<i>In Situ</i> Monitoring of Hypochlorite Decay under Radiation Using Differential Pulse Voltammetry

Understanding how concentrations of corrosive oxidants evolve under γ-radiation is essential for assessing long-term material performance in nuclear environments. This work integrates <i>in situ</i> differential pulse voltammetry (DPV) with finite-element kinetic modeling to track and interpret the decay of hypochlorite (OCl<sup>-</sup>) in aerated 0.1 M NaCl at pH ∼9.9 under a dose rate of 725 Gy h<sup>-1</sup>. Using a three-electrode setup inside a <sup>60</sup>Co γ-cell, OCl<sup>-</sup> was quantified from calibration curves, where concentrations were validated <i>ex situ</i> by UV-vis spectroscopy. For an initial OCl<sup>-</sup> added concentration of 10 mM, both methods showed a decrease to ∼1 mM after 24 h. Kinetic analysis based on a radiolysis/halogen reaction scheme indicates that HOCl consumption is dominated by OH<sup>•</sup> abstraction (∼71%), with a secondary contribution from O<sub>2</sub> <sup>•-</sup> reduction (∼22%) and a minor Cl<sup>-</sup>-mediated pathway (∼7%); contributions from e<sup>-</sup> and H<sup>•</sup> are negligible at the steady state. The added HOCl drives a pronounced rise in OCl<sup>•</sup> that feeds back to lower the steady-state OH<sup>•</sup> level and modulates H<sub>2</sub>O<sub>2</sub> formation. From these kinetics, it is estimated that <i>g</i> <sub>HOCl</sub> ≈ -0.53 μmol J<sup>-1</sup>. Beyond validating DPV as an <i>in situ</i> radiation electroanalytical method, the combined measurements and modeling provide a mechanistic basis for OCl<sup>-</sup> transformation in saline waters, establishing a general radiation-electrochemistry platform for time-resolved detection of radiolysis products relevant to nuclear-waste containment.

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Journal
ACS electrochemistry.
Published
2026-02-02
DOI
https://doi.org/10.1021/acselectrochem.5c00338
Primary Topic
Advanced oxidation water treatment
Type
article
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article

In Situ Monitoring of Hypochlorite Decay under Radiation Using Differential Pulse Voltammetry

Reza Moshrefi, Samantha Michelle Gateman, Peter Keech, Mehran Behazin et al.
ACS electrochemistry.
Advanced oxidation water treatment
article

In Situ Monitoring of Hypochlorite Decay under Radiation Using Differential Pulse Voltammetry

Reza Moshrefi, Samantha Michelle Gateman, Peter Keech, Mehran Behazin, Taras Skotar, Emmanuel Mena-Morcillo, Fraser King, Scott Briggs
article en

Abstract

Understanding how concentrations of corrosive oxidants evolve under γ-radiation is essential for assessing long-term material performance in nuclear environments. This work integrates <i>in situ</i> differential pulse voltammetry (DPV) with finite-element kinetic modeling to track and interpret the decay of hypochlorite (OCl<sup>-</sup>) in aerated 0.1 M NaCl at pH ∼9.9 under a dose rate of 725 Gy h<sup>-1</sup>. Using a three-electrode setup inside a <sup>60</sup>Co γ-cell, OCl<sup>-</sup> was quantified from calibration curves, where concentrations were validated <i>ex situ</i> by UV-vis spectroscopy. For an initial OCl<sup>-</sup> added concentration of 10 mM, both methods showed a decrease to ∼1 mM after 24 h. Kinetic analysis based on a radiolysis/halogen reaction scheme indicates that HOCl consumption is dominated by OH<sup>•</sup> abstraction (∼71%), with a secondary contribution from O<sub>2</sub> <sup>•-</sup> reduction (∼22%) and a minor Cl<sup>-</sup>-mediated pathway (∼7%); contributions from e<sup>-</sup> and H<sup>•</sup> are negligible at the steady state. The added HOCl drives a pronounced rise in OCl<sup>•</sup> that feeds back to lower the steady-state OH<sup>•</sup> level and modulates H<sub>2</sub>O<sub>2</sub> formation. From these kinetics, it is estimated that <i>g</i> <sub>HOCl</sub> ≈ -0.53 μmol J<sup>-1</sup>. Beyond validating DPV as an <i>in situ</i> radiation electroanalytical method, the combined measurements and modeling provide a mechanistic basis for OCl<sup>-</sup> transformation in saline waters, establishing a general radiation-electrochemistry platform for time-resolved detection of radiolysis products relevant to nuclear-waste containment.

ACS electrochemistry.Vol. 2(3)
Western University (CA), Nuclear Waste Management Organization (CA)
Openalex Percentile: Top 71%
Advanced oxidation water treatment
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