A mass spectrometry method for quantitative and kinetic analysis of gas release from nuclear materials and its application to helium desorption from UO₂and fission gas release from irradiated fuel

Abstract

(2014) A mass spectrometry method for quantitative and kinetic analysis of gas release from nuclear materials and its application to helium desorption from UO 2 and fission gas release from irradiated fuel, Journal A new system has been developed to determine absolute quantities of gas (mainly noble gases) released during thermal desorption in the range from 10 −12 to 10 −5 mol with a precision of few percent. The system is actually designed for simultaneous measurement of gaseous elements like He, Xe, Kr, thermally released from nuclear fuel samples and also allows the determination of the release kinetics as a function of time. This system, called Quantitative GAs MEasurement System (Q-GAMES), is based on the principle of collecting, purifying and spiking the sample gas in a "high-pressure" chamber, and continuous sampling of the gas for mass spectrometric analysis without sample depletion during the experiment. It is equipped with its own spike generator and with different gas purification systems. It is shown that this system fulfills the requirement to work with two existing very high-temperature gas desorption facilities for nuclear materials. This paper describes the Q-GAMES principle, the spiking system, its calibration, its operative mode, the different quantification techniques, as well as its technical data, in combination with some examples of typical application.

Colloquium: 100 years of mass spectrometry: Perspectives and future trends

“…Mass spectrometers are utilized in a wide range of applications in the chemical, electronics, food processing, petroleum, and pharmaceutical industries. They are routinely used to monitor nuclear facilities (Colle et al, 2014), detect environmental pollutants (Richardson, 2012), diagnose drug abuse (Ojanperä, Kolmonen, and Pelander, 2012), and monitor residual gas in vacuum systems (Sulzer et al, 2012). Mass spectrometers are deployed in environments as diverse as the ocean depths for identifying trace chemicals (Bell et al, 2007) and also in space for extra-terrestrial exploration (Petrie and Bohme, 2007;Hoffman, Chaney, and Hammack, 2008).…”

The dissolution of helium in La-doped UO2 as a surrogate of hypo-stoichiometric UO2

“…The released He gas was collected and quantitatively measured by Quantitative Gas Measurement System with its own mass spectrometer (Pfeiffer-vacuum qma 400 quadrupole mass spectrometer) by spiking a known quantity of helium gas. The details of the set-ups used can be found in ref [30,31].…”

“…Three different UO 2 samples, containing 6, 11, and 22 mol% lanthanum, respectively, were examined. Helium was introduced in the samples by the infusion technique, and its release rate as a function of annealing temperature and quantitative measurements were performed by Laser Knudsen Cell and Quantitative Gas Measurement Systems, respectively [30,31]. Characterization of the samples was performed by scanning electron microscopy (SEM) and transmission electron microscopy (TEM).…”

Properties of the high burnup structure in nuclear light water reactor fuel

“…In addition to the analyses of fission gas by EPMA and SIMS some thermal desorption analyses were performed using a Knudsen cell device 33 . Fig.…”

“…Based on the new model for the HBS formation as a function of temperature and burnup, a new model for the release from this structure under design basis accident conditions is being developed, which depends on the local temperature levels, the effective burnup and should account for any constraint effect. It relies on local experimental data obtained from HBS samples in a Knudsen Cell that is coupled with a mass spectrometer 33 , as well as on the basis of integral results observed in fuel rod segments. The internal gas pressure, especially after a reactivity insertion accident, is remarkably enhanced by the burst release of fission gas following the grain separation, and is generally correlated with the peak fuel enthalpy.…”