Bioresource Technology Volume 102 Issue 2 2011 [Doi 10.1016%2Fj.biortech.2010.08.125] Yuyi Yang; Guan Wang; Bing Wang; Zeli Li; Xiaoming Jia; Qifa Zho -- Biosorption of Acid Black

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Biosorption of Acid Black 172 and Congo Red from aqueous solution by nonviablePenicillium YW 01: Kinetic study, equilibrium isotherm and articial neuralnetwork modeling

Yuyi Yang, Guan Wang, Bing Wang, Zeli Li, Xiaoming Jia, Qifa Zhou, Yuhua Zhao

College of Life Sciences, Zhejiang University, Hangzhou, Zhejiang Province 310058, PR China

a r t i c l e i n f o

Article history:Received 8 June 2010Received in revised form 27 August 2010Accepted 31 August 2010Available online 6 September 2010

Keywords:Nonviable Penicillium YW 01Congo RedAcid Black 172Biosorption isothermsArticial neural network

a b s t r a c t

The main objective of this work was to investigate the biosorption performance of nonviable PenicilliumYW 01 biomass for removal of Acid Black 172 metal-complex dye (AB) and Congo Red (CR) in solutions.Maximum biosorption capacities of 225.38 and 411.53 mg g 1 under initial dye concentration of 800 mg L 1, pH 3.0 and 40 C conditions were observed for AB and CR, respectively. Biosorption data weresuccessfully described with Langmuir isotherm and the pseudo-second-order kinetic model. TheWeber-Morris model analysis indicated that intraparticle diffusion was the limiting step for biosorptionof AB and CR onto biosorbent. Analysis based on the articial neural network and genetic algorithmshybrid model indicated that initial dye concentration and temperature appeared to be the most inuen-tial parameters for biosorption process of AB and CR onto biosorbent, respectively. Characterization of thebiosorbent and possible dye-biosorbent interaction were conrmed by Fourier transform infraredspectroscopy and scanning electron microscopy.

2010 Elsevier Ltd. All rights reserved.

1. Introduction

Dyes are synthetic chemical compounds having complex aro-matic structures which are extensively used in the textile, cos-metic, plastic, food, and pharmaceutical industries ( Forgacs et al.,2004 ). The dye-containing wastewater discharged from the indus-tries can adversely affect the aquatic environment by impedinglight penetration. Moreover, most of the dyes are toxic, carcino-genic and harmful to human health. Even at low concentration(1 mg L 1), dyes could be highly noticeable, and could cause anaesthetic pollution and disturbance to the ecosystem and watersources ( Vimonses et al., 2010 ). Therefore, there is an increasingdemand of efcient and economical technologies for removingdyes from water environment in the world.

Biosorption has been found to be one of the prominent tech-niques for dye wastewater treatment in terms of cost and opera-tion. Activated carbon is an effective adsorbent for dyes and hasbeen widely used in wastewater treatment. However, this adsor-bent has been limited in practice because of high cost and prob-lems with its disposal ( Xiong et al., 2010). Therefore, low-costand effective materials used for dyes removal from large volumesof wastewater have been of great concerns for environmental sci-entists. Recently, chitin ( Dolphen et al., 2007 ), jute stick powder

(Panda et al., 2009 ), cattail root ( Hu et al., 2010), various fungi(Arica and Bayramoglu, 2007; Binupriya et al., 2008; Akar et al.,2009), etc., have been investigated for removal of dye fromwastewater.

Penicillium is one of the most widespread fungi in the terrestrialenvironment. Penicillium has been widely used for dye removal viabiodegradation or biosorption ( Iscen et al., 2007; Shedbalkar et al.,2008; Gou et al., 2009 ). Dried Penicillium restrictum had been re-cently used for biosorption of Reactive Black 5 ( Iscen et al.,2007). In this study, we investigated Penicillium YW 01 for biosorp-tion capacities of AB (C.I. Acid Black 172, chemical formula:C40H20O14N6S2Na2Cr, molecular weight: 970) metal-complex dyeand CR (C.I. Direct Red 28, chemical formula: C32H22N6Na2O6S2,molecular weight: 697) under different conditions, the biosorptionkinetics for the two dyes and the characteristics of the fungus bio-mass related to the interaction between the dyes and the biomass,and the effects of the operational parameters on the biosorptioncapacity was also analyzed by using articial neural network(ANN) and Genetic Algorithms (GAs) hybrid model. AB having Cr(VI) in its structure was chosen in this study because it is one of the anionic metal-complex dyes and widely used in tanning andtextile industries in China, as the metal-complex dyes dischargedinto the environment could cause more serious problem, and CR,a benzidine-based azo dye, was selected in this study as a modelanionic dye because of its complex chemical structure, persistenceand carcinogenicity, which has been widely used in textiles, paper,rubber and plastic industries.

