Surfactant Selection for the Enhanced Biological Degradation of Toluene

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1 w w m y wz Vol. 10, No. 4, pp. 26~32, 2005 œ Toluene w w w w y ½ 1 Á ³ 1 Á½ x 1 Á x 2 * 1š w zy lœw, 2 w m y œw Surfactant Selection for the Enhanced Biological Degradation of Toluene Yongsik Kim 1 ÁYounggyu Son 1 ÁJeehyeong Khim 1 ÁJihyeon Song 2 * 1 Dept. of Civil & Environmental Engineering, Korea University 2 Dept. of Civil & Environmental Engineering, Sejong University ABSTRACT Surfactants can be used to enhance the mass transfer rate of hydrophobic compounds into the biologically active liquid phase, resulting in an increase in biodegradation rate of toluene. In this study, the mass transfer rate and the biocompatibility of toluene in the presence of various surfactants were evaluated. Four anionic and nonionic surfactants were tested: sodium dodecyl sulfate (SDS), TritonX-100, Tween 80, and. Experimental results showed that at the critical micelle concentration (CMC) enhanced the solubility of toluene. However, there was no increase in the solubility of toluene by SDS and TritonX-100 at their CMCs. With the addition of each surfactant into deionized water the mass transfer rate became faster than that of the case with no surfactant. A bottle study using toluene-degrading microorganisms showed that SDS seriously reduced toluene removal presumably due to the toxicity of the anionic surfactant and/or the substrate competition between the surfactant and toluene. In addition, the degradation rate of toluene was decreased in the presence of, indicating that adversely affects the activity of microorganisms. However, TritonX-100 and Tween 80 did not decrease the degradation rate of toluene significantly. Rather, at the low concentration of TritonX-100 toluene degradation rate was even increased. Overall the experimental results suggest that TritonX-100 be the appropriate surfactant for enhanced biological degradation of toluene. Key words : Surfactant, Biocompatibility, Toluene solubility, Mass transfer rate y (m ) ƒ g ƒ w w w ƒ k. y ƒ w m w wƒ w w y : Sodium Dodecyl Sulfate (SDS), TritonX-100, Tween 80, (silicone y ). x critical micelle concentration (CMC) m w ƒ g. w, SDS TritonX-100 CMC m w ƒ j w. y ƒw m (K L a) ƒ w. m w w z x SDS m w g. SDSƒ» š,» m» y w x m wƒ w ƒ y ƒw w» w, TritonX-100 Tween 80 m wƒ j w û TritonX-100 m w ƒw. mw m w w w ƒ w y TritonX-100 *Corresponding author : songjh@sejong.ac.kr š : : m : ¾ 26

2 Toluene w w w w y 27 : y, ey, m w, 1. y x ù, t, de-emulsifiers, penetrants» w (Muligan and Gibbs, 1993). p, yw w ƒ g z ƒ j y w (Falatko, 1991). w, y œw z x column x mw y ƒ ü w PAHs (poly aromatic hydrocarbons) w k ƒ k m ü PAHs m l ý z m y y w š (Deshpande et al., 1999 Muligan et al., 2001; Chang et al., 2000; Huang et al., 2001; Edwards et al., 1991). w y w y ƒ w ƒ, t, t (Muligan et al., 2001). w y p» volatile organic compounds (VOCs) wwš w z» p w w y p t w ƒ (Maurice, 1994; Chang et al., 2000; Huang et al., 2001; Deshpande et al., 1999). y w t» t ƒ g» (K L a) ƒ k (Muligan et al., 2001).» w VOCs k,» VOCs k w w w wr, w ƒ critical micelle concentration (CMC) ƒ y ƒ micelle x wš micelleü» w» w ƒ j x y w» VOCs w g w w w VOCs w w j y w z l w, w y ƒ w ƒ š, y ù w e w w. y w ƒƒ y ƒ š, w y ƒ y w w e š w. š k toluene VOCs w w j š w w w y w š w. 2. x 2.1. x y x y» m ù w w m w xw y SDS (Sigma-Aldrich Co.) (Chang et al., 2000; Huang et al., 2001; Deshpande et al., 1999), TritonX-100 (Sigma-Aldrich Co.) (Chang et al., 2000; Hiller and Wandruszka, 1995; Edwards et al., 1991), Table 1. Chemical properties of sufactants used in this study Surfactants Properties Molecular formula Molecular weight Critical micelle concentration (CMC) SDS Anionic CH 3 (CH 2 ) 11 OSO 3 Na 288 g/mol 8.2 mm TritonX-100 Non-ionic C 9 H 17 C 6 H 4 O(CH 2 CH 2 0) 9.5 H 628 g/mol 0.25 mm Tween80 Non-ionic C 18 S 6 EO g/mol mm Goudar, 1999 Non-ionic EO = ethylene oxide group Polyether modified poly-dimethyl-siloxane 2700~4700 g/mol 1.5 mm Reference Heyder er al., 1997; Hill, 1999; Hiller and Wandruszka, 1995 Heyder er al., 1997; Huang er al., 2001; Kim et al., 2001 Deeb and Alvarez-Cohen, 1999; Falatko, 1991

