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H6 824 Viscosity & Apparent Molal Volume of Potassium Chloride in Acetone-. Dioxane- & Methyl Alcohol-Water

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H6 824 Viscosity & Apparent Molal Volume of Potassium Chloride in Acetone-. Dioxane- & Methyl Alcohol-Water INDIAN J. CHEM., VOL. 15A, SEPTEMBER 1977 been interpolated from the data8,9 reported in the 5. SMITH,B. C., THAKUR,L. & ROCH, D. P., Cherny Ind. literature assuming that the presence of uranyl (1965), 1787. 6. THAKUll,L., AHMAD,M. F. & PRASAD,R., Indian J. nitrate bis-alcohol will have no effect on the heat Chcm., 15A (1977), in press. of solution. /::"H6 thus estimated for methanol 7. STAVELF.YL, A. K., MAUKHAM,D. R. & JONES,M. R., and ethanol complexes, respectively, are 0·42 and .f. iuorg. nucl, Chem., 30 (1968), 231. 1·5 KJ mol'<. Hence /::"H, for U02(N03)2.2CHaOH(c) 8. LANGE,N. A., Handbook of chemistry, 11th cdn (McGraw Hill. ~;cw York), 1974, 9. and U02(N03)2.2C2H50H(c) are -80·8 and -60,6 9. VVAGMANN,D. D., EVANS,vV. H., HALOW,1., PARKER, KJ mol>, respectively. V. B., BAILEY,S. M. & SCHUMMR, . R., Selected values Standard heats of formation of uranyl nitrate bis- of chemical thermodynamic p·ropcrties, NBS Technical Note' 270-1, 1965, 107. alcohols - The heats of formation of the his-alcohol 10. Cox, J. D. & PILCHER,G., Thermochemistry of organic and compounds have been calculated from the relation (8). organometallic compounds (Academic Press, London), 1970, 200. ll.H,= 'E.ll.H/ (products)-'E.ll.Ht (reactants) ... (8) 11. SMITH,B. c., THAKUR,L. & WASSEF,M., Indian J. Chern., Therefore 7 (1969), 1157. 12. ASHCROFT,S. J. & MORTrMER,C. T., 'Thermochemistry of ll.H/UO.(N03) a- 2ROH (e) = ll.H/UO.(N03).(e) transition metal complexes (Academic Press, London). +2ll.Hj ROH(I)+ll.H ... (9) 1970, 414. 13. VDOVENKO,V. M., SI;GLOBOVA1., G. & SUGLOBOV& By computing /::"H; U02(N03)z(c) from Lange8 D.HYUK, Y. Y., Radiokhimiya, 5 (1963), 739. and /::"H; ROH(l) from Cox and Pilcher!", /::"H; U02(N03)2.2CH30H(c) and /::"H; U02(NOa)2.2C2H5- OH(c) come out to be -1935·4 and -1993·2 KJ Viscosity & Apparent Molal Volume of mol", respectively. Potassium Chloride in Acetone-. Dioxane- & The mean bond dissociation energy of uranium- oxygen (alcohol) bond has been calculated from Methyl Alcohol-Water Mixtures the following well-knowrr'! steps (10-14): N. C. DAS & P. B. DAS UO.(N03).(e) +2ROH(I) = UO.(N03).·2ROH(e); MI, (10) Department of Chemistry, S.C.S. College, Puri U02(N03h.2ROH(c) = U02(N03) a- 2ROH(g); su; (11) Received 13 December 1976; accepted 15 June 1977 UO.(N03)2(C)= U02(N031.(g); sn; (12) 2ROH(I)=2ROH(g); 2ll.Hv (13) The viscosity and apparent molal volume of potas- UO.(N03).(g) +2ROH(g) =UO.(N03).·2ROH(g); MI g (14) sium chloride in acetone-, dioxane- and methyl where /::"H; and /::"H; are the heats of sublimation alcohol-water rnixtures containing 10, 20, 30, 40 and of uranvl nitrate his-alcohol and uranyl nitrate, 50% (w/w) of the organic components have been respectively; /::"H", the heat of vaporization of the measured at 35° and the data analysed in terms of alcohol; and /::"Hr., is the gas-phase molecular Jones-Dole epuation. The values of the constants A dissociation energy. Whence, /::"Hg= /::"HI +/::"H;- and B of Jones-Dole equation and the apparent molal /::"H;-2I::,Hv• volume have been explained in terms of ion-ion and As pointed out earlier" the heats of sublimation ion-solvent interactions. data are assumed to be the same for uranyl nitrate and the bis-complexes. Hence I::,H , for the his- g ISCOSITY and apparent molal volume (~) of methanol and bis-ethanol are -155·6 and -145,8 V electrolyte solutions in aquo-organic solvents KJ mol+; and the uranium-oxygen (alcohol) bond- have been studied with a view to understand ing strength, E(O-U)=,-/::"H and 72·9 KJ g/2=77·8 the nature of ion-ion and ion-solvent interaction mol'<, respectively for methanol and ethanol respectivcly-"!'