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Interactions of Uranium and Reactive Oxygen Species.

紀錄類型:	書目-電子資源 : Monograph/item
正題名/作者:	Interactions of Uranium and Reactive Oxygen Species./
作者:	Kravchuk, Dmytro V.
面頁冊數:	1 online resource (333 pages)
附註:	Source: Dissertations Abstracts International, Volume: 85-01, Section: B.
Contained By:	Dissertations Abstracts International85-01B.
標題:	Chemistry. -
電子資源:	http://pqdd.sinica.edu.tw/twdaoapp/servlet/advanced?query=30425107click for full text (PQDT)
ISBN:	9798379794040

Interactions of Uranium and Reactive Oxygen Species.
Kravchuk, Dmytro V.

Interactions of Uranium and Reactive Oxygen Species. - 1 online resource (333 pages)

Source: Dissertations Abstracts International, Volume: 85-01, Section: B.

Thesis (Ph.D.)--The University of Iowa, 2023.

Includes bibliographical references

Meeting global energy needs requires development of sustainable and affordable power options with minimal carbon footprint. As the world is moving away from traditional fossil-fuel-based energy sources, nuclear power emerges as a promising alternative providing reliable baseload energy without emission of greenhouse gases. While nuclear energy has been integrated in the United States energy grid since the late 1950s, the nuclear industry still faces challenges with the long-term storage and reprocessing of spent nuclear fuel, and legacy waste from the Manhattan project and plutonium production facilities. Such waste forms present a unique chemical challenge due to radiation fields inducing unexpected chemical reactions on the surface of stored materials. Radiolysis products on the surface of either spent nuclear fuel or stored nuclear waste are typically oxidized forms of uranium as peroxide- or carbonate-bearing alteration phases. As a result, there is a critical need to evaluate various mechanisms that lead to the formation of such alteration phases in the back-end of the nuclear fuel cycle, thus addressing potential challenges in the long-term storage or reprocessing efforts.The objective of my thesis is to explore various synthetic pathways towards uranium alteration phases found on the surface of spent nuclear fuel and nuclear waste via generation or introduction of reactive oxygen species in the presence of hexavalent uranium. I have reported successful synthesis of uranyl peroxide species using: (i) in-situ generation of organic peroxide via autoxidation of benzaldehyde; (ii) photochemical uranyl-mediated H-abstraction in the solid state resulting in uranyl peroxide dimers; (iii/iv) mechanochemical reactivity of U(IV) and U(VI) oxides with solid alkali metal peroxides. Along with uranyl peroxide phases, we managed to (v) isolate the first uranyl superoxide (O2-●) compound that exhibits direct air capture of carbon dioxide, as well as (vi) demonstrate the behavior and thermodynamic stability of this uranyl superoxide material at elevated temperatures. This thesis presents a significant contribution to our understanding of reactions between reactive oxygen species (peroxide O22- and superoxide O2-●) and uranium, which provide a plausible mechanism for the formation of uranium-bearing alteration phases found on real-life samples of spent nuclear fuel and nuclear waste.

Electronic reproduction.
Ann Arbor, Mich. :
ProQuest,
2023

Mode of access: World Wide Web

ISBN: 9798379794040Subjects--Topical Terms:

516420
Chemistry.
Subjects--Index Terms:

Carbon captureIndex Terms--Genre/Form:

542853
Electronic books.

Interactions of Uranium and Reactive Oxygen Species.
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504 $a Includes bibliographical references
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653 $a Uranium
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