Research Journal of Chemical Sciences ______________________________________________ ISSN 2231-606X Vol. 4(3), 45-53, March (2014) Res. J. Chem. Sci. International Science Congress Association 45 Study of Molecular Interaction in Binary Mixture of Dimethyl Acetamide with Diethyl ether using Ultrasonic and Viscosity Probes Dash Ashok Kumar and Paikaray Rita2 Department of Physics, L.N. College, Patkura, Kendrapara, Odisha, INDIA Department of Physics, Ravenshaw University Cuttack, Odisha, INDIA Available online at: www.isca.in, www.isca.me Received 27th January 2014, revised 11th February 2014, accepted 17th March 2014Abstract The ultrasonic velocity (U), density () and coefficient of viscosity () of binary mixture of dimethyl acetamide (DAMC) and diethyl ether at temperature 308K have been measured at different frequencies (2MH, 4MHz 6MHZ and 8MH). Adiabatic compressibility (K), intermolecular free length (L), free volume (V), internal pressure () and their respective excess values have been computed for entire range of concentration and are interpreted to explain molecular interaction occurring in the liquid mixture. Relaxation time (), excess enthalpy (H) and absorption coefficient (/f) have been calculated and discussed. Key words: Internal pressure, relaxation time, excess enthalpy and absorption coefficient. Introduction The acoustical study of liquids plays an important role to understand the nature and strength of molecular interactions. Ultrasonic velocities have been adequately employed in order to explain the nature of molecular interaction in pure liquids, binary and ternary mixture1-10. The investigation regarding the study of molecular interaction in binary liquid mixture with dimethyl acetamide (DMAC) and diethyl ether as the components is of particular interest, becauce DMAC is a dipolar aprotic solvent with high boiling point and having good thermal and chemical stability. It has large dipole moment and dielectric constant (µ = 3.7 D and € = 37.8). It is used in industry and medicine. It is also used as solvent for the production of acrylic fibres, elasthane fibres, polymide resins and various pharmaceuticals. It is an excellent proton donor as well as proton acceptor and hence it is strongly associated through intermolecular hydrogen bond. It is highly soluble in a variety of polar and nonpolar solvents and readily suitable to explore solute solvent interactions. Diethyl ether is a non-polar solvent. It has small dipole moment and dielectric constant (µ = 1.15 D and € = 4.34 ). It is used in the production of cellulose plastics. An attempt has been taken to explain the molecular interaction in binary mixture of dimethyl acetamide (DMAC) and diethyl ether at different frequencies at 308K. Departure from linearity in the acoustical parameters versus mole fraction in binary mixture of DMAC is considered as an indication of the presence of molecular interaction between different liquid molecules11-20. The physiochemical properties of binary mixture is studied by nonlinear variation of ultrasonic velocity and other acoustical parameters with structural changes occurring in a liquid and the liquid mixture. Theory: Using the measured data the acoustical parameters such as adiabatic compressibility (K) intermolecular free length (L), free volume (V) and internal pressure () have been calculated from the following equations. = (U-1 (1) = k (K1/2 (2)f = (MU/K3/2 (3) = bRT(K/U)1/2( 2/3/M7/6) (4) Where k, M and R are temperature dependent constant, effective molecular weight and universal gas constant respectively. K is a temperature