adsorption_biodegradation_orshansky

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War. Res. Vo l. 31, No. 3, pp. 391-39 8, 1997 1997 ElsevierScience LtdPergamon Printed in G reat Britain. All rights reservedP l l : S00 43 -13 54 (96 )00 22 7-8 0043-1354/97 $17.00 + 0.00

C H A R A C T E R I S T IC S O F O R G A N I C S R E M O V A L B Y P A CTS I M U L T A N E O U S A D S O R P T I O N A N D B I O D E G R A D A T I O N

F R I E D A O R S H A N S K Y a n d N A V A N A R K IS * @E nvi ronm en ta l and W ate r R esources E ng inee r ing , T echn ion- - I s r ae l I ns t i tu t e o f T echno logy ,Tech nion Ci ty , Ha ifa 32000, Israel

(First received Augu st 1995; accepted in revised orm July 1996)A bs t r ac t - -T he use o f pow dered ac t i va t ed ca rbon t r ea tm en t (P A C T ) , based on s im ul t aneous adso rp t i onand biode gradat io n, i s effective for t reat ing orga nic toxic pol lutants , present in indu st r ia l wastewaters .R em ova l o f pheno l and an i l i ne f rom aq ueous so lu t i ons by b io log ica l t r ea tm en t a lone , by adso rp t i on onpow dered ac t iva t ed ca rbon (P A C ) a lone and by s im ul t aneous adso rp t i on and b iodegrada t i on w erecomp ared. In the adso rpt ion experiments , Lang mu ir adsorp t ion i sotherms were obta ined, f rom which Qo,the l imi t ing adso rpt ion capacit ies , a nd b , the cons tant re la ted to the energy of adsorpt io n, weredetermined. Q values of phen ol and ani l ine were foun d to b e s imi lar , whi le the energy-re la ted con stantfor an i l ine was f ive t imes higher than for phenol . A ddi t io n of mineral nut r ients , needed for the biologicalt reatmen t , a nd inact ivated microbial ce ll s increased the l imi t ing adsorpt io n capacit ies and s igni ficant lydecreased the energy re la ted constants . In b iological t reatm ent a lone, kinet ic studies showed that ani l inew as m ore r e s i st an t t o b iodegrada t i on t han pheno l . I n t he s im ul t aneous adso rp t i on and b iodegrada t i onprocess , the PAC presence di f ferently af fected the b ioox idat ion of pheno l and ani l ine . Wh i le the PACenhanced the microbial respi ra t ion in the phenol bioreactor , i t s igni f icant ly reduced the microbialrespi ra t ion in the an i l ine bioreactor . Dif ferent organ ic removal mecha nisms are suggested in P AC T forphen ol and ani l ine , due to thei r d if ferent energy of adsorpt ion. The respi rometr ic studies are recomm endedas an adequ ate tool for p redic t ion of toxic organics remova l capabi l i t ies f rom ind ust r ia l wastewaters byPA CT . 199 7 Elsevier Science Ltd. A ll rights reservedKey words--powdered ac t i vat ed ca rbon t r ea tm en t (P A C T ) , m echan i sm s , s im ul t aneous adso rp t i on an db iodegrada t i on , pheno l , an i l i ne

N OM EN CL ATU RE s i m u l t a n e o u s a d s o r p t i o n a n d b i o d e g r a d a t i o n . W a s t e -Ads or p t i on w a t e r p u r i f i c a t i o n , b y p o w d e r e d a c t i v a t e d c a r b o nt r e a t m e n t ( P A C T ) , w h i ch w a s in t r o d u c e d b y D u P o n tb = energy re la ted Langmuir constant (L / rag)C = l iq u i d p h a se c o n c e n t ra t i o n o f p o l lu t a n t a t ( H u t t o n a n d R o b e r t a c c i o , 1 9 7 5 ) h a s b e e n b a s e de q u i li b r iu m ( m g /L ) o n t h e s e t w o p r o c e s s e s . T h e m e c h a n i s m s i n v o l v e dq~ = a d s o r b e n t p h a se c o n c e n t r at i o n o f p o l l u t an t a t i n t h e c o m p l i c a t e d s i m u l t a n e o u s a d s o r p t i o n a n d

e q u i li b r iu m ( m g/ g) b i o d e g r a d a t i o n p r o c e s s s t i ll n e e d t o b e s t u d i e d .Q " = m a x i m u m , o r l im i t in g , a d s o r p ti o n c a p a ci ty ( mg /g T w o d i f f e r e n t P A C T m e c h a n i s m s a r e f o u n d i n t h eP A C ) l i t e r a t u r e . T h e f i r s t o n e ( K a l i n s k e , 1 9 7 2 ; P e r r o t t i a n dBiodegradation R o d m a n , 1 9 7 4 ; S p e t i e l , 1 98 9 ) s u g g e s t s a m u t u a l e f fe c tB OD r**v = R esp i rom e tr i c B iochem ica l O xygen D em and o f t he m ic ro b i a l ce l l s an d t he po w d ere d ac t i va t ed(mgO2 uptake/ rag subst ra te removed )

