从电导率评价放射性废物包封BaO - FeOx - P2O5玻璃的降解

IF 3.5 3区材料科学 Q1 MATERIALS SCIENCE, CERAMICS

Journal of the American Ceramic Society Pub Date : 2025-02-24 DOI:10.1111/jace.20434

Kazuki Mitsui, Nobuyasu Nishioka, Hiromichi Takebe, Richard K. Brow, Akira Saitoh

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引用次数: 0

摘要

本文报道了放射性废物封装玻璃的候选材料——磷酸铁钡玻璃的电导率。由于FeO（OH）稳定水化层在玻璃表面的沉淀提高了玻璃的水耐久性，因此优化了玻璃组合物在热水中的缓慢溶解。假设该玻璃的导电机理是在Fe （II）和Fe （III）离子的电子能级之间发生电子跳变，服从Fe （II）→Fe (III) + e−的载流子生成。在200至550℃范围内，基底玻璃的电导率为~ 3.2 × 10−7至~ 5.0 × 10−4 S/cm，而在耐水试验后具有表面水化层的样品的电导率比基底玻璃样品低一个数量级。结晶样品在400℃时的电导率为~ 0.8 × 10−7 S/cm。x射线光电子能谱分析表明，试样中存在Fe （II）和Fe （III）键，P−O−Fe （Ba）键和P−O−P键，电导率随试样体积、腐蚀和结晶的增大而增大。

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Degradation of radioactive waste encapsulation of BaO−FeOx−P2O5 glass evaluated from electrical conductivity

We report on the electrical conductivity of barium iron phosphate glass, a candidate for radioactive waste encapsulating glass. The glass composition has been optimized for slow dissolution in hot water because the precipitation of a stable hydration layer of FeO(OH) on the glass surface enhances the water durability of the glass. The mechanism of electrical conductivity of the glass is assumed to be an electron hopping between the electronic energy levels of Fe (II) and Fe (III) ions, obeying the electron carrier generation of Fe (II) → Fe (III) + e⁻. The electrical conductivity of the base glass was ∼3.2 × 10⁻⁷ to ∼5.0 × 10⁻⁴ S/cm, from 200 to 550°C, whereas samples with surface hydration layers after the water durability tests had conductivities one order of magnitude lower than the base glass sample. The electrical conductivity of a crystallized sample was ∼0.8 × 10⁻⁷ S/cm at 400°C. X-ray photoelectron spectroscopy revealed the existence of Fe (II) and Fe (III), and P−O−Fe (Ba) and P−O−P bonds, and it was found that electrical conductivity increased in the order of increasing Fe (II)/Fe (III) ratio for the bulk, the corroded, and the crystallized samples.

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来源期刊

Journal of the American Ceramic Society 工程技术-材料科学：硅酸盐

CiteScore

7.50

自引率

7.70%

发文量

590

审稿时长

2.1 months

期刊介绍： The Journal of the American Ceramic Society contains records of original research that provide insight into or describe the science of ceramic and glass materials and composites based on ceramics and glasses. These papers include reports on discovery, characterization, and analysis of new inorganic, non-metallic materials; synthesis methods; phase relationships; processing approaches; microstructure-property relationships; and functionalities. Of great interest are works that support understanding founded on fundamental principles using experimental, theoretical, or computational methods or combinations of those approaches. All the published papers must be of enduring value and relevant to the science of ceramics and glasses or composites based on those materials. Papers on fundamental ceramic and glass science are welcome including those in the following areas: Enabling materials for grand challenges[...] Materials design, selection, synthesis and processing methods[...] Characterization of compositions, structures, defects, and properties along with new methods [...] Mechanisms, Theory, Modeling, and Simulation[...] JACerS accepts submissions of full-length Articles reporting original research, in-depth Feature Articles, Reviews of the state-of-the-art with compelling analysis, and Rapid Communications which are short papers with sufficient novelty or impact to justify swift publication.