المؤلفون: Barr, Logan, Conrad, Jacy K., McGregor, Christine, Perron, Randy, Yakabuskie, Pamela A., Stuart, Craig R.

المساهمون: Idaho National Laboratory, Atomic Energy of Canada Limited, Laboratory Directed Research and Development

المصدر: Physical Chemistry Chemical Physics ; volume 26, issue 5, page 4278-4283 ; ISSN 1463-9076 1463-9084

الوصف: The mechanism of the reaction of OH radicals with Fe 2+ ions changes from hydrogen atom transfer to dissociative ligand interchange above 150 °C. The activation energies of the mechanisms are different, leading to non-Arrhenius temperature dependence.

الإتاحة: https://doi.org/10.1039/d3cp03819jTest
http://pubs.rsc.org/en/content/articlepdf/2024/CP/D3CP03819JTest

المؤلفون: Sterniczuk, Marcin, Yakabuskie, Pamela A., Wren, J. Clara, Jacob, Jasmine A., Bartels, David M.

المساهمون: Department of Energy, National Science and Engineering Research Council of Canada (NSERC)

المصدر: Radiation Physics and Chemistry ; volume 121, page 35-42 ; ISSN 0969-806X

مصطلحات موضوعية: Radiation

الإتاحة: https://doi.org/10.1016/j.radphyschem.2015.12.007Test
https://api.elsevier.com/content/article/PII:S0969806X15301353?httpAccept=text/xmlTest
https://api.elsevier.com/content/article/PII:S0969806X15301353?httpAccept=text/plainTest

المؤلفون: Yakabuskie, Pamela A

المصدر: Electronic Thesis and Dissertation Repository

مصطلحات موضوعية: Radiation chemistry, water radiolysis, kinetics, mass transport, colloid formation, corrosion, Physical Chemistry

الوصف: This thesis presents work focusing on the long-term effect of gamma-radiation on aqueous solution kinetics. Ionizing radiation drives the decomposition of water to form both oxidizing (•OH, O2, H2O2) and reducing (•eaq−, •O2−, •H, H2) chemical species. Over time, these radiolysis products can react with dissolved solutes and participate in interfacial reactions. This can lead to significant changes in the eventual solution redox condition, and gas phase composition, and in certain cases result in the formation of solid species. Understanding the long-term solution kinetics for radiolysis systems is particularly important for the improvement of chemistry control and activity transport models, such as those employed in the nuclear power industry. In order to study the chemical changes induced by exposing these aqueous systems to gamma‑radiation, species in the aqueous, gaseous and solid phases (where applicable) were monitored by a variety of techniques as a function of irradiation time. Chemical kinetics modeling was performed to both validate obtained experimental results, as well as aid in the interpretation of these results. The presence of dissolved solutes was found to impact the steady-state concentrations of the molecular water radiolysis products by competing with them for reaction with radical species. This radical scavenging lowers the rate of removal of the molecular products and allows their concentrations to reach higher levels, however the increase observed relative to pure water is dependent on pH and solute concentration. Redox active solutes that can undergo pseudo-catalytic reaction cycles with the radical species can also significantly affect the concentrations of water radiolysis products without experiencing a significant change in their net speciation. Irradiation studies with transition metal solutes were shown to generate uniform sized colloidal species in solution. The radiolytic oxidation of soluble ferrous ions to less soluble ferric species leads to the homogeneous condensation of ...

وصف الملف: application/pdf

العلاقة: https://ir.lib.uwo.ca/etd/2669Test; https://ir.lib.uwo.ca/context/etd/article/4107/viewcontent/PYThesis_FINAL2015_01_28.pdfTest

الإتاحة: https://ir.lib.uwo.ca/etd/2669Test
https://ir.lib.uwo.ca/context/etd/article/4107/viewcontent/PYThesis_FINAL2015_01_28.pdfTest

المؤلفون: Sterniczuk, Marcin, Yakabuskie, Pamela A., Wren, J. Clara, Jacob, Jasmine A., Bartels, David M.

وصف الملف: application/pdf

العلاقة: http://www.osti.gov/servlets/purl/1359809Test; https://www.osti.gov/biblio/1359809Test; https://doi.org/10.1016/j.radphyschem.2015.12.007Test

الإتاحة: https://doi.org/10.1016/j.radphyschem.2015.12.007Test
http://www.osti.gov/servlets/purl/1359809Test
https://www.osti.gov/biblio/1359809Test

المؤلفون: Yakabuskie, Pamela A., Joseph, Jiju M., Stuart, Craig R., Wren, J. Clara

المصدر: The Journal of Physical Chemistry A ; volume 115, issue 17, page 4270-4278 ; ISSN 1089-5639 1520-5215

الإتاحة: https://doi.org/10.1021/jp200262cTest

المؤلفون: Yakabuskie, Pamela A., Joseph, Jiju M., Clara Wren, J.

المصدر: Radiation Physics and Chemistry ; volume 79, issue 7, page 777-785 ; ISSN 0969-806X

مصطلحات موضوعية: Radiation

الإتاحة: https://doi.org/10.1016/j.radphyschem.2010.02.001Test
https://api.elsevier.com/content/article/PII:S0969806X1000112X?httpAccept=text/xmlTest
https://api.elsevier.com/content/article/PII:S0969806X1000112X?httpAccept=text/plainTest

المؤلفون: Yakabuskie, Pamela A.¹, Joseph, Jiju M.¹, Stuart, Craig R.², Wren, J. Clara¹ jcwren@uwo.ca

المصدر: Journal of Physical Chemistry A. May2011, Vol. 115 Issue 17, p4270-4278. 9p.

مصطلحات موضوعية: *RADIATION chemistry, *IRRADIATION, *CHEMICAL kinetics, *NITRATES, *NITRITES

مستخلص: Radiolysis kinetics in NO3– and NO2– solutions during γ-irradiation were studied at an absorbed dose rate of 2.1 Gy&bull s-1 at room temperature. Air- or argon-saturated nitrate or nitrite solutions at pH 6.0 and 10.6 were irradiated, and the aqueous concentrations of molecular water decomposition products, H2 and H2O2, and the variation in the concentrations of NO3– and NO2– were measured as a function of irradiation time. The experimental data were compared with computer simulations using a comprehensive radiolysis kinetic model to aid in interpretation of the experimental results. The effect of nitrate and nitrite, present at concentrations below 10-3 M, on water radiolysis processes occurs through reactions with the radical species generated by water radiolysis, *eaq , *O2 , and *OH. The changes in H2 and H2O2 concentrations observed in the presence of nitrate and nitrite under a variety of conditions can be explained by a reduction in the radical concentrations. The kinetic analysis shows that the main loss pathway for H2 is the reaction with *OH and the main loss pathways for H2O2are reactions with *eaq– and *OH. Nitrate and nitrite compete for the radicals leading to an increase in the concentrations of H2 and H2 and H2O2. Post-irradiation measurements of H2, H2O2, NO2– and NO3– concentrations can be used to calculate the radical concentrations and provide information on the redox conditions of the irradiated aqueous solutions. [ABSTRACT FROM AUTHOR]