K , = H a l d a n e i n h i b i to r c o n s t a n t ( ra g/ L) c a r b o n ( P A C ) . T h e p r e s e n c e o f P A C i n c r e a s e s t h e#ma~ = m ax im um spec if ic b iom ass g row th r a t e (h -~) l i q u id - so l i d su r f ace s , on w h ich m i c ro b i a l ce l l s ,R = re s p ir o m e tr ic b i o m a ss e q u i v al e n t ( m gO 2 u p t ak e / e n z y m e s , o r g a n i c m a t e r i a l s a n d o x y g e n a r e a d s o r b e d ,m g b io m a ss f or m ed ) p r o v i d i n g a n e n r i c h e d e n v i r o n m e n t f o r m i c r o b i a lY = ce ll y i e ld coef fi ci en t (m g b iom ass fo rm ed /m g m e tab o l i s m . S u r f ace ca t a lys i s o f ph ys i c o -c hem ica lsubst ra te removed) r e a c t i o n s i s a l so p o s s i b l e o n t h e s u r f a c e o f a c t i v a t e d

c a r b o n ( K a l i n s k e , 1 9 72 ), M i c r o b i a l e n z y m e s , e x -INTRODUCTION c r e t e d i n t o c a r b o n m i c r o p o r e s , b r i n g a b o u t e x t r a -I n m a n y n a t u r a l e c o s y s te m s a c o m b i n a t i o n o f c e l lu l a r b i o d e g r a d a t i o n o f a d s o r b e d o r g a n i c s a n d

b i o lo g i c a l a n d a d s o r p t i o n p r o ce s se s i s a c o m m o n b i o r e g e n e r a t i o n o f t h e a c t iv a t e d c a r b o n . T h e c a r b o np h e n o m e n o n . O r g a n i c p o l l u ta n t s , d is c h a rg e d f r o m a d s o r p t i o n c ap a c i ty , c o n t r o l le d b y t h e b i o r e g e n e ra -i n d u s tr i e s, a r e r e m o v e d f r o m th e e n v i r o n m e n t d u e to t i o n , is h ig h l y in c r e a se d a n d t h e c a r b o n a d s o r p t i o n

c o l u m n c y c le i s p r o l o n g e d , a s c o m p a r e d t o p u r e*A uthor t o w hom a l l co r r e spondence shou ld be addres sed ad so rp t i o n sys t e m s a lon e . A s a r e su l t , w h en[ Fa x: + 9 72 4 8 2 2 8 8 98 ]. s i m u l t a n e o u s b i o d e g r a d a t i o n a n d a d s o r p t i o n o c c u r s ,

391


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392 F . Orshansky and N. Nark i sthe o rg an ic co n t am in an ts r em ov a l e f f i c ien cy an d the Table 1. Composi tion o f minera l nu tr ien tsin the synthetic aqu eou s solutions, atf i n a l w a t e r q u a l i t y a r e s u b s t a n t i a l l y i m p r o v e d p H 7.2(P er r o t t i an d R od m an , 1974) . Cons ti tuent Concen trat ionT h e s e c o n d m e c h a n i s m i s s u g g e s t e d b y s e v e r a l (NH4)2 SO4 500 mg /La u t h o r s ( E h r h a r d t a n d R e h m , 1 9 8 5 ; C r a v e i r o a n d M gSO 4"V H20 2 00 m g/ LM a l i n a , 1 9 9 1 ; X i a o j a n e t a l . , 1991) . Th ey re po r te d on Phospha te buffer 30 m t / tCaCI2 27.5 mg /Lo p p o s i t e r e s u l t s , w h i c h s h o w e d a g r a d u a l d e c r e a s e i n F eC h .6 H 20 0 .5 m g /Lo r g a n i c s u b s t a n c e s e l i m i n a t i o n , a f t e r s e v e r a l a d s o r p -t i o n c y c l e s i n t h e p r e s e n c e o f m i c r o o r g a n i s m s . T h i sp h e n o m e n o n w a s ex p l a in e d a s P A C sur face sa tu - suspensions were in the range o f 30-40 mg ce l l s/L . At ther a t i o n , w h i c h b r o u g h t a b o u t r e d u c t i o n o f o r g a n i c s e n d o f U V r a d ia t io n , t h e c o m p l e t e m i cr o b ia l ce ll sr e m o v a l e f f i c i e n c i e s , i n d i c a t i n g t h e a b s e n c e o f t h e i n a c ti v a ti o n w a s c o n f ir m e d b y s ee di ng t h e m o n s o li d D i f c ob i o r e g e n e r a t i o n p h e n o m e n o n . X i a o j i a n e t a l . (1991) nu t r i en t agar . Ba tch adsorp t ion experiments were ca r r i edou t , a s desc r ibed by Nark i s and Ben-David (1985) . To as u g g e s t e d t h a t e x t r a - c e l l u l a r e n z y m a t i c r e a c t i o n s s er ie s o f 5 00 m l E rl en m ey er -f la sk s c o n t a in i n g 2 5 0 m L o fc a n n o t t a k e p l a c e w i t h i n t h e s o r b e n t ' s t i n y m i c r o - s t o ck s o l ut i on s o f 1 6 00 m g / L p h e n o l o r 12 00 m g / L a n i li n ep o r e s , s i n c e t h e e n z y m e ' s m o l e c u l e s a r e l a r g e r t h a n i n di st il le d w a t e r o r in t h e n u t ri e n t s o lu t io n , p re ci se lyweigh ted BDH powdered ac t iva ted ca rbon doses , be tweent h e m i c r o p o r e s ' s i z e . T h u s , t h e i m p r o v e m e n t o f 4 a n d 2 4 g / L , w e r e a d d e d a n d w e r e s h a ke n i n a s h a k e r f o rw a s t e w a t e r p u r i f i c a t i o n i s c o n s i d e r e d a s a r e s u l t o f a 2 4 h a t 2 5 + I C . A p r e li m i n a r y te s t s h o w e d t h a t t h es i m p l e c o m b i n a t i o n o f a d s o r p t i o n a n d b i o d e g r a d a - a d s o r p t io n e q u i li b r iu m w e r e r e a ch e d a f t er 6 h c o n t a c t t im e .t i o n , w i t h o u t m u t u a l e n h a n c e m e n t . B o t h t h e o r i e s d o T h e r e f o re , i n o r d e r t o e n s u re t h a t t h e a d s o r p ti o n s ys te m sn o t s u p p l y e n o u g h q u a n t i t a t i v e a d s o r p t i o n a n d r e a ch e d e q u i li b r iu m , t h e f la sk s w e r e s h a k en f o r 2 4 h . A t t h eend o f this period, th e solut ions were f i ltered an d th eb i o k i n e t i c d a t a i n o r d e r t o e v a l u a t e t h e P A C r o l e i n r e si d u al p h e n o l o r a n i li n e c o n c e n t r at i o n a t e q u i li b r iu m int h e r e m o v a l o f o r g a n i c s b y P A C T . t h e f i lt r at e s o l u ti o n s w e r e d e t er m i n e d. L i n e ar i ze d L a n g m u i rT h e a i m s o f t h i s r e s e a r c h w e r e t o s t u d y t h e a d s o r p t io n i s o th e r m s w e r e o b t a in e d f r o m w h i c h t h e l im i t in gm e c h a n i s m s a n d p h y s i o l o g i c a l a s p e c t s o f t h e s i m u l - a d s o r p t io n c a p a c it y Q , i n m g a d s o rb e d o r g a n ic m a t t e r p e rt a n e o u s a d s o r p t i o n a n d b i o d e g r a d a t i o n p r o c e s s f o r g r a m P A C , b th e co n s ta n t r el at ed t o t h e e n er g y o fadsorption, in L/mg, and the correlat ion coeff icient r , werer e m o v a l o f p h e n o l a n d a n i l i n e f r o m a q u e o u s c a lc u la te d .s o l u t i o n s ( N a r k i s a n d O r s h a n s k y , 1 9 9 3 a , b , 1 9 95 ). B i o o x i d a ti o n k i n et ic p a r a m e t er s w e re d e t e rm i n e d i n b a t c hreac to rs (Er lenmeyer f la sks o f 500 mL vo lume) , mixed by ashaker , which con ta ined 250 mL media o f nu t r ien t so lu t ionEXPERIMENTAL wi th an in i ti a l mic rob ia l b iomass be tween 30 and 40 mg /LM a t e r i a l s and va r ious pheno l o r an i l ine concen t ra t ions , f rom 50 to500 mg /L. In paral lel , biod egrad ation k inet ic s tudies w ereThe fo l lowing chemica l s were used in th i s r e sea rch : ex t ra ca r r i ed ou t by an "02 su r roga te" t echn ique (Gaud y et al . ,pure an i l ine , manufac tu red by Merck , Darm stad t , 198 8) us ing Saprom at e lec t ro ly t i c r esp i romete r . S tandardGerm any; ana ly t i cal g rade pheno l , manufac tu red by dev ia t ion o f oxygen up take resu lt s were ca lcu la ted to beRiede l -de -Haen , Hano ver , Germ any; powdered ac t iva ted +2 .5% . Biok ine t ic cons tan t s ca lcu la t ions (Gaud y ' s ap -ca rbon , p roduc t o f BDH C hemica l s L td , Poo le , Eng land ; p roach) were ca r r i ed ou t accord ing to Gau dy e t a l . (1988)4-aminoan t ipyr ine , p rodu c t o f Janssen , Gee l , Be lgium; and Roz ich and Gaudy (1992). A ca l ib ra t ion curve o f2-naphtho l-3.6 disulfonic acid disod ium sal t , produ ct of micro bial suspension optical densi ty at 2 = 560 nm as aF luka Chem ika , Swi tze rland . func t ion o f d ry ce l l mass concen t ra t ion had been p repared

