DYE SOLUBILITY IN SUPERCRITICAL CARBON DIOXIDE FLUID

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1 THERMAL SCIENCE, Yer 2015, Vol. 19, No. 4, pp DYE SOLUBILITY IN SUPERCRITICAL CARBON DIOXIDE FLUID by Jun YAN, Li-Jiu ZHENG *, Bing DU, Yong-Fng QIAN, nd Fng YE Lioning Provincil Key Lbortory of Textile Clening, Dlin Polytechnic University, Dlin, Chin Originl scientific pper DOI: /TSCI Y Supercriticl crbon dioxide fluid is n lterntive solvent for the wter of the trditionl dyeing. The solubility of dyestuff ffects gretly the dyeing process. A theoreticl model for predicting the dye solubility is proposed nd verified experimentlly. The pper concludes tht the pressure hs greter impct on the dyestuff solubility thn temperture, nd n optiml dyeing condition is suggested for the highest distribution coefficient of dyestuff. Key words: supercriticl CO 2, disperse dyes, solubility, phse equilibrium, Chrstil ssocition model, distribution coefficient Introduction Crbon dioxide cpture, storge, nd utiliztion become the hottest topic in the world s one of the min lterntives for sustinble energy infrstructure development [1, 2]. Supercriticl crbon dioxide (SC-CO 2 ) dyeing is new clen technology for textile industry, nd the dyestuff is recyclble [3]. Solubility of dyestuff is extremely importnt to develop the SC-CO 2 dyeing process, nd much preliminry work ws conducted [4-11]. The ffinity between dyes nd fbric in SC-CO 2 is usully expressed by distribution coefficient of dyestuff, the higher of the coefficient, the higher efficiency of dye utiliztion nd better dyeing effect. However, the theoreticl insight into the coefficient is rre nd very much preliminry. Therefore, the theoreticl nd experimentl studies on the coefficient re much needed. This pper develops theoreticl model, nd n experiment is verified by experimentl dt. Experimentl Cotton/polyester (65/35) fbrics, C. I. disperse red 127 ( 98%), fig. 1, nd pure CO 2 (99.99%) were used in the experiment. Experimentl set-up includes the rection unit, control unit, recycle unit, pressure unit, nd temperture unit [1].The rection unit ws Figure 1. The constitutionl formul of C. I. consisted of high pressure rection kettle for disperse red 127 dyestuff dissolving. The control unit took the monitoring role of the whole rection process by controlling the flow rte of CO 2, pressure * Corresponding uthor; e-mil:

2 1312 THERMAL SCIENCE, Yer 2015, Vol. 19, No. 4, pp nd temperture. The recycling unit referred to seprte the dyestuff nd CO 2 by decresing the pressure nd temperture, which the dyestuff could be gthered. After recycled, the CO 2 could be used gin by incresing pressure, chieving the effect of recycle utiliztion. There were two kinds of solubility mesurement equipment for the disperse dyestuff in SC-CO 2 : continuous nd intermittent. Intermittent smpling ws referred to put the dyestuff in seled continer first nd the CO 2 is introduced through the pipe. The dyestuff ws tken out for nlysis fter the conditions of high pressure rection kettle reched the phse equilibrium. But becuse of the intermittent smpling ws more difficult to judge whether ll dyestuff is dissolved in the kettle or not, so the continuous smpling device ws dopted in this work. Solubility of dyestuff The solubility of dyestuff cn be expressed by the Chrstil eqution [10]: lnc= kln + + b T where c is the solubility of solid solute, the fluid density, T the temperture, nd k,, nd b re constnts. Peng-Robison eqution of stte (PR-EOS) is dopted hereby: where RT P = v b v( v+ b) + b( v b) 2 2 Tc (1) (2) R α ( Tr) = (3) P c r α ( T ) = [1 + m(1 T )] (4) r m= f( w) = w w (5) RT b = c (6) P where nd b re the grvity prmeter nd repulsion prmeter, respectively, R is the universl gs constnt for the vlue of J/molK, P the pressure, T the temperture, v the molr volume, P C the criticl pressure, T C the criticl temperture, T r the reduced temperture, nd w the centric fctor. Compression fctor Z is expressed in the form: PV Z = (7) RT The density of CO 2 is defined s: M = (8) V where M is g/mol, nd V is the molr volume of CO 2 [cm 3 mol 1 ]. c 2