3 28 ½ Á ³Á½ xá x Tween 80 (Sigma-aldrich Co.) (Yeh et al., 1999), (silicone surfactant, BYK-Chemie) (Hill, 1999; Maurice, 1994) 4ƒ ƒƒ y w Table 1 ùkü w w 6 r k, w toluene k / w w 6L» w (Song, 2001; Yang and Zhu, 2004) g/l KH 2 PO 4, 1.42 g/l Na 2 HPO 4, 0.5 g/l (NH 4 ) 2 SO 4, 3.03 g/l KNO 3 1 ml/l 50 g/l MgSO 4 7H 2 O, 14.7 g/l CaCl 2 2H 2 O, 2.86 g/l H 3 BO 3, 1.54 g/l MnSO 4 H 2 O, 2.5 g/l FeSO 4 7H 2 O, g/l CuCl 2 2H 2 O, g/l ZnSO 4 7H 2 O, g/l CoCl 2 6H 2 O, g/l Na 2 MoO 4 2H 2 O, 0.02 g/l NiCl 2 6H 2 O» 20 š, m 200 ppm v 2.2. y z x 250 ml s» k 45 ml Table 2. Surfactant concentrations used in this study Surfactant Concentration range (%) SDS CMC : wt% TritonX-100 CMC : v/v% Tween80 CMC : v/v% CMC : v/v% z, w y wì vƒ 50 ml w» gastight w» toluene z stirrer bar w 1 g» toluene sx k wš, z w w» toluene d w» toluene FIDƒ HP6890 GC manual injection w w w toluene Purge & Trap GC/FID w w x ƒ y Table 2 ùkü 3. š 3.1. y w toluene w y y CMC micelle x w š micelle ü» k» w ƒ k y ƒ toluene w ù ƒ k y w» v 200 ml, v 50 ml wš ƒ y ƒ x CMCƒ w z,» toluene» w» toluene s x w sx k w z» w toluene d w, x x (1-1) (Deeb and Alvarez-Cohen, 1999) (1-2) (Staudinger and Roberts, 2001) w w x w H atm m 3 ( mol) e ( A B T) H atm = ( ) ( ) = 10 A B T (1-1) (1-2) (1-1) toluene A š B Table 3. Toluene concentrations in the liquid and the gas phase using surfactants Surfactant Toluene injection (ppm v ) Gas phase conc. at equilibrium (ppm v ) Liquid phase conc. measured at equilibrium (mg/l) Liquid phase conc. (mg/l) calculated by H (equation, 1-1) deviation(%) Liquid phase conc. (mg/l) calculated by H (equation, 1-2) deviation(%) Deionized water SDS TritonX

