Acta Scientiae Circum stantiae. Rem ova l of arsena te from wa ter by using the syn thetica l iron2a lum inum hydrox ide com plexes

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1 Acta Scientiae Circum stantiae Vol. 26, No. 3 Mar., 2006,,, (V) [ J ]., 26 (3) : L iang M N, L iu H L, Zhu Y N, et al Removal of arsenate from water by using the synthetical iron2alum inum hydroxide comp lexes[ J ]. Acta Scientiae Circum stantiae, 26 (3) : ( V) 1, 2, 2, 3, 1, 1 1., , : : : : Fe ( ) A l( ), 9 Fe ( ) A l( ). X, 5 2.,,.,,, ; ph mg L - 1, mg L - 1, Fe ( ) /A l( ) 7 3. ph Freundlich Langmuir. : ; ; : (2006) : X13112 : A Rem ova l of arsena te from wa ter by using the syn thetica l iron2a lum inum hydrox ide com plexes L IANG Meina 1, 2, L IU Hailing 2, 3, ZHU Yinian 1, WANG Dan 1 1. Department of Resources and Environmental Engineering, Guilin University of Technology, Guilin Department ofmaterials and Chem ical Engineering, Guilin University of Technology, Guilin Received 12 Sep tember 2005; rece ived in revised form 18 January 2006; accepted 22 January 2006 Abstract: Based on the strong affinities of Fe ( ) and A l( ) to arsenate, nine iron2alum inum hydroxide comp lexes were synthesized as adsorbents for the arsenic removal. The scanning electron microscopy ( SEM ) images and X2ray diffraction ( XRD ) spectra demonstrated that five iron - alum inum hydroxide complexes had the m inicrystal - amorphousmorphology. of these complexes were lower than those of the pure iron hydroxide synthesized under the same conditions. The nitrogen sorption experiments indicated that the pore volume and the pore diameter The addition of alum inum hydroxide into iron hydroxide could change the superficial characteristic and crystal frame. Moreover, the adsorption experiments showed that all iron - alum inum comp lexes could adsorb aqueous arsenate effectively and with a high capacity. W hen an arsenic solution of 2 mg L - 1 was added with anyone of these comp lexes at ph , the arsenic concentration could be decreased to less than mg L - 1, the standard for drinking water set by the World Health O rganization. Among these absorbents, the comp lex with the Fe ( ) /A l( ) molar ratio of 7 /3 owned the highest adsorp tion capacity. adsorp tion isotherm s of arsenic on these comp lexes agreed well with the Freundlich or Langmuir equations at ph Keywords: iron2alum inum hydroxide complex; adsorbent; arsenate; aqueous solution Furthermore, the, (CDC) (LARC) (, 2002).,, (WHO) 1993, 50 g L g L - 1 (, : (No ) ; ( ) ; ( ) Supported by the Natural Science Foundation of China ( No ) ; the Scientific Research Foundation for the Returned Overseas Chinese Scholars, MOE of China (No ) ; the Provincial Education Department of Guangxi (No ) : (1974 ),, ; 3 ( ), E2mail: liuhailing998@ sina. com B iography: L IANG Meina (1974 ), female, engineer; 3 Correspond ing author, E2mail: liuhailing998@ sina. com

2 3 : (V) ),. (, 2004),., (, 2004), ( Halser et al., 2001 ), (, 2003), (, 2003)., (, 2002; Fendorfet al., 1997 ). Raven (1998) ; Grossl (1997) ; Fendorf (1997) X ( EXAFS), ; Halter ( 2001 ) A s (V) 2A l 2 O 3.,. (2005) 2, ; (2003) 2,, ; Lenoble (2002), m 2 g - 1, A s(v ) ph 3 6.,., mg L - 1.,,.,, X,. 1 ( Experiments) 1. 1 FeCl 3 6H 2 O A lcl 3 6H 2 O NaOH HNO 3 HCl A s 2 O 5,. : PHS23 ( ), PE2 AA700 ( Perkin2Elmer), ( C2EDL ), X (R IGAKU, CuK, nm ), NOVA 1200e ( Quantachrome), VECTOR 22 FT2IR ( B ruker) ( SEM, Joel JSM25610LV) , Fe ( III) A l ( III), A l ( III),,. ph 7. 4, FeCl 3 6H 2 O A lcl 3 6H 2 O, 1 mol L - 1, Fe ( III) /A l( III) 0. 9: : : : : : : : : 0. 9, 9 FeCl 3 6H 2 O A lcl 3 6H 2 O,, 500 ml, ml, 3 mol L - 1 NaOH ph , 30 m in, 0. 1 mol L - 1 HNO mol L - 1 NaOH ph h,,,. 105 o C 20 h, 180,. 9, Fe2A l201 Fe2A l202 Fe2A l203 Fe2A l204 Fe2A l205 Fe2A l206 Fe2 A l207 Fe2A l208 Fe2A l209, ( Fe2A l200) ( Fe2A l210). 1. 3, Fe ( ) A l ( ) K 2 CrO 7 EDTA ; X

