyes and also critically analysed and identified various operation conditions and their maximum adsorption capacity. Authors also tried to analyse the scattered available information on dye adsorption by wide range of adsorbents
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since last two decades.
ACCEPTED MANUSCRIPT 1.1Classification of dyes There are several ways for classification of commercial dyes. It can be classified in terms of
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structure, colour and application method [23]. However, due to the complexities of the colour
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nomenclature from the chemical structure system, the classification based on application is often favourable [14]. The classification based on chemical structure for the common class of
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the dyes is presented in Table 1.Table 2 represents the different application based classification. Other than the above, dyes are also usually classified based on their particle charge upon dissolution in aqueous application medium [24, 25] such as cationic (all basic
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dyes), anionic (direct, acid, and reactive dyes), and non-ionic (dispersed dyes).
ACCEPTED MANUSCRIPT Table 1:Classification of dyes according to the chemical structure adopted from [21] Chromospheres
Example
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Class
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Azo dyes
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Reactive Black 5
Reactive Blue 4
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Anthraquinone dyes
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Indigoid dyes
Acid Blue 71
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Nitroso dyes
Acid green 1
Nitro dyes
Acid Yellow 24
Triarylmethane dyes
Basic red 9
ACCEPTED MANUSCRIPT Table 2:Classification of dye based on their chemical nature adopted from [26]
Direct
Generally from neutral to acidic bath.
Anthraquinone, xanthene, azo (including, nitroso, premetallized), nitro, and tryphenylmethane.
Nylon, rayon, paper, leather and cotton.
Polyamide, acrylic polyester, acetate, and plastics
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Applied from acidic dye baths.
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Inks, paper, polyacrylonitrile, treated nylon, and polyester
Sulphur
Vat
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Wool, cotton, silk and nylon.
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Reactive
Rayon and Cotton.
Wool and cotton.
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Wool, nylon, silk, inks, leather and paper.
Applied from neutral or a little alkaline baths containing additional electrolyte. Fine aqueous dispersions often applied by high temperature/pressure or lower temperature carrier methods; dye maybe padded on cloth and thermo fixed.
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Disperse
Chemical types
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Basic
Method of application
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Acid
Substrate
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Class
Reactive site on dye reacts with functional group on fibre to bind dye covalently under influence of heat and pH. Aromatic substrate vatted with sodium sulphide and reoxidized to insoluble sulfur-containing products on fibre Water-insoluble dyes solubilised by dropping with sodium hydrogensulfite, then exhausted on reoxidized and fibre.
Hemicyanine, azo, cyanine, diazahemicyanine, azine diphenylmethane, xanthene, triarylmethane, acridine, anthraquinone and oxazine. Phthalocyanine, azo, oxazine, and stilbene.
Benzodifuranone, azo, anthraquinone, nitro, and styryl.
anthraquinone, formazan, phthalocyanine, Azo, oxazine and basic.
Indeterminate structures
Indigoids and Anthraquinone.
Several industries such as dyestuff, textile, paper, printing, carpet, plastic, food and cosmetic industry are used dyes to provide colour to their products. These dyes are always left in industrial waste and consequently discharged generally to the water body [19, 27-29].
ACCEPTED MANUSCRIPT 1.2Toxicity effects of Dyes Basic dyes have high intensity of colours and are greatly visible even in very little
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concentration [23, 30-35]. The complex dyes are generally chromium based, which is
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carcinogenic [23, 24, 30, 36]. Dyes may affect the photosynthetic activity in aquatic life due to decreased light penetration and may also be toxic to some aquatic life due to the presence
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of metals, aromatics, etc. [23, 24, 30-32, 36, 37]. Furthermore, dyes are also carcinogenic, mutagenic, or teratogenic in various microbiological, fish species. Additionally it also can cause severe damage to human beings such as dysfunction of kidney, reproductive system,
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liver brain and central nervous system [38]. Azo dyes are toxic because of the presence of toxic amines in the effluent [39]. Similarly anthraquinone-based dyes are most resistant to degradation and remains colour for a large time in effluents [39]. Reactive dyes are water
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soluble and 5-10 % of the dyes go in the dye bath giving highly coloured effluent causing serious troubles in the environment [40]. Additionally, reactive dyes being chemically stable
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and having little biodegradability are likely to pass through conventional treatment plants
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untreated, so their elimination is of great importance. Due to the dyes toxic effects, dyes have generated much concern regarding its use. It has
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been informed to cause mutagenesis, chromosomal fractures, carcinogenesis, and respiratory toxicity. Therefore focuses on specific methods and technologies to remove dyes from
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different kinds of wastewater streams is desired.
2.0 Present Treatment methods for Dye Removal There are numerous methods to treat dye bearing effluents. In spite of the availability of many techniques to remove dye contaminants from wastewaters, such as coagulation, chemical oxidation, membrane separation process, electro chemical and aerobic and anaerobic microbial degradation, and each of these methods have inherent limitations. The technologies can be divided into three categories: physical, chemical and biological [41]. All of these methods have their own advantages and disadvantages. Table 3 shows the advantages and
disadvantages of different dye removal methods.