4 Toluene w w w w y T (1-2) toluene A š B 1745 T Table 3 w x 22 C o š (1-1) (1-2) w w x ƒ ƒ mg/l/atm mg/l/atm Table 3 ù x 21 C o (1-1) (1-2) mw w x ƒƒ mg/l/ atm mg/l/atm x mw s x k» toluene» d toluene x mw toluene ƒ ù SDS, TritonX-100 d ƒ x w w ù w ùkþ. w, d ƒ x w d x mw ƒ y w ƒ z w ƒ toluene x SDS TritonX-100 w ƒ z ƒ š, silicone y w ƒ z ƒ, SDS ù TritonX-100 w ƒ x ù» w ƒ CMC { w w. w w y CMC y CMC w w ƒ ƒ j ù toluene micelleü w ww w»» 3.2. y w y Toluene VOCs w w w» ƒ w w g w w w w. z x» ù VOCs (2), (3), (4) w (Heyder et al., 1997). dc g V g = 0 V l dc l dt dc g dt C l * = dt V l * K a ( L C l C ) l V g C g = H» (K L a)» (1/hr), C l w (µg/l), C l» sx k * (2) (3) (4) Fig. 1. Changes in toluene concentration in the liquid phase during the abiotic bottle teste The symbols represent experimental data while lines illustrate simulated results. Table 4. Mass transfer coefficients (K L a) determined using the experimental data from the bottle studies and the nonlinear regression Surfactant K L a (1/hr) Deionized water SDS TritonX (µg/l), C g» (ppm), V l v(ml), V g» v(ml), H» sx k d» w ƒ w w H w. w K L a ùkü ƒ ƒƒ y w (K L a) w y y» 200 ml, 50 ml xwš, ƒ y x CMC w» w toluene w z 28 o C w w» d w toluene w. k y w Fig. 1 ùkü w Fig. 1 ùkù y k (2), (3), (4) w x z» w (K L a) w, w toluene w Fig. 1 Table 4 ùkü

5 30 ½ Á ³Á½ xá x Fig. 2. Biological toluene degradation in the presence of (a) SDS, (b) TritonX-100, (c) Tween 80, and (d) Silicone surfactant. Table 4 toluene» silicone y ƒ jš TritonX-100 SDS w w š ƒ û y» toluene ƒ ƒw š w 3.3. w toluene w y ƒ e w y w» toluene w z, w w j ƒ w ƒw y w y ƒ w w y ƒ e w» w y, w vƒ 50 ml wš» vƒ 200 ml w z,»» toluene w y d w. ƒ y w xw» sampling w x y w w y w š, ƒ x w w x y ƒw k w toluene w d w Fig 2(a)~(d), y ƒ ƒ k» toluene, toluene w 36 mg/l/hr w y ƒ (pure culture) toluene w w (Deeb and AlvarezCohen, 1999), w yw y ƒ y w y SDS w Fig 2(a) zw y ƒ 0.1%w/w w x» w toluene wƒ w y w w x SDS CMC 0.25%w/w x ùkù y w, y SDS w w toluene

6 Toluene w w w w y 31 wƒ ƒw w ƒ, SDSƒ cell membrane ù enzyme g y» toluene wƒ (Cserhati et al., 2002)., SDS w w y toluene w SDS» w» toluene w ƒ û (Goudar et al., 1999). TritonX-100 y w Fig 2(b) ùkù y w y ƒ j w y w TritonX-100 ƒ û w j ƒ» TritonX-100 w y š w Tween 80 y w Fig 2(c) y w y ƒ j w y w. Tween 80 w w toluene w, ƒ ƒw TritonX-100 toluene wƒ Tween 80ƒ TritonX-100 w»» š q (Kim et al., 2001). Silicone y w»» toluene ƒ w ƒ w ƒ»» toluene w w w» w» w toluene» d x y» toluene ùkû. w,» toluene š ú» toluene ƒ w y ƒ w» š q, silicone y y w w w ww 4. Toluene VOCs w ww l w y w» w x mw ƒ w š ƒ y w ƒ ƒ w š, y ƒ y e w w z 1) ƒ y ƒ CMC silicone y toluene w ƒ g SDSù TritonX -100 w toluene w ƒ 2)» toluene ƒ w y ƒ sw ùkû. w, TritonX-100, SDS j 3) SDS y w g w toluene wƒ š, silicone y y w g toluene w g. TritonX-100 Tween80 y j, TritonX-100 û toluene w ƒ ƒw y w toluene VOCs w» w l y w toluene w ƒ d silicone y BYK- 345ƒ ƒ ww y y w j TritonX-100 ww w š x Chang, M.C., Huang, C.R., and Shu, H.Y., 2000, Effects of surfactants on extraction of phenanthrene in spiked sand, Chemosphere, 41, Cserhati, T., Forgacs, E., and Oros, G., 2002, Biological activity and environmental impact of anionic surfactants, Environ. International, 28, Deeb, R.A. and Alvarez-Cohen, L., 1999, Temperature effect and substrate influence during the aerobic biotransformation of BTEX mixtures by toluene-enriched consortia and Rhodococcus rhodochrous, Biotechnol. Bioeng., 62(5), Deeb, R.A. and Alvarez-Cohen, L., 1999, Temperature effects and substrate interactions during the aerobic biotransformation of BTEX mixtures by toluene-enriched consortia and Rhodococcus rhodochrous. Biotechnol. Bioeng., 62(5), Deshpande, S., Shiau, B.J., Wade, D., Sabatini D.A., and Harwell, J.H., 1999, Surfactant selection for enhancing ex situ soil

