Equilibrium Kinetics and Isotherm Studies of Cu (II) Adsorption from Waste Water onto Alkali Activated Oil Palm Ash

Transcription

1 Amrican Journal of Applid Scincs 8 (3): , 20 ISSN Scinc Publicaions Euilibrium Kinics and Isohrm Sudis of Cu (II) Adsorpion from Was War ono Alkali Acivad Oil Palm Ash Zaira Zaman Chowdhury, Sharifuddin Mohd. Zain, Rashid Aa Khan and 2 Abdulbari Abdulrahman Ahmd Dparmn of Chmisry, Faculy of Scinc, Univrsiy Malaya, Kuala Lumpur, Malaysia 2 Dparmn of Chmical Enginring, Faculy of Enginring, Pnang, Univrsiy Scinc, Malaysia Absrac: Problm samn: Havy mal accumulaion in was war could affc auaic lif, human halh and ovrall cosysm advrsly. Thrfor, in rcn yars much mphasis has bn givn for h us of indusrial was marial as low cos adsorbns for rmoval of mallic conaminans from was war. Approach: Prsn sudy dals wih h adsorpion uilibrium and kinics of Cu (II) caion using sodium hydroxid acivad Oil Palm Ash (OPA). Adsorpion was invsigad in a bach sysm wih rspc o various paramrs such as iniial mal ion concnraion, conac im and ph of h soluion. Surfac characrizaion of h prpard adsorbn was don by using surfac ara analyzr, Scanning Elcron Microscop (SEM) and X-ray Fluorscnc and compard wih naural oil palm ash. Th adsorpion uilibrium daa wr bs rprsnd by Langmuir, Frundlich and Tmkin modl. Euilibrium kinics sudis wr prformd by Psudo firs ordr, Psudo scond ordr and Inra-paricl diffusion. Rsuls: Maximum monolayr adsorpion capaciy obsrvd a 30 C was 8.86 mg g. Kinic daa corrlad wll wih h psudo scond ordr modl, suggsing ha h adsorpion procss migh b chmical sorpion. Th linar plos of inra paricl diffusion rvald ha h adsorpion procss was mainly govrnd by por diffusion. Euilibrium upak was incrasd wih incras of iniial concnraion and conac im. Exprimnal daa showd ha abou 96.03% of coppr can b rmovd a ph 5.5. Conclusion: Th rsarch concludd ha acivaion by alkali ramn of naural OPA would produc sufficin porosiis and surfac ara and i has go good ponial o rmov Cu (II) from was war. Ky words: Oil Palm Ash (OPA), Scanning Elcron Microscop (SEM), World Halh Organizaion (WHO), Empy Frui Bunch (EFB), Palm Shll (PS), Langmuir uaion, uilibrium daa, Empy Frui Bunch (EFB), sodium hydroxid INTRODUCTION Auous ffluns manaing from many indusris conain havy mals dissolvd in i. If hs dischargs ar mid wihou purificaion, hy may hav svr impac on nvironmn (Krim al., 2006). Primarily som anhropognic aciviis, such as wahring of rocks and volcanic aciviis play a vial rol for nriching h war rsrvoirs wih havy mals (Yisa, 200; Ong and Kamruzzaman, 2009). Numrous mals such as mangans (Mn), mrcury (Hg), lad (Pb), cadmium (Cd), arsnic (As), coppr (Cu). ar known o b significanly oxic du o hir non-biodgradabiliy and oxiciy (Ghaly al., 2008; Omar and Al-Iawi, 2007). Among hs havy mals, coppr is considrd as on of h mos oxic on. Th ponial sourc of coppr in indusrial ffluns includs papr and pulp, frilizr, wood prsrvaivs, rfinris, mal claning and plaing bah c. Th xcssiv inak of coppr may caus rnal and hpaic damag, svr mucosal irriaion, wid sprad capillary damag, gasroinsinal irriaion and possibly ncroic changs in kidny and livr. World Halh Organizaion (WHO) has rcommndd ha maximum accpabl limi for Cu (II) concnraion in drinking war should b.5 mg L. Consunly, i is ssnial ha h poabl war should b givn som ramn bfor domsic supply. Many convnional mhods including oxidaion, mmbran filraion, coagulaion, rvrs osmosis, adsorpion, ion xchang, prcipiaion. hav bn Corrsponding Auhor: Zaira Zaman Chowdhury, Dparmn of Chmisry, Faculy of Scinc, Univrsiy Malaya, Malaysia, Tl: Fax: /