ACCEPTED MANUSCRIPT Table3: Advantages and disadvantages of dyes removal methods [18]. Methods
Advantages
Disadvantages
Chemical treatments (H2O) agent needs to activate by some means Sludge generation
Simplicity of application
H2O2+Fe(II) salts (Fenton’s reagent)
Fentons reagent is a suitable chemical means
Ozonation
Ozone can be applied in its gaseous state and does not increase the volume of wastewater and sludge
Photochemical
No sludge is produced and foul odors are greatly reduced
Formation of by-products
Sodium hypochloride (NaOCl)
Initiates and accelerates azobond cleavage
Release of aromatic amines
Electrochemical destruction
No consumption of chemicals and no sludge build up
Relatively high flow rates cause a direct decrease in dye removal
Other microbial Cultures (Mixed bacterial)
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White-rot fungi are able to degrade dyes using enzymes
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Decolourization by white-rot fungi
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Adsorption by living/dead microbial biomass
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Short half-life (20 min)
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Biological treatments
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Oxidative process
Enzyme production has also been shown to be unreliable
Decolorized in 24–30 h
Under aerobic conditions azo dyes are not readily metabolized
Certain dyes have a particular affinity for binding with microbial species
Not effective for all dyes
Anaerobic textile- dye Allows azo and other waterbioremediation soluble dyes to be decolorized systems
Anaerobic breakdown yields methane and hydrogen sulphide
Physical treatments Adsorption by activated carbon Membrane filtration
Good removal of wide variety of dyes Removes all dye types
Very expensive
Ion exchange
Regeneration: no adsorbent loss Effective oxidation at lab scale
Not effective for all dyes
Economically feasible
High sludge production
Irradiation Electrokinetic coagulation
Concentrated sludge production
Requires a lot of dissolved O2
ACCEPTED MANUSCRIPT 3.0 Adsorption The term adsorption refers to the accumulation of a substance at the interface between two phases (liquid-solid interface or gas-solid interface). The substance that accumulates at the
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interface is called adsorbate and the solid on which adsorption occurs is adsorbent [42].
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Adsorption can be classified into two types; chemical sorption and physical sorption. Chemical adsorption or chemisorption is illustrated by the formation of strong chemical
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associations between molecules or ions of adsorbate to adsorbent surface, which is generally due to the exchange of electrons [43] and thus chemical sorption generally is irreversible. Physical adsorption or physisorption is characterized by weak Van der Waals intraparticle
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bonds between adsorbate and adsorbent and thus reversible in most cases [43]. Adsorption on most of the adsorbent including agricultural by-products is controlled by physical forces with
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some exception of chemisorption. The main physical forces controlling adsorption are Van der Waals forces, hydrogen bonds, polarity, dipole-dipole ∏-∏ interaction, etc.[21].This process provides an attractive alternative for the treatment of polluted waters, especially if the
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sorbent is inexpensive and does not require an additional pre-treatment step before its
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application [42].As for environmental remediation purpose, adsorption techniques are widely used to remove certain classes of chemical contaminants from waters, especially those that
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are practically unaffected by conventional biological wastewater treatments [42, 43]. Adsorption has been found to be superior to other techniques in terms of flexibility and simplicity of design, initial cost, insensitivity to toxic pollutants and ease of operation. Adsorption also does not produce the harmful substances [19].Factors that influence the
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adsorption efficiency include adsorbate adsorbent interaction, adsorbent surface area, adsorbent to adsorbate ratio, adsorbent particle size, temperature, pH and contact time [19, 43] etc.
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Factors Affecting Adsorption of Dye
There are many factors affecting dye adsorption such as solution pH, temperature, initial dye concentration, etc. Thus, the effects of these parameters are to be taken into account.
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Optimization of such conditions will greatly help in the development of industrial-scale dye
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removal treatment process. In this section, some of the factors affecting adsorption of dyes
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are discussed below: 3.1.1 Effect of solution pH
One of the most important factors affecting the capacity of adsorbent in wastewater treatment
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is solution pH. The efficiency of adsorption is dependent on the solution pH, since variation in pH leads to the variation in the degree of ionization of the adsorptive molecule and the
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surface properties of adsorbent [44].
Chowdhury et al.[45] studied the effect of solution pH on the adsorption of Basic Green 4
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dye by Ananas comosus leaf powder and they noticed that at a pH range from 2 to 10, the dye removal ratio was maximum at a pH 10. Dawood and Sen [46] studied the effect of solution
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pH on the adsorption of Congo red by pine cone and they noticed that the adsorption was maximum at pH of 3.5. Ibrahim et al.[47] studied the adsorption of RB4 dye by modified
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barley straw and they found that RB4 gives a complete removal of 100% at pH of 3 and decreased value below 50% as the pH was increased. Yagub et al. [13] reported that adsorption of cationic dye MB onto raw pine leaves biomass was increased with increase in
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solution pH (Figure1). Table 4 reported the compilation of different studies on the effect of solution pH on dye adsorption.
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35
80
30
70
25
60
20
%
10
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Amunt of Adsorption 15 qe(mg/g)
Percent of 50 Adsorptin % 40
qe
10 0
5 0
0
2
4
6
8
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Initial pH
10
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Fig. 1 Effect of initial solution pH on the adsorption of Methylene Blue (MB) on pine leaves [13].
The adsorption ability of the surface and the type of surface active centres are indicated by
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the significant factor that is the point of zero charge (pHpzc) [48]. The pH at which the surface
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charge is zero is called the point of zero charge (pzc) and is typically used to quantify or define the electrokinetic properties of a surface. The value of pH is used to describe pzc only
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for systems in which H+/OH− are the potential determining ions. Many researchers studied the point of zero charge (pHpzc) of various adsorbents prepared from agricultural solid wastes; in order to understand the adsorption mechanism. Due to presence of functional group such
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as OH−group, cationic dye adsorption is favoured at pH>pHpzc, whereas, anionic dye adsorption is favoured at pH
