천연산점토광물을이용한폐 - 유기염료제거

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1 Printed in the Republic of Korea 천연산점토광물을이용한폐 - 유기염료제거 * w œw ( ) The Removal of Organic Dye Waste using Natural Clay Minerals Jung-Chul Park* Department of Electronic Materials Engineering, Silla University, Busan , Korea (Received May 17, 2006). w M78 KJ, 2 m w y CTMA(M-1, KJ-1), DSDMA(M-2, KJ- 2) š TMSA(M-3, KJ-3) w mÿ w w. w mÿ w s wù œ š acid blue 92 acid red 1 x mw M-1, M-3, KJ-1 KJ-3 w m M KJ 0% ƒ¾ ƒ. w M-1 KJ-3 w 100% w w mƒ œ w» w ƒ š w. :, m, y ABSTRACT. Acid red 1 and acid blue 92, anionic dyes, were removed from synthetic wastewater by the surfactantmodified clay minerals. Two different clays, such as Korean clay(m78) and Japanese clay(kj) were treated with three different sulfactants, CTMA, DSDMA and TMSA. The surfactant-modified clay minerals such as M-1(CTMA), M-3(TMSA), KJ-1(CTMA) and KJ-3(TMSA), showed high removal efficiencies with dyes, while M-2(DSDMA) and KJ-2(DSDMA) could adsorb both dyes with relatively low efficiencies. Furthermore, almost 100% absorption of both dyes onto M-1(CTMA) and KJ-3(TMSA) revealed the possibility that these materials can be used for the removal of hazardous organic dyes from wastewater. Keywords: Surfactants, Clays, Removal of Dyes ƒ s» s j z w wš w k w y w š k q w x w ƒ. t œ s w s», ww w ƒ ƒ w j š. s», šx s» e w m ƒ z š. w w w ¾ j š š w «xw 321

2 322. ƒ» w ƒ ƒw š ƒ y w w š. 1-19, y w mw ú w ƒ. ƒ» ƒ š. w l w. ù x s w w p. ÿw ù y wš y» w wƒ» w ƒ. w mÿ w z ƒ š. e m e» w w», w ƒ y w w š d ³ Ÿ, (plane) š q(sheet) w ww,, q s w. d(layer) q w. mÿ pw yw w w y w -. w d w t, j»ù ey w. xk, y,,, t, q. y yw š. d ³ w w mÿ ù» w Ÿ t w ey ƒ š w. w» mÿ w w.» m w» w ƒ w 4. Boyd ƒ 4ƒ w m e» w» w ww Evans 5» mü y» m œ q w» w œ f ƒ w» w š w. Smith 6 10 w mù p w tetrachloromethane w w w w. mÿ w - z» w mÿ Cetyltrimethylammonium Bromide(CTMA), Distearyldimethylammonium Chloride (DSDMA), Trimethylstearylammonium Chloride(TMSA) w e» jš, mÿ w s wù œ š acid blue 92 acid red 1 w š w. x x m M78(w ), KJ( ) 2 m w. m wì w, <2 µm» w Fig. 1. Structures of acid red 1 and acid blue 92.

3 w.» w» w 6% H 2O 2 k» 1 ƒ ò 1 N- NaCl ƒw d +xk Na y k. óù z, NaCl w» w m n (dialysis membrane) AgCl e» ¾ n yw. mass cylinder stokes law w w k z CTMA, DSDMA TMSA m y š w 1.5 v v g(75%) w g m 10 g g. 65 C w 3 o k z CTMA, DSDMA TMSA yw 3 65 o C» g. óù z AgBr(y AgCl)e» ¾ v v g(75%) w g. z y w m ƒƒ M y KJ š CTMA w m ƒƒ M-1, KJ-1 DSDMA w m M-2, KJ-2 TMSA w m M-3, KJ-3» w. X- z (XRD) Ÿ xk XRD ww. d»» Shimadzu 6000 w. d Fig. 2. Structures of cationic sulfactants. mÿ w s-» 323 Ni fiterƒ Cu Kα w. X- p 30 kv 16 ma g. n-alkylammonium w d w d 7 n-alkylammonium chloride (the number of the carbon=4, 6, 8, 10, 12, 14, 16, 18) 6 ml m 200 mg š 65 C o 48 k z z 48 g. óù z k k w» w k AgCl e» ¾ 10z w. z 65 C o 0.01 torr w œ w. k - m basal spacing X- z» d w. x e» m, 100 mg 50 ml x š 500, 1000, 1500, 2000 ppm acid blue acid red ƒƒ 4 ml ƒw 16» w k z 10,000 rpm 20 g. w UV Ÿ» w acid blue 92 q 571 nm acid red nm ƒƒ Ÿ d w w. m Fig. 3 k - m w k k w basal spacing w., m KJ k Å ƒ k d xk m d œ swš, k ƒ ƒw d ƒw k Å ƒ k d xk m d œ ssw. l, m s³ w 0.36 eq/(si,al) 4O 10 w. w, ü m, M78 k Å ƒ k d xk m d œ swš, k ƒ ƒw d

