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Effects of Gamma Radiation and Gamma-Induced Species on Water Chemistry, Polymers and Fe-, Ni- and Zr-Based Alloys
KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry. Chalmers University of Technology. (Mats Jonsson)ORCID iD: 0000-0002-7393-9583
2026 (English)Doctoral thesis, comprehensive summary (Other academic)
Sustainable development
SDG 7: Affordable and clean energy, SDG 6: Clean water and sanitation, SDG 13: Climate action, SDG 9: Industry, innovation and infrastructure
Abstract [en]

Nuclear energy is expected to play an important role in the transition toward low-carbon energy systems. Light Water Reactors (LWRs) dominate the global nuclear fleet, and their safe, reliable, and long-term operation depends on understanding the interactions between radiation, water chemistry, and structural materials that govern corrosion and material degradation.

This thesis investigates the effects of direct gamma irradiation and gamma-induced radiolysis on polymers, aqueous systems, and metallic alloys relevant to LWR operation. Particular attention is given to hydrogen peroxide and other reactive species produced during water radiolysis and their interactions with materials commonly present in reactor systems and laboratory irradiation experiments. The results demonstrate that material interfaces strongly influence the chemistry of irradiated aqueous systems. Investigations of polymer sealing materials revealed that hydrogen peroxide accumulation depends significantly on material choice, highlighting how experimental design and material selection can affect radiation chemistry measurements and contribute to reproducibility challenges. Studies of reactor-relevant alloys further showed that hydrogen peroxide accumulation depends on alloy composition and is governed primarily by radiation-induced processes in solution. Surface analyses indicated only minor modifications of oxide films during irradiation, suggesting that changes in water chemistry are linked more closely to species released into solution than to extensive alterations of alloy surfaces under the investigated conditions. In situ electrochemical measurements under intermittent gamma irradiation revealed an immediate dose-rate-dependent response associated with radiolytically generated reactive species. The results distinguished the roles of short-lived radicals and longer-lived oxidants, identifying hydrogen peroxide as the primary driver of the longer-term electrochemical evolution of the investigated alloy surface. Overall, this thesis shows that the behaviour of irradiated aqueous systems is governed by the interplay between radiation, water chemistry, and material interfaces. The findings contribute to a deeper understanding of radiation chemistry and corrosion-related phenomena in LWR environments and provide guidance for the design and interpretation of future irradiation experiments.

Abstract [sv]

Kärnenergi förväntas spela en viktig roll i omställningen till energisystem med låga koldioxidutsläpp. Lättvattenreaktorer (Light Water Reactors, LWR) dominerar den globala kärnkraftsflottan, och deras säkra, tillförlitliga och långsiktiga drift är beroende av en god förståelse av de interaktioner mellan strålning, vattenkemi och konstruktionsmaterial som styr korrosion och materialdegradering. Denna avhandling undersöker effekterna av direkt gammastrålning och gammastrålningsinducerad radiolys på polymerer, vattenbaserade system och metalliska legeringar som är relevanta för drift av lättvattenreaktorer. Särskild uppmärksamhet ägnas åt väteperoxid och andra reaktiva specier som bildas vid vattenradiolys samt deras interaktioner med material som vanligtvis förekommer i reaktorsystem och i laboratoriebaserade bestrålningsexperiment. Resultaten visar att materialgränsytor har ett starkt inflytande på kemin i bestrålade vattenbaserade system. Studier av polymera tätningsmaterial visade att ackumuleringen av väteperoxid i hög grad beror på materialvalet, vilket belyser hur experimentell utformning och materialval kan påverka mätningar inom strålningskemi och bidra till utmaningar kopplade till reproducerbarhet. Undersökningar av reaktorrelevanta legeringar visade vidare att ackumuleringen av väteperoxid beror på legeringens sammansättning och i huvudsak styrs av strålningsinducerade processer i lösningen. Ytanalyser indikerade endast mindre förändringar i oxidfilmerna under bestrålning, vilket tyder på att förändringar i vattenkemin är närmare kopplade till arter som frigörs till lösningen än till omfattande förändringar av legeringsytorna under de undersökta förhållandena. Elektrokemiska in situ-mätningar under intermittent gammastrålning visade en omedelbar dosrathastighetsberoende respons associerad med radiolytiskt genererade reaktiva specier. Resultaten särskilde rollerna hos kortlivade radikaler och mer långlivade oxidationsmedel och identifierade väteperoxid som den huvudsakliga drivkraften bakom den långsiktiga elektrokemiska utvecklingen hos den undersökta legeringsytan. Sammanfattningsvis visar denna avhandling att beteendet hos bestrålade vattenbaserade system styrs av samspelet mellan strålning, vattenkemi och materialgränsytor. Resultaten bidrar till en djupare förståelse av strålningskemiska och korrosionsrelaterade fenomen i lättvattenreaktormiljöer samt ger vägledning för utformning och tolkning av framtida bestrålningsexperiment.

