<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.
Authors
- Reza Moshrefi (ORCID: https://orcid.org/0000-0002-2969-2341)
- Samantha Michelle Gateman (ORCID: https://orcid.org/0000-0002-3889-9926)
- Peter Keech (ORCID: https://orcid.org/0000-0001-8435-628X)
- Mehran Behazin (ORCID: https://orcid.org/0000-0001-5245-4256)
- Taras Skotar
- Emmanuel Mena-Morcillo
- Fraser King
- Scott Briggs
Institutions
- Western University (CA)
- Nuclear Waste Management Organization (CA)
Publication Details
- Journal
- ACS electrochemistry.
- Published
- 2026-02-02
- DOI
- https://doi.org/10.1021/acselectrochem.5c00338
- Primary Topic
- Advanced oxidation water treatment
- Type
- article
- Field-Weighted Citation Impact
- 0.00