independent constant equal to 4.28 × 10 where as b is the cubic packing factor equal to 2 for all liquid mixtures. Excess values of the above acoustical parameters have been calculated from the following relations. = Aexp – (X + X) (5) Where X1, and X are mole fractions of DMAC and diethyl ether respectively and A is any acoustical parameter. Relaxation time(),excess enthalpy(H) and absorption coefficient(/f), have been calculated from the following relations. = (4/3) K (6) =(X1 i1 Vm1 + X2 i2m2) - (7) /f = 2/U (8) Material and Methods Liquid mixtures of various concentrations in mole fraction were prepared by taking chemicals of analytical reagent(AR) and Research Journal of Chemical Sciences ___________________________________________________________ ISSN 2231-606XVol. 4(3), 45-53, March (2014) Res. J. Chem. Sci. International Science Congress Association 46 spectroscopic reagent(SR) grades with minimum assay of 99.9% (E-Merck Ltd, India) which were used as such without further purification. Liquid mixture of different mole fractions were prepared on concentration scale with a precision 0.0001g using an electronic digital balance. The density of liquid mixture was determined by a specific gravity bottle of 10ml capacity. The specific gravity bottle with the liquid mixture was immersed in a temperature controlled water bath. The density was determined using the relation. 2 = (/w1) 1 (9) Where w1, w, and 2 are mass of distilled water, mass of liquid mixture, density of distilled water and density ofliquid mixture respectively. The coefficient of viscosity () of pure liquids and liquid mixture was determined by an Ostwald’s viscometer calibrated with distilled water. The Ostwald’s viscometer containing the liquid was immersed in a temperature controlled water bath and the time of flow was measured by a Racer stop watch. The coefficient of viscosity was determined using the relation. 2 = ( 1 /t1) t (10) Where , , t, and t2 arecoefficient of viscosity of distilled water, coefficient of viscosity ofliquid mixture, time of flow of distilled water and time of flow of liquid mixture respectively. The velocity ofultrasonic waves in the binary liquid mixture was determined by using a multi frequency interferometer (Model M-82S) with a high degree of accuracy operating at different frequencies supplied by Mittal Enterprises, New Delhi. The measuring cell of the interferometer is a specially designed double walled vessel with provision to circulate water at constant temperature i.e.308K. The high frequency generator excites a quartz crystal fixed at the bottom of the vessel, at its resonant frequency. A fine micrometer screw at the top of the cell is used to raise or lower the reflector plate in the liquid through a known distance. The measuring cell is connected to the output terminals of the high frequency generator through a cable. Ultrasonic waves normal to quartz crystal are reflected from the reflector plate. Stationary waves are formed in the region between reflector plate and the quartz crystal. The micrometer is slowly moved till a number of maximum readings (N) of the anode current is passed. The total distance (d) moved by the micrometer is noted. The velocity ofultrasonic waves in the binary liquid mixture was determined using the relation. U = ƒ (11) Where = 2d/N = wavelength of the ultrasonic waves in the binary liquid mixture and ƒ is the frequency of the generator. Results and Discussion Density , coefficient of viscosity and ultrasonic velocity U increase with the increase in mole fraction of DMAC as shown in table-1 and in figure-1, figure-2 