Chemical mitigation of the transmutation problem in crystalline nuclear waste radiophases

Vance, E. R.; Roy, Rustum; Pepin, John G.; Agrawal, Dinesh Kumar

doi:10.1007/bf00543512

Cited by 22 publications

(14 citation statements)

References 9 publications

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“…The Cs 1+ decays to Ba 2+ with a decrease in ionic radius of 20%, and Sr 2+ decays to Y 3+ , which in turn decays to Zr 4+ with a final ionic radius decrease of 29%. One way to mitigate the effects of such transmutations is through the use of multiple cation waste forms with one or more variable valence cations [Vance et al 1982], which are plentiful in HLW glasses. Thus, unlike crystalline waste forms, transmutations products can be readily accommodated in complex glasses.…”

Section: Beta Decay Effectsmentioning

confidence: 99%

Radiation and Thermal Ageing of Nuclear Waste Glass

Weber

2014

Procedia Materials Science

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Section: Beta Decay Effectsmentioning

confidence: 99%

Radiation and Thermal Ageing of Nuclear Waste Glass

Weber

2014

Procedia Materials Science

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“…38 One way to mitigate the effects of such transmutations is through the use of multiple cation waste forms with one or more variable-valence cations. 39 In addition, helium atoms, formed by α particles capturing two electrons, are also produced in actinidebearing waste forms and must be accommodated. For high actinide loadings, the He concentrations can become quite high (several atomic percent) and difficult to accommodate within both glass and ceramic structures.…”

Section: Radiation Effectsmentioning

confidence: 99%

Materials Science of High-Level Nuclear Waste Immobilization

Weber¹,

Navrotsky²,

Stefanovsky³

et al. 2009

MRS Bull.

319

219

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With the increasing demand for the development of nuclear power comes the responsibility to address the issue of waste, including the technical challenges of immobilizing high-level nuclear wastes in stable solid forms for interim storage or disposition in geologic repositories. The immobilization of high-level nuclear wastes has been an active area of research and development for over 50 years. Borosilicate glasses and complex ceramic composites have been developed to meet many technical challenges and current needs, although regulatory issues, which vary widely from country to country, have yet to be resolved. Cooperative international programs to develop advanced proliferation-resistant nuclear technologies to close the nuclear fuel cycle and increase the efficiency of nuclear energy production might create new separation waste streams that could demand new concepts and materials for nuclear waste immobilization. This article reviews the current state-of-the-art understanding regarding the materials science of glasses and ceramics for the immobilization of highlevel nuclear waste and excess nuclear materials and discusses approaches to address new waste streams.

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“…While somewhat more challenging because of the large change in charge, the initial work focused on the decay of 90 Sr 2+ to 90 Zr 4+ in a titanate model material. The variable valence state of Ti may serve to compensate for some of the charge imbalance (Vance et al 1982). …”

Section: +mentioning

confidence: 99%

Chemical and Charge Imbalance Induced by Radionuclide Decay: Effects on Waste Form Structure

Jiang¹,

Ginhoven²

2012

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SUMMARY ExperimentalIn this section, the experimental results for the Radiation Effects task are summarized. Zr + ion implantation at 550 K was performed and Zr and O atomic concentrations of up to 1.5 at% each in STO were achieved. Effects on the crystal structure, chemistry, and charge states in the implanted STO were studied. A number of analytical methods were employed to characterize the implanted STO, including secondary-ion mass spectroscopy, multiaxial ion-channeling analysis, transmission electron microscopy, X-ray diffraction, X-ray photoelectron spectroscopy, and Raman spectroscopy. The results show that, in contrast to the observed mobile Sr interstitials in STO, the implanted Zr does not diffuse noticeably during the ion implantation or thermal annealing up to 1423 K. A defect concentration was generated and accumulated in STO during the ion implantation, but the crystal structure was not rendered fully amorphous. Thermal annealing at 1273 K leads to a significant defect recovery at the surface with little recovery occurring at the damage peak, where a modest recovery occurs upon further annealing at 1423 K. The blocking ratio of Zr in STO, as observed along the <001> axis, is ~0.4 and ~0.5 after annealing at 1273 and 1423 K, respectively. Nearly all the implanted Zr species are not located exactly at the original lattice site due to structural distortion. A high density of dislocations was observed in the damage layer, where there were also Zr-containing superlattice structures and voids (or oxygen blisters). Results show that Zr is located at every other Sr site in the superlattice structure. Larger voids and dislocation loops exist beyond the damage layer. There was a minor phase with a tetragonal structure in the damage layer, where the implanted Zr was distributed. The tetragonal phase has the <001> axis parallel to that of the STO host. It survived thermal annealing at 1423 K with only a small decrease in the c value. Changes in chemical states or formation of new chemical bonding were not observed in this study because of the thin implanted layer and limited detection sensitivity. Discussion about the results and a general assessment of the model waste form are also provided in this report.

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Chemical mitigation of the transmutation problem in crystalline nuclear waste radiophases

Cited by 22 publications

References 9 publications

Radiation and Thermal Ageing of Nuclear Waste Glass

Radiation and Thermal Ageing of Nuclear Waste Glass

Materials Science of High-Level Nuclear Waste Immobilization

Chemical and Charge Imbalance Induced by Radionuclide Decay: Effects on Waste Form Structure

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