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Report/Internal Report | FZJ-2019-03205 |
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2019
Report No.: NTRD-MRWFD-2019- M3FT-19IN030102018
Abstract: The radiation chemistry of a series of hydrophilic DGAs (TEDGA, Me-TEDGA, Me2-TEDGA, and TPDGA) has been investigated under neutral pH, concentrated (5.0 M), aqueous nitrate solution conditions. A combination of steady-state gamma and time-resolved pulsed electron irradiation experiments, supported by advanced analytical techniques and multi-scale modeling calculations, have demonstrated that: (i) the investigated hydrophilic DGAs undergo first-order decay with an average dose constant of (3.48 ± 0.28) × 10–6 Gy–1; (ii) their degradation product distributions are similar to those under pure water conditions, except for the appearance of NOx adducts; and (iii) radiolysis is driven by hydroxyl and nitrate radical oxidation chemistry moderated by secondary degradation product scavenging reactions. Overall, the radiolysis of hydrophilic DGAs in 5.0 M nitrate solutions is significantly slower and less structurally sensitive than under pure water conditions, but similar to their lipophilic analogs. These findings are promising for the deployment of hydrophilic DGAs as actinide aqueous phase stripping and hold-back agents, due to the presence of nitrate in envisioned large-scale process conditions.
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