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Desalination of Dye by Charged Mosaic Membrane

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) 8 1 0 2 O S M ( n o it a z i m it p O d n a n o it a l u m i S , g n il e d o M n o e c n e r e f n o C l a n o it a n r e t n I 8 1 0 2 8 7 9 : N B S

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s e c r u o s e R r e t a W f o y ti s r e v i n U a n i h C h t r o N , g n i r e e n i g n E l a p i c i n u M d n a l a t n e m n o ri v n E f o e t u ti t s n I n a n e H , u o h z g n e h Z , r e w o P c i r t c e l E d n

a ,450011,China

d r o w y e

K s:ChargedMosaicMembrane(CMM), D , ye Desailnaitonandpuriifcaiton.

t c a r t s b

A . Desalination and purification of dye c an improve tis quality and value .Membrane n i a m e h t f o e n o s i y g o l o n h c e t n o i t a r a p e

s technologies of dye desalination and purificaiton .The e n a r b m e m c i a s o m d e g r a h

c (CMM)is preparedbyinterfacia lpolymerization(IP)inthispaper .A nd t nh te i isapplied in desalination and purification ofcrudedye .TheresultsshowsRejection ofthe

d n a l C a N r o f M M

C Reactive Ligh tYellow F( -P 6GS) is 13.2% and 99.2% ,respectively .Itsflux e s a e r c n

i s from 6.22L·m-2·h-1to18.5L·m-2·h-1when theoperatingpressureincreases from0.2MPa

. a p M 5 . 0 o

t I ts flux reduces from 13.32 L·m-2·h-1 to 11.11 L· m-2·h-1 and it s rejection for NaC l

y l l a u d a r

g improves from12.5% to 13.7% when NaC lconcentraiton increases from 500 mg·L- 1to

g m 0 0 0

2 ·L-1 .Itsflux gradually reduces from10.17L·m-2·h-1 to 8.21 L·m-2·h-1 and therejection for

e y d e h

t a ll exceeds 99 . % 00 when the PF-6GS concentration increases from 500mg·L-1 to

g m 0 0 0

2 ·L-1. Aftert hecrudedyeisdesalinate adv i fivet imest heNaC lconcentrationindyesoluiton

e c u d e

r s from8775mg·L- 1to658mg·L-1 ,theconductivityofd yesoluitonreduces from28.6ms/m to

2 9 .

8 sm / ,m dyepurityi ncreases from72.6%t o97. %. 0

n o it c u d o r t n I e y d e h

T prepared by "satling-out"methodcontainslargeamountsofs s atl and rawmaterialsand y

b products .Thesei mpuritiescandecreased yesolubilityandfastness ,andmaketheprintedproduc t s

a

e i ly appear color point and color stain. So i t has grea t significance for desalination and n o i t a c i f i r u

p ofcrudedye.

0 0 2 n e e w t e b s i ) F N ( e n a r b m e m n o it a r tl i f o n a n f o ) C W M ( f f o t u c t h g i e w r a l u c e l o m e h

T -1000 .I tcan

tl a s e t a r a p e s l l e

w s and mos tdyes. iL ][1 prepared a negaitvely charged N F membrane via phase

. x d o h t e m n o i s r e v n

i TheNFmembranepurewaterfluxcouldreach269.5L·m-2 h· - 1andt herejecitons

s tl a s f o s e p y t l l a r o

f candecilnetounder11%, da sn ti rejecitonforReacitveRed49 wasintherange 0

8 f

o -90%.Wei[2]fabricatedhollow fiberNF membraneand appiled theNF membraneto desailnate

