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Spectroscopie Infrarouge et Rayonnements Ionisants – SPIRIT

Submission summary

Despite its utility (nuclear industry, medicine...), radiation chemistry is still a science facing challenges that are relevant to fundamental science. Our project is dedicated to the introduction of vibrational spectroscopy in this field because this technique is an efficient probe of the nature of chemical bonds. We have recently carried out the first coupling between our 10 MeV linear accelerator and a FT-IR spectrometer. This coupling made it possible to obtain information on chemical reactions induced by ionizing radiations. However, in this setup, the sample must be thin enough (in the 1-100 µm range) to transmit infrared light. With such thinness, only a small fraction of the initial electron energy (0.1%) is used to induced chemical reactions. Therefore, it would be tremendously advantageous to perform similar experiments with less energetic electrons. 60 keV electrons would have in water or organic materials a maximum penetrating range of about 30 µm, which is sufficient for all IR experiments. We propose to develop a coupling between a 60 keV electron gun (having a pulsed structure) and an infrared detection. This will enable us to get kinetics in a time scale ranging from microseconds to minutes. Systems of interest deal first with organometallic complexes. The experimental setup will enable us to characterize the reactivity of these complexes after irradiation. Moreover, in collaboration with our partners from CEA/Marcoule, we are interested in the behaviour of ionic liquids under irradiation. Although ionic liquids are known to be quite stable towards irradiation, their strong infrared bands will enable us to understand their degradation pathways, for example by detecting carbenes which are postulated in the alkylimidazolium radiolysis. Last, the search for complexant molecules which specifically bind actinides and separate them from other cations (lanthanides) is a challenge in the context of nuclear waster separation and also from a fundamental point of view. It is therefore of interest to perform time-resolved experiments to track the reaction mechanisms. We will focus our attention on phosphates (especially tributylphosphate) and on malonamides, these latter molecules being used in the DIAMEX process. Last, calculations will be performed in order to identify species (especially reaction intermediates) formed under irradiation thanks to their vibrational signatures.

Project coordinator

The author of this summary is the project coordinator, who is responsible for the content of this summary. The ANR declines any responsibility as for its contents.


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Beginning and duration of the scientific project: - 0 Months

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