Authors: Pietro Brazzale
Source: SPIRE - Sciences Po Institutional REpository (preprint, 2020-11-12)
Field: Materials Science — Materials Chemistry

Numerical and experimental study at the pilot scale of the hydrogen injection into liquid sodium by permeation through nickel membrane In the framework of the SFR (Sodium-cooled Fast Reactors), the management of tritium contamination in sodium circuits and the control of its release in atmosphere is fundamental. In order to capture and recover the tritium, it is necessary to maintain a certain amount of hydrogen dissolved in the liquid sodium stream. The hydrogen injection by permeation through nickel dense membranes has been proposed to provide a continuous hydrogen intake to liquid sodium stream, thus allowing the desired hydrogen concentration to be reached. Similar nickel-based membranes have been developed in the past for SFR (i.e. hydrogen-meters), but a lack of knowledge and applications is found for what concerns the hydrogen injection by permeation. In this study, an original permeator prototype has been designed and an experimental activity at pilot-scale has been carried out on an experimental sodium loop, under different operating conditions (temperature: 375°C-450°C; hydrogen supply partial pressures: 5 kPa-28 kPa). A dedicated measurement system, based on the gas chromatography on the retentate side, coupled to the hydrogen detection inside sodium (through a dedicated hydrogen-meter using mass spectrometry), has provided an accurate estimation of the hydrogen permeation flowrate. Tests are carried out for both a gas-vacuum and a gas-sodium configuration: in both cases, the global hydrogen permeation flowrate depends linearly on the square root of the hydrogen partial pressure in the feed side up to 20 kPa, thus demonstrating that the process in this range is limited by the hydrogen diffusion inside the nickel membrane. In particular, the presence of sodium in the permeate side does not affect significantly the whole mass transfer process. The results, compared to the permeation theoretical laws, provide an experimental permeability coefficient, specific to the prototype geometry and configuration. Comparison to values from the literature results for small nickel samples, showed that some metal-lattice phenomenon, probably linked to the membranes deformation by cold-working, could affect the hydrogen permeation in this study. In fact, slightly higher permeation coefficient with a lower activation energy is found here if compared to the literature. Finally, the experimental process has been successfully validated, thus demonstrating the feasibility of this application at the pilot-scale. An analytical 1D model has been set up with a multi-physics approach, in order to assess the radial hydrogen mass transfer in steady conditions over three physical domains, including gas, nickel and liquid sodium. It includes benchmark literature correlations for the convective mass transfer inside gas and sodium phase in tubular geometry, the Sieverts law for the H-Ni and H-Na equilibrium, coupled to the Richardson’s law for the hydrogen permeation through the nickel membrane, assumed to be diffusion-limited. CFD simulations, performed in a 2D axial-symmetric geometry with the software Comsol Multiphysics, have provided a better comprehension of the transport phenomena taking place and have confirmed the results of the straightforward 1D model under certain conditions, specific to the experimental prototype. Finally, the experimental results have shown a good agreement with the 1D model and CFD simulations in the whole temperature interval and up to a hydrogen partial pressure of 20 kPa. By resuming all the elements provided by this study, both at the experimental and numerical stage, a single equation law has been defined to describe the prototype performance and to enhance the industrial scale-up design activity Permeation ; Chemistry ; Sodium ; Nuclear chemistry ; Humanities ; Physical chemistry ; Membrane ; Art ; Organic chemistry Fusion materials and technologies ; Chemical Synthesis and Characterization