4 324 Fig. 3. Variation of basal spacings and charge densities of RNH 3-aluminosilicates with the number of carbon atoms in RNH 3 +. Fig. 4. XRD patterns of M78, M78-1(CTMA), M78-2 (DSDMA) and M78-3(TMSA). ƒw k Å ƒ k d x k m d œ ssw. l, m s³ w 0.33 eq/(si,al) 4O 10 w. w w ƒ p ù p ü m, M78 m, KJ m +ù w w y ƒ w», Na K +, Ca 4ƒ 2+ y y w e». m w ey jš» 4,6 w ey ù y w m mü k w ƒw» w ƒw w» w. w j 12,13 y w bentonite y w q š ü» w. Na y w m d + y w ùkù d y Fig. 4 5 w. Fig. 4 ùkù ü m M78, y k d yƒ ùkù. M78-1(CTMA) M78-3(TMSA) y k ƒ w 21 Å d ùküš k ƒ j M78- Fig. 5. XRD patterns of KJ, KJ-1(CTMA), KJ-2(DSDMA) and KJ-3(TMSA). 2(DSDMA) 32 Å j ù kùš Fig. 5 w w ùküš. md Ì 9.6 Å ƒƒ d 9.6 Å m d y ƒ w., X- z m d y ƒ w. Table 1 2 y» m M KJ, š ƒƒ CTMA, DSDMA š TMSA m M-1, M-2, M-3, KJ-1, KJ-2, KJ-3 ƒ, acid red 1 acid blue 92 ùkü. y» m M KJ CTMA TMSA M-1, M-3, KJ-1

5 Table 1. Removal efficiencies of acid red 1 onto various clays m 500 ppm 1000 ppm 1500 ppm 2000 ppm M 0 % 0 % 0 % 0 % M % 100 % 100 % 100 % M % 72.3 % 40.4 % 25 % M % 99.7 % 98.3 % 96.9 % KJ 0 % 0 % 0 % 0 % KJ % 99.5 % 96.1 % 90.4 % KJ-2 84 % 50 % 24.3 % 16.5 % KJ % 99.9 % 99.9 % 95.7 % mÿ w s-» 325 Table 2. Removal efficiencies of acid blue 92 onto various clays m 500 ppm 1000 ppm 1500 ppm 2000 ppm M 0 % 0 % 0 % 0 % M % 99.9 % 99.8 % 100 % M % 97.5 % 86.3 % 81.6 % M % 99.9 % 99.2 % 98.9 % KJ 0 % 0 % 0 % 0 % KJ % 100 % 99.4 % 98.5 % KJ % 51.6 % 43.1 % 26 % KJ % 100 % 99.9 % 99.8 % š KJ-3 ù. w m M M-1 š KJ KJ-3ƒ ƒ 100% w š w. DSDMA x M-2 KJ-2 ƒƒ CTMA TMSA m w x w. w y DSDMAƒ CTMA y TMSA w w œ j bulky y w, DSDMAƒ m d œ m w ƒ» j w DSDMA m w j w š w. wr Fig. 6ƒ 7 acid red1 acid blue 92 UV rp M, M-3, KJ, KJ-3 x z UV rp š. surfactants Fig. 6. (a) UV spectra of the resiclual concentration after treatment of the acid red 1 (1000 ppm) using M or M-3, (b) UV spectra of acid blue 92 (1000 ppm) in the presence of KJ or KJ-3. w m w m acid blue acid red ƒƒ 4 ml ƒw 16» w k z 10,000 rpm 20 k z w UV Ÿ» w Ÿ d w. acid blue 92 q 571 nm acid red nm ƒ ƒ Ÿ ùkü. surfactant w m w w TMSAƒ M-3 KJ-3 100% ƒ¾ ùkü. y x m M-1, M-3, KJ-1, KJ-3 w ƒ k p M-1 KJ-3 w 100% w w mƒ œ

