Gamma Radiolysis of TODGA and CyMe4BTPhen in the Ionic Liquid Tri-n-Octylmethylammonium Nitrate

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Gamma Radiolysis of TODGA and CyMe4BTPhen in the Ionic Liquid Tri-n-Octylmethylammonium Nitrate. / Zsabka, Peter; Van Hecke, Karen; Wilden, Andreas; Modolo, Giuseppe; Hupert, Michelle; Jespers, Vincent; Voorspoels, Stefan; Verwerft, Marc; Binnemans, Koen; Cardinaels, Thomas.

In: Solvent extraction and ion exchange, 20.01.2020.

Research output: Contribution to journalArticle

Harvard

Zsabka, P, Van Hecke, K, Wilden, A, Modolo, G, Hupert, M, Jespers, V, Voorspoels, S, Verwerft, M, Binnemans, K & Cardinaels, T 2020, 'Gamma Radiolysis of TODGA and CyMe4BTPhen in the Ionic Liquid Tri-n-Octylmethylammonium Nitrate' Solvent extraction and ion exchange. DOI: 10.1080/07366299.2019.1710918

Vancouver

Zsabka P, Van Hecke K, Wilden A, Modolo G, Hupert M, Jespers V et al. Gamma Radiolysis of TODGA and CyMe4BTPhen in the Ionic Liquid Tri-n-Octylmethylammonium Nitrate. Solvent extraction and ion exchange. 2020 Jan 20. Available from, DOI: 10.1080/07366299.2019.1710918

Author

Zsabka, Peter; Van Hecke, Karen; Wilden, Andreas; Modolo, Giuseppe; Hupert, Michelle; Jespers, Vincent; Voorspoels, Stefan; Verwerft, Marc; Binnemans, Koen; Cardinaels, Thomas / Gamma Radiolysis of TODGA and CyMe4BTPhen in the Ionic Liquid Tri-n-Octylmethylammonium Nitrate.

In: Solvent extraction and ion exchange, 20.01.2020.

Research output: Contribution to journalArticle

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@article{2ca7d1eb14f3468db5b1d7587f040761,
title = "Gamma Radiolysis of TODGA and CyMe4BTPhen in the Ionic Liquid Tri-n-Octylmethylammonium Nitrate",
keywords = "Solvent extraction, TODGA, CyMe4BTPhen, gamma radiolysis, ionic liquids, HPLC-ESI-MS",
author = "Peter Zsabka and {Van Hecke}, Karen and Andreas Wilden and Giuseppe Modolo and Michelle Hupert and Vincent Jespers and Stefan Voorspoels and Marc Verwerft and Koen Binnemans and Thomas Cardinaels",
note = "Score=10",
year = "2020",
month = "1",
doi = "10.1080/07366299.2019.1710918",
journal = "Solvent extraction and ion exchange",
issn = "1532-2262",
publisher = "Taylor & Francis (CRC)",

}

RIS - Download

TY - JOUR

T1 - Gamma Radiolysis of TODGA and CyMe4BTPhen in the Ionic Liquid Tri-n-Octylmethylammonium Nitrate

AU - Zsabka,Peter

AU - Van Hecke,Karen

AU - Wilden,Andreas

AU - Modolo,Giuseppe

AU - Hupert,Michelle

AU - Jespers,Vincent

AU - Voorspoels,Stefan

AU - Verwerft,Marc

AU - Binnemans,Koen

AU - Cardinaels,Thomas

N1 - Score=10

PY - 2020/1/20

Y1 - 2020/1/20

N2 - Radiolytic stability of the extractants N,N,N’,N’-tetraoctyl diglycolamide (TODGA) and 2,9-bis(5,5,8,8-tetramethyl-5,6,7,8-tetrahydro-1,2,4-benzotriazin-3-yl)-1,10-phenanthroline (CyMe4BTPhen) in the ionic liquid tri-n-octylmethylammonium nitrate ([N1888][NO3]) was studied via the combination of a steady-state irradiation by cobalt-60 gamma-radiation, followed by solvent extraction and identification of radiolysis products by High-Performance Liquid Chromatography coupled to Electro Spray Ionisation Mass Spectrometry (HPLC-ESI-MS). The observed trend for the distribution ratios of trivalent minor actinides and Eu(III) showed a decrease as a function of absorbed dose in the case of the TODGA solvent. The gamma irradiations were conducted in the presence or absence of an acidic aqueous phase. The determined dose constants for TODGA under neutral or acidic conditions were up to four times lower than the values reported in aliphatic diluents under comparable conditions. The degradation patterns were similar to those found by former studies on TODGA diluted in n-dodecane; only de-alkylation and bond ruptures within the diglycolamide core were observed. The presence of an acidic aqueous phase during irradiation resulted in a different relative abundance of certain radiolysis products of both the diluent and TODGA and a higher dose constant compared to the neutral irradiation conditions. A quantification of CyMe4BTPhen in irradiated samples with the [N1888][NO3] diluent was not possible, but the effect on its extraction properties was evaluated. The distribution ratios slightly increased under the effect of absorbed dose, indicating the formation of radiolysis products that are efficient extractants as well.

AB - Radiolytic stability of the extractants N,N,N’,N’-tetraoctyl diglycolamide (TODGA) and 2,9-bis(5,5,8,8-tetramethyl-5,6,7,8-tetrahydro-1,2,4-benzotriazin-3-yl)-1,10-phenanthroline (CyMe4BTPhen) in the ionic liquid tri-n-octylmethylammonium nitrate ([N1888][NO3]) was studied via the combination of a steady-state irradiation by cobalt-60 gamma-radiation, followed by solvent extraction and identification of radiolysis products by High-Performance Liquid Chromatography coupled to Electro Spray Ionisation Mass Spectrometry (HPLC-ESI-MS). The observed trend for the distribution ratios of trivalent minor actinides and Eu(III) showed a decrease as a function of absorbed dose in the case of the TODGA solvent. The gamma irradiations were conducted in the presence or absence of an acidic aqueous phase. The determined dose constants for TODGA under neutral or acidic conditions were up to four times lower than the values reported in aliphatic diluents under comparable conditions. The degradation patterns were similar to those found by former studies on TODGA diluted in n-dodecane; only de-alkylation and bond ruptures within the diglycolamide core were observed. The presence of an acidic aqueous phase during irradiation resulted in a different relative abundance of certain radiolysis products of both the diluent and TODGA and a higher dose constant compared to the neutral irradiation conditions. A quantification of CyMe4BTPhen in irradiated samples with the [N1888][NO3] diluent was not possible, but the effect on its extraction properties was evaluated. The distribution ratios slightly increased under the effect of absorbed dose, indicating the formation of radiolysis products that are efficient extractants as well.

KW - Solvent extraction, TODGA, CyMe4BTPhen, gamma radiolysis, ionic liquids, HPLC-ESI-MS

UR - https://ecm.sckcen.be/OTCS/llisapi.dll/overview/36869727

U2 - 10.1080/07366299.2019.1710918

DO - 10.1080/07366299.2019.1710918

M3 - Article

JO - Solvent extraction and ion exchange

T2 - Solvent extraction and ion exchange

JF - Solvent extraction and ion exchange

SN - 1532-2262

ER -

ID: 5956166