2 Am. J. Applid Sci., 8 (3): , 20 rpord in h liraur o rmov coppr along wih ohr havy mals from was war. Ths mhods may b inffciv or xrmly xpnsiv spcially whn h was sram conains rlaivly low an improvd acivaion sragy for oil palm ash by using sodium hydroxid which can nhanc is surfac ara significanly and consunly incras is adsorpion capabiliy. concnraion of mal (-00ppm) dissolvd in larg volum. Howvr, adsorpion can b rgardd as on MATERIALS AND METHODS of h mos popular mhod for h rmoval of havy mals from h waswar du o is low cos, asy Chmicals: Coppr (II) sulfa, CuSO 4.5H 2 O, sodium availabiliy, biodgradabiliy, simpliciy of dsign and hydroxid (NaOH) and Hydrochloric Acid (HCl) wr high rmoval fficincy (Azhar al., 2005; Esmaili purchasd from Mrck, Grmany. Sock soluion of al., 2005; Shakr, 2007). Morovr, i dos no produc Coppr (II) sulfa having concnraion of abou 000 harmful subsancs. Thrfor, adsorpiv rmoval of mg L was prpard by using doubl disilld war. havy mals including coppr from auous srams Various concnraions of s soluion of Cu (II) by using agriculural and indusrial was producs ranging from mg L wr prpard by which ar abundan in naur and ruirs lil subsun diluion of h sock soluion whil h procssing has rcivd much anion in rcn yars ( iniial ph was adjusd o 5.5 using a ph mr (Mls Zuorro and Lavcchia, 200). Svral adsorbn Toldo, Modl: Ross FE 20, USA). Frsh diluion of drivd from low cos marial such as agaros, za h sock soluion was don for ach sorpion sudy. All mays Tassl (Caliphs al., 200), sa mussl and ragns usd hr wr of AR grad chmicals. whi clay, Spirogyra nglca (Modhr al., 2009), drid acivad sludg (Solani al., 2009), a was (Amarasingh and Williams, 2007; Mahvi al., 2005) volcanic uff (Mihaly-Cozmua al., 2005). for raing was war a h solid-soluion inrfac hav bn rpord. Abov prusal of h liraur rflcs ha svral yps of adsorbns hav bn usd for rmoval of havy mals from was war. Acivad oil palm ash posssss som uniu propris du o is xndd surfac ara, porosiis and oxid conn on is surfac. Ths propris significanly can conribu for is nhancd upak capaciy. Thrfor, oil palm ash was akn for h prparaion of adsorbn and is applicabiliy for h rmoval of coppr ion from was war was valuad. Malaysia has hug supply of agro-basd was biomassgnrad from oil palm indusris which consiss of Empy Frui Bunch (EFB), Palm Shll (PS) and Oil Palm Ash (OPA) acivaion: Th palm oil ful ash usd hr was akn from h middl of h flu owr and was collcd from Eas oil Mill, Goldn Hop Planaion Sdn. Bhd, Pulau Cary, Slangor. Th adsorbn hus obaind was sivd hrough siv no 200µm. I was washd wih dionizd war for svral ims o rmov forign paricls and ovn drid a 0 C ovr nigh. Th raio of oil palm ash wih causic soda was kp 5: ha is 50 grams of oil palm ash wr addd wih 0 gm of NaOH in 250 ml disilld war. Thn h mixur was rfluxd a 60 C for 8 h in a round boom flask wih a magnic sirrr placd insid i. Th slurry was allowd o cool a room mpraur and filrd. Th filr cak was rpadly washd wih dionizd war unil nural ph of h filra was obsrvd. Thn i was drid in an ovn a 0 C for 2 h bfor us and sord in dsiccaors ovr frsh silica gl for furhr applicaion. msocarp fibr. This biomass is burn in boilr o produc sam for lcriciy