X n a d e n i a t n o c h c i h w n o it u l o s s u o e u q a d e x i m e t a r t n e c n o c d n

a -BRandNaCl .Afterdesailnaiton and e r s a w l C a N % 3 . 5 9 r e v o d n a , % 4 . 1 9 o t p u s a w e y d f o e t a r y r e v o c e r e h t n o it a r t n e c n o

c movedfromthe

. s e r u t x i m t l a s / e y

d iL[3]prepared ahollowfibercompostiemembranemodified wtih nano- OTi 2. T he

e n a r b m e m F

N rejeciton for CR , MO and MB was 94±2.57% , 52.1±2.45% , and 92±2.20% , y l e v it c e p s e

r ,bu t ti had no rejeciton to satls(NaC,lNa2SO4) u. Y [ ]4 fabricated a high flux posiitvely

e s o o l d e g r a h

c N F membrane via “blending-phase inversion” method. TheNF membranepossesse s s e y d e v it c a e r r o f n o it c e j e r r e h g i h y l e v it a l e r d n a y ti li b a e m r e p t l a s r e h g i

h .These NF membranes

d e y a l p s i

d outstandingadvantagestobeappiledt odesailnateandpurifythecrudedye. ) M M C ( e n a r b m e m c i a s o m d e g r a h c e h

T is one of NF membranes . It contains both anion e g n a h c x

e group and caiton exchange group .Inorganicionscan easily penetratethrough CMM by g n i d n o p s e r r o c h ti w g n i n i b m o

c exchanged group ,so i thas lower rejection for inorganic ions .Bu t y l l a r e n e g t o n e r a y e h t e s u a c e b d n u o p m o c c i n a g r o r o f n o i t c e j e r h g i h s a h M C

C charged [5] .This

e r u t a e

f makeCMMbemoresuitablefordesalinationandpurificationofcrudedye. t , t n e s e r p t

A hepreparaiton methods ofCMMhav ephaseinversion[6] ,composition[7] ,interfacia l

n o i t a z i r e m y l o

p [8] ,thehybrid[9]and cross-linking[ 01 ] da n soon .Inthisstudy, theCMMw asfirslty

d e r a p e r

p byIPwhich ah d highrejectionfordyes andl owerrejectionforNaCl .

Thenthemembrane aw sappliedi ndesailnaitonandpurificationofPF-6GScrudedye .T heaimi s s e i g o l o n h c e t d n a s l a i r e t a m w e n e d i v o r p o

(2)

n o it c e S l a t n e m i r e p x E

sl a i r e t a M

b o s a w ) I E P ( e d i m i r e h t e y l o

P tained from Guangzhou Hengda surface technology Co. , Ltd . m-Phenylenediamine m( -PDA)waspurchasedfromShangha iShanpuchemicalCo. ,Ltd .Trimesoy l

o b i Z y b d e i l p p u s s a w ) C M T ( e d i r o l h

C Dalong pharmaceuticals technology Co. ,Ltd .Sodium S

D S ( e t a f l u s l y c e d o

d ) was purchased from Shangha iYingpeng Addiitves chemica lcompany . e

t a n o b r a c m u i d o

S (Na2CO3) wasobtained from Tianjin Jingdachemicalcompany .N-hexane was

g n o t i a K n i j n a i T m o r f d e s a h c r u

p chemica lreagentsCo. ,Ltd. Reactive Ligh tYellow (P -F 6GS) ,its m eol cular weight is 796 ,which is provided by a dye Co. ,Ltd. The dye purity is 72.6% ,the

o d n a l C a N f o n o i t a r t n e c n o

c theri mpuritiesis17.6%and9.8% ,respectively.

f o n o it a r a p e r

P PolysufloneSuppor tMembrane

i r t e h

T -channe lhollow fiber ultrafitlration (UF) membrane was prepared by dry/je twe tspinning d

n a ) % 8 ( P V P , l a i r e t a m e n a r b m e m a s a d e s u s a w ) % 2 2 ( F S P h c i h w n i , y g o l o n h c e

t acetone(0.5%)

s a w e n a r b m e m t r o p p u s f o e c n a m r o f r e p e h T . t n e v l o s s a d e s u s a w c M A D , s e v i t i d d a s a d e s u e r e w

n i w o h

s Table1 .