0960-8524/$ - see front matter 2010 Elsevier Ltd. All rights reserved.doi:10.1016/j.biortech.2010.08.125

Corresponding author. Tel./fax: +86 571 88206995.E-mail address: [email protected] (Y. Zhao).

Bioresource Technology 102 (2011) 828834

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2. Methods

2.1. Preparation of biosorbent

The Penicillium YW 01 (GenBank accession No. GU944770) usedin this work was grown in the potato-dextrose broth (made in lab-oratory according to descriptions for ATCC media number 336

without incorporating agar) at pH 5.5, 30

C and shaken at200 rpm for 5 days. The biomass was separated from the culturebroth by ltration, and washed with generous amounts of distilledwater. Then, the pretreated biomass was autoclaved at 121 C for20 min and dried overnight at 50 C. The dried biomass was groundto power in a disintegrator and sieved through a No. 60 standardsieve to obtain uniform size for biosorption studies. The volumeweight and the bulk porosity of the biomass powder were0.32 g cm 3 and 76.38%, respectively.

2.2. Preparation of dye solution and determination of dyeconcentrations

The dyes AB and CR were obtained from Shanghai Sangon Bio-logical Engineering Technology & Services Co., Ltd, China. Stocksolutions (1000 mg L 1) of dyes were prepared in deionized anddouble distilled water and diluted to get the desired concentrationof dyes. Calibration curves for dyes were prepared by measuringthe absorbance of different concentrations of the dyes. 570 and497 nm were used to measure the absorbance of CR at pH 1.03.0 and pH 4.010.0, respectively. The AB was measured at597 nm to determine the concentration in the solution.

2.3. Biosorption studies

Biosorption experiments were carried out with 100 ml dye solu-tion of desired concentration mixing 0.1 g adsorbent in a 250 mlErlenmeyer ask. The mixture was agitated (200 rpm) at 30 Cfor 6 h unless otherwise stated. The inuence of hydrogen ion con-centration on the biosorption process was studied over a pH rangeof 1.010.0, with adjustments being made using 0.1 mol L 1 HCl or0.1 mol L 1 NaOH. The effect of dye concentration was studied inthe range from 50 to 800 mg L 1 at pH 3.0. The effect of tempera-ture on the biosorption capacity of each adsorbent was investi-gated in the temperature range from 20 to 40 C at pH 3.0.

The biosorption capacity, Q e (mg g 1), was calculated as follows:

Q e C o C eV

M 1

where, C o and C e are the initial and nal concentrations (mg L 1),respectively, M is the adsorbent dosage ( g ) and V the volume of solution ( L).

All the experiments were carried out at least three times andthe data were analyzed by SigmaPlot software (Version 10.0,USA). MATLAB (Version R2009a, USA) software was used to modelthe biosorption process of dyes onto fungal biomass by articialneural network.

2.4. Characterization of the adsorbent

Surface morphology of the biosorbent was determined usinghanging drop method by SEM at 20 kV and 6000 magnication.FTIR spectra of virgin and dye-loaded biosorbent were recordedby PerkinElmer spectrum spectrophotometer in the region of 4004000 cm 1.