and used fo r eva lua t ion o f the b iomass inc rement ra te .M e t h o d s The s imul taneous adsorp t ion and b iodegrada t ion p rocessHete rogeneous mic rob ia l cu l tu re , ob ta ined f rom raw resp i romet r ic s tud ies were pe r fo rmed in Saprom at ' s ba tchsewage , passed th rough adap ta t ion dur ing a 2 -mon th reac to r s con ta in ing 250 mL so lu tions , w i th the fo l lowingperiod, to gradu ally increasing phen ol or an i l ine concen- ingredients: phenol or ani l ine (500 mg/L ), mine ral nutr ients ,t r a t ions in a con t inuous f low reac to r , chemos ta t . The acc l imated mic rob ia l b iomass (30-40 mg/L ) and va r iousadap ta t ion s ta r ted wi th feed ing media conce n t ra t ions o f PA C concen t ra t ions between 0 .74 and 3 .68 g /L . One ba tch200 mg /L pheno l o r an i l ine, which was inc reased by reac to r d id no t con ta in PAC and se rved as a con t ro l .100 mg/L each week , up to 1000 mg/L . The feed ing so lu t ion Pheno l concen t ra t ions were de te rmined by a 4 -aminoan-con ta ined , besides pheno l and an i l ine , nu t r i en t s in t ipyr ine metho d and by CO D (S tandard Metho ds fo r theconcen t ra t ions as wi ll be fu r the r desc r ibed . The vo lume of Exam ina t ion o f W ate r and Was tewate r , 1992) . Ani l inethe reac to r was 2 .15L . concen t ra t ion was de te rmined by d iazo coup l ing wi thAdsorp t ion i so the rms were de te rmined separa te ly fo r 2 -naph tho l -3 ,6 -d i su l fon ic ac id d i sod ium sa lt (Korenm an ,pheno l and an i l ine in d i s t il l ed wa te r so lu t ions , a s we l l a s in 19 75 ) and by d i rec t UV absorp t ion a t 2 = 230 nm.aqueous so lu t ions con ta in ing m inera l nu t r i en t s and Spec t ropho tom et r ic measurements were ca r r i ed ou t byinac t iva ted mic rob ia lce l l s . Fo r example , the com pos i t ion of us ing M i l ton Roy Spec t ron ic 6 01 . Al l the da ta a reminera l nu t r i en t s used in the case o f 500 mg/L pheno l r epresen ta tive o f r epea ted exper iments .s tudies is given in Table 1. The same nutr ients were addedto al l the s tudied systems, in pro por t ion to the organ ic RESULTS AND DISCUSSIONsubs t ra te concen t ra t ions . The s tock so lu t ion o f thep h o s p h a t e b u f fe r w a s p r e p a re d a c c o r d in g t o t h e B O D t e st , T h e a i m s o f t h i s r e s e a r c h w e r e t o s t u d y t h ea s d e sc r ib e d i n t h e S t an d a rd M e t h o d s f o r t h e E x a m i n at io n s i m u l t a n e o u s a d s o r p t i o n a n d b i o d e g r a d a t i o n p r o c e s so f W a te r a nd W a s t ew a t er ( 19 9 2) . T h e in a c ti v at io n o f t h e f o r t h e r e m o v a l o f t o x i c o r g a n i c c o m p o u n d s , p h e n o lmic rob ia l b iomass w as ca r r i ed ou t a t 30 min o f U Vr a d i a ti o n o f t h in l ay er s, 7 - 9 r a m , o f m i c r o b ia l s us pe ns io n s a n d a n i l i n e , f r o m p o l l u t e d w a t e r s . I n t h e f i r s t s t a g e o fd i sp e r se d i n t a p w a t e r. T h e c o n c e n t r a ti o n o f t h e m i c r o b ia l t h i s r e s e a r c h e a c h p r o c e s s , a d s o r p t i o n a n d b i o d e g r a -


