极高剂量率对超临界水在400°C和25 MPa下辐射分解的影响

IF 1.1 4区 化学 Q3 CHEMISTRY, MULTIDISCIPLINARY
A. Sultana, J. Meesungnoen, J. Jay-Gerin
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引用次数: 0

摘要

采用蒙特卡罗多道化学模拟方法,结合圆柱形“瞬时脉冲”辐照模型,研究了高剂量率对超临界水(SCW)在400℃、25 MPa压力下辐射分解“初级产物”(e-aq、H•、H2、•OH、H2O2、h30 +、OH-等)的早期瞬态产率(G值)的影响。我们的模拟模型是用单脉冲入射300 mev质子随机照射SCW,模拟60Co γ/快速电子辐照的低线性能量转移。通常,高剂量率有利于自由基-自由基反应,增加了分子产物的比例,牺牲了自由基产物的比例。然而,作为例外,G(H•)在放射性溶解的径迹阶段随着剂量率的增加而增加,这主要是由于水合电子与水合氢离子(h30o +)的反应。此外,还研究了物理化学阶段质子转移反应引起的酸性峰的产生。有趣的是,在整个辐照体积中,在高辐射剂量率下观察到早期、短暂的强酸性(pH ~ 3.5)反应。目前的工作提出了一个问题,即潜在的氧化物质•OH和H2O2以及高剂量率下的高酸性pH峰值是否会在拟议的第四代scw冷却反应堆或小型模块化反应堆操作条件下促进腐蚀环境,从而导致材料的逐步降解。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
Effect of very high dose rates on the radiolysis of supercritical water at 400 °C and 25 MPa
Monte Carlo multi-track chemistry simulations were used in combination with a cylindrical, “instantaneous pulse” irradiation model to study the effect of high dose rates on the early, transient yields (G values) of the “primary products” (e-aq, H•, H2, •OH, H2O2, H3O+, OH-,…) of the radiolysis of supercritical water (SCW) at 400 °C and 25 MPa pressure. Our simulation model consisted of randomly irradiating SCW with single pulses of N incident 300-MeV protons, which mimic the low linear energy transfer of 60Co γ/fast electron irradiations. The effect of dose rate was studied by varying N. Generally, high dose rates were found to favor radical-radical reactions, which increases the proportion of the molecular products at the expense of the radical products. However, as an exception, G(H•) increases with increasing dose rate in the track stage of radiolysis, predominantly due to the reaction of hydrated electrons with hydronium ions (H3O+). In addition, the generation of acidic spikes due to proton transfer reactions in the physicochemical stage was also examined. Interestingly, an early, transient, very acidic (pH ~ 3.5) response was observed at high radiation dose rates across the entire irradiated volume. The present work raises the question of whether the potential oxidizing species •OH and H2O2 and these highly acidic pH spikes at high dose rates could promote a corrosive environment under proposed Generation-IV SCW-cooled reactor or small modular reactor operating conditions that would lead to progressive degradation of materials.
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来源期刊
Canadian Journal of Chemistry
Canadian Journal of Chemistry 化学-化学综合
CiteScore
1.90
自引率
9.10%
发文量
99
审稿时长
1 months
期刊介绍: Published since 1929, the Canadian Journal of Chemistry reports current research findings in all branches of chemistry. It includes the traditional areas of analytical, inorganic, organic, and physical-theoretical chemistry and newer interdisciplinary areas such as materials science, spectroscopy, chemical physics