and figure-3 respectively. The increase in density with the increase in mole fraction of DMAC indicates that dipole-induced dipole interactions increases with the increase in concentration of DMAC in the liquid mixture. The increase in ultrasonic velocity at a particular frequency indicates the presence of dipole-induced dipole interactions in the liquid mixture. The increase in coefficient of viscosity with the increase in mole fraction of DMAC indicates the presence of solute-solvent interactions in the liquid mixture. DMAC is a polar molecule and when it is associated with nonpolar solvent diethyl ether, the diethyl ether molecule tends to break the DMAC- DMAC dipolar association and releases several DMAC dipoles. Free DMAC dipoles would induce moments in the neighboring diethyl ether molecules resulting dipole-induced dipole interactions in the liquid mixture. Consequently the binary liquid mixture has dipole-dipole interactions between DMAC molecules as well as dipole-induced dipole interactions between DMAC and diethyl ether molecules. This leads to contraction in volume and it causes decrease in adiabatic compressibility Ks and intermolecular free length L with the increasing molar concentration of DMAC which are depicted in table-2 and shown graphically in figures-4 and 5. Table-1 Values of density,coefficient of viscosity and ultrasonic velocity at 308K Mole Fraction of DMAC(X 1 ) Kgm-3 × 10-3 Nsm-2U ms - 1 2MHz 4MHz 6MHz 8MHz 0 693 0.279 928 912 904 880 0.219 743 0.346 1032 1024 1008 992 0.327 768 0.387 1094 1076 1068 1056 0.428 792 0.471 1152 1136 1116 1104 0.529 815 0.567 1198 1182 1160 1150 0.631 839 0.631 1252 1240 1224 1216 0.733 862 0.725 1296 1288 1272 1264 0.826 883 0.809 1356 1344 1332 1328 0.917 904 0.863 1416 1396 1386 1372 1 925 0.946 1488 1472 1464 1440 Research Journal of Chemical Sciences ___________________________________________________________ ISSN 2231-606XVol. 4(3), 45-53, March (2014) Res. J. Chem. Sci. International Science Congress Association 47 Figure-1 Variation of Versus X1 Figure-2 Variation of Versus X1 Figure-3 Variation of U Versus X1 Figure-4 Variation of K Versus X1 Table-3 and figure-6 show that the values of free volume Vf decrease with the increase in mole fraction of DMAC for a particular frequency. The decrease in free volume with the increase in mole fraction of DMAC is because of (i) contraction due to the free volume difference of unlike molecules. (ii) contraction due to the hydrogen bond formation between unlike molecules. (iii) specific interactions between unlike molecules in the binary liquid mixture. Table-2 Values of adiabatic compressibility and free length at 308K Mole Fraction of DMAC(X) ×10-10 m-1 ×10-10 m 2MHz 4MHz 6MHz 8MHz 2MHz 4MHz 6MHz 8MHz 0 16.756 17.3491 17.6575 18.6338 0.8195 0.8338 0.8412 0.8642 0.219 12.6372 12.8355 13.2462 13.6769 0.7116 0.7172 0.7286 0.7403 0.327 10.8794 11.2464 11.4155 11.6765 0.6603 0.6713 0.6688 0.6764 0.428 9.5141 9.784 10.1379 10.3594 0.6175 0.6262 0.6374 0.6443 0.529 8.5492 8.7822 9.1185 9.2778 0.5853 0.5932 0.6045 0.6097 0.631 7.6037 7.7516 7.9556 8.0606 0.552 0.5573 0.5646 0.5683 0.733 6.9068 6.9929 7.1699 7.261 0.5261 0.5294 0.536 0.5394 0.826 6.1591 6.2696 6.383 6.4216 0.4968 0.5012 0.5057 0.5073 0.917 5.517 5.6762 5.7584 5.8765 0.4702 0.4769 0.4804 0.4853 1 4.8826 4.9893 5.044 5.2135 0.4423 0.4471 0.4496 0.4571 Research Journal of Chemical Sciences ___________________________________________________________ ISSN 2231-606XVol. 4(3), 45-53, March (2014) Res. J. Chem. Sci. International Science Congress Association 48 Figure-5 Variation of L Versus