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Char ac te r is t ic s o f or gan ic s r e mo val by P A CT 39310, 700

9 C J q e . 0 . 3 6 0 3 + 7 . 3 6 9 x 1 0 3 . C / 6 0 0( ~ - 1 3 5 . 7 engJO . a ( - - 4 0 0 m ~e b - 0.02o4 L/m0 ~ a , " "7 " " E 5 0 0 ~ 3 0 0 m o l L~ 6 ~ ~ " ' t ' = l H ' ' ' ' ' ' ~

3 . e . ~ f e , . ~ . ~ . , , . . . . . . ; : 1 -O 0 ~- m =o lL ; . ; ; ; : ~ : . :

l q0 0 . . . . , . . . . i . . . . , . . . . . . . . . i . . . . , -

2 0 0 4 0 0 6 0 0 8 0 0 1 0 0 0 1 2 0 0 0 5 1 0 1 5 2 0 2 5 3 0T I M E ( h r s . )C P H E N O L E Q U I L I B R IU M C O N C E N T R A T I O N ( ra g /L ) F i g . 3 . O x y g e n u p t a k e d u r i n g b i o d e g r a d a t i o n a l o n e o fF i g . 1. L i n e a r iz e d L a n g m u i r a d s o r p t i o n i s o t h e r m o f p h e n o l v a r i o u s i n i t i a l p h e n o l c o n c e n t r a t i o n s i n b a t c h b i o l o g i c a lin d i s t i l l e d wate r s o lu t ion on pow de r e d ac t ivate d c ar bon , r e actors .

2.0'C , ./ qe - 7 . 4 7 6 x 1 0 - 2 + 7.907. x 10 3. C Adsorption alone( l o . 1 2 6 . s m g /gb-010S~L/m. / Adso rpt ion isothe rms of phenol and ani l ine on

1.s. -, PAC were studied in disti l led water aqu eou s~, solut ions, in the absence and presence of mineral- nutr ients, and inact ivated microbial cel ls . Theo~ 1.0. l inearized form of Lan gmui r adso rpt i on isother mo equat i ons were obta ined, as sho wn in Figs 1 and 2,o from which the l imi t ing adso rpt io n capaci ties Qo and

0.s. the energy re la ted Lang muir consta nts b werecalcula ted and are summarized in Table 2. Acompar i s on of t hese pa ramete rs , fo r phenol and

0.0 . . . . . . . . . . . . . . . . . . . aniline in distilled water solut ions, sh owed a lmos t0 5 0 1 0 0 1 5 0 2 0 0 s i m i l a r l i m i t i n g a d s o r p t i o n c a p a c i t y v a l u e s , a n dC ANILINE EQUILIBRIUM CONCENT RATION (mgtL) __ s u b s t a n t i a l l y d i f f e re n t e n e r g i e s o f a d s o r p t i o n . T h e

Fig . 2 . Linear ized Langmui r adsorpt ion i sotherm of anil ine ani l ine b va lue was fo un d to be f ive t ime s highe r thani n d is ti ll ed w a te r s o lu t ion on pow der ed a c t i va te d c a r bon , f o r phe no l . The p r e s e n c e o f t he m i ne r a l nu t r i e n t s a n di n a c t i v a t e d m i c r o b i a l c e l l s i n c r e a s e d t h e a d s o r p t i o nc a p a c i ti e s o f P A C a n d c o n s i d e r a b l y re d u c e d t h e

d a t i o n , w a s s t u d i e d s e p a r a t e l y . I n t h e s e c o n d s t a g e e n e r g y o f a d s o r p t i o n . H o w e v e r , t h e e n e r g y o fs i m u l t a n e o u s a d s o r p t i o n a n d b i o d e g r a d a t i o n w a s a d s o r p t i o n f o r a n i li n e i n s a li n e s o l u t io n s ti ll r e m a i n e di n v e s t i g a t e d , t w i c e a s h i g h a s f o r p h e n o l .