3 THERMAL SCIENCE, Yer 2015, Vol. 19, No. 4, pp Combining eqs. (7) nd (8), eq. (8) becomes: MP = (9) ZRT When the criticl temperture is K, criticl pressure is 7.39 MP, c is g/m 3, Z c is The density of the CO 2 is given in tb.1. Tble 1. The density of SC-CO [K] [K] [K] [K] P [MP] P [MP] P [MP] P [MP] Results nd discussion The solubility of C. I. disperse red 127 in SC-CO 2 ws mesured under CO 2 flow rte of 500 kg/h, t the temperture of K to K nd pressure of 21 MP to 25 MP in the work. The results of the solubility under different condition were shown in fig. 2. Comprison between the experimentl solubility nd theoreticl prediction is presented s AAD%, which is defined s: np exp clc y2i + y2i exp i= 1 y2i 1 AAD% = 100 (10) np where np is the experimentl number of points, exp clc nd y 2i nd y 2i re the solubility of dyestuff obtined from experimentl dt nd clculted by C. I. disperse thermodynmic model, respectively. The vlues of red 127 AAD% re listed in tb. 2. The continuous smpling method ws used to mesure the solubility dt of C. I. disperse red 127 in SC-CO 2, it is concluded tht the solubility in the Figure 2. The experimentl vlues of C. I. disperse red 127 in SC-CO 2 Tble2. The prmeters of Chrstil eqution nd verge reltive error K b K AAD% K K K K Averge vlue

4 1314 THERMAL SCIENCE, Yer 2015, Vol. 19, No. 4, pp rnge of mol/mol in the work. The solubility ws incresing when the pressure incresed. And becuse of the solubility incresed obviously between 23 MP nd 24 MP, it indicted tht the trnsition pressure of C. I. disperse red 127 ws 23 MP. The distribution coefficient between fbric nd CO 2 : The cotton/polyester (65/35) fbric ws dyed with C. I. disperse red 127 by selfdeveloped SC-CO 2 dyeing equipment. According to the dt, the reltion mong temperture, pressure nd distribution ws shown in fig. 3. From fig. 3, the distribution coefficient (K eq ) reched the highest t the pressure of 23 MP. But with the increse of temperture, the distribution coefficient decresed nd the chnge of distribution coefficient ws reltively stble under the rnge of high pressure, Figure 3. The reltion chrt between showing the rte of dye uptke on the fbric distribution coefficient nd pressure in ternry lmost equl to the dissolved rte of dyestuff system of C. I. disperse red 127, fbric nd SC-CO in CO 2 2. At the temperture of K, pressure of MP, the concentrtion of dyestuff both in CO 2 nd fbric increse nd K eq incresed obviously. It ws shown tht most of dyestuffs dissolved in CO 2 were in combintion with fbric nd this process ws the key period to the dyeing. However, the rte of dyes uptkes on the fbric slowed down with the increse of pressure, even dyestuff desorption ppered. And the distribution coefficient decresed. Conclusions The mesurement of solubility in SC-CO 2 ws studied in this pper. In the experimentl conditions, the solubility rnge of C. I. disperse red 127 ws mol/mol for the SC-CO 2 -dyestuff binry phse equilibrium system. At the sme temperture, when the pressure ws lower thn 23 MP, the increse rte of solubility ws slower, but the pressure ws higher thn 23 MP, the increse rte of solubility ws quicker. At the sme pressure, with the increse of the temperture, the solubility incresed smoothly. From mentioned bove, the pressure hd greter impct on the dye solubility reltive to the temperture. The results showed tht the turning point of C. I. disperse red 127 pressure ws 23 MP. Chrstil ssociting model, cube stte model PR eqution nd Vn der Wls mixed rules were used to do experimentl dt correltion. Through the model bove, the verge reltive error between the clculted vlue nd experimentl vlue ws less thn 10%. It ws proved to be successful through correltion clcultion. The distribution coefficient of C. I. disperse dyes between fbric nd SC-CO 2 ws lso discussed. Combining with the dyeing dt of C. I. disperse red 127 nd cotton/polyester (65/35) fbric in SC-CO 2, it ws showed tht t the temperture of K, pressure of MP, the distribution coefficient of SC-CO 2 -dyestuff-fbric ternry phse equilibrium system ws At the temperture of K, the pressure of 23 MP, the distribution coefficient ws highest, showing the dyestuff hd good ffinity on the fbric. The concentrtion of dyestuff in fbric ws higher thn in SC-CO 2, which is bout 10 2 ~ 10 4 orders of mgnitude. Becuse of SC-CO 2 dyeing is n exothermic chemicl process, rising temperture will reduce distribution coefficient t the sme pressure.