gnraion which producs Surfac characrizaions: Scanning Elcron a lo of solid was- oil palm ash. Th uilizaion of palm ash provids wo-fold advanag wih rspc o nvironmnal conaminaion. In ha cas, solid was Microscop (SEM) was usd o sudy h morphological changs of unrad and rad oil palm ash. X-ray fluorscnc (XRF, Rigaku RIX, 3000, Japan) was usd disposal problm can b parly rducd and o idnify h chmical composiion of h acivad simulanously i can b convrd o valu addd, adsorbn. Surfac ara, por volum and por diamr asily availabl, co-frindly adsorbn. of h prpard adsorbn was masurd by Auosorb, Prsn rsarch aims o rmov Cu (II) from was Quanachrom Auosorb Auomad gas sorpion sysm war by using chmically rad palm oil ash and o supplid by Quanachrom. Bfor prforming h invsiga h influnc of all h physicochmical nirogn gas adsorpion, h acivad OPA was paramrs involvd during h sorpion procss. Th ougassd undr vacuum a mpraur 300 C for 4 h. o rsarch focuss on adsorpion kinics and isohrm rmov any moisur conn from h solid surfac. sudis of h prpard adsorbn. W ar rporing hr Surfac ara and por volum wr calculad by 23

3 Brunaur Emm Tllr (BET). Abov mniond procdur was auomaically prformd by sofwar (Micropor vrsion 2.26) availabl wih h insrumn. Am. J. Applid Sci., 8 (3): , 20 Euilibrium sudis: Each of h bach xprimn was carrid ou by adding 0.2 gm of OPA wih 50 ml of diffrn concnraion of Cu (II) soluion a 50 rpm. Th rsidual concnraion of Cu (II) was analyzd afr prdrmind inrval of im unil h sysm rachd uilibrium by using aomic absorpion spcrophoomr (Prkin-Elmr Modl 300). (a) Isohrm sudis: For isohrm gnraion ach xprimn was conducd a 30 C in a hrmorgulad war bah (Haak Wia Modl, Japan) wih shakr covr in ordr o prvn ha loss o h surroundings. Th uilibrium adsorpion amoun ( ) is calculad according o E. : (c c )v w i = () Hr, is h adsorpion amoun of mal ion (mg g ) a uilibrium conac im, W is h wigh of adsorbn (g), V is h volum of soluion (ml). Th rmoval fficincy of h mal ion was calculad by using E. 2: Fig. : (a) Naural oil palm ash (b) Acivad oil palm ash (b) c c w i R moval% 00 = (2) RESULTS SEM was usd o sudy h changs in morphology of unrad OPA and chmically rad sampl of OPA which was shown by Fig. a and b. Th figur clarly rvals ha surfac morphologis of boh h sampl wr diffrn. I was obsrvd ha naural palm ash had rough srucur wihou any cracks and crvics. Howvr significan numbr of pors wih diffrn srucur was obsrvd afr acivaion of h sampl. Du o his wll dvlopd porosiis crad by sodium hydroxid, acivad oil palm ash had high surfac ara and adsorpion capaciy. Afr acivaion, h major chmical consiun of modifid oil palm ash (w%) obsrvd was: SiO 2 (5.70), Al 2 O 3 (5.50), F 2 O 3 (5.77), Na 2 O(2.00), K 2 O(5.69), MgO(.20), CaO(0.90), P 2 O 5 (5.95), SO 3 (0.0), TiO 2 (0.4) and MnO (0.44). Th high oxid conn of silica along wih ohr oxid has givn h srucur of palm ash o b usd as good adsorbn for mal. 232 Fig. 2: Effc of iniial mal ion concnraion wih uilibrium conac im Th phnomnon of adsorpion is mainly dpndn on surfac ara and por srucur. Th calculad BET surfac ara for h naural sampl was m 2 g, bu i incrasd o 467. m 2 g afr acivaion. This nlargmn of surfac ara is probably du o incras in micro por volum and micro por surfac ara. Th micro por volum and micro por surfac ara of naural sampl of OPA obsrvd was cm 3 and m 2 g rspcivly which wr incrasd o 0.99 cm 3 g and 56.9 m 2 g afr chmical ramn.