it a r a p e r

P onoft heCMM

i r t e h

T -channe lhollowfiberCMMwaspreparedby IP ,whichthetri-channe lPSFhollowfiberUF d

n a ) F B ( n i s h c u f c i s a b , e n a r b m e m t r o p p u s e h t s a d e s u s a w e n a r b m e

m P EIand2 ,5-diaminobenzene s

a C M T , r e m o n o m e s a h p s u o e u q a s a ) A I D ( d i c a c i r u f l u

s organicphasemonomer .BF c an provide e

g n a h c x e n o i n

a group ; DIA can provide cation exchange group . The concentration of acid a

N ( t n e b r o s b

a 2CO3)andsurfactan t(SDS)inwatersolutionwas0.45%and0.2% ,respectively .The

o e c n a m r o f r e p e h T . n i m 3 d e t c a e r P

I f CMM prepared under differen tconditions was shown in .

1 e l b a T

F P d n a l C a N r o f 2 M M C f o n o it c e j e r t a h t s w o h s 1 e l b a

T -6GS is13.2%and 99.2% ,respectively , e

y d e v o r p m i n a c y l n o t o n h c i h

w recovery ratebu talso canacceleratethespeed ofdesalinationand u

p rification. Iti smoresuitablefordesalinationandpurificationofPF-6GScrudedye .SoCMM2is F

P r o f y f i r u p d n a e t a n i l a s e d o t d e t c e l e

s -6GScrudedye .

1 e l b a

T . Theperformanceofsuppor tmembraneandCMM. O

N Membrane D IA F B P EI NaCl P -F6GS conduct Jv

) %

( (%) (%) (%) (%) (%) (L·m-2·h-1)

1 S M 0 0 0 0 4 1 4 .8 37.2

2 CMM1 1 .5 0 .2 1 .2 2 .5 6 0 9 .3 22.8

3 CMM2 2 0 .2 1 .5 13.2 99.2 3 9 13.7

n o it a n il a s e D e y D

F P f o n o it a r t n e c n o c e h t h c i h w n i d e r a p e r p s a w s u o e u q a e y d e h

T -6GS crudedyewas5% .And then p

s a w t

i umpi ntomembranemodulet odesalinate .Thesamevolumeofdemonizedwaterwasj oined .

L 4 . 0 d e h c a e r e t a e m r e p n e h w n

(3)

l a c it y l a n

A Methods

e t e m y t i v it c u d n o c a y b d e r u s a e m s a w n o i t a r t n e c n o c t l a s e h

T r (Shangha i Dazhong analysis S

D D : l e d o M , y n a p m o c s t n e m u r t s n

i -12A) .The dye concentration was analyzed by UV/visible n

o i s i c e r P i a h g n a h S ( r e t e m o t o h p o r t c e p

s InstrumentCo. ,Ltd. ,Model :722S).

s tl u s e

R andDsicus ison e

n a r b m e

M Performance

f o t c e ff

E Opera itng Pressure .TheCMM wasfirstly pre-pressured for30 mina t0.5MPawith M

M C n o e r u s s e r p g n i t a r e p o f o t c e f f e e h t n e h t d n a , r e t a w e r u

p performance was analyzed under .

1 . g i F n i n w o h s e r e w s t l u s e r e h T . e r u t a r e p m e t m o o r

2 .

0 0.3 0.4 0.5 4

6 8 0 1

2 1

4 1

6 1

8 1

0 2

·

·

-1

a P M / P

e f f E . 1 e r u g i

F c tofoperatingpressureonfluxoft heCCM.

m · L 2 2 . 6 m o r f s e s a e r c n i M M C e h t f o x u l f e h t t a h t s w o h s 1 . g i

F -2·h- 1to 18.5 L·m-2·h- 1when the

g n i t a r e p

o pressurei ncreasesfrom0.2MPat o0.5MPa. o

s l a t l u s e r e h

T nc a beexplained yb theKedem-Katchalskyequation [11].

E ffec to fNaC lConcentra iton .The NaCl soluiton was prepared in which its concentration m

o r f d e s a e r c n

i 500mg·L-1 ot 2000mg·L-1 .Theeffec tofNaC lconcentration on CCMperformance

a

w sshowi nFig.2.