6 326 w y CTMA (M-1, KJ-1), DSDMA (M-2, KJ-2) š TMSA (M-3, KJ-3) w mÿ w. X- z m d y ƒ w ƒƒ d w ý. w mÿ w s wù œ š acid blue 92 acid red 1 x mw M-1, M-3, KJ-1 KJ-3 w m M KJ 0% ƒ¾ ƒ. w M-1 KJ-3 w 100% w w mƒ œ» w ƒ š w. x Fig. 7. (a) UV spectra of the resiclual concentration after treatment of the acid blue 92 (1000 ppm) using M or M-3, (b) UV spectra of acid blue 92 (1000 ppm) in the presence of KJ or KJ-3.» w ƒ š w. w» w ƒ ƒw š ƒ y w w š. p ù œ» ù j wù w ƒ w. e m w e» w w», w tw. w M78 KJ, 2 m 1. Jordan, J. W., Organophilic bentonites. Swelling in organic liquids, J. Phys. Colloid Chem., 1949, 53(2), Snoeyink, V. L., Weber, W. J. and Maj, H. B., Sorption of phenol and nitrophenol by active carbon, Environ. Sci. and Eng., 1969, 3, Knettig, E., Thomson, B. M., Hrudey, S. E., Competitve activate carbon adsorption of phenolic compounds, Environ. Pollute. Ser. B, 1986, 12, Boyd, S. A., Lee, J. F. and Mortland, M. M., Attenuating organic contaminant mobility by soil modification, Nature, 1988, 333, Evans, J. C. and Pancoski, S. E., January 22-26, Organically modified clays, Paper No , Transportation Research Board, 68th Annual Meeting, Washinton, D.C Smith, J. A. and Gaian, A., Sorption of nonionic organic contaminants to single and dual organic cation bentonites from water, Environ. Sci. Technol., 1995, 29, Lagaly, G. A. and Weiss, A., Neue Methoden zur Characterizierung und Identifizierung queiiungsfahiger Dreischichttonminerale, Z. Pflanzenernahrung u. Bodenkunde, 1971, 130, Cadena F., Use of tailored bentonite for selective removal of organic pollutants, J. Enveron, Eng., 1989, 155,

7 mÿ w s-» Brownawell, B. J., Chan, H., Collier, J. M. and Westal, J. C., Adsorption of organic cations to natural materials, Enveron. Sci. Technol., 1990, 24, Keeran, R. S. and Fogler, H. S., Use of inorgano-organoclays in the removal of periority pollutants from industrial wastewater; structural aspects, Clays and Clay Mineral, 1990, 38, Lee, J. F., Mortland, M. M. and Boyd, S. A., Shapeselective adsorption of aromatic molecules from water by tetramethlyammonium-smectite, J. Chem. Soc., Faraday Trans., 1989, 85(9), Lee, J. F., Crum, J. R. and Boyd, S. A., Enhanced retention of organic contaminants by soil exchanged with organic cations, Environ. Sci. Technol., 1989, 23, Jeon, Y. W., Curtis, C. W. and Kiggun, B. M., An investigation of the effect of antistripping agents on silica adsorption of asphalt functionalities, Fuel Sci. Tech. Int., 1990, 8(3), Beall, G. W., March 17, Method of immobilizing organic contaminants to form non-flowable matrix thereform, U. S. Patent Number 4,650, Beall, G. W., October 29, Method of removing organic contaminants from aqueous compositions, U. S. Patent Number 4, Smith, J. A., Jaffe, P. R. and Chiou, C. T., Effects of ten quaternary ammonuim cation on tetrachlorometane sorption to clay from water, Environ. Sci. Technol., 1990, 24, Holsen, T. M., Taylor, E. R., Seo, Y. C. and Anderson., P. R., Removal of organic chemicals from aqueous solutions with surfactant-coated ferrihydrite, Environ. Sci. Technol., 1991, 25, Zhang, Z. Z., Sparks, D. L., Scrivner, N. C., Sorption and desorption of quarternary amine cations on clays, Environ. Sci. Technol., 1993, 27, ½,» ù p w r, w w ½w,,, y ƒ gq m w ù», J. Korea Ind. & Eng. Chem., 1995, 6,

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