4 Fig. 3: Effc of ph on rmoval % of coppr Figur 2 shows h ffc of iniial mal ion concnraion and upak wih uilibrium conac im. I is clar from h graph ha amoun of upak (mg gm ) incrasd wih incrasd agiaion im and afr crain priod of im; i rachd o a consan valu byond which no furhr adsorpion ook plac. Th rsuls showd ha, h adsorpion was fas a iniial sag of conac priod and afr ha nar h uilibrium i bcam slowr. Th ra of upak was iniially high du o h availabiliy of largr surfac ara of modifid oil palm ash for adsorpion. Wih h laps of im, h surfac adsorpion sis wr xhausd. Th rmaining vacan sis wr difficul o b occupid by h caion du o rpulsiv forcs bwn adsorba prsn in solid and bulk phass. As h concnraion of h mal ion is incrasing, h sorpion capaciy by h sorbn is also incrasing. Similar rnd was obsrvd for phnol adsorpion ono ric husk and ric husk ash (Mahvi al, 2004).Th plo rvals ha wihin 80 min h sysm rachd uilibrium and afr ha h adsorpion bcam mor or lss sam. Howvr, hr xprimnal daa wr masurd for 3 h o nsur ha full uilibrium was aaind. In ordr o sudy h ffc of ph, h soluion ph was varid from 2-8 whil kping h ohr variabl consan. Figur 3 dpics h ffc of ph on rmoval% of coppr. I was found ha adsorpion of Cu (II) ion from h soluion was srongly ph dpndn. A ph 2-3 rang h adsorpion was low and rapidly incrasd bwn ph 4-7 rsuling grar rmoval fficincy. This phnomnon can b xplaind by h prsnc of H + and H 3 O + ions in h soluion a lowr ph. A ph lss han 4, hydrogn proons may comp wih mal ions for aciv binding sis on h surfac of palm oil ash, which lads o fwr binding sis bing Am. J. Applid Sci., 8 (3): , availabl o bind mal ions, so h adsorpion amoun of Cu (II) was vry lil. As h ph incrass, h adsorpion surfac bcam lss posiiv and hrfor lcrosaic aracion bwn mal ions and h surfac of palm oil ash was incrasd rsuling grar rmoval fficincy bwn ph 4-8. Th rsul dpics ha rmoval% was incrasd sadily up o ph 8, aains maximum valu of abou 94.56%. Howvr, afr ph 8, hr is a sharp dcras in adsorpion. This dcras is may b du o formaion of solubl hydroxyl complxs. Afr ph 8, hr is again incras of rmoval % which rsuls S-lik adsorpion curv. This S-lik curv rflcs cumulaiv ffc of adsorpion and prcipiaion. Thrfor h adsorpion of Cu (II) ion ono oil palm ash was sudid a ph 5.5 for subsun xprimns a uilibrium. To dsign h sorpion sysms, chmical kinics is vry imporan as i xplains how slow and fas h ra of chmical racion occurs and h facors which affc h racion ra. In ordr o gain som insigh ino h sorpion procss of Cu (II) ions ono h surfac acivad palm oil ful ash, psudo firs ordr and psudo scond ordr kinic modls wr implmnd. Th psudo firs ordr uaion (Ong al, 200) basd on basd on uilibrium adsorpion is xprssd as: k = (3) 2,303 log ( ) log Whr, and ar h amoun of adsorbd (mg g ) a uilibrium and a any im, k is h firs ordr ra consan (min ). Th plo of log ( - ) vrsus (Fig no shown) gav h slop k and inrcp of log. Tabl- shows h co-rlaion cofficin R 2 and ra consan k for diffrn iniial concnraion a 30 C. Psudo scond ordr uaion (Ho and McKay, 999) can b givn by: k k, = + (4) Hr, k 2 is h ra consan of scond ordr adsorpion. Th linar plo of vrsus gav as k slop and as inrcp. This modl is mor likly o prdic h bhavior ovr h whol rang of adsorpion. Th linar plos of psudo scond ordr modl is shown in Fig. 4 and h modl paramrs ar lisd in Tabl.