Table 2. Effect of aqueous solution compositions on PAC adsorption characteristics of aniline and phenol in a single andbi-solute systemsLangmuir linearized isotherm equations rC 1 Cqc bQ "~ Qo Qo b Correlation

m~ organics (L/mg) coetf icien tedia Sorbate (g/L) g PACDistilled water Phenol C/q~ = 0.3603 + 7.3690 10-3C 135.7 0.0204 0.999Aniline C /q , = 7.476 10 2 + 7.9019 x 10-3C 126.6 0.1057 0.996Distilled water + mineral nutrientsPhenol C /q , = 0.5003 + 6.0117 10-3C 166.3 0.0121 0.995Aniline C/q~ = 0.3187 + 7.9319 10-3C 126.1 0.0249 0.997Distilled water + inactivated microbial cellsPhenol C /q , = 0.5996 + 6.6527 10-3C 150.3 0.0111 0.998Aniline C/q~ = 0.1613 + 7.5863 10-~C 131.8 0.0470 0.997Distilled water + mineral nutrients + inactivated microbial cells

Phenol C /q , = 0.6480 + 6.3732 10-3C 156.9 0.0098 0.998Aniline C /q , = 0,3673 + 7.2917 x 10-3C 137.1 0.0200 0.996


4/8

394 F. Orshansky and N. Narkis1000" 800 a/900 700" y-15.900+1.5930C /~ ~ ~" -.

. S00mglL"~ 4 0 0 ] ~ _1_0_0_re_g_/L00molL ~.,~ 300"- = = = = = = = = = = = = = = = = = = = = = Z: >. 200"o . . . . . . . . . . . . . . 8

1 0 0 1 0 0 .

0 - 0 . . . . - , - , - , -0 1 0 2 0 3 0 4 0 5 0 6 0 7 0 0 100 200 300 400 500 600

TIME (hrs.) INITIAL AN ILINE CONCENTRATION (m01L)Fig. 4. Oxygen uptak e during biodeg radatio n alone of Fig. 6. Oxygen uptake as a function of ini t ial ani linevar ious initial aniline concentrations in ba tch biological concentration.reactors.

Biotreatment alone F o r a n i l i n e :I n t he s t ud y o f t he b i o l o g i c a l t r e a t m e n t a l one , t he O 5 . . . . . . . ~ = 15 .900 + 1 .593C ; r = 0 .997 ( 2 )o x y g e n c o n s u m p t i o n d u r i n g t h e b i o o x i d a t i o n o fv a r i o u s i n i t i a l c o n c e n t r a t i o n s o f a q u e o u s p h e n o l a n d w h e r e C i s t h e i n i ti a l s u b s t r a t e c o n c e n t r a t i o n i n t h ea n i l i n e s o l u t i o n s w e r e d e t e r m i n e d i n S a p r o m a t l i q u i d p h a s e .r e s p i ro m e t e r . T h e o x y g e n u p t a k e , a s a f u n c ti o n o f O x y g e n u p t a k e a n d b i o m a s s i n c r e m e n t r e s ul ts w e r et i m e a n d i n i t i a l o r g a n i c s u b s t r a t e c o n c e n t r a t i o n a r e u s e d f o r k i n e t i c p a r a m e t e r s c a l c u l a t i o n s , a s s u m m a r -s h o w n i n F i g s 3 a n d 4 . T h e i n it ia l s u b s t r a te i z ed i n T a b l e 3 . T h e b i o k i n e t i c p a r a m e t e r s , Y a n d p . ~c o n c e n t r a t i o n a f fe c te d t h e a m o u n t o f o x y g e n w e r e d e t e r m i n e d f r o m t h e b i o m a s s i n c re m e n t , w h i lec o n s u m e d a n d t h e ti m e f o r c o m p l e t e o x y g e n u p t a k e . B O D r , p a n d R , t h e r e s p i ro m e t r i c b i o m a s s e q u i v a le n t ,C o m p l e t e b i o o x i d a t i o n f o r a n i l i n e t o o k a l o n g e r t i m e w e r e c a l c u l a t e d f r o m t h e r e s p i r o m e t r i c d a t a .t h a n f o r p h e n o l a t t h e s a m e i n i t ia l c o n c e n t r a t i o n s . A r e l a t i o n s h i p b e t w e e n t h e v a l u e s o f t h e b i o -

T h e a s y m p t o t i c v a l u e s o f o x y g e n u p t a k e w e r e k i n e ti c p a r a m e t e r Y , d e t e r m i n e d f r o m t h e b i o -r e c o r d e d w h e n c o m p l e t e b i o o x i d a t i o n t o o k p l a ce . A m a s s i n c r e m e n t o b s e r v e d , a n d t h o s e c a l c u l a te dl i n e a r r e l a t i o n s h i p w a s f o u n d b e t w e e n t h e a s y m p t o t i c f r o m r e s p i r o m e t r i c d a t a , B OD r+ +p a n d R c a n b ev a l u e s o f t h e o x y g e n u p t a k e a n d t h e in i t i a l p h e n o l e x p r e s s e d b y e q u a t i o n ( 3 ).a n d a n i l i ne s ub s t r a t e s c on c e n t r a t i on , a s s how n i n Y phenol B O D re spanm ne R a n i l i n eF i g s 5 a n d 6 a n d e q u a t i o n s ( 1 ) a n d ( 2 ). x ( 3 )F o r p h e n o l : Yaniline B O D r, o ph0.o~ Rpho,o~

B y s u b s t i t u t i n g t h e e x p e r i m e n t a l re s u l t s f r o m T a b l e 30 2 . . . . . . ~ = - 2 . 5 6 9 5 + 1 .3 4 5 7C ; r = 0 . 99 9 ( 1 ) i n t o t h e r i g h t p a r t o f e q u a t i o n ( 3 ), th e f o l l o w i n g

r e l a t i o n s h i p w a s f o u n d , a s s h o w n i n e q u a t i o n ( 4 ) .80 o 0.659 1.59

" y. .2 .SSOS+1.34src 0.389 x ~ = 2 .00 (4)700 r - 0 . 9 9 9 T h e c a l c u l a t e d v a l u e 2 . 0 0 i s i n c o m p l e t e a g r e e m e n t6oo - w i t h t he r a t i o o f R a,m .0 t o R ph~ .o ], ob t a i n e d f r om t he

g e x p e r i m e n t a l r e s u l ts o f t h i s r e s e a r c h , w h i c h e q u a l sI~1 500-~" 2 . 00 . T h e s e d a t a p r o v e t h a t r e s p i r o m e t r i c t e c h n i q u e i s,,~ 3 0 0 - T a b l e 3 . K i n e t i c p a r a m e t e r s d e t e r m i n e d i n b i o l o g i c a l t r e a t m e n t a l o n eo f p h e n o l a n d a n i l i n e>~ 2 0 0 . P a r a m e t e r U n i t P h e n o l A n i l i n eO