0 0

5 1000 1500 2000 0

. 0 1

5 . 0 1

0 . 1 1

5 . 1 1

0 . 2 1

5 . 2 1

0 . 3 1

5 . 3 1

0 . 4 1

· g m / C

·

·

0 . 2 1

5 . 2 1

0 . 3 1

5 . 3 1

0 . 4 1

5 . 4 1

0 . 5 1

%/

R

g i

F ure2 .Effec tofNaC lconcentrationontheCCMperformance.

t

I canbeseenfromFig.2tha tthefluxdecreases from13.32L·m-2·h- 1t o11.11L·m-2·h-1 sa NaC l

n o i t a r t n e c n o

c increases from 500mg·L- 1to 2000mg·L-1. tI can beexplainedby KedemKatchalsky

n o it a u q

e [ 1]1 .

a 2 . g i

F lso shows that CMM rejection for NaCl increases from 12.5% to 13.7% when si t m

o r f s e s a e r c n i n o i t a r t n e c n o

c 500mg·L- 1to 2000mg·L-1 .Th echargecapacityinCMMdecreases as

s e v o r p m i n o i t a r t n e c n o c l C a

N becauseanion exchange group and cation exchange group adsorbes .

n o i e t y l o r t c e l e e t i s o p p o y l l a c i r t c e l

e The character ofCMM decreases ,and which makes rejeciton s

e s a e r c e d l C a N r o f M M C f

o .Theresulti sdifferentt oordinarynanfitlrationmembrane[12]. f

o t c e ff

E Dye Concentra iton .The effect of dye concentraiton on CMM performance was .

0 t a d e t c u d n o

(4)

0 .

0 0.5 1.0 1.5 2.0 2.5

0 . 8 5 . 8 0 . 9 5 . 9 0 . 0 1

5 . 0 1

0 . 1 1

·

·

2-·

1-0 . 8 9

5 . 8 9

0 . 9 9

5 . 9 9

0 . 0 0 1

%/

R

e c n a m r o f r e p M C C e h t n o n o i t a r t n e c n o c e y d f o t c e f f E . 3 e r u g i

F .

e h t t a h t s w o h s 3 . g i

F flux fo CMMslowlydropsfrom 01 .17L·m-2·h-1to8.21 L·m-2·h- 1whendye

e v o r p m i n o i t a r t n e c n o

c s from 500 mg·L-1 to 2000mg·L-1 .This is due to tha tpolarization and

g n i l u o f e n a r b m e

m wil lbestrong as dye concentration increases[13] .T heflux decreasecan also be

t o m s o e h t o t e u d y l l a i t r a

p icpressureofsolutionincreases sa thedyeconcentrationincreases. e

y d r o f e n a r b m e m f o n o i t c e j e r e h t t a h t 3 . g i F m o r f n e e s e b o s l a n a c t

I iskep tbetween99.24% da n e

v o r p m i n o i t a r t n e c n o c e y d n e h w % 8 3 . 9

9 s from500mg·L-1to2000mg·L-1 .I thelpstoimprovedye

y r e v o c e

r erat .

n o it a n il a s e

D o fDye

f o t c e ff

E Opera itng Time on Flux .TheCMMwasappiled in thedesailnation and purification F

P r o

f -6GS crudedyesa t0.35MPaunder room temperature .Thecrude dye concentration in feed .

% 5 s a w n o i t u l o

s Effec tofoperatingt imeonCCMfluxwasshowni nFig.4 .

0 5 10 15 20 25 30 35 40 0

. 6 5 . 6 0 . 7 5 . 7 0 . 8 5 . 8

·

·

e r u g i

F 4. Effect fo operatingt imeonCMMflux.

