Oxidation and/or reduction of manganese species by γ-ray and He2+ particle irradiation in highly concentrated carbonate media

Ghalei, Mohammad; Vandenborre, Johan; Blain, Guillaume; Haddad, Férid; Mostafavi, Mehran; Fattahi, Massoud

doi:10.1016/j.radphyschem.2015.10.009

Cited by 5 publications

(5 citation statements)

References 30 publications

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“…The presence of radionuclides in the waste container induces radiations due to their radioactive disintegration. Moreover, numerous studies have dealt with the radiation chemistry effects on carbonate ions solutions. − The first step of the degradation of carbonate ions leads to the formation of two radicals ,,,− (CO 2 –• and CO 3 –• ) either by direct effect of the ionizing radiation or by the reaction of carbonate ions with the species formed by water radiolysis (e aq – , H • , OH • , H 2 , and H 2 O 2 ). Then, recombination reactions occur between these radicals (eq ), or between these radical and molecular species (eq ) or radical products of water radiolysis (eq ).…”

Section: Introductionmentioning

confidence: 99%

Radiolytic Dissolution of Calcite under Gamma and Helium Ion Irradiation

et al. 2017

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Samples of calcite have been irradiated using both the 60.7 MeV helium ion beam of the ARRONAX (Nantes, France) cyclotron and 661.7 keV gamma radiations. The irradiation of calcite pellets results mainly in radiolytically generated gas (H2, CO2). The presence of superficial water during the calcite irradiation in a humid atmosphere is a key factor for the production of radiolysis gases. Besides, the irradiation of calcite–water biphasic media was performed. The gas released after these irradiations is quantified. No significant amount of CO2 has been detected, whereas carbonate ions act as OH• scavengers, thus inducing an increase of H2 production. The amount of hydrogen peroxide created confirms this scavenging mechanism. Finally, ionic chromatography experiments with irradiated solutions allow us to quantify the organic anions (formate HCOO–, acetate CH3COO–, propionate CH3-CH2COO–, and oxalate C2O4 2–) formed by calcite and/or carbonate ion radiolysis and study the variation of calcium carbonate solubility under irradiation. Formate and acetate ions are formed at low irradiation doses, whereas oxalate is favored at high irradiation doses. The increase of calcium ions in solution during the irradiation of calcite–water media indicates that calcite is progressively dissolved during the irradiation. The main difference between calcite–water media and carbonate ion solutions is that calcite acts as a carbonate ion supply in the radiolysis mechanisms.

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Section: Introductionmentioning

confidence: 99%

Radiolytic Dissolution of Calcite under Gamma and Helium Ion Irradiation

et al. 2017

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“…To conceptualize the radiation-based charging for the Mn–Fe RFB, we obtained radiolysis evidence of reported yield and stability for the reduction of ferric (Fe 3+ ) ions to ferrous (Fe 2+ ) ions and oxidation of Mn 2+ ions to MnO 2 . The radiolytic oxidation of Mn 2+ to Mn 4+ precipitate and the radiolytic reduction of Fe 3+ to Fe 2+ ions, , were noted as charging cycle reactions for the proposed approach. Thus, from the confirmed recharged ion yield and stability metric, the Mn–Fe couple was noted as a feasible RFB system for charging by ionizing radiation.…”

Section: Resultsmentioning

confidence: 99%

“…Ghalei et al 28 studied the oxidation of Mn 2+ to Mn 4+ using manganese carbonate (MnCO 3 ) in carbonate solution and Cs-137 as the radioactive source. Upon the fast oxidation of Mn 2+ to Mn 3+ , further irradiation caused the oxidation of Mn 3+ ions to soluble Mn 4+ ions, which precipitated as insoluble Mn 4+ .…”

Section: Resultsmentioning

confidence: 99%

Perspective on Radiolytic Charging for Redox Flow Battery Electrolytes Using the Nuclear Decay Energy of Spent Nuclear Fuel/Radionuclides

et al. 2022

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The conversion of nuclear energy into electricity is facilitated by chemical intermediates and molecular products formed during the radiolysis of water. In this work, we hypothesize a novel radiolytic charging approach for redox flow battery electrolytes. Radiolytically produced ionic intermediates and molecular products oxidize or reduce the metal ion solutes in the electrolytes. A qualitative study for choice of redox couples based on electrochemical principles followed by a feasibility study of radiolytic conversion of active material is presented. A framework for an empirical investigation of radioactive source, equipment and dose, and product characterization techniques is discussed. The proposed method finds application in the utilization of spent nuclear fuel (specifically gamma emissions from fission products in early activity stages) as a radiolysis radiation source for electrolyte charging. We present a perspective on future investigations that are required to harness nuclear energy for charging electrolytes and developing a self-operating RFB system.

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“…In our previous studies about concentrated sulfuric acid, it was possible to estimate the yield of radical formation through oxidation by water hole through measuring directly the yield of sulfate radical in neat sulfuric acid on the picosecond range. For these systems, it was shown that the electron transfer reaction from the solute to the water hole could be more rapid than a proton transfer reaction. − In the present work, a picosecond pulse radiolysis study of four highly concentrated K 2 CO 3 solutions has been carried out in order to find the time dependent oxidation radiolytic yield in perspective for allowing the evaluation on the redox reactions of solutions containing Tc radioelement containing also high concentration of carbonate anion . For this purpose, the mechanism and the yield of carbonate radical formation are discussed.…”

Section: Introductionmentioning

confidence: 95%

“…10−16 In the present work, a picosecond pulse radiolysis study of four highly concentrated K 2 CO 3 solutions has been carried out in order to find the time dependent oxidation radiolytic yield in perspective for allowing the evaluation on the redox reactions of solutions containing Tc radioelement containing also high concentration of carbonate anion. 17 For this purpose, the mechanism and the yield of carbonate radical formation are discussed.…”

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confidence: 99%

Picosecond Pulse Radiolysis of Highly Concentrated Carbonate Solutions

Ghalei

Schmidhammer

et al. 2016

J. Phys. Chem. B

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Highly concentrated potassium carbonate aqueous solutions are studied by picosecond pulse radiolysis with the purpose of exploring the formation processes of carbonate radical CO3(•-). The transient absorption band of solvated electron produced by ionizing is markedly shifted from 715 to 600 nm when the solute concentration of K2CO3 is 5 mol L(-1). This spectral shift is even more important than that observed for the solvated electron in 10 mol L(-1) KOH solutions. The broad absorption band of solvated electron in K2CO3 solutions overlaps with that of carbonate radical CO3(•-) formed at ultrashort time. Nitrate ion is used to scavenge the solvated electron and to observe the contribution of carbonate radical CO3(•-). The analysis of the amplitude and the kinetics of carbonate radical formation in highly concentrated solutions shows that CO3(•-) is formed within the electron pulse (7 ps) by two parallel mechanisms: a direct effect on the solute and the oxidation of the solute by water radical hole H2O(•+). These two mechanisms are followed by an additional one, by reaction between the solute and OH(•) radical especially in lower concentration. The radiolytic yield of each process is discussed.

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Oxidation and/or reduction of manganese species by γ-ray and He2+ particle irradiation in highly concentrated carbonate media

Cited by 5 publications

References 30 publications

Radiolytic Dissolution of Calcite under Gamma and Helium Ion Irradiation

Radiolytic Dissolution of Calcite under Gamma and Helium Ion Irradiation

Perspective on Radiolytic Charging for Redox Flow Battery Electrolytes Using the Nuclear Decay Energy of Spent Nuclear Fuel/Radionuclides

Picosecond Pulse Radiolysis of Highly Concentrated Carbonate Solutions

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