3. Results and discussions

3.1. Effect of pH on biosorption capacity

As shown in Fig. 1a, the biosorption capacity of Penicillium YW01 increased from pH 1.0 to pH 3.0, and reached maximum at pH3.0 (46.95 and 48.83 mg g 1 for AB and CR, respectively), and thendeclined sharply with further increase in pH for both of the twodyes, indicating that the optimal pH for biosorption of PenicilliumYW 01 is 3.0 for both of the two dyes under the experimental con-ditions. The change pattern of the biosorption capacity with pHcould be associated with the effects of pH on both the activity of functional groups in the biosorbents and the chemical propertiesof dyes. Acidic conditions could be favorable for the biosorption be-tween the two dyes and the fungal biomass, because a signicantlyhigh electro-static attraction could exist between the positivelycharged surface of the adsorbent under acidic conditions and theanionic dyes (AB and CR are anionic dyes in solution for -SO 3 groupin their structure). At pH 10.0, the biosorption values were 22.56and 21.67 mg g 1 for AB and CR, which were 44% and 48% of max-imum values, respectively. The low biosorption capacity underalkaline conditions could be mainly attributed to that the increas-ing number of negative charge on the surface of the fungal surfacecould result in electrostatic repulsion between the adsorbent anddye molecules ( Aksu and Donmez, 2003 ) and that the existenceof excess OH- ions may compete with the anionic dyes for thedecreasing number of positively charged sites on the fungal surfaceas the pH increased. A similar trend was observed for the biosorp-

Fig. 1. Effect of initial pH (a) and initial dye concentration and temperature (b) on biosorption capacity of the Penicillium YW 01 biomass for AB and CR.

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Table 2) at all the dye concentrations of AB and CR. The results sug-gested the boundary layer resistance was not the rate limiting stepsince the dye-biosorption follows pseudo-second order kinetics(Xiong et al., 2010).

The Weber-Morris model could be used to investigate the masstransfer mechanism in the dye-fungus system and is expressed as

Q t K w t 1=2 I 3

where K w is the intraparticle rate constant, t 1/2 is the square root of time, Q t is the amount of adsorbed dye per unit weight of adsor-bent at time t (mg g 1) and I is the value of intercept. The interceptgives an idea about the thickness of the boundary layer, i.e. thelarger is the intercept, the greater is the boundary layer effect(zer et al., 2006). The Weber-Morris plots were presented inFig. 3 and the parameters were summarized in Table 3. TheWeber-Morris plots for biosorption of AB and CR at 50 mg L 1 werelinear and did not pass the origin ( Fig. 3a), indicating the signi-cance of intraparticle diffusion existed in the biosorption of dyesonto the fungal biomass ( zer et al., 2006). Higher interceptsindicated that the boundary layer effect could not be ignored forbiosorption of AB and CR at initial concentration of 50 mg L 1(Table 3). Fig. 3b showed that the intraparticle diffusion of AB

and CR within fungus biomass at initial concentration of 100 mg L 1 occurred in two stages. The rst straight portion couldbe attributed to macropore diffusion (stage I), i.e. transport of dyemolecules from bulk solution to the surface of the adsorbent, andthe second linear portion could be attributed to micropore diffu-sion (stage II), i.e. the binding of the dye molecules on the activesites of biosorption. Since the kw, 2 values were smaller than thekw ,1 values (Table 3), the intraparticle diffusion should be the lim-iting step for the biosorption of AB and CR onto fungal biomass.Similar trend was observed with biosorption of CR and rhodamineB onto jute stick power ( Panda et al., 2009 ). All the intercepts cal-culated at 100 mg L 1 were higher than that of 50 mg L 1 (Table 3),indicating that the boundary layer effect had more inuence on thebiosorption process at higher concentrations.

3.4. Biosorption isotherms

To investigate the biosorption mechanisms, the surface proper-ties and the capacity or afnity of nonviable Penicillium YW 01 forAB and CR, the Langmuir, Freundlich and Dubinin-Radushkevichadsorption isotherms were selected to explicate the dye-fungussystem in this study.

3.4.1. Langmuir isothermThe Langmuir theory assumes a homogeneous type of adsorp-

tion. That is, once a dye molecule occupies a binding site, no fur-ther adsorption can occur at that site ( Langmuir, 1918 ). Thelinearized equation is given as

C eQ max

1Omax K L

C eQ max 4

where C e is the equilibrium dye concentration in the solution(mg L 1), Q e is the equilibrium dye uptake on the biosorbent

Fig. 3. Weber-Morris plots for biosorption of AB and CR onto the Penicillium YW 01 biomass at 50 mg L 1 (a) and 100 mg L 1 (b).

Table 3

Parameters of Weber-Morris model for adsorption of AB and CR onto fungal biomass.

