A Comparison of the<font>γ</font>-Radiolysis of TODGA and T(EH)DGA Using UHPLC-ESI-MS Analysis

Zarzana, Christopher A.; Groenewold, Gary S.; Mincher, Bruce J.; Mezyk, Stephen P.; Wilden, Andreas; Schmidt, H.; Modolo, Giuseppe; Wishart, James F.; Cook, Andrew R.

doi:10.1080/07366299.2015.1012885

Cited by 67 publications

(107 citation statements)

References 26 publications

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“…[16] However, no equivalent kinetics for CMPO have been reported, nor for any acid contacted ligand-containing solvents. Therefore in this study, the importance of the dodecane radical cation reaction with CMPO, and the impact of nitric acid contract with both CMPO and TODGA was elucidated by measurement of absolute second-order rate constants.…”

Section: Resultsmentioning

confidence: 99%

“…5. The non-acid (zero concentration) contact data point was taken from Zarzana et al [16], the acid-contacted measurements were performed in this study. Again the acid-contact data show minimal reactivity change, as observed for CMPO.…”

Section: Resultsmentioning

confidence: 99%

“…1), [14,15] and Zarzana et al reported the rate constant for the TODGA reaction with this species to be diffusion limited. [16] However, no corresponding work has been done for CMPO. Here we report the measurement of dodecane radical cation reactions with CMPO, both in the pure organic phase and when in contact with aqueous nitric acid.…”

Section: Introductionmentioning

confidence: 98%

“…[17,18] This protection was not observed for TODGA, indicating that an equivalent nitric acid complex was not formed in the organic phase. [16]. The goal of this work was to further investigate the chemistry involved in ligand degradation occurring in the organic phase due to the dodecane radical cation.…”

Section: Introductionmentioning

confidence: 99%

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The role of organic solvent radical cations in separations ligand degradation

Mezyk

Mincher

Dhiman

et al. 2015

J Radioanal Nucl Chem

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The dodecane radical cation reaction rate constant with CMPO was measured using ps electron pulse radiolysis/ absorption spectroscopy as k = (1.30 ± 0.11) 9 10 10 M -1 s -1 in dodecane/0.10 M CH 2 Cl 2 solution. No reactivity increase occurred when these solutions were pre-contacted with nitric acid, similar to the behavior observed for TODGA. To corroborate these kinetic data with steady-state radiolysis measurements, where acid pre-contacted CMPO showed significantly less degradation, it is proposed that the dodecane radical cation always reacts directly with TODGA, but for CMPO the charge-transfer occurs with the CMPOÁHNO 3 complex formed in the acid contacted solvent.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 98%

Section: Introductionmentioning

confidence: 99%

See 2 more Smart Citations

The role of organic solvent radical cations in separations ligand degradation

Mezyk

Mincher

Dhiman

et al. 2015

J Radioanal Nucl Chem

Self Cite

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show abstract

“…Earlier, the radiolytic stability of a number of extraction systems developed for both the group separation of An(III)/Ln(III) and their individual element's separation has been studied in details. [3][4][5][6][7] The classical experimental approach for testing of the radiation stability is an external gamma irradiation of organic extractant solutions, subsequent extraction experiments and determination of qualitative and quantitative composition of radiolysis products. However only few studies were performed on the theoretical predictions of irradiation effects and the most radiation-stable ligands.…”

Section: Introductionmentioning

confidence: 99%