. g i

F 4 shows tha tthe flux of CMM ed creases in every cycle sa operating time prolongs .T he l

l i w l C a N d n a e y d f o n o i t a r t n e c n o

c increase w ith prolong of operaitng time in very cycle, which s

e v o r p m

i osmoitcpressureofsoluitonandconcentrationpolarization oftheCMM. .

g i

F 4 also shows that the CMM flux is higher than the flux of the previous cycle. tI can be d

e n i a l p x

e thattheconcentrationofNaC landdyereduces bydesalination ,whichdecreasesosmotic e

r u s s e r

p ofsolutionandconcentrationpolarization oftheCMM.

f o t c e ff

E Opera itngTimeonDyeConcentra iton.Effec tofoperatingtimeondyeconcentration n

i feedsolutionwasshowni nFig.5duringdesalinationandpurificationprocess.

5

- 0 5 10 15 20 25 30 35 40 0

0 0 0 3

0 0 0 5 3

0 0 0 0 4

0 0 0 5 4

0 0 0 0 5

0 0 0 5 5

0 0 0 0 6

(5)

. g i F m o r f n e e s e b n a c t

I 5 tha tthedye concentraiton i n feed solutionincreasesineverycycle as a

c e b s g n o l o r p e m i t g n i t a r e p

o use of dewatering .The dyeconcentration in feed solution is smaller n

a h

t that of the previous cycle .I tcan be explained tha ta ny dye losse s and tota ldye moun t e

y d e m o s e s u a c e b s e s a e r c e

d be discharged with permeaitng solution. The dye purity can reach 7

9 0. %byfive itmesdesalinationandpurificaiton.

f o t c e ff

E Opera itng Time on NaCl Concentra iton .The NaC lconcentration in feed sioluiton d

e r u s a e m s a

w . Itsremova lrateandt ota lremovalrateweremeasuredaftereverydesalinationcycle . Theresult wasshowni nTable2 .

e h t t a h t s w o h s 2 e l b a

T concentration of NaC ldecreases from 8775mg·L- 1to 658mg·L-1 and the

l a v o m e r l a t o

t ratereaches92.48%byfive itmesdesalination.

2 e l b a

T . ThechangeofNaC lconcentrationandrejectionwithoperatingt ime. .

O

N time h

( ) concNenaCtrlation (m Lg· -1)

l C a N

e t a r l a v o m e r

) % / R (

l a t o t l C a N

e t a r l a v o m e r

) % / R (

0 0 8775 0

0

1 8 .5 4964

1 5 . 3

4 43.51

2 15.9 2783

3 8 . 4

2 68.34

3 22.8 1617

2 3 . 3

1 81.66

4 29.7 1033

1 6 .

6 88.27

5 36.2 6 65 4.21 92.48

n o e m it g n it a r e p o f o t c e ff

E conduc itvtiy .The conducitvity v y ar trend of feed solution w as e

l b a t n i n w o h

s 3 .Table3 shows that et h conduciton offeedsolution decreases from32.8ms·m-1 to

2 9 .

8 ms·m-1anditstota lremovalreaches67.07% byfivetimesdesailnation .I tcanbeseentha tthe

l a v o m e r e h t n a h t r e w o l s i e t a r l a v o m e r y t i v it c u d n o

c rateofNaC lbycomparing Table2t o Table3 . t

I isbecauset hedyet akes chargeandhascertainconducitvity .

3 e l b a

T . Thechangeoft hedyesolutionconductionwithoperatingt ime. .

O

N time ) h (

u d n o

c ctivity

(ms·m-1) creomndouvcati lvraittye

) % / R (

l a t o

T conductivity e t a r l a v o m e r

) % / R (

0 32.8 0

0

1 8 .5 24.1 26.52 26.52

2 15.9 16.27 23.87 50.39

3 22.8 12.92 13.26 63.65

4 29.7 10.20 2 .2 65.85

5 36.2 8.92

2 2 .

(6)

u l c n o

C s ni o

) 1

( The rejection oft he CMM prepared by IP forNaC land Reactive Ligh tYellow i s13.2% and t

I . y l e v it c e p s e r , % 2 . 9

9 si verysuitabletopurify FP -6GScrudedye. e

h T ) 2

( increase of pressure is beneficia lfor increase of flux and production capactiy of the .

