Effect of structural disorder induced by external irradiation with heavy ions on the alteration of a four oxide borosilicate glass

IF 6.6 2区 材料科学 Q1 MATERIALS SCIENCE, MULTIDISCIPLINARY
Stéphane Gin, Mélanie Taron, Hélène Arena, Jean-Marc Delaye
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Abstract

The irradiation of glass by heavy ions induces structural damage, generally leading to a decrease in its chemical durability whose amplitude strongly depends on the glass chemical composition. Here, we investigate the effects of irradiation by 7 MeV Au ions (simulating the main ballistic effects induced by self-irradiation in nuclear glass) on the behavior of a 4-oxide borosilicate glass in both the initial and residual dissolution regimes. The comparison between irradiated and non-irradiated glasses provides insights into the predominant atomic mechanisms governing glass alteration processes. The most pronounced effect is observed on interdiffusion in acidic conditions, with the rate increased by more than an order of magnitude for the irradiated glass. We show that both the interdiffusion regime and the residual regime are controlled by the hydrolysis of the B—O—Si linkages, whereas under initial dissolution rate regime in basic conditions the rate-limiting step becomes the hydrolysis of Si—O—Si linkages. Overall, the observations suggest structural disorder due to external irradiation by Au ions primarily affects the kinetics of glass alteration without changing the fundamental nature of the limiting reactions.

Abstract Image

重离子外部辐照引起的结构紊乱对四氧化物硼硅酸盐玻璃变化的影响
重离子辐照玻璃会诱发结构损伤,通常会导致其化学耐久性下降,其幅度与玻璃的化学成分密切相关。在这里,我们研究了 7 MeV Au 离子(模拟核玻璃自辐照引起的主要弹道效应)辐照对 4 氧化物硼硅玻璃在初始和残余溶解状态下的行为的影响。通过对比辐照玻璃和非辐照玻璃,可以深入了解玻璃改变过程的主要原子机制。在酸性条件下,对相互扩散的影响最为明显,辐照玻璃的相互扩散速率增加了一个数量级以上。我们发现,相互扩散机制和残留机制都是由 B-O-Si 链接的水解作用控制的,而在碱性条件下的初始溶解速率机制中,限速步骤变成了 Si-O-Si 链接的水解作用。总之,这些观察结果表明,金离子外部辐照导致的结构紊乱主要影响玻璃改变的动力学,而不会改变限制反应的基本性质。
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来源期刊
npj Materials Degradation
npj Materials Degradation MATERIALS SCIENCE, MULTIDISCIPLINARY-
CiteScore
7.80
自引率
7.80%
发文量
86
审稿时长
6 weeks
期刊介绍: npj Materials Degradation considers basic and applied research that explores all aspects of the degradation of metallic and non-metallic materials. The journal broadly defines ‘materials degradation’ as a reduction in the ability of a material to perform its task in-service as a result of environmental exposure. The journal covers a broad range of topics including but not limited to: -Degradation of metals, glasses, minerals, polymers, ceramics, cements and composites in natural and engineered environments, as a result of various stimuli -Computational and experimental studies of degradation mechanisms and kinetics -Characterization of degradation by traditional and emerging techniques -New approaches and technologies for enhancing resistance to degradation -Inspection and monitoring techniques for materials in-service, such as sensing technologies
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