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Standard Potential of the Silver-Silver-Chloride Electrode from 0° to 95° C and the Thermodynamic Properties of Dilute Hydrochloric Acid Solutions

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Standard Potential of the Silver-Silver-Chloride Electrode from 0° to 95° C and the Thermodynamic Properties of Dilute Hydrochloric Acid Solutions Journal of Research of the National Bureau of Standards Vol. 53, No.5, November 1954 Research Paper 2546 Standard Potential of the Silver-Silver-Chloride Electrode from 0° to 95° C and the Thermodynamic Properties of Dilute Hydrochloric Acid Solutions Roger G . Bates and Vincent E. Bower From electromotive-force measurements of the cell withou t liquid junction: Pt; H 2, HCI (m), AgCI; Ag thro~l gh the range 0° to 95° C, calculations have been made of (1) t he standard potential of the s Ilver-silver-chloride electrode, (2) the activity coefficient of hydrochloric acid in aqueous solutIOns from m (molality) = 0 t.o m ~ O .l and from 0° to 90° C, (3) the relative partial molal hcat content of hydrochIol'lc aCId , and (4) the relatIve partial molal heat capacity of hydrochloric acid. The extrapolati?ns were made by the method of least squares with the a id of punch-card techl1lqu es . Data from at least 24 cells were analyzed at eaeh temperature and 81 cells were studied at 25 ° C. The value of the standard potential was [ound to be 0.22234 absolute volt at 25° C, and t he standard deviation was 0.02 millivolt at 0° C 0.01 milli volt at 25° C and 0.09 millivolt at 95° C. The resul ts from 0° to 60° C are compared with earlier d ete rll1ina~ t lOns of the sta ndard potential and other quantities derived from the electromotive force. 1. Introduction cells tudied ranged from 24 at 45° 0 and 55° 0 to 80 at 60° 0 and 81 at 25° O. The equations used The silvel'- silver-chloride electrode is employed for extrapolation were obtained by the method of extensively in the dctermination of ionization con­ least squares. Punchcard techniques aided in the stants and other thermodynamic data by the electro­ calculatiol1. motive-force method [1].1 It is therefore important that the standard potential of this electrode be 2 . Experimental Procedures known as accurately as possible over a wide range of tempcrature. Hydrochloric acid of reagent grade was distilled Electromotive-force measmemen Ls of cell A in .an all-gla s still ; the middle fraction (about two­ thu'ds) of the distillate wa collected andl'edistilled. Pt; Hi (g, 1 atm ), HCl (m) , AgOl; Ag, (A ) The middle fraction of the distillate from the second distillation was diluted, a needed, with water to at value of m suffi cien tly low to be useful in deter­ about .O.~ m ~nd was s~andard iz ed gravimetrically mining the tandard potential by extrapolation to by wmghmg SlIver chlonde. Test of the undiluted zero molality have been made by a number of acid revealed no bromide [18]. One of th e three investigators [2 to 16]. 2 The measurements of Glin­ O.l-m stock solutions was tandardized three time telberg were made at 20 ° 0, and all of the other over a period of 8 months ; the concentration ap­ investigations, except that of Harned and Ehlers peared to have changed only 0.02 percent in tbat which covered the range 0° to 60° 0, were confined time. to 25 ° O. R ecently, Harned and Paxton [17] have The cell solutions were prepared as needed by calculated the standard potential for the range 0° diluting portions of the stock solutions with water to 50 ° 0 from the electromotive force of cells of that had a conductivity of about 0.8 X 10- 6 ohm- 1 type A containing aqueous mixtures of hydrochloric cm- 1 at room temperature. Dissolved air was re­ acid and stron tium chloridc. In connection wi th moved from most of the solutions by bubbling the establishment of pH standards, the standard mtrogen; the rest of the solutions were saturated potential was n eeded in the range 60° to 95° O. In with hydrogen or boiled under vacuum. When the view of the extensive use of this electrode in electro­ latter procedure was used, the weight of the solution chemical studies, it was deemed desirable to redeter­ was determined after boiling so that the final con­ mine the standard potential at lower temperatures centratiol?