The Radiation Chemistry of Ionic Liquids and its Implications for their Use in Nuclear Fuel Processing

Wishart, James F.; Shkrob, Ilya A.

doi:10.1021/bk-2009-1030.ch008

Cited by 32 publications

(45 citation statements)

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“…Applications of ionic liquids (ILs) in spent nuclear fuel reprocessing, , energy storage, and other electrochemical processes warrant the necessity to investigate the primary redox active species produced upon radiolysis of these media. Further, understanding of the kinetics and reactivity of these transient species would provide an insight into the radiolytic impact and the stability of this class of liquids .…”

Section: Introductionmentioning

confidence: 99%

Pulse Radiolysis and Computational Studies on a Pyrrolidinium Dicyanamide Ionic Liquid: Detection of the Dimer Radical Anion

et al. 2018

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A pulse radiolysis study on pyrrolidinium cation based ionic liquids is presented herein. Time-resolved absorption spectra for 1-methyl-1-propylpyrrolidinium dicyanamide (DCA) at 500 ns after the electron pulse show broad absorption bands at wavelengths below 440 nm and at 640 nm. In pyrrolidinium bis(trifluoromethylsulfonyl)imide (NTf) and tris(perfluoroethyl)trifluorophosphate (FAP) ILs, the transient absorption below 440 nm is much weaker. The absorption at 500 ns, which increases with wavelength from 500 nm to beyond 800 nm, was assigned to the tail of the solvated electron NIR absorption spectrum, since it disappears in the presence of NO. In the DCA IL, the presence of a reducing species was confirmed by the formation of pyrene radical anion. The difference in the transient species in the case of the DCA IL compared to other two ILs should be due to the anion, with cations being similar. In pseudohalide ILs such as DCA, radicals are formed by direct hole trapping by the anion (X + h → X), followed by addition to the parent anion. Prediction of the UV/vis absorption spectra of the dimer radical anion by computational calculation supports the experimental results. The oxidizing efficiency of (DCA) and its reduction potential ( E) have been determined.

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Section: Introductionmentioning

confidence: 99%

Pulse Radiolysis and Computational Studies on a Pyrrolidinium Dicyanamide Ionic Liquid: Detection of the Dimer Radical Anion

et al. 2018

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“…[14][15][16][17] For example, ILs have been shown to protect an extractant (tributylphosphate) from radiolytic damage, whereas the standard kerosene solvent used in the PUREX process (to separate U and Pu) directs damage into the extractant. [18,19] However, under fuel recycling conditions ILs will be exposed to a wide variety of radioactive fission products that can induce chemical changes to the IL that will hamper the performance of the separation system. [20] Therefore, an understanding of the radiation effects on ILs is essential for their successful use in radiation filled environments.…”

Section: Introductionmentioning

confidence: 99%

Gamma and heavy ion radiolysis of ionic liquids: A comparative study

Dhiman

Goff

Runde

et al. 2014

Journal of Nuclear Materials

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A variety of imidazolium, quaternary ammonium, and phosphonium cation based ionic liquids were irradiated with -rays, 2-15 MeV protons and 5-20 MeV helium ions in order to examine their relative radiation stability and potential hazards for application in advanced nuclear fuel cycles. Molecular hydrogen production can be taken as an overall indicator of radiation stability, and was found to be considerably lower for the -irradiated aromatic imidazolium based compounds when compared to the other aliphatic based media. Increasing the length of the aliphatic side chain increases the H 2 yields for all the compounds examined. Little difference is found in the production of H 2 between the quaternary ammonium and phosphonium based ionic liquids with similar length side chains. Yields of H 2 increase substantially from rays to 5 MeV He ions for the imidazolium based ionic liquids, but little variation with radiation type is observed for the quaternary ammonium and phosphonium based ionic liquids. The imidazolium based ionic liquids show a darkening with increasing dose and the UV-visible spectra show an increase in absorption from 240 to 400 nm that is probably due to induced changes in the cation. FTIR spectra show little variation with radiolysis, which is consistent with the low H 2 yields. The formation of a new peak at 1658 cm-1 is attributable to the formation of acyclic disubstituted alkene bonds in the irradiated imidazolium based compounds.

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“…The particular reactivities of various classes of anions and cations will also be examined. To save space, some aspects of ionic liquid radiation chemistry are included here by reference to previous reviews. − …”

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Ionic Liquids and Ionizing Radiation: Reactivity of Highly Energetic Species

Wishart

2010

J. Phys. Chem. Lett.

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Due to their unique properties, ionic liquids present many opportunities for basic research on the interactions of radiation with materials under conditions not previously available. At the same time, there are practical applied reasons for characterizing, understanding, and being able to predict how ionicliquid-based devices and industrial-scale systems will perform under conditions of extreme reactivity, including radiation. This perspective discusses current issues in ionic liquid physical chemistry, provides a brief introduction to radiation chemistry, draws attention to some key findings in ionic liquid radiation chemistry, and identifies some current hot topics and new opportunities.

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The Radiation Chemistry of Ionic Liquids and its Implications for their Use in Nuclear Fuel Processing

Cited by 32 publications

References 0 publications

Pulse Radiolysis and Computational Studies on a Pyrrolidinium Dicyanamide Ionic Liquid: Detection of the Dimer Radical Anion

Pulse Radiolysis and Computational Studies on a Pyrrolidinium Dicyanamide Ionic Liquid: Detection of the Dimer Radical Anion

Gamma and heavy ion radiolysis of ionic liquids: A comparative study

Ionic Liquids and Ionizing Radiation: Reactivity of Highly Energetic Species

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