100 . ,u ,~, h -] 0 .458 0.228K~ mg /L 60 .7 49 .00 y m ~ b i o m a s s f o r m e d 0 .6 5 9 0 . 3 8 90 100 200 300 400 500 m g s u b s t r a t e r e m o v e dm~ 02 upta ke 1.34 1.59INITIAL PHENOL C O N C E N T R A T I O N ( m 0 1 L ) BOD~p .... mg substrate removed

Fig. 5. Oxyg en up tak e as a function of initial phenol R.~ mg O~ uptake 2.25 4.50concentration, mg biomass formed


5/8

Characteristics of organics remo val by PA CT 395

. PAC C0NC. (g /L )

d o " t - * - , + ' J - ~ lI D ~ 0 0 ' ~ l l 2 . 2 15 0 0 2 . 1 IS

' - " " I < " h ' , / Il ' / ' I d t Z " , o , zt ~ 2 o o A7 1 " .4 ; ' .~ ~74O 1 0 0 2 .9 s

S , 6 80 . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . i 5 2 ' 0 2 ' 5 3 0 3 5 4 ' 0 4 5

5 1 0 1 5 2 0 2 5 3 0 3 5 T I M E ( h r s . )T I M E ( h r s . ) Fig. 9 . Oxygen uptake by m icrobia l cul ture dur ing

Fig . " i. Oxygen uptake by microbia l cul ture du r ing s imul taneous adsorpt ion and biodegradat ion of 500m g/Lsimultaneous ad sorp tion and biodeg rada tion of 500 mg /L aniline in batch reactors containing various PA C concen-phenol in batch reactors containing various PA C concen- t rations. Reac tor volume 250 mL.trat ions. Reactor volume 250 mL.

a r e l ia b l e m e t h o d w h i c h c a n b e u s e d f o r P A C T b i o d e g r a d a t i o n o f c o n s t a n t in i t ia l p h e n o l c o n ce n -e v a l u a t i o n , t r a ti o n , o f 5 00 m g / L , a n d v a r i o u s c o n c e n t r a t io n s o f

P A C , f r o m 0 . 0 0 t o 3 . 6 8 g / L .Simultaneous adsorption and biotreatment I n t h e a b s e n c e o f P A C t h e a s y m p t o t i c o x y g e nS i m u l t a n e o u s a d s o r p t i o n a n d b i o d e g r a d a t i o n o f u p t a k e o c c u rr e d a f t e r 3 0 h . P A C a d d i t i o n e n h a n c e d

p h e n o l a n d a n i l i n e w a s s t u d i e d i n a s e r ie s o f b a t c h t h e r e s p i r a t i o n r a t e . T h e h i g h e r t h e P A C c o n c e n -r e s p i r o m e t r i c e x p e r i m e n t s . I n th e a b s e n c e o f m i c r o - t r a t i o n t h e s h o r t e r th e t i m e re q u i r e d f o r g e tt i n g a nb i a l c e l ls a n d s u b s t r a t e s , t h e t o t a l o x y g e n u p t a k e o f a s y m p t o t i c o x y g e n u p t a k e , a n d t h e s h a r p e r t h e s l o p eP A C a l o n e i n d i s ti l l e d w a t e r w a s i n t h e r a n g e o f o f i n c r e a s e d o x y g e n u p t a k e c u r v e s .6 . 0 - 1 7 . 0 m g O 2 / L , d e p e n d i n g o n P A C c o n c e n t r a t i o n , T h e o x y g e n u p t a k e r a te s w e r e c a lc u l a t e d inw h i c h w a s r e l a t i v e ly l o w . i n t e r v a l s o f l h e a c h , d u r i n g p h e n o l b i o o x i d a t i o n i n

Phenol. F i g u r e 7 s h o w s t h e o x y g e n u p t a k e a s a s i m u l t a n e o u s a d s o r p t i o n a n d b i o d e g r a d a t i o n p ro ce ss +f u n c t io n o f t i m e d u r i n g s i m u l t a n e o u s a d s o r p t i o n a n d f o r 5 00 m g / L p h e n o l a q u e o u s s o l u t io n a n d v a r i o u si . . A A

. . + t- I 7 0 ' 0 . 0 0 P A C I L 7 0 . t 0 . 7 4 0 P A C I L 1 . 4 7 0 P A C / t~ e o . E 6 0- 4O t5 0 5 0

4 o ~ 4 o ~ ,o1 . . / ~ 3 o\ "2 0 . -20 os 20

" = 1 0 ' ~ 1 0 1O ~ 0 . . . . , . . . . , . . . . , . . . . , . . . . i . . . . , . . . . N

0 5 1 0 1 5 2 0 2 5 3 0 3 5 4 ~ n ! . . . . , . . . . , . . . . , . . . . , . . . . , . . . . 1 ~ . . . . O " " - : ; " . . . . ' . . . . ' . . . . ' . . . . ' . . . . ' . . . . '0 5 1 0 1 5 2 0 2 5 3 0 5 0 5 1 0 1 5 2 0 2 5 3 0 5T I M E ( h r s . ) T I M E ( h r s . ) T I M E ( h r s . )

~ " : ~ a o = . ,~ : ~ 7 0 " 2 . 2 1 0 P A C I L " ] 7 0 ' 2 . 9 5 0 P A C I L " J 7 0 " 1 3 . 6 8 0 P A C / L

- / \S O - 5 0 . SO' != 30. ~ 201 ~a 20. 20. 20

1 0 1 0 ' " 1 0e 4 0 - - , . . . . = . . . . , . . . . , . . . . i . . . . , . . . . 0 ' . . . . M O / . . . . , . . . . , . . . . , . . . . , . . . . + . ~ . . . , . . . .o s l o i s = 0 m s 3 0 a s o s 1 o I S 2 0 m s a o s o o s ~o i s = 0 m s ~ , o a s

T I M E ( h r s . ) T I M E ( h r s . ) T I M E ( h r s . )F i g . 8 . O x y g e n u p t a k e r a te s , f o r e a c h 1 h i n t e r v a l , d u r i n g s i m u l ta n e o u s a d s o r p t i o n a n d b i o d e g r a d a t i o no f 5 0 0 m g / L p h e n o l s in g l e s o lu t e s o l u t io n a n d v a r i o u s P A C c o n c e n t r a t i o n s i n b a t c h r e a c to r s .


