An experimental and computational look at the radiolytic degradation of TODGA and the effect on metal complexation

Abstract

Diglycolamide extractants, and in particular N,N,N’N’- tetraoctyl diglycolamide (TODGA), are currently under investigation for use in nuclear fuel reprocessing by liquid-liquid separations. Several processes, such as ARTIST, i-Sanex, and EURO-GANEX...

Effect of metal complexation on diglycolamide radiolysis: a comparison between ex situ gamma and in situ alpha irradiation

“…Overall, the identified radiolysis products are identical to the ones formed when irradiating DGA solutions without metallic ions with gamma rays. 23,27,28,33,37,39,41,42,45,46,59 As after gamma irradiation of TODGA solution without metallic ions, DPXIII has not been observed alone in the solution. It has, however, been observed complexed to Am (Table 5).…”

“…Fukui functions can be used to determine the likely sites for electrophilic, nucleophilic, or radical attack on a molecule 59,75,76 The Fukui function used is composed of 3 separate equations listed as follows:…”

“…alters the site for radical attack and leads to various distributions of degradation products depending on the experimental conditions. 59 TODGA is in a very different conformation when complexed to metal ions than when free in solution, so it is expected that the presence of metal will change TODGA stability and the degradation products formed.…”

Gamma radiolytic stability of the novel modified diglycolamide 2,2′-oxybis(N,N-didecylpropanamide) (mTDDGA) for grouped actinide extraction

“…Especially, the presence of nitric, the formation of aggregates, adducts and different conformers of the diglycolamide are of particular interest. 52 …”

“… 43 Also Kimberlin et al reported a slight protective effect of nitric acid. 52 For CMPO, nitric acid showed a strong protective effect. 49 …”