Dye Concentration(mg L 1)

Initial linear portion Second linear portion

K w ,1 I 1 R2 K w ,2 I 2 R2

AB 50 0.1113 47.23 0.887 100 3.9091 62.214 0.905 0.1349 95.477 0.829CR 50 0.1319 46.97 0.962

100 3.6818 65.593 0.936 0.0994 92.716 0.949

Table 4

Biosorption isotherm parameters for the adsorption of AB and CR onto Penicillium YW 01 at various temperatures.

Dye T ( C) Q exp (mg g 1) Langmuir constants Freundlich constants Dubinin-Radushkevich (D-R) constants

Q max (mg g 1) K l (L mg 1) R2 n K F (L g 1) R2 Q max (mg g 1) b (mol 2 KJ 2) R2 E (kJ mol 1)

AB 20 182.31 185.19 0.057 0.997 9.93 93.69 0.997 162.40 0.0004 0.868 35.3530 220.26 222.22 0.058 0.995 7.78 97.51 0.986 192.48 0.0006 0.903 28.8740 225.38 227.27 0.060 0.993 7.02 92.76 0.911 200.34 0.0008 0.946 25.00

CR 20 355.43 357.14 0.042 0.977 4.94 100.48 0.918 281.46 0.001 0.899 22.3630 383.09 384.62 0.046 0.975 5.14 112.16 0.883 304.91 0.0008 0.904 25.0040 411.53 416.67 0.054 0.989 4.30 104.59 0.901 340.35 0.0011 0.918 21.32

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(mg g 1), Q max is the maximum biosorption capacity (mg g 1), andK L is the Langmuir constant (L mg 1).

The Langmuir model has a high R2 values (Table 4), indicatingthe formation of a monolayer of AB and CR covering the PenicilliumYW 01 surface. Q max and K L reached maximum values of 227.27 mg g 1 and 0.060 L mg 1 at40 C for AB, respectively (Table4). Q max and K L reached maximum values of 416.67 mg g 1 and0.054 L mg 1 at 40 C for CR, respectively (Table 4). These valuesindicated that the dye molecules exhibited the highest afnityfor the adsorbent at 40 C and agreed with the experimental results(Q exp values in Table 4).

The suitability of the adsorbent for the sorbate can be expressedusing the Hall separation factor ( RL, dimensionless), which can becalculated in the following equation ( Hall et al., 1966)

RL 1

1 K LC 05

where K L and C 0 are the Langmuir constant (L mg 1) and initial dyeconcentration (mg L 1), respectively. All the RL values (data werenot shown) for AB and CR were in the range 01, indicating thatthe biosorption process was favorable.

3.4.2. Freundlich isothermThe Freundlich isotherm assumes a heterogeneous surface with

a nonuniform distribution of heat of adsorption ( Freundlich, 1906 ).The equation of Freundlich isotherm is given as below:

InQ e InK F 1n

lnC e 6

where K F (L g 1) and n (dimensionless) are characteristic con-stants that indicate the extent of the biosorption, the degree of nonlinearity between solution concentration and biosorption,respectively.

The values of Freundlich constant n for AB and CR (Table 4)were all in range 210, indicating that good biosorption occurred.In addition, n values were greater than unity, indicating that the

dyes were favorably adsorbed by the fungus biomass. The high val-ues of K F (Table 4) for AB and CR implied ready uptake of the dyesfrom the solution with high adsorptive capacities of these biosor-bents. Similar trend were observed for biosorption of Remazol Bluereactive dye onto dried yeasts ( Aksu and Donmez, 2003 ), Bromo-phenol Blue Dye onto Phizopus stolonifer , Fusarium sp. Geotrichumsp. and Aspergillus fumigatus (Zeroual et al., 2006 ).

3.4.3. Dubinin-Radushkevich isothermThe Dubinin-Radushkevich (D-R) isotherm model is more

general than Langmuir isotherm, because it does not assume ahomogeneous surface or constant sorption potential ( Dubininand Radushkevich, 1947 ). The D-R model is postulated withinadsorption space close to the adsorbent surface ( Akar et al.,

2009 ), which was applied to distinguish the nature of biosorptionas physical or chemical. The model can be linearized as follows:

InQ e InQ max be2 7

where e is Polanyi potential, Q max is the theoretical saturationcapacity of biomass (mg g 1), b is a constant related to the energyof transfer of the solute from bulk solution to solid adsorbent. Theconstant b gives us the information about the mean energy of bio-sorption ( E ), which can be calculated from the following equation(Akar et al., 2009):

E 1

2b1=2 8

The magnitude of E value is useful for estimating the type of bio-

sorption process. It was found the estimated values of E for ABand CR were in the range between 21.32 and 35.35 kJ mol 1

(Table 4), which is not within the energy range of ion-exchangereactions, 816 kJ mol 1. This implied that physical adsorptionmay be one of the mechanisms for the biosorption for AB and CR.Similar results were observed for the adsorption of uranium ontoamberlite IR-118 resin ( Kilislioglu and Bilgin, 2003).