. The viscosity and apparent molal adducts, The values compare well with the alcohol volume of KCl in acetonc-, dioxane- and methyl and LlCl, bond strength-! in UCI .4ROH and with 4 alcohol-water mixtures containing 10, 20, 30, 40 the uranium-oxygen (water) bond strength reported and 50% of the organic solvent have now been, earlier12,la. The bond strengths in bis-a1cohol are measured at concentrations <O'lM at 35° ± 0.001 0. stronger than the uranium-water bond strengths KC1, acetone, dioxane and methyl alcohol used on account of the electron donating effect of the were of E. Merck; (extra pure) qualities. Puri- alkyl groups. It can be seen that the steric effect fication of the solvents and preparation of mixed due to long-chain ethyl group slightly opposes the solvents and solutions were carried out as reported positive inductive effect of the ethyl group producing earlier+'. The procedures for viscosity measurement a lower bond strength in his-ethanol. were the same as described by Prasad et al.13• The The authors thank the UGC, New Delhi, for density measurements were made by pyknometer contingent grant and the award of a JRF to one (50 ml) with buoyancy correction and the values of them (M.F.A.). are accurate up to 4 in 106• The concentration References range was from 0·1 to O·OOIM. The applicability of the jones-Dole equation- is 1. BAGNALL,K. W., The actinide elements (Elsevier, New York), 1969, 154. shown by the linear plot of Yj,-l/O versus O. The 2. COMYNS,A. E., cu«. ta«, 60 (1960), 125. values of the constants A and B, given by the 3. CORDFUNKEE., H. P., The chemistry of uranium (Elsevier, intercept and slope of the plots respectively are New York), 1969, 124. given in Table 1. The calculated B values are in 4. CHERNYAEV, 1. 1., Complex compounds of U1'anium, translated by Israel Program for Scientific Translations, acceptable agreement with those obtained from Jerusalem, 1966, 240. these plots. 824 NOTES TABLE 1 - A AND B VALUES FOR DIFFERENT TABLE 2 - SV AND <pO VALUES FOR DIFFERENT AQUO-ORGANIC SOLVENTS AQUO-ORGANIC SOLVENTS Organic A x103 B x102 Organic Sv solvent solvent (w/w.%) I II III I II III (wJw. %) I II III I II III 10 5·0 5·5 6·1 3·2 2·8 0·0 10 1·08 1·23 1·35 26·00 25·35 24-50 20 6·0 6·2 7·0 6·9 3·9 0'0 20 1·12 1·20 1·41 25·30 24·25 23·86 30 6'5 7·1 7·8 7·3 5·3 0·0 30 1·00 1·36 1·48 26·30 22·35 23'23 40 7'5 8·0 8·6 12·6 10·0 2·0 40 1·03 1-45 1·55 26·70 21·45 22'56 50 9·1 9·7 10·0 13·8 12·6 6·3 SO 1·19 1'51 1·63 25·50 20·75 21·20 The values of A (at 25°) and B (at 25°) are 0·0049 and The value of <po ill water at 25° is 26·81 (ref. 17). 0·009 respectively (ref. 17). I = acetone-water; II = dioxane-water and III = methyl I = acetone-water; II = dioxane-water and III = methyl alcohol-water. alcohol-water. organic mixtures containing 10% organic com- The different A values for different mixed solvents ponents were linear and the values of the limiting indicates its dependence on ionic interaction (Table apparent molal volume (<po) in acetone-water, 1). The values of A in different solvents follow dioxane-water and methyl alcohol-water mixtures the order: MeOH-H20 > dioxane-Hgo .» acetone- at different solvent compositions obtained from H20. It is also seen that the A values increase the extrapolation of the plot of <p versus Ct to zero with the increase in organic solvent in the solvent concentration are sumrnarised in Table 2 along with mixture. This may be attributed to the change the limiting slope (5v). The limiting experimental in the mobility of the ions with a change in the slope is positive suggesting electrostatic ion-ion dielectric constant of the medium. interaction. If the dielectric constant of the solvent H According to Stokes and Mills , the viscosity is not very high as in mixed solvent or if it is fairly of the dilute electrolyte solution incorporate that high as in water, and the ions are small, the electro- of the solvent plus the contribution from three other static ion-ion interaction will be appreciable and factors, viz. 'Y)E the viscosity increase due to the shape an ion will have strong influence On its neighbour and size of an ion; 'I)A the increase due to the align- if actual association does not occur. Ion association ment or orientation of the polar molecules by the ma y be expected in mixed solvents like acetone-Hjr), ionic field and TJD the decrease in viscosity due to dioxane-Hgt) and MeOH-H20 but in pure water the distortion ot the solvent structure by the ions. actual association is very unlikely at moderate con- In the present case the B values are always positive centrations. This effect coupled with ion-solvent except for MeOH-H20 mixtur:s (10. 20 and 30% interaction seems to be responsible for the positive and where it is zero, B values mcrease III the order slope in the <p versus Ct plots in these systems. acetone-Hjf) > dioxane-Hsf) > MeOH-H20. Potas- Also it can be noted from Table 2 that as the sium ion with greater crystal radii and smaller dielectric constant decreases with the increase in charge density would have a weak orie~ting effect organic solvent, the S; values also increase slightly.
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