6/8

396 F. Orshansky and N. Nark isTable 4. Simultaneous adsorption and biodegradation reatment of p henol and aniline aqueous solutions. Da ta determined n SapromatRespirometerbatch reactors n the presenceof various PAC concentrations. n itialconcentration:phenol 500.00 mg/L, aniline 504.00 mg/L.Reaction time: phen ol 30 h, aniline 42 hPAC Oxygen consumed Biooxidized Residual co nc en trati on s Ca lc ul at edesidualsConc. by biooxidation substrate in liquid phase adsorbed on PAC

Phenol Aniline Phenol Aniline Phenol Aniline Phenol Anilineg/L mgO~/L mgO2/L mg/L mg/L mg/L m g /L m g /g P A C mg/gPA C0.0000 567 794 489.30 502.80 10.70 1.02 - - - -0.7368 642 672 479.10 425.80 0.10


7/8

Characteristics of organics removal by PA CT 397b e t w e e n 0 . 7 4 g / L a n d 3 . 68 g / L , v e r y l o w o r g a n i c ~-om a t e r i a l s r e s i d u a l s w e r e f o u n d i n t h e l i q u i d p h a s e , p A c c o n c . g/Lb e t w e e n 0 . 0 5 a n d 0 . 1 5 m g / L p h e n o l a n d l e ss t h a n 1 ~ 7040 .01 t o 0 .04 m g / L a n i l i ne . A l m os t a l l t he r e s i du a l ~ 1 .s . 0 .n o n - b i o d e g r a d e d p h e n o l a n d a n i l in e re m a i n e d a d - ~ -.---o--- 1.47Z ~ --"'4"-" 2.21s o r b e d o n t h e P A C s u r fa c e . T h e a m o u n t o f t h e a 1.0' \ x 2.95a d s o r b e d o r g a n i c s i s g i v e n i n T a b l e 4 , a n d i n F i g . 1 0. ~ - -- 0 -- - 3 .mF i g u r e 1 0 s h o w s t h e r e s i d u a l p h e n o l a n d a n i l i n e a s a o ~ [ ~f u n c ti o n o f P A C d o se s , w h i ch r e m a in e d o n t h e P A C ~ a x . Z 7 7 7 7 Zi n t h e m i x e d l i q u o r , e x p r e s s e d a s m g / L a n d a s m g o 0 . sa d s o r b e d p h e n o l o r a n i l i n e p e r g r a m p o w d e r e d , i o n ,a c t i v a t e d c a r b o n . T h e a m ou n t o f n o n - b i o d e g r a d e d ~ . , " ~ ' ~ " ~ ~a n i l i n e w a s m u c h h i g h e r t h a n o f p h e n o l . T h e 0.0 . . . . . . . . . . . . . . . . . . . ~ ,. . . . . . . . . . . . . . . . . . ~ . . . . . . ~=:..7.-.7 ..... ....p e r c e n t a g e o f t h e n o n - b i o o x i d i z e d p h e n o l r e m a i n e d 1 9o 2 1o 2 a o 2 50 2 t o 2 g o a l O a a oa d s o r b e d o n P A C , w a s in t h e r a n g e o f 4 - 9 % a n d o f WAVELENGTHrim)15 -32 % for ani l in e , as a fun ct io n o f P A C Fig . 12. UV spect ra of soluble organics remaining af ter 42 hco nc en t ra t io n, of s imul taneous adsorpt ion and biodegradat ion and af terTh e r e m a i n i n g a n i l i ne w a s s t r on g l y a d s o r be d on b i o tr e a tm e n t a l one o f a n il ine s ing le s o l ut e a que oussolutions. C ell length 1 cm.t h e P A C s u r fa c e , n o t b e i n g a v a i l a b l e f o r b i o d e g r a d a -t i o n . T h i s f a c t i s i n a g o o d a g r e e m e n t w i t h t h e h i g h e re n e r g y o f a d s o r p t i o n o f a n i li n e t h a n o f p h e n o l , as P A C T ( K a l i n s k e , 1 97 2; P e r r o t t i a n d R o d m a n , 1 97 4;d e t e r m i n e d f r o m t h e a d s o r p t i o n i s o th e r m s . W h e n th e S p e i te l e t a l . , 1989) . I n t he c a s e o f a n i l i ne , on on ea d s o r b e d n o n - b i o d e g r a d e d o rg a n i c s w e r e e x p r e ss e d h a n d , P A C a d d i t i o n r e d u c e d t h e m i c r o b i a l r e s p ir -i n m g / L m i x e d l i q u o r , t h e h i g h e r t h e P A C a t i o n , w h i l e o n t h e o t h e r h a n d , v e r y l o w r e s i d u a lc o n c e n t r a t i o n , t h e l a r g e r t h e r e s i d u a l o r g a n i c s a n i l i n e c o n c e n t r a t i o n s w e r e f o u n d in t h e t r e a t e dc o n c e n t r a t i o n . W h e n t h e r e s i d u a l s w e r e e x p r e s s e d a s w a t e r . H e n c e , a s i g n i f ic a n t p a r t o f t h e a n i l i n e w a sm g o r g a n i c s p e r g r a m P A C , a s t h e P A C c o n c e n - a d s o r b e d a n d r e m a i n e d n o n - b i o o x i d i z e d .t r a t io n s w e r e h i g h e r , t h e a m o u n t s o f r e m a i n e d T h e r e f o re , t h e a n i li n e r e m o v a l b y P A C T c a n b eo r g a n i c s b e c a m e l o w e r. T h e r e s p i ro m e t r i c e x p e r- c o n s i d e r e d a s a si m p l e c o m b i n a t i o n o f a d s o r p t i o ni m e n t s re s u l t s, a s w e l l a s t h e r e s i d u a l p h e n o l a n d a n d b i o d e g r a d a t i o n , w i t h o u t m u t u a l e n h a n c e m e n t .a n i l i n e i n t h e l i q u i d p h a s e , d e t e r m i n e d b y c h e m i c a l T h i s f a c t i s i n a g r e e m e n t w i t h t h e s u g g e s t i o n s o fa n a l y si s , a n d t h e c a l c u la t e d n o n - b i o d e g r a d e d r e- X i a o j i a n e t a l . (1991).s i d u a l s a d s o r b e d o n t h e P A C , e n a b l e d t h e c o m p a r i -s o n o f t h e b e h a v i o u r o f p h e n o l a n d a n i li n e in t h e T r e a t e d w a t e r q u a l i t ys i m u l t a n e o u s a d s o r p t i o n a n d b i o d e g r a d a t i o n s y s- T h e s i m u l t a n e o u s a d s o r p t i o n a n d b i o d e g r a d a t i o nt e m s . p r o c e s s , p r o v e d t o b e a s u i t a b l e t r e a t m e n t i n o r d e r t o