X1 Figure-6 Variation of V Versus X1 Figure-7 Variation of Versus XTable-3 and figure-7 show that the values of internal pressure increase with the increase in mole fraction of DMAC for a particular frequency. The increase in internal pressure with the increase in mole fraction of DMAC indicates the increase in cohesive forces in the binary liquid mixture. With the increase of frequency from 2MHz, to 8MHz ultrasonic velocity decreases at a fixed concentration of DMAC. The decrease in ultrasonic velocity is perhaps due to the decrease in molecular interaction in the binary liquid mixture at higher frequencies. Consequently, the values of adiabatic compressibility, intermolecular free length and internal pressure increase but free volume decreases with the increase in frequency for a particular mole fraction of DMAC. Table-3 Values of free volume and internal pressure at 308KMole Fraction of DMAC(X 1 ) V f m 3 mol - 1  i ×10 4 Nm - 2 2MHz 4MHz 6MHz 8MHz 2MHz 4MHz 6MHz 8MHz 0 0.0138 0.0134 0.0132 0.0127 9.47 9.553 9.595 9.725 0.219 0.0124 0.0122 0.0119 0.0116 10.037 10.072 10.155 10.237 0.327 0.0117 0.0114 0.0113 0.0111 10.319 10.405 10.444 10.503 0.428 0.0097 0.0095 0.0092 0.0091 11.108 11.184 11.284 11.345 0.529 0.0079 0.0078 0.0076 0.0075 11.95 12.03 12.144 12.196 0.631 0.0074 0.0073 0.0071 0.0071 12.336 12.395 12.476 12.517 0.733 0.0065 0.0064 0.0063 0.0062 12.988 13.029 13.11 13.152 0.826 0.006 0.0059 0.0058 0.0058 13.404 13.463 13.524 13.544 0.917 0.0059 0.0058 0.0057 0.0057 13.541 13.637 13.686 13.756 1 0.0057 0.0056 0.0055 0.0054 13.826 13.901 13.939 14.055 Research Journal of Chemical Sciences ___________________________________________________________ ISSN 2231-606XVol. 4(3), 45-53, March (2014) Res. J. Chem. Sci. International Science Congress Association 49 Figure-8 Variation of Versus X1 Figure-9 Variation of UE Versus X1 Table-4, figure-8 and figure-9 show that the excess values of coefficient of viscosity and excess values of U are negative for the entire range of concentration of DMAC for all frequencies. The negative excess values of indicate the presence of dispersion, induction and dipolar forces21 and the negative excess values of U indicate the presence of dispersion interactions in the binary liquid mixture. It is evident from table-5, figure-10 and figure-11 that the values of excess adiabatic compressibility and excess free length are negative for the entire range of concentration of DMAC for frequencies 2MHz, 4MHz, 6MHz and 8MHz. The negative excess values of adiabatic compressibility (K) indicate the existence of strong interactions in the binary liquid mixture. It also indicates tightly packed molecules in the liquid mixture. The negative excess values of free length (L) predict the existence of strong interactions in the binary liquid mixture due to charge transfer, dipole-induced dipole, dipole-dipole interactions, interstitial accommodation and orientational ordering. Table-4 Excess values of coefficient of viscosity and velocity at 308K Mole Fraction of DMAC(X) × 10-3 Nsm-2 E ms - 1 2MHz 4MHz 6MHz 8MHz 0 0 0 0 0 0 0.219 -0.0787 -17.712 -9.728 -17.736 -9.76 0.327 -0.1093 -16.192 -18.208 -18.216 -6.24 0.428 -0.0932 -14.752 -14.768 -26.776 -14.8 0.529 -0.0645 -25.312 -25.328 -39.336 -25.36 0.631 -0.0686 -28.432 -24.448 -32.456 -16.48 0.733 -0.0426 -41.552 -33.568 -41.576 -25.6 0.826 -0.0206 -33.632 -29.648 -33.656 -13.68 0.917 -0.0273 -24.592 -28.608 -30.616 -20.69 1 0 0 0 0 0 Table-5 Excess values of adiabatic compressibility and free length at 308K Mole Fraction of DMAC(X 1 ) K s E ×10 - 10 m 2 N - 1 L f E ×10 - 10 