- could be calculated accurately. The as well. elec.trolytlC hydrogen, obtained in cylinders, was pUrIfied by passage over a platinum catalyst at The measurements reported here were made at 17 room temperature and then over copper at 500° C. temperatures from 0° to 95 ° 0 and were limited to .Each of the cells, described elsewhere [19], con­ molalities between 0.001 and 0.12. The number of tamed two hydrogen electrodes and two silver­ 1 Figures in brackets indicate the literatlUc references at the end of this paper. silver-chloride electrodes. The latter were of the ' T he calculation of the standard poten Ual from the data of Ham cd and Ehlcrs thermal-electrolytic type [2 , 20]. The silver oxide has been exa mined by Hamcd and Wright flO]. Prentiss and Scatchard [11) Hamel', Bunoll, and Acroe [12). Hills and I ves [13). and Swinehart [14). ' from which theYa:were prepared was wa hecl40 times 283 with distilled water. The ] -1\1£ hydrochloric acid in used in this work, h was about 40 mm. The cor ­ which they were chloridized was a distilled sample rection therefore amounts to 0.02 m v at 25° C, 0.03 free of bromide. The electrodes were prepared at mv at 6Co C, 0.( S mv at 90 ° C, and 0.] 6 mv at 95° C. least 24 hours before use. For the high-temperature Nevertheless, the corrections were not applied to the series (60° to 95° C), the cells were provided with electromotive-force da ta and standard poten tials extra hydrogen saturators eonsistin.g of three cham­ reported here, in order that these results could be bers, as described by Bates and Pinching [21 ). used directly in other studies where the average jet Two calibrated potentiometers were used. The dep th is about the same (namely, 4 em) as in this standards of electromotive force were a pair of satu­ inves tigation. The th ermodynamic constants for rated Weston cells maintained at a temperature hydrochloric acid solutions are unaff ected, as they near 36° C in a th ermostated box of th e type de­ depend upon the difference E - E O and its change scribed by Mueller and Stimson [22) . Three con­ with temperature. stant-temperature baths were employed ; water baths were used from 0° to 60 ° C and an oil bath from 60 ° to 95° C. The temperature was regulated to 'the 3 . Standard Potential of the Cell desired even temperature within the limits of ± 0.02 deg C from 25° to SO° C and ± 0.03 deg C from 0° From the equation for the electromotive force, E , to 20° C and above SO° C. T emperature measure­ of cell A one can write ments wer e made with a platinum r esistance ther­ mometer. The difference of temperature between th e oil bath and the solu tion in a cell immersed in the bath was found to be less th an 0.1 deg C at 90° C. where E O is the standard poten tial of th e cell, 'Y± is The cells from which the data for th e range 0° to the stoichiometric mean ionic molal activity co­ 60° C were obtained were measured initially at 25 ° C. effi cien t of hydrochloric acid, and the other symbols The constant-temperature water th ermostat was h ave their usual significance. H arned and Owen lowered to near 0° C overnigh t , and the measure­ [1, chap. ll) have shown that experimental activity ments from 0° to 30° C were made on th e second coeffi cien ts of uni-univalent strong electrolytes up day , fo llowed on th e third day by th e measure­ to 1 m can be expressed wi th high accuracy by an ments from 30° to 60 ° C. A final check of 34 of the equation of the form cells was made at 25° C. The average differen.ce between initial and final values was O.IS mv. The log 'Y± _ - _A_·V,-,'c_r;: +Cc+ (e xt.)-lO g (1 + 0.03604 m), final value was almost alwavs lower than th e initial I + Ba*, c value, and there was some" indication th at a con­ (2) siderable time was required for equilibrium to be establish ed after the rapid drop from the higher where c is the molar concentration, A and B are temperature. Seven of th e cells were measured constants of the D ebye-Hiickel theory, C is an ad­ only in th e range 25° to 60° C. The data for th e j us table parameter, and a * is the ion-size param eter, high range, 60 ° to 95 ° C, were obtained from a and (ext.) represents the total contribution of the separate group of cells immersed in an oil bath. extended terms in the D ebye-Hiickel theory. The initial measurements of th ese cells were made at 25 ° C or at 60 ° C, and the other temperatures ' 'V'hen m do E' S no t exceed 0. 1, c differs from were studied in ascending order. A final check at J mdo, wh ere dO is the density of pure water, b.\' 60° C was sometimes but not always made. less than 1 par t in 1,000. Substitution of mdo The electromotive-force values were corrected to a for c in eq (2) an d combination with eq (1 ) gives par tial pressure of hydrogen of 1 atm.
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