M M

C Itsflux reduced and tis rejeciton forsolute gradually improved as concentration NaC land e

y

d increased.

(3 )Afterthecrudedyeisdesailnated and purifi aed v i fivetimest eh NaC lconcentration reduce L

· g m 5 7 7 8 m o r

f - 1to 658mg·L-1and conduction reducefrom 28.6m ms· -1 to 8.92 ms·m-1 ,thepurity

f

o ed y increases from72.6%t o97.0% .

s t n e m e g d e l w o n k c A

h c r a e s e r s i h t g n i d n u f r o f e c n i v o r P n a n e H f o t n e m t r a p e D n o it a c u d E e h T o t l u f e t a r g e r a s r o h t u a e h T

t n a r g a i

v 12A560007and WaterResourcesDepartmen tof Guizhou Provinceforfunding viagran t a i v g n i d n u f r o f r e w o P c i r t c e l E d n a y c n a v r e s n o C r e t a W f o y t i s r e v i n U a n i h C h t r o N d n a 5 1 3 1 0 2 T K

. 2 4 2 1 0 2 t n a r g

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p h t i w g n i d n e l b y b e n a r b m e

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[ Xiuzhen Wei ,Xin Kong ,Chengtian Sun ,e tal .Characterizaiton and application ofa thin-film n

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[5] MitsuruHiga ,D aiMasudaa ,EisukeKobayashi ,e tal .Chargemosaicmembranespreparedfrom A

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m e

s -interpenetratingnetworkstructures[J] .2013 ,428: 72 – 46 2 . 7

[7 R] .H. Lajimi ,A.B. Abdallah , . E Ferjan P. ,e tal .Change of the performance properties of e

c a f r u s y b s e n a r b m e m e t a t e c a e s o l u l l e c n o it a r t l i f o n a

n adsorptionofpolyelectrolytemulitlayers[J] . 1

( 3 6 1 , 4 0 0 2 , n o it a n il a s e

D - :3 3) 1 -9 202.

[8] J.Y. Zhang ,Y.W. Zhang ,H.Q. Zhang ,e tal .Preparation and Characterization of a Nove l c

i a s o M d e g r a h C e d i m a y l o

P Membrane[J] .ChineseJourna lofChemica lEngineering ,2010 ,18(4) : 9

6 5 -576.

[9] Xu Tongwen ,Liu Junsheng ,Fu Yanxun .A Hybrid amphoteric ion-exchange membrane , 2 3 8 4 6 8 1 N C . t n e t a P a n i h C . d o h t e m n o it a r a p e r p s ti d n a p u o r g c i d i c a t n e r e f f i d g n i s i r p m o c

6 0 0

(7)

[ 01 ] Mitsuru Higa ,Mayumi Kobayashi ,Yuriko Kakihana ,e tal .Charge mosaic membranes with i

m e

s -interpenetratingnetworkstructurespreparedfromapolymerblendofpoly(viny lalcohol)and s

e t y l o r t c e l e y l o

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[ 1] I . Koyuncua , D . Topacika , M.R . Wiesner , Factors influencing flux decline during h

c r a e s e R r e t a W . s tl a s d n a s e y d g n i n i a t n o c s n o i t u l o s f o n o it a r t l i f o n a

n , 2004, 38(2): 24 –3 440. 1

[ 2] Y iHe ,Guang-Ming Li ,HuaWang, te al .Experimenta lstudy ontherejection ofsal tanddye r

t l i f o n a n e t a t e c a e s o l u l l e c h t i

w aiton membrane . Journa lof the Taiwan Institute of Chemica l 9

0 0 2 , s r e e n i g n

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[ 3] Jian Huang ,Kaisong Zhang .Thehigh flux poly (m-phenyleneisophthalamide)nanofiltraiton 1

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: r o h t u

A Deng Jianmian ,Doctor ,Associate Professo ,r Graduate direction: Water Treatmen tand e

n a r b m e

References

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