5 THERMAL SCIENCE, Yer 2015, Vol. 19, No. 4, pp Acknowledgments This reserch is supported by the Science Fund (No. 2014A11GX030) from Dlin City in Reference [1] Shim, S. M., et l., A Numericl Evlution of Prediction Accurcy of CO 2 Absorber Model for Vrious Rection Rte Coefficients, Therml Science, 16 (2012) 3, pp [2] Koukouzs, N., et l., CO 2 Cpture nd Storge in Greece: Cse Study from Komotini NGCC Power Plnt, Therml Science, 10 (2006), 3, pp [3] Yn, J., et l., Study on Dyeing of the Plsm Modifiction Silk Fbric in Supercriticl Crbon Dioxide, Advnced Mteril Reserch, (2011), Jn., pp [4] Zhen, H., et l., Representing Dyestuff Solubility in Supercriticl Crbon Dioxide with Severl Density- Bsed Correltions, Fluid Phse Equilibrium Fluid Properties Simultion Chllenge, 236 (2005), 1-2, pp [5] Muthukumrn, P., et l., Dye Solubility in Supercriticl Crbon Dioxide. Effect of Hydrogen Bonding with Cosolvents, Koren Journl of Chemicl Engineering, 16 (1999), 1, pp [6] Bo, P., et l., Reltionships between the Solubility of C. I. Disperse Red 60 nd Uptke on PET in Supercriticl CO 2, Journl of Chemistry & Engineering Dt, 50 (2005), 3, pp [7] Lee, J. W., et l., Mesurement nd Correltion of Dye Solubility in Supercriticl Crbon Dioxide, Fluid Phse Equilibri, 179 (2001), 1, pp [8] Ferri, A., et l., An Experimentl Technique for Mesuring High Solubility of Dyes in Supercriticl Crbon Dioxide, Journl of Supercriticl Fluids, 30 (2004), 1, pp [9] Ferri, A., et l., Dye Uptke nd Prtition Rtio of Disperse Dyes between PET Yrn nd Supercriticl Crbon Dioxide, Journl of Supercriticl Fluids, 37 (2006), 1, pp [10] Kim, T., et l., Solubility Mesurement nd Dyeing Performnce Evlution of Armid NOMEX Yrn by Dispersed Dyes in Supercriticl Crbon Dioxide, Industril & Engineering Chemistry Reserch, 45 (2006),10, pp [11] Mishim, K., et l., Mesurement nd Correltion of Azo Dyes nd Anthrquinone Solubility in Supercriticl Crbon Dioxide, Fluid Phse Equilibri, 194 (2002), 1, pp Pper submitted: Februry 6, 2015 Pper revised: Mrch 18, 2015 Pper ccepted: April 20, 2015

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