5 Am. J. Applid Sci., 8 (3): , 20 Tabl : Comparison of psudo-firs ordr and psudo-scond ordr adsorpion ra consan for diffrn iniial concnraion Psudo-firs ordr kinics Psudo-scond ordr Kinics C 0 (xp) (cal) K (cal) K 2 (mgl ) (mg g ) (mg g ) (min ) R 2 (mg g ) (min ) R Fig. 4: Psudo Scond ordr Kinics for adsorpion of Cu (II) ono Acivad Palm Ash a 30 Tmpraur a ph 5.5 Th plo of vrsus 0,5 as shown by Fig. 5. Th slop of h plo has bn dfind o yild h inraparicl diffusion paramr K id (mg min 0,5 ). On h ohr hand, h inrcp of h plo rflcs C, h boundary layr ffc. Th largr h inrcp, h grar h conribuion of h surfac sorpion in h ra-conrolling sp. Th calculad inraparicl diffusion cofficin K id valus ar lisd in Tabl 2. Th salin faurs of isohrm sudis ar ssnial for h adsorpion procss o b inrprd adualy. Many modls hav bn proposd by h rsarchrs o xplain adsorpion uilibrium. Th mos commonly usd isohrm modls for solid-liuid adsorpion ar h Langmuir, Frundlich and Tmkin isohrms. Th Langmuir isohrm is basd on monolayr adsorpion (consan ha of adsorpion for all sis) on h aciv sis of h adsorbn and i is xprssd by following uaion: kc L = (6) + alc by: Th linar form of h Langmuir isohrm is givn Fig. 5 : Inra-Paricl diffusion for adsorpion of Cu (II) ono Acivad Palm Ash a 30 C Tmpraur a ph 5.5 Th prdicion of h ra-limiing sp is a ky facor o b drmind in h adsorpion procss. Th mos commonly usd chniu for idnifying h mchanism involvd in h adsorpion procss is by fiing an inraparicl diffusion plo. An inraparicl diffusion cofficin K id is givn by h uaion: = k (5) 0,5 id 234 C = + C (7) K m ax L m ax Whr: = Th uilibrium caion on h adsorbn (mg g ) C = Th uilibrium caion concnraion in soluion (mg L ) max = Th maximum monolayr adsorpion capaciy of h adsorbn (mg g ) and K L = Th Langmuir adsorpion consan (L mg )

6 Am. J. Applid Sci., 8 (3): , 20 Tabl 2: Inra paricl ra consan for diffrn iniial concnraion Iniial concnraion Corrlaion (mg L ) C K dif (mg/gh 0.5 ) cofficin,r Tabl 3: Essnial characrisics of langmuir isohrm Valu of R L Typ of Isohrm R L > Unfavorabl R L = Linar 0<R L < Favorabl R L = Irrvrsibl Tabl 4: Isohrm modl paramrs and corrlaion cofficin a 30 C Tmpraur Isohrm modl Paramrs valus R 2 Langmuir m,maximum monolayr adsorpion capaciis(mg g ) R L, sparaion facor K L, Langmuir consan Frundlich K F, Affiniy Facor (mg/gm(l mg ) /n ) /n, Frundlich xponn 0.20 Tmkin K T, (l mg ) B Fig. 7: Frundlich Isohrm a ono acivad palm ash a 30 C Tmpraur a ph 5.5 Fig. 6: Langmuir Isohrm a ono acivad palm ash a 30 C Tmpraur a ph 5.5 = (9) k C / n f And can b linarizd as: Whn C / is plod agains C, a sraigh lin wih slop / max and inrcp of / max K L is obaind. Th ssnial characrisics of h Langmuir uaion (ALzaydin, 2009) can b xprssd in rms of a dimnsionlss facor, R L which is givn blow: R L = + K C L o (8) Co is h highs iniial caion concnraion (mg L ). Th valu of sparaion facor R L, can b rprsnd by following Tabl 3. Th linar plo of Langmuir Isohrm a 30 C mpraur is shown on Fig. 6 and h modl paramrs a 30 C ar lisd in Tabl 4. Frundlich isohrm givs h rlaionship bwn uilibrium liuid and solid phas capaciy basd on h mulilayr adsorpion (hrognous surfac) propris. This isohrm is drivd from h assumpion ha h adsorpion sis ar disribud xponnially wih rspc o h ha of adsorpion and is givn by: 235 In k InC n = + (0) f whr, K f (mg g ) and rlas h mulilayr n adsorpion capaciy and innsiy of adsorpion. Th linar plo of Frundlich Isohrm a 30 C mpraur is shown on Fig. 7 and h modl paramrs a 30 C ar lisd in Tabl 4. Tmkin isohrm, which considrs h ffcs of h ha of adsorpion of all molculs in h layr would dcras linarly wih covrag du o h adsorba and adsorbn inracions and is givn by: RT InAC b = () Euaion can b linarizd as: RT RT = InA+ In C b b (2)

