Interfacial redox reactions, X-ray absorption spectroscopy, and how they can contribute to the safety of radioactive-waste repositories


Interfacial redox reactions, X-ray absorption spectroscopy, and how they can contribute to the safety of radioactive-waste repositories

Scheinost, A. C.

The safe enclosure of nuclear waste in deep-geological repositories is not only a challenge for engineers to build it, but also for geoscientist to predict that the eventually forming leaks do not lead to a contamination of the biosphere – and this for a period of up to one million years, as dictated by the slow decay of long-lived radionuclides. A precise, molecular-scale understanding of the retention processes at water/mineral interfaces is one of the fundamental requirements to improve the prediction of radionuclide migration by (reactive) transport models. These processes include physical and chemical sorption, and structural incorporation by existing or neoforming mineral phases. Interfacial redox reactions with structural or sorbed Fe(II) play a pivotal role during these processes, since Fe(II) is the most ubiquitous redox agent in the deep anoxic underground, and is released from steel canisters corroding under radiolytic H2 production. Synchrotron-based X-ray absorption spectroscopy is ideally suited to elucidate such processes, since it provides information on oxidation state, bonding and short-range structure of an element at the same time, and this in situ due to the high penetration depth and element-specifity of the used synchrotron radiation. I will show selected examples for a range of metals occurring in radwaste (Tc, U, Np, Pu, Am), while the observed processes are transferable to many other metals and metalloids of general geochemical interest.

Keywords: nuclear waste; XAFS; Redox

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