3.5. Sample characterization

It can be found from the SEM image in Fig. 4 that the surface of the fungus biomass was heterogeneous, smooth and porous. Theporous characteristics of the biomass with a bulk porosity of 76.38% indicated the biomass has a large surface area for dye inter-action and a great capacity for dye holding.

The band positions in the FTIR spectra of the biosorbent beforeand after AB and CR biosorption were presented in Table 5. Thebands at 3415 and 3418 observed after biosorption were corre-sponded to the stretching vibration of NH in the structure of CR (Wang and Wang, 2008 ) and OH formation in the structure of AB, respectively, attributing to the biosorption of AB and CR ontobiomass. The strong biosorption bands of OH and/or NH groupswere observed at 3275 cm 1 for virgin biosorbent, but this biosorp-tion peak could not be observed for the dye-loaded biomass. Theresults, with acid condition enhancing the biosorption, implicatedthat NH groups may be responsible for the dye-biosorption in thebiomass. The changes observed in the band 2920, 2925 and2851 cm 1 indicated that ion-exchange between protons of sym-metric or asymmetric CH and the symmetric stretching vibrationof CH2, respectively, of aliphatic acids ( Wahab et al., 2010 ). Thesechanges observed between 1660 and 1500 cm 1 might be due tothe electrostatic forces of attraction between the negative chargeof carboxylate anion and positive group of dyes ( Farinella et al.,

Fig. 4. SEM image of the Penicillium YW 01 biomass.

Table 5The FTIR spectral characteristics of nonviable Penicillium YW 01 biomass before andafter biosorption of AB and CR.

Suggested assignment Band positions (cm 1)

Unloadedbiomass

AB-loadedbiomass

CR-loadedbiomass

-OH and/or NH stretching 3415 3418-OH and/or NH stretching 3275 -CH symmetric stretching 2920 2925 2925-CH asymmetric stretching 2851 Amid-I 1649 1660 1633Amid-II 1541 1549 1548-CH bending vibrations 1456 1410 1411-CH bending vibrations 1398 1378 1378-SO3 stretching 1260 1230 -C-O stretching 1027 1038 1041-CH bending vibrations (aromatic) 931692

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numbers, respectively. The initial concentration of AB with a rela-tive importance of 41.43% appeared to be the most inuentialparameter in the biosorption process for AB, followed by pH(23.45%), temperature (19.17%) and time (15.95%). Temperaturewith a relative importance of 36.76% appeared to be the most inu-ential parameter in the biosorption process for CR, followed by pH(29.83%), time (24.30%) and initial concentration (9.11%). The re-sults also indicated that all of the variables have strong effects onthe biosorption capacity for AB and CR.

4. Conclusions

The inactive Penicillium YW 01 biomass was efcient as anadsorbent for the removal of AB and CR form aqueous solutions.The maximum biosorption capacity of CR was 411.53 mg g 1,which was best among the reported fungi. Kinetic study revealedthat intraparticle diffusion was the limiting step for biosorptionof AB and CR. The performance of ANN-GA appeared to be betterthan that of ANN to get the net weights which were used to assessthe relative importance of operational parameters. The dye-biosor-bent interactions were conrmed by FTIR and heterogeneous,

smooth and porous structure were observed by SEM technique.

Appendix A. Supplementary data

Supplementary data associated with this article can be found, inthe online version, at doi:10.1016/j.biortech.2010.08.125 .

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Bioresource Technology Volume 102 Issue 2 2011 [Doi 10.1016%2Fj.biortech.2010.08.125] Yuyi Yang; Guan Wang; Bing Wang; Zeli Li; Xiaoming Jia; Qifa Zho -- Biosorption of Acid Black