7 Am. J. Applid Sci., 8 (3): , 20 Fig. 8: Tmkin Isohrm ono acivad palm ash a 30 C Tmpraur a ph 5.5 Hr RT/b = B (j mol ), which is Tmkin consan rlad o ha of sorpion whras a (L g ) is h uilibrium binding consan corrsponding o h maximum binding nrgy. R (8.34 J mol k) is univrsal; gas consan and T(K) is absolu soluion mpraur. Figur 8 dpics Tmkin modl undr h concnraion rang sudid hr. DISCUSSION Th rsuls from h xprimn s dscribd in his sudy show ha coppr ions can b absorb fficinly on acivad oil palm ash. Howvr, h abiliy of acivad oil palm ash is h rsul of a numbr of mchanisms, including surfac adsorpion, chmisorpions, complxaion, ion xchang, microprcipiiaion and mal hydroxid complxaion. In ordr o undrsand h daild mchanism by which coppr ion has bn rmovd from h soluion by adsorpion, i is ssnial o idnify h chmical consiun prsn on h adsorbn. Th high prcnag of SiO 2 may also b involvd in h adsorpion phnomna hrough SiO bond wih coppr (II) ions, as prsnd by following schm: cofficin, R 2 of psudo firs ordr kinics ar bwn This confirms ha i is no appropria o us h Lagrgrn firs ordr kinic modl o prdic h adsorpion kinics for Cu (II) ono acivad palm oil ash for h nir sorpion priod. On h conrary, h corrlaion cofficin, R 2 for h scond ordr kinic modl wr almos ual o uniy for all coppr concnraions indicaing h applicabiliy of h modl. Thus i appard ha h sysm undr sudy is mor approprialy dscribd by psudo scond ordr kinics which was basd on h assumpion ha h ra limiing sp may b chmisorpions involving valncy forcs hrough sharing and xchang of lcrons. From h plo of inra-paricl diffusion, i is obsrvd ha h lins did no pass hrough h origin. This indicad ha h ra limiing procss is no only govrnd by inra paricl diffusion. Som ohr mchanism along wih inraparicl diffusion was involvd. Th validiy of h Langmuir modl hr suggsd ha h adsorpion procss was monolayr and adsorpion of ach molcul had ual acivaion nrgy. Th R L valu obaind is bwn 0- indicaing ha h adsorpion of coppr ono acivad oil palm ash is favorabl. Th Langmuir modl was found o fi h daa significanly br han Frundlich modl, which showd h mor homognous naur of acivad palm ash. Frundlich xponn, n ranging bwn 0 and is a masur of adsorpion innsiy or surfac hrogniy. Th valu n blow on indicas favorabl adsorpion of coppr ono acivad oil palm ash. Th Tmkin isohrm showd a highr rgrssion cofficin, which may b du o h linar dpndnc of ha of adsorpion a low or mdium covrag. This linariy may b du o rpulsion bwn adsorba spcis or o inrinsic surfac hrogniy. Th rgrssion cofficin of hs modls showd a srong affiniy for h adsorpion of Cu (II) ono acivad palm ash. CONCLUSION -SiO 2 +H 2 O=-SiO - +H 3 O + (I) This sudy invsigad h adsorpion of Cu (II) -SiO - +Cu 2+ =-SiOCu 2+ (II) from auous soluion using surfac modifid palm oil ful ash a iniial ph of 5.5 of h soluion. Th -SiOH+Cu 2+ =-SiO - Cu 2+ (III) adsorpion was found o b srongly dpndn on ph, conac im and iniial mal ion concnraion. Psudo scond ordr gav br R 2 valus confirming Th rsuls obaind from Psudo firs ordr chmisorpions ono h surfac. Euilibrium was kinics dmonsrad ha h xprimnal (mg g ) aaind wihin 3 h. Boh Frundlich and Langmuir valus did no agr wll wih h calculad valus modl can b usd o fi h daa and sima modl obaind from h linar plos. Th corrlaion paramrs bu h ovrall daa is slighly br fid 236

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