Place, publisher, year, edition, pages
Stockholm: KTH Royal Institute of Technology, 2026. , p. 81
Series
TRITA-CBH-FOU ; 2026:37
Series
Ny Serie ; 5930
Keywords [en]
Gamma radiation, Hydrogen peroxide, Polymer degradation, Electrochemistry, Radiolysis
National Category
Inorganic Chemistry Physical Chemistry Other Chemistry Topics
Research subject
Chemistry
Identifiers
URN: urn:nbn:se:kth:diva-387424DOI: 10.63959/chalmers.dt/5930ISBN: 978-91-8103-473-8 (print)OAI: oai:DiVA.org:kth-387424DiVA, id: diva2:2093875
Public defence
2026-09-18, Lecture hall Viva, Kemigården 4, floor 10, Göteborg, https://chalmers.zoom.us/j/67220245604, 13:00 (English)
Opponent
Supervisors
Funder
Swedish Centre for Nuclear Technology (SKC)
Note

QC 20260828

Available from: 2026-08-28 Created: 2026-08-20 Last updated: 2026-09-07Bibliographically approved
List of papers
1. How septum materials affect H2O2 accumulation under gamma-irradiation of water in sealed vials: A comparative study on polysiloxane rubber, PTFE, and aluminium
Open this publication in new window or tab >>How septum materials affect H2O2 accumulation under gamma-irradiation of water in sealed vials: A comparative study on polysiloxane rubber, PTFE, and aluminium
2026 (English)In: Radiation Physics and Chemistry, ISSN 0969-806X, E-ISSN 1879-0895, Vol. 238, p. 113196-113196, article id 113196Article in journal (Refereed) Published
Abstract [en]

This study investigates the influence of septum materials on the radiolytic generation and steady-state concentration of hydrogen peroxide (H2O2) in deionized water produced through γ-irradiation with a Co-60 source at a dose rate of 3 kGy/h. The experimental findings reveal that polysiloxane rubber septa significantly reduce the steady-state concentration of H2O2 by up to 90 % compared to polytetrafluoroethylene (PTFE) and aluminium septa when in contact with the headspace above the solution. The suppression of H2O2 accumulation was observed exclusively during irradiation. This indicates a radiation-mediated interaction between the silicone rubber and the air-saturated, closed system of the irradiated vials. A plausible explanation is that the O2 in the headspace reacts with Si- and C-centered radicals formed upon irradiation of the silicone. The consumption of the O2 from the head space will lead to the depletion of O2 in the solution as the equilibrium between the gas phase and the liquid must be maintained. This, in turn, explains the lower H2O2 concentrations in the liquid phase since O2 is a precursor for H2O2. These results have implications for the design of experimental setups and the choice of materials in systems where radiolytic processes are significant.

