Determination of ultra-low concentrations of gaseous 14C-bearing hydrocarbons produced during corrosion of irradiated steel using accelerator mass spectrometry

Guillemot, T.; Salazar, G.; Cvetković, B. Z.; Kunz, D.; Szidat, S.; Wieland, E. (2020). Determination of ultra-low concentrations of gaseous 14C-bearing hydrocarbons produced during corrosion of irradiated steel using accelerator mass spectrometry. Analyst, 145(24), pp. 7870-7883. Royal Society of Chemistry 10.1039/d0an01517b

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Compound-specific radiocarbon analysis (CSRA) was developed to identify and quantify gaseous 14Cbearing carbon compounds at the pico- to femtomolar concentration range and employed in a corrosion experiment with small specimens of irradiated steel. The approach is based on gas chromatographic separation of single 14C-bearing carbon compounds, their oxidation to 14CO2, sampling with a custom-made fraction collector and quantification by accelerator mass spectrometry (AMS). In addition to CSRA, a method allowing the quantification of the total 14C content of the gas phase was developed and tested. After validation of the two set-ups with standards, the gaseous 14C-bearing carbon compounds produced during alkaline anoxic corrosion of irradiated steel were quantified. Small hydrocarbons (HCs) like methane (14CH4) and ethane (14C2H6) were the only 14C-bearing compounds identified in the gas phase above the detection limit. 14CH4 was the main species (on average 5.4 × 10−14 mol L−1 gas) and contributed >90% to the total 14C content, whereas the concentration of 14C2H6 was much lower (7.9 × 10−16 mol L−1 gas). To our knowledge, this is the first study reporting CSRA of gaseous 14C-bearing HCs produced during anoxic corrosion of irradiated metallic radioactive waste at ultra-low concentrations.

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