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CCXL1.- the Electrochemistry of Solutions in Acetone. Part I

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CCXL1.- the Electrochemistry of Solutions in Acetone. Part I View Article Online / Journal Homepage / Table of Contents for this issue 2 I38 ROSHDESTWENSKY AND LEWlS THE CCXL1.- The Electrochemistry of Solutions in Acetone. Part I. By ALEXANDERROSHDESTWENSEY and WILLIAM CUDMORE MCCULLAGHLEWIS. WHILSTa considerable amount of attention has been directed to the electrochemical behaviour of methyl and ethyl alcohols, rela- tively few measurements are recorded in the caw of solutions in acetone. The present paper contains the resulk of an investigation undertaken to supply to a certain extent this deficiency. The solutes employed were lithium nitrate and silver nitrate, the latter being examined in greater detail. Before giving our own meamrements, it is necessary to indicate briefly some of the results obtained by other observers which bear directly on the results obtained by us.* As regards the electrolysis of saturated silver nitrate solutions in acetone, Kahlenberg (J. physicd C‘Aem., 1900,4, 349) found that the metal was precipitated in a coherent form, but “the solution conducts so poorly ” that it was impossible to verify Faxaday’s law. In the same paper Kahlenberg gives some results of electromotive force measurements of Ag i AgNO, concentration cells in pyridine and acetonitrile respectively, with regard to which he concludes that the Nernst expressions are inapplicable. Kahlenberg asumes that the liquid/liquid potential difference is negligible, which, in the case of acetone at least, we shall show later is not the case. The specific conductivity of acetone itself has been meamred by Dutoit and Levier (J. Chim. phys., 1905, 3,435), the value obtained Published on 01 January 1911. Downloaded by Freie Universitaet Berlin 09/04/2018 17:53:03. being (2 - 0.48) x 10-7 mho at the ordinary temperature (using unplatinised platinum electrodes). H. C. Jones and C. A. Rouiller (Amer. Chem. J., 1906, 36, 427) obtained the value 1.0 x 10-6 at Oo, our own result being 6 x at 18O (using unplatinised elec- trodes t). As regads the molecular conductivity of sokutes at infinite dilution (A ) in acetone, considerable vagueness exists. Carrara (Zoc. cit.) states that A, for triethylsdphine iodide is 167 (it9 deter- mined by direct experiment). Walden (Zeitsch. physikal. Chem., 1906, 54, 222) found for tetraethylammonium iodide at 25O * For a general account of the electrochemistry of non-aqueous solutions, conqare Cerrara : ‘‘ Elektrochemie der nichtwassrigen Losungen,” Ahrens’ Samm- lung, 12 ; also Neustadt, Diss., Breslau, 1909. t These are preferable to ylatiiiised ones, as they eliminate the poasibility of catalytic reactions when the solvent is an organic snlc,tnnce. View Article Online ELECTROCHEMISTRY OF SOLUTIONS IN ACETONE. PART I. 2139 A, =225. Dutoit and Levier (Zoc. cit.) give the following values for some simple salts at 18O : Li . Na. K. NH,. Br ............... 155 158 155.5 157’5 I .............. 157 155 157-5 157’5 CNS ........... - 169 170.0 171.0 NO,* ............ 132 - - - * Benz, Diss., Lausnnne, 1905. From thae results Dutoit and Levier conclude that Kohlrausch’s law of the independent migration of the ions is valid for solutions in acetone. The same authors have applied Ostwald’s dilution law to some of the above salts, but find that the ‘I wnstant ” falls with increasing dilution. In conmxion with the question of transport numbers, Carrara (Zoc. cit.) draws the conclusion that in general there is a tendency on the part of each ion to reach a limiting value independent of the nature of the solvent. This scarcely seems to be borne out in the case of acetone, however. In the particular instance of silver nitrate, Jones and Rouiller (Zoc. cit.) state that the solubility of the salt in acetone is too slight to make a direct determination of the transport number, but that a value may be obtained by extra polation from results obtained in’ acetone-water mixtures, the acetone concentration rising from zero to 75 per cent. Naturally, the extrapolation is a rather large one, and Jones and Rouiller have only felt justified in giving the result as an inequality, namely, the transport number of NOd at 25O in acetone )0*62. Experiments with methyl alcohol-acetone mixtures also lead on extrapolation to a value for the transport number greater than 0.6. Published on 01 January 1911. Downloaded by Freie Universitaet Berlin 09/04/2018 17:53:03. EXPERIMENTAL. Kahlbaum’s acetone was twice distilled over metallic calcium, the middle fraction being kept in a glass bottle, from which moisture was carefully excluded by calcium chloride tubes. The most concentrated solution of silver nitrate conveniently prepared was O*O%N. The solvent and solutions were kept, and the measurements carried out in weak artificial light, as it was noticed that on exposure to sunlight a brown precipitate forms in the solutions. Under the conditions specified the solutions remain permanently homogeneous. I.--Conductivity Measurements. The usual Wheatstone bridge and telephone method was employed. The cell, from which moisture waa excluded, contained 7a2 View Article Online 2140 ROSHDESTWENSKY AND LEWIS : THE two large unplatinised platinum plates close together, the cell constant being small, namely, 0.09213. The measurements were made at 1S0, an oil-bath being employed as the resistances were in all cases fairly large. The following table contains the specific and molecular conductivities of silver nitrate. TABLEI. Concentration Specific conductivity A". in gram-mols./litre. (mhos) x lo5. Molecular conductivity. 0.02 14-37 7-19 0.01 10'17 10.17 0.007 7 -42 10 60 0.005 5-50 11'00 0.0035 3-97 11'34 0'002 2.51 12*54 0.001 1-46 14'62 0*0005 0.98 19.68 Our values at 18O are slightly lower than those of Laszczynski, and slightly higher than those of Jones and Rouiller (at 25O). The value of A, for silver nitrate cannot be obtained directly. The empirical expression A, q =constant (compare Walden, Zeitsch. physikd. Chem., 1906, 55, 207) independent of the solvent, q being the viscosity of the solvent, does not appear to hold for acetone; thus, on oomparing the viscosities of water and acetone, one finds that A, for silver nitrate in acetone= 371, a value which is certainly too great. Again, Kohlrausch's expression, A, = A - a 7~;where a is a constant and c the concentration, has found application in those cases in which hV is a linear function of 3;; although this condi- tion is approximately fulfilled in the present instance, the values for A, given by the formula vary from 45 to 78. Published on 01 January 1911. Downloaded by Freie Universitaet Berlin 09/04/2018 17:53:03. A moderate approximation may, however, be obtained in the following way : According to Laszczynski, A, for simple salts in Getone is 1.3 times that in water. For silver nitrate at 18O, X = 116, and hence in acetone h, = 151. This is not very different from the directly determined values for alkali bromides and iodides in acetone (ha =155-160, Dutoit and Levier), and since in water the A, for silver nitrate does not differ much from that of these salts, we have assumed that the same holds for wetone solution and have taken h ,for silver nitrate = 150. The conclusions which we draw from the results in which h is employed are not invalidated, even if a large percentage error (up to 30 per cent.) were involved in this quantity ; further, the majority of the electre motive force measurements given later are independent of A,. The following table contains the degrees of dissociation of silver nitrate in acetone, the Ostwald dilution law a2/(1- a)v, and the View Article Online ELECTHOCHEMISTRY OF SOLUTIONS IN ACETONE, PART I. 2141 empirical expressions a3i (1 - a)% and a2/(1- a) Jiof van't Hoff and RudoIphi respectively. TABLE11. Molar concen trrttion. a=A,/A,. Ostwald K. van't Hoff K. Rudolphi K. 0.02 0.048 0'04,48 0'0,244 0 '0,342 0 *01 0.068 50 362 496 0.007 0.070 37 27 7 442 0 ~~05 0.073 29 226 407 0-0035 0.075 21 173 360 0.002 0.084 15 141 345 O'OOi 0.097 14 102 329 0*0005 0.131 09 149 441 The Ostwald constant falls steadily as the dilution increases. The van't Hoff constant is also not very satisfactory, the most consistent values being given by Rudolphi's formula. It is thus apparent that silver nitrate in acetone behaves like a strong electrolyte in not obeying Ostwald's law, but at the same time the extent of the dissociation is that of a weak electrolyte (in water). This opens the question adsto what is the criterion to be employed to decide whether an electrolyte is " weak " or " strong." The conductivity of lithium nitrate in acetone (which is required in connexion with the E.M.F. measurements) was also determined, with the following result. TABLE111. Lithium iVit,.de in Acetone at 18O. Molar Specific concentration. cone. x lo3. Av. a = A,/&. Ostwald K. Rudolphi K. 0*343* 2.4 7.0 0.068 0 '02,101 0'0,176 0-1715 1.39 8-1 0.061 067 160 Published on 01 January 1911. Downloaded by Freie Universitaet Berlin 09/04/2018 17:53:03. 0.0858 0.82 9'54 0'072 048 - 0.0429 0.60 11.6 0.088 036 - 0,0214 0.31 14'5 0'110 029 0~0,200 0 *0107 0 -20 19'0 0.144 026 - 0.0053 0.13 24.5 0.186 022 - 0-0026 0.087 33-4 0.253 022 0 -0,430 0*0013 0.057 44 -0 0.333 022 - 0 '00065 0.037 57.0 0.432 021 0-0,840 0-00032 0-024 75.0 0.568 023 0-0120 Saturated.
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