Frank Druyts, Sébastien Caes, Wouter Van Renterghem and Peter Thomas

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Presentation transcript:

Carbon-14 release and speciation from carbon steel in highly alkaline conditions Frank Druyts, Sébastien Caes, Wouter Van Renterghem and Peter Thomas Belgian Nuclear Research Centre, SCK•CEN, Mol, Belgium E-mail: fdruyts@sckcen.be Introduction We investigated (i) the release of carbon-14 from carbon steel representative for the reactor pressure vessel (RPV) steel of Belgian nuclear power plants and (ii) the carbon-14 speciation in a cementitious environment under anaerobic conditions representative for the Belgian geological disposal concept, which involves placing the RPV steel in a concrete monolith. To achieve this, we designed static and accelerated corrosion tests, and we obtained irradiated reference material representative for the RPV steel at end-of-life conditions in the Belgian power plants. Objectives To perform metallographic analyses of unirradiated and irradiated material in order to investigate the influence of irradiation on the metallic structure of carbon steel To measure the corrosion rate of carbon steel in a highly alkaline environment To determine the speciation of released carbon species from carbon steel in a highly alkaline environment representative for geological disposal conditions Materials and methods Tests were performed on JRQ carbon steel* Main experimental techniques were: Cobalt-60 measurements to determine the corrosion rate Static corrosion tests to determine the corrosion rate and carbon-14 speciation with gas chromatography (GC) Accelerated corrosion tests (by imposing a pre-determined potential) to determine the carbon-14 speciation with GC Gas chromatograph: tailor-made Shimadzu GC-2010 Plus. The gas sample can be injected manually (1) or automatically (2). *JRQ steel is an internationally accepted reference material for RPV steels. JRQ is th IAEA designation for the ASTM A533 grade B class 1 steel. Electrochemical cell for accelerated testing Results Metallographic analysis Little influence of irradiation Mo2C and Fe3C type carbides are detected Only effect of irradiation: limited number of small dislocation loops Corrosion rates Cobalt-60 activity measurements: parabolic rate law, after one year 7 nm is dissolved GC: total dissolved carbon yields a corrosion rate of 68 to 117 nm/year Carbon-14 speciation Methane, carbon dioxide, ethane and ethene detected, leached from carbon steel Hydrogen gas detected as a result of anaerobic corrosion of carbon steel Bright field micrographs (A and B) of Mo2C carbides and EDS spectrum (C) proving the higher Mo concentration after irradiation. Linear fit of the released Cobalt-60 activity as a function of the square root of the elapsed time. Gas chromatograms obtained after the corrosion tests with JRQ carbon steel (duration 231 days) steel (duration 231 days) Conclusions Measurement of the Cobalt-60 release of JRQ carbon steel in pure portlandite water confirmed that the corrosion rate obeys a parabolic law. Gas chromatography revealed that during long-term static corrosion tests, hydrogen, methane, ethene, and ethane were produced. Acknowledgements: This research was conducted with the financial support of the European Commission and ONDRAF/NIRAS. SCK•CEN || Boeretang 200 || BE-2400 Mol || www.sckcen.be || info@sckcen.be || Posternr: