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Limiting Conductivities of Univalent Cations and the Chloride Ion in H2O and D2O Under Hydrothermal Conditions

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Abstract

Frequency-dependent electrical conductivities of aqueous sodium chloride, potassium chloride, cesium chloride, potassium iodide and cesium iodide have been measured in both H2O and D2O between T = 298 and 598 K at p ~ 20 MPa at a ionic strength of ~10−3 mol·kg−1 using a high-precision flow-through AC electrical conductance instrument. Experimental values for the molar conductivity, Λ, of each electrolyte were used to calculate their molar conductivities at infinite dilution, Λ°, with the Fuoss–Hsia–Fernández-Prini conductivity model. Single-ion limiting conductivities for the chloride ion in H2O, λ°(Cl−), were derived from Λ° by extrapolating literature values for the transference number of Cl−, t°(Cl−), in aqueous solutions of KCl and NaCl from ~400 and ~390 K up to the experimental conditions. Values for λ°(Cl−) in D2O were determined from literature values of t°(Cl−) for KCl in D2O near ambient conditions, assuming the same temperature dependence as in H2O. The results were used to calculate values for the single ion limiting conductivities λ°(Na+), λ°(K+), λ°(Cs+), λ°(Cl−), and λ°(I−) in both light and heavy water. The values of λ° in D2O are the first to be reported at temperatures above 338 K. The temperature dependence of the isotopic Walden product ratio, \( (\lambda^\circ \eta )_{{{\text{D}}_{2} {\text{O}}}} /(\lambda {^\circ }\eta )_{{{\text{H}}_{2} {\text{O}}}} \), indicates that differences in the hydration of Cl−, K+ and Cs+ ions between light and heavy water at ambient conditions associated with hydrogen-bonding, the so-called “structure breaking” effects, largely disappear at temperatures above ~400 K. The value of \( (\lambda^\circ \eta )_{{{\text{D}}_{2} {\text{O}}}} /(\lambda {^\circ }\eta )_{{{\text{H}}_{2} {\text{O}}}} \) for the “structure making” ion Na+ rises from 0.98 at 298.15 K to ~1.04 ± 0.02 at temperatures above ~375 K and remains approximately constant up to 600 K.

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Acknowledgments

The authors express their deep gratitude to Prof. Robert H. Wood, University of Delaware, for donating the AC conductance cell to the Hydrothermal Chemistry Laboratory at the University of Guelph. We are grateful to both Professor Wood and Professor Greg Zimmerman for providing us with the benefit of their extensive operating experience, and for many fruitful discussions. We also thank Mr. Ian Renaud and Mr. Casey Gielen of the electronics shop and machine shop in the College of Physical and Engineering Science at the University of Guelph for their very considerable expertise in maintaining and modifying the instrument and its data acquisition system. This research was supported by the Natural Science and Engineering Research Council of Canada (NSERC), Ontario Power Generation Ltd. (OPG), and the University Network of Excellence in Nuclear Engineering (UNENE). Technical advice and encouragement were provided by Dr. Dave Guzonas, Atomic Energy of Canada Ltd.; Dr. Dave Evans, Ontario Power Generation Ltd.; and Dr. Mike Upton, Bruce Power Ltd.

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  1. Department of Chemistry, University of Guelph, Guelph, ON, N1G 2W1, Canada

    J. Plumridge, H. Arcis & P. R. Tremaine

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Plumridge, J., Arcis, H. & Tremaine, P.R. Limiting Conductivities of Univalent Cations and the Chloride Ion in H2O and D2O Under Hydrothermal Conditions. J Solution Chem 44, 1062–1089 (2015). https://doi.org/10.1007/s10953-014-0281-1

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