m 2MHz 4MHz 6MHz 8MHz 2MHz 4MHz 6MHz 8MHz 0 0 0 0 0 0 0 0 0 0.219 - 1.5017 - 1.7894 - 1.6312 - 1.9992 - 0.0244 - 0.031 - 0.026 - 0.0338 0.327 - 1.9772 - 2.0437 - 2.3519 - 2.5502 - 0.035 - 0.0352 - 0.0359 - 0.0461 0.428 - 2.1433 - 2.2577 - 2.1033 - 2.5118 - 0.0397 - 0.0412 - 0.0353 - 0.0448 0.529 - 1.909 - 2.0112 - 1.8488 - 2.238 - 0.0338 - 0.0352 - 0.0287 - 0.0382 0.631 - 1.6434 - 1.7811 - 1.7251 - 2.0863 - 0.0286 - 0.0316 - 0.0286 - 0.0381 0.733 - 1.1292 - 1.2791 - 1.2242 - 1.517 - 0.016 - 0 .0201 - 0.0173 - 0.0255 0.826 - 0.7727 - 0.8529 - 0.838 - 1.1084 - 0.0103 - 0.0123 - 0.0112 - 0.0197 0.917 - 0.3343 - 0.3216 - 0.3148 - 0.4322 - 0.0025 - 0.0014 - 0.0008 - 0.0047 1 0 0 0 0 0 0 0 0 Research Journal of Chemical Sciences ___________________________________________________________ ISSN 2231-606XVol. 4(3), 45-53, March (2014) Res. J. Chem. Sci. International Science Congress Association 50 Figure-10 Variation of KE Versus XFigure-11 Variation of LE Versus XTable-6 and figure-12 show that the values of excess free volume V are positive between 0 to 0.327 mole fraction of DMAC and negative between 0.428 to 1 mole fraction of DMAC. The values of excess free volume are influenced by i. the specific interactions between the component molecules and weak physical forces like dipole-dipole or dipole-induced dipole interactions or vander Waal’s forces ii. The dispersive forces, steric hindrance of component molecules, unfavorable geometric fitting and electrostatic repulsion. The former effect leads to contraction of volume and the latter effect leads to expansion of volume. In the present investigation the positive values of V may be interpreted as the expansion of volume and the negative values of V may be interpreted as the contraction of volume of the binary liquid mixture of DMAC and diethyl ether. The positive values of VE at lower concentration of DMAC are favorable for the latter effect which accounts for the weak molecular interactions and the negative values of VE at higher concentration of DMAC are favorable for the former effect which accounts for the strong molecular interactions in the binary liquid mixture22. Figure-12 Variation of VE Versus XFigure-13 Variation of E Versus X1 Table-6 and figure-13 show that the values of excess internal pressure are negative within 0 to 0.428 mole fraction of DMAC and positive within 0.529 to 1 mole fraction of DMAC. The negative values of E at lower concentration of DMAC indicate the presence of dispersion and dipolar forces but the positive values of E at higher concentration of DMAC indicate the existence of strong interactions in the binary liquid mixture23. Tables-4, 5, and 6 show that the excess values of velocity, coefficient of viscosity, adiabatic compressibility, free length, free volume and internal pressure are changed with the increase in frequency due to the decrease in ultrasonic velocity in the binary liquid mixture. Research Journal of Chemical Sciences ___________________________________________________________ ISSN 2231-606XVol. 4(3), 45-53, March (2014) Res. J. Chem. Sci. International Science Congress Association 51 Table-7 and figure-14 show that the relaxation time varies nonlinearly with the increase in concentration of DMAC for a fixed frequency. The relaxation time increases with the increase in frequency for a fixed mole fraction DMAC. The relaxation time is in the order of 10-12s may be due to the structural relaxation process showing the existence of molecular interactions and in such a case it is suggested that the molecules are rearranged due to co-operative process. The