3 ; ;. 1. 4,. A s(v) A s 2 O 5, 1 mol L - 1,. ( 25 1) g 100 ml, ph, 50 ml A s(v ),, 5 d (, 2 m in)., ph ( ph = 6), 0. 1 mol L - 1 HNO mol L - 1 NaOH, 6 h 1 h ph, 6 h ph. 5 d, m ( 2 3 ml ), 0. 2% HNO 3, A s(v ) Fe ( ) A l ( ).., g 50 ml, A s (V ) 2 mg L - 1, ph : (25 1), g, mmol L - 1, 50 ml PE, ( PE ), 380 ma, nm, 0. 7 nm, 0. 2%, 20 L, 2 L 4 g L - 1 PbCl 2 5 L 3 g L - 1., s, s, s, s. 2 (Results) , Fe ( ) /A l ( ), 1. 1 Fe A l Fig. 1 Theoretic and measured Fe and A l molar valu of the synthetical adsorbents XRD, 1. Fig. 2 2 X XRD spectra of the iron - aluminum hydroxide comp lexes

4 3 : (V) Fig. 3 IR spectrum of the iron - alum inum hydroxide comp lexes 1 Table 1 Surface structure of the iron - alum inum hydroxide comp lexes Fe2A l200 Fe2A l201 Fe2A l202 Fe2A l203 Fe2A l204 Fe2A l205 Fe2A l206 Fe2A l207 Fe2A l208 Fe2A l209 Fe2A l210 Fe /A l BET / (m 2 g - 1 ) BJH / (m 2 g - 1 ) BJH / ( cm 3 g - 1 ) /nm Fig. 4 SEM images of some synthetical iron - alum inum hydroxide comp lexes

5 ph 5. 5 ph Fig. 5 Adsorp tion efficiency of arsenic on the iron - alum inum hydroxide comp lexes at different ph, Fe2A l202 Fe2A l203 Fe2A l205 Fe2A l200 ( ), ph 7, ( 6) ; ph Fe2A l2 03 ( 7). 7 Fe2A l203 ph Fig. 7 Adsorp tion isotherm s of arsenic on Fe2A l203 at different ph 6 ( ph = 7) Fig. 6 Adsorp tion isotherm s of arsenic on the iron - alum inum hydroxide comp lexes (ph = 7) Freundlich (Q e = k n c ), logq e logc e, k n, 2. Langmuir C e /Q e = 1 / ( bq m ) +C e /Q m, C e /Q e, C e, 6 7, O rigin Fe2A l Freundlich Table 2 Freundlich isotherm parameters for the arsenic adsorp tion on Fe2A l200, 02, 03 and 05 ph k n R 2 p n Fe2A l Fe2A l Fe2A l Fe2A l Fe2A l Fe2A l

6 3 : (V) 443, Langm u ir ( ph = 7) Fig. 8 Langmuir adsorp tion model of arsenic on the iron - aluminum hydroxide comp lexes (ph = 7) 1 / bq m 1 /Q m, b Q m. 95%, Langmuir 9 Fe2A l203 ph Langm u ir Fig. 9 Langmuir adsorp tion model of arsenic on Fe2A l203 at different ph, ph = 7, Fe2A l200 Fe2A l202 Fe2A l203 Fe2A l205, ph = 5 ph = 7 ph = 9 Fe2 A l203 Q m, 3. 3 Fe2A l Langm u ir Table 3 Langmuir isotherm parameters for the arsenic adsorp tion on Fe2A l and 05 ph Q m / (mol kg - 1 ) b R 2 p n Fe2A l200 7 y = x < Fe2A l202 7 y = x < Fe2A l203 7 y = x < Fe2A l205 7 y = x < Fe2A l203 5 y = x < Fe2A l203 9 y = x < (D iscussion) 3. 1 Fe ( ) /A l( ) 1, Fe ( ) A l ( ), Fe ( ) A l( ) Fe A l ; Fe ( ) /A l( ),. Fe (OH ) 3 K sp, Fe = , A l (OH ) 3 K sp, A l = (, 1990)., OH -, FeOOH, A l ( ), A l (OH) 3 ; A l ( ) FeOOH, Fe m A l n (OH) k.,,. XRD IR. ph, Fe ( ) A l ( ), A l (OH) 3,, Fe ( ) /A l( ) d. ( Fe2A l200 ) d : nm nm nm. X (, 1978),

