A technique for uranium and plutonium determination using coulometric potentiostatic facility UPK-19 for analysis of mixed-oxide fuel

Abstract

The content of uranium and plutonium is the main characteristic of mixed uranium-plutonium oxide fuel, which is strictly controlled and has a very narrow range of the permissible values. We focused on developing a technique for measuring mass fractions of uranium and plutonium by controlled potential coulometry using a coulometric unit UPK-19 in set with a R-40Kh potentiostat-galvanostat. Under conditions of sealed enclosures, a special design of the support stand which minimized the effect of fluctuations in ambient conditions on the signal stability was developed. Optimal conditions for coulometric determination of plutonium and uranium mass fractions were specified. The sulfuric acid solution with a molar concentration of 0.5 mol/dm3 was used as a medium. Lead ions were introduced into the background electrolyte to decrease the minimum voltage of hydrogen reduction to –190 mV. The addition of aluminum nitride reduced the effect of fluoride ions participating as a catalyst in dissolving MOX fuel samples, and the interfering effect of nitrite ions was eliminated by introducing a sulfamic acid solution into the cell. The total content of uranium and plutonium was determined by evaluation of the amount of electricity consumed at the stage of uranium and plutonium co-oxidation. Plutonium content was measured at the potentials, at which uranium remains in the stable state, which makes it possible to subtract the contribution of plutonium oxidation current from the total oxidation current. The error characteristics of the developed measurement technique were evaluated using the standard sample method and the real MOX fuel pellets. The error limits match the requirements set out in the specifications for MOX fuel. The technique for measuring mass fractions of uranium and plutonium in uranium-plutonium oxide nuclear fuel was certified. The relative measurement error of the mass fraction of plutonium and uranium was ±0.0070 and ±0.0095, respectively. The relative error of the ratio of the plutonium mass fraction to the sum of mass fractions of uranium and plutonium was ±0.0085.