values of excess enthalpy H are positive for 0 to 0.428 mole fraction of DMAC and negative for 0.529 to 1 mole fraction of DMAC for frequencies 2MHz, 4MHz ,6MHz and 8MHz as shown in Table-8 and Figure-15. The positive excess values of H at lower concentration of DMAC indicate the existence of dispersion interactions and the negative excess values of H at higher concentration of DMAC indicate the presence of strong interactions in the liquid mixture24. Table-6 Excess values of free volume and internal pressure at 308K Mole Fraction of DMAC(X 1 ) f E m 3 mol - 1  i E ×10 4 Nm - 2 2MHz 4MHz 6MHz 8MHz 2MHz 4MHz 6MHz 8MHz 0 0 0 0 0 0 0 0 0 0.219 0.00038 0.00052 0.0004 0.00051 -0.377 -0.423 -0.381 -0.426 0.327 0.00056 0.00056 0.00063 0.0008 -0.565 -0.56 -0.561 -0.628 0.428 -0.00062 -0.00055 -0.00069 -0.00046 -0.216 -0.22 -0.16 -0.223 0.529 -0.0016 -0.00146 -0.00151 -0.00133 0.185 0.186 0.26 0.19 0.631 -0.00128 -0.00116 -0.00123 -0.00098 0.126 0.107 0.149 0.069 0.733 -0.00135 -0.00127 -0.00124 -0.00114 0.334 0.298 0.34 0.262 0.826 -0.0011 -0.00104 -0.00103 -0.00086 0.345 0.328 0.35 0.252 0.917 -0.00046 -0.00043 -0.00043 -0.00029 0.086 0.106 0.117 0.07 1 0 0 0 0 0 0 0 0 Table-7 Values of relaxation time at 308K Mole Fraction of DMAC(X 1 ) ×10 - 12 s 2MHz 4MHz 6MHz 8MHz 0 0.623 0.645 0.656 0.693 0.219 0.582 0.591 0.61 0.63 0.327 0.52 0.551 0.575 0.602 0.428 0.597 0.614 0.636 0.65 0.529 0.646 0.663 0.689 0.701 0.631 0.639 0.652 0.669 0.677 0.733 0.667 0.675 0.692 0.701 0.826 0.664 0.676 0.688 0.692 0.917 0.634 0.652 0.662 0.676 1 0.615 0.629 0.636 0.657 Table-8 Values of excess enthalpy and absorption coefficient at 308K Mole Fraction of DMAC(X 1 ) E J mol - 1 /f 2 )×10 - 15 2MHz 4MHz 6MHz 8MHz 2MHz 4MHz 6MHz 8MHz 0 0 0 0 0 13.264 13.975 14.348 15.557 0.219 0.036 0.041 0.037 0.042 11.156 11.418 11.972 12.562 0.327 0.054 0.053 0.053 0.06 9.399 10.118 10.65 11.267 0.428 0.017 0.017 0.013 0.019 10.242 10.68 11.251 11.638 0.529 -0.023 -0.021 -0.028 -0.021 10.654 11.092 11.735 12.045 0.631 -0.015 -0.013 -0.017 -0.009 10.09 10.387 10.799 11.013 0.733 -0.035 -0.032 -0.036 -0.028 10.173 10.365 10.761 10.966 0.826 -0.037 -0.035 -0.037 -0.027 9.675 9.937 10.208 10.301 0.917 -0.01 -0.012 -0.013 -0.008 8.853 9.24 9.441 9.733 1 0 0 0 0 8.174 8.442 8.582 9.018 Research Journal of Chemical Sciences ___________________________________________________________ ISSN 2231-606XVol. 4(3), 45-53, March (2014) Res. J. Chem. Sci. International Science Congress Association 52 Figure-14 Variation of Versus X1 Figure -15 Variation of H Versus X1 Figure-16 Variation of /f Versus X1 Table-8 and figure-16 show that the values of absorption coefficient /f decrease non-linearly with the increase in mole fraction of DMAC for a fixed frequency indicating the increase in molecular interaction. The increase in absorption coefficient with the increase in frequency for a fixed concentration of DMAC indicates the reduction in molecular interaction in the binary liquid mixture25 at higher frequencies. Conclusion On the basis of the experimental values of density, ultrasonic velocity, related acoustical parameters and their excess values for the binary liquid mixture, it is concluded that there exists dipole-dipole, dipole-induced dipole and dispersion interactions in the binary liquid mixture of DMAC diethyl ether. Further, it is concluded that the molecular interaction increases with the increase in mole fraction of DMAC for a fixed frequency and decreases with the increase in frequency for a fixed concentration of DMAC in the binary mixture. 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