7 Fe2A l203 Fe2A l2 04 Fe2A l205,, ; A l ( ). A l( ), ( 2 Fe2A l Fe2A l ), d. A l( ) A l( ) /Fe ( ) 8 /1 ( Fe2A l208), 2 = 13. 7, A l ( ),.,, 2 = = A l ( ), A l ( ),,.,,.,, A l( ) A l( ),. 3, IR ( Fe2A l200), 1000 cm - 1, 530 cm cm cm - 1 2Fe2OH, cm - 1 2A l2oh., Fe2A l2 06 Fe2A l207 Fe2A l208 Fe2A l cm - 1,. - OH ( cm - 1 ) - OH ( cm - 1 ), ( : ) (, 1982), Fe2A l203 Fe2A l204 Fe2A l205 Fe2A l2 06 Fe2A l207 Fe2A l208 Fe2A l209 2A lo OH 2FeO OH,. 1,,,, Fe2A l202 Fe2A l2 03 Fe2A l205. Dubinin (, 2003) ( < 1. 5 nm) ( nm ) ( > 100 nm). Dubinin, Fe2A l202,,, Fe2A l203 Fe2 A l205,,,. Fe2A l2 03 Fe2A l204 Fe2A l205 X,, Fe2A l202 Fe2A l203 Fe2A l204 Fe2A l205,,., Fe2 A l206 Fe2A l209,,, , ph ,, A s (V ), 99. 5%, mg L - 1. ph = 5. 0 ph = 9. 0,. Raven Jain (1998), ph , mg L - 1. Raven Jain ( A s (V ) mmol L - 1, 20 mg L - 1 ),.,,,,. 6, Fe ( ) /A l ( ),. 3, ph = 7, A s(v ) : Fe2A l203 > Fe2A l202 > Fe2A l205 > Fe2A l200,. Fe2A l202 Fe2A l203, Fe2A l202 Fe2A l203, Fe2A l203 Fe2A l202, 4, Fe2A l202

8 3 : (V) 445,,, 1 m ; Fe2A l203,, Fe2 A l203 Fe2A l202. Fe2A l205 Fe2A l202 Fe2A l203, Fe2A l202 Fe2A l , Fe2A l205.,. 2, ph = 7. 0, Fe2A l200 Fe2 A l202 Fe2A l203 Fe2A l205 Freundlich. ph = 5 ph = 7 ph = 9, Fe2A l203 Freundlich. 7 3, Fe2A l203 ph Q m (ph = 5) > Q m (ph = 7) >Q m (ph = 9). Langmuir b,, (, 1992). 3, b ph,,,. ph = 5, Fe2A l203, mol kg - 1. (2004), mol kg - 1, mol kg - 1. ( 2002), Fe ( ) La ( ) mol kg - 1., A s(v ). 4 (Conclusions) 1) ph, Fe ( ) /A l ( ) 9, A s(v ). A s (V ) 2 mg L - 1, ph , 99. 5%,, mg L - 1., A s (V ). 2) 5,,.,,,. 3) A s (V ) Langmuir Freundlich. References: Chen J J, Jiang B Q, W ang W Status and progress of arsenic removal [ J ]. Jiangxi Chem ical Industry, 2: 1 4 ( in Chinese) Fendorf S, Eick M J, Grossl P, et al A rsenate and Chromate Retention Mechanism s on Goethite. 1. Surface Structure [ J ]. Environ Sci Technol, 31 (2) : Grossl P R A rsenate and Chromate Retention Mechanism s on Goethite. 2. Kinetic Evaluation U sing a Pressure - Jump Relaxation Technique [ J ]. Environ Sci Technol, 31 (2) : Gu T R, Zhu Y, L i W L, et al Surface Chem istry [ M ]. Beijing: Science Press, ( in Chinese) Guiyang Institute of Geochem istry of Chinese Academy of Sciences Handbook for M ineral Identification U sing Powder X - ray D iffraction [M ]. Beijing: Science Press, ( in Chinese) HalserW E, Pfeifer H R A rsenic (V ) adsorp tion onto 2A l 2 O 3 between 25 and 70 [ J ]. App lied Geochem istry, 16 ( 7 8 ) : Han L J, Cui Y Q, Lui D X, et al Study on the removal of arsenic in waste waters from compound sem i - conductor manufacturing [ J ]. Journal of Q ingdao University ( E&T), 19 (1) : ( in Chinese) Jiang H, L iao L B, W ang S P Adsorp tion of arsenic on Fe oxyhydroxide - montmorillinitre comp lex [ J ]. Geochim ica, 31 (6) : ( in Chinese) Lenoble V, Bouras O, Deluchat V, et al A rsenic adsorption onto p illared clays and iron oxides [ J ]. Journal of Colloid and Interface Science, 255 (1) : L iao L B, Donald G F Adsorption of arsenate and chromate on Hydroxy2Fe2Montmotillonite [ J ]. Science in China ( Ser. D Earth Science), 35 (8) : ( in Chinese) M inistry of Health of the Peop le Public of China GB Hygienic Standard of Bottled Purified W ater for D rinking [ S ]. Beijing: Standards Press( in Chinese) PengW S, L iu G G Collection of Infrared Spectra of M inerals [ Z]. Beijing: Science Press, ( in Chinese) Raven K P, Jain A, Loeppert R H A rsenite and A rsenate Adsorption on Ferrihydrite: Kinetics, Equilibrium, and Adsorp tion Envelopes [ J ]. Environ Sci Technol, 32 (3) : Staff Room for Inorganic Chem istry of Dalian University of Technology Inorganic Chem istry 3 rd edition [ M ]. Beijing: H igher

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