7 32 ½ Á ³Á½ xá x washing, Water Res., 33(2), Edwards, D.A., Luthy, R.G., and Liu, Z., 1991, Solubilization of polycyclic aromatic hydrocarbons in micellar nonionic surfactant solutions, Environ. Sci. Technol, 25(1), Falatko, D.M., 1991, Effects of biologically reduced surfactants on the mobility and biodegradation of petroleum hydrocarbons, MS thesis, Virginia Polytechnic Institute and State University, Blackburg, VA. Goudar, C., Strevett, K., and Grego, J., 1999, Competitive substrate biodegradation during surfactant- enhanced remediation, J. Environ. Eng., 125(12), Heyder, B.D., Vanrolleghem, P., and Lagenhove, H.V., 1997, Kinetic characterization of mass transfer limited biodegradation of a low water soluble gas in batch experiments-necessity for multiresponse fitting, Biotechnol. Bioeng., 55(3), Hill, RM, 1999, Siloxane surfactant. In: Hill RM, editor. Silicone surfactants, New York: Marcel Dekker Inc. Hiller G.K. and Wandruszka R.V., 1995, Decontamination of oilpolluted soil by cloud point extraction. Talanta, 42(1), Huang, H.L., Lee, W.M., and Grace, 2001, Enhanced naphthalene solubility in the presence of sodium dodecyl sulfate: effect of critical micelle concentration, Chemosphere, 44, Kim, I.S., Park, J.S., and Kim, K.W., 2001, Enhanced biodegradation of polycyclic aromatic hydrocarbons using nonionic surfactants in soil slurry. Appl. Geochem., 16, Maurice, R., Porter & Associates Handbook of Surfactants, 2nd ed., Muligan, C.N., Yong, R.N., and Gibbs, B.F., 2001, Surfactantenhanced remediation of contaminated soil: A review, Eng. Geol., 60, Muligan. C.N. and Gibbs, B.F., 1993, Factors influencing the economics of biosurfactants, In: Kosaric, N (Ed.), Biosurfactants, Production, Properties, Applications. marcel Dekker, New York, p Song, J.H., 2001, Control and characterization of biomass activity and distribution in vapor-phase bioreactor for VOC removal, Doctoral thesis, the University of Texas at Austin. Staudinger, J. and Roberts, P.V., 2001, A critical compilation of Henry`s law constant temperature dependence relations for organic compounds in dilute aqueous solutions, Chemosphere, 44, Yang, C. and Zhu, X., 2004, Removal of a volatile organic compound in a hybrid rotting drum biofilter, J. Environ. Eng., 130(3), Yeh, D.H., Pennell, K.D., and Pavlostathis, S.G., 1999, Effect of Tween surfactants on methanogenesis and microbial reductive dechlorination of hexachlorobenzene, Environ. Toxicol. Chem., 18(7),

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