I n t h e c a s e o f p h e n o l , P A C a d d i t i o n e n h a n c e d t h e a c h i e v e h i g h q u a l i t y e f fl u e n ts , w i t h b e t t e r r e m o v a l s o fb i o o x i d a t i o n p r o c e ss e s a s c o m p a r e d t o b i o t r e a t m e n t p h e n o l a n d a n i li n e th a n b y b i o t r e a t m e n t a l o n e , a sa l o n e . T h i s f a c t c a n c o n f i r m t h e a p p r o a c h i n w h i c h c o n f i r m e d b y th e r e s u l t s p r e s e n t e d i n F i g s 11 a n d 1 2.a c t i v a t e d c a r b o n e n h a n c e s e n z y m a t i c r e a c t i o n s i n T h e s o l u b l e C O D , d e t e r m i n e d i n t h e f i lt e r e d l i q u i d ,

a f t e r 30 h o f s im u l t a n e o u s a d s o r p t i o n a n d b i o d e g r a -d a t i o n o f p h e n o l, w i t h v a r i o u s P A C c o n c e n t r a t io n s ,

407 i s s h o w n i n F i g . 1 1. A s t h e P A C c o n c e n t r a t i o n s

!b e c a m e h i g h e r , t h e r e s id u a l C O D b e c a m e l o w e r . F o r

- - ' c o m p a r i s o n , t h e s o l u b l e C O D o f 3 7. 7 m g O ~ / L , w h i c h_1 3 0. w a s f o u n d a f t e r 3 0 h i n t h e b i o r e a c t o r i n t h e a b s e n c eo f P A C , w a s a l s o g i v en . T h e b i o l o g i c a l l y t r e a t e d~ , l i q u i d c o n t a i n e d 1 0. 7 m g / L r e s i d u a l p h e n o l , d e t e r -

a 2 o m i n e d b y c h e m i c a l a n a l y s i s ( T a b l e 4 ) , a s c o m p a r e dOo ~ w i t h 0 . 15 m g / L r e s i d u a l p h e n o l , a f t e r s i m u l t a n e o u s


8/8

398 F. Orshansky and N. Nark isb i o d e g r a d a t i o n , w i t h v a r i o u s P A C c o n c e n t r a t i o n s . Acknowledgements - -The research was supported by TheTh e U V o p t i c a l de n s i t y a f t e r b i o t r e a t m e n t a l o ne w a s Mi n i s tr y o f Sc ie nce a nd A r t s , The P r og ra m f o r I m m i gr a n tAbso rpt ion and the Center for A bsorpt ion in Science , Theh i gh e r t ha n i n t he p r e s e n c e o f PA C . Th e s e r e s u l t s , a s Mi n i s tr y o f I m m i gra n t A bs o r p ti on , St at e o f I sr ae l. Thewel l as the CO D resul t s , pr ov ed th a t f ina l wa ter o f grant s f rom both Minist ri es a re gra tefully acknowledged.h i g h e r q u a l i t y c a n b e o b t a i n e d i n s i m u l t a n e o u sa d s o r p t i o n a n d b i o d e g r a d a t i o n o f p h e n o l o r a n i l in es o l u t i o n s , t h a n i n b i o l o g i c a l t r e a t m e n t a l o n e .

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SUMMARY Craveiro F. A. and M alina J. F. , Jr (1991) Ana erobicdegra dation of phenol and bioregeneration of granu larS i m u l t a n e o u s a d s o r p t i o n a n d b i o d e g r a d a t i o n a c ti v at ed c a rb o n . J. Hazard. Wat. 28, 189-190.t r e a t m e n t o f phe no l a nd a n i l i ne i n s yn t he t i c a que ous Ehr ha r d t H . M. a nd R e hm H . J . ( 1985) Phe no l de g r a da ti ons o l u t i ons p r o ve d t o r e m ove e ff i c i e n t ly t he s e t ox i c by m i cr oo r ga n is m s a ds o r be d on a c ti va te d c a r bon.Appl. Microbiol. Biotech. 21, 32-35.o r ga n i c s . H i gh e r f i na l w a t e r qua l i t y w a s a c h i e ve d by G a udy A . F . , Eka m ba r a m A . a nd R ozi ch A . F . 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