Place, publisher, year, edition, pages
Elsevier BV, 2026
National Category
Materials Chemistry Polymer Chemistry Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-387310 (URN)10.1016/j.radphyschem.2025.113196 (DOI)001694097800001 ()2-s2.0-105012622174 (Scopus ID)
Funder
Chalmers University of Technology
Note

QC 20260820

Available from: 2026-08-20 Created: 2026-08-20 Last updated: 2026-08-20Bibliographically approved
2. Study of H2O2 Production and Consumption in γ-Irradiated Aqueous Systems in Contact with Zircalloy, Inconel, and AISI Alloys. An Electrochemical Approach
Open this publication in new window or tab >>Study of H2O2 Production and Consumption in γ-Irradiated Aqueous Systems in Contact with Zircalloy, Inconel, and AISI Alloys. An Electrochemical Approach
2025 (English)In: The 23rd International Conference on Water Chemistry in Nuclear Reactor Systems, Busan, Korea, 2025, article id 1279Conference paper, Published paper (Refereed)
Abstract [en]

This study investigates the steady-state concentration of radiolytic H2O2 produced by γ-radiolysis of water in contact with stainless steel, Inconel and Zircalloy materials. The findings reveal that the alloys lead to different hydrogen peroxide concentrations under γ-irradiation up to a total received dose of 2.2 MGy, with a maximum reduction of 40 % with respect to the control sample achieved by stainless steel and no tangible difference induced by Zircalloy. Without γ-irradiation, H2O2 reactivity is instead minimal and homogeneous toward all the alloys. No evidence of material oxidation was found on the surface of the irradiated samples. Further electrochemical investigations evidenced a shift of the Electrochemical Corrosion Potential (ECP) toward more positive values under γ-irradiation for both stainless steel and Zircalloy, with stainless steel showing a larger drift and higher current than Zircalloy. The results indicate that simple use of H2O2 solutions may not correctly mimic the effect of water radiolysis products and γ-irradiation on the alloys object of this study.

Place, publisher, year, edition, pages
Busan, Korea: , 2025
Keywords
Radiolysis, Gamma Radiation, Hydrogen Peroxide, Electrochemistry
National Category
Inorganic Chemistry Materials Chemistry Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-387312 (URN)
Conference
The 23rd International Conference on Water Chemistry in Nuclear Reactor Systems
Projects
SKC Project - Impact of radiation chemistry on surface processes in LWRs
Funder
Swedish Centre for Nuclear Technology (SKC)
Note

QC 20260820

Available from: 2026-08-20 Created: 2026-08-20 Last updated: 2026-08-20Bibliographically approved
3. Impact of Alloy Composition on the Steady-State Concentration of Hydrogen Peroxide in Water under Gamma Irradiation
Open this publication in new window or tab >>Impact of Alloy Composition on the Steady-State Concentration of Hydrogen Peroxide in Water under Gamma Irradiation
(English)Manuscript (preprint) (Other academic)
National Category
Inorganic Chemistry Physical Chemistry
Identifiers
urn:nbn:se:kth:diva-387320 (URN)
Projects
SKC project: "Impact of radiation chemistry on surface processes in LWRs" "
Funder
Swedish Centre for Nuclear Technology (SKC)
Note

QC 20260820

Available from: 2026-08-20 Created: 2026-08-20 Last updated: 2026-08-20Bibliographically approved
4. In Situ Electrochemical Investigation of 316L Alloy under Intermittent Gamma Irradiation in Water Solutions – Direct Assessment of the Relative Impact of Radiolytic Oxidants
Open this publication in new window or tab >>In Situ Electrochemical Investigation of 316L Alloy under Intermittent Gamma Irradiation in Water Solutions – Direct Assessment of the Relative Impact of Radiolytic Oxidants
(English)Manuscript (preprint) (Other academic)
National Category
Inorganic Chemistry Physical Chemistry Other Chemistry Topics
Identifiers
urn:nbn:se:kth:diva-387423 (URN)
Projects
SKC project: "Impact of radiation chemistry on surface processes in LWRs"
Funder
Swedish Centre for Nuclear Technology (SKC)
Note

QC 20260820

Available from: 2026-08-20 Created: 2026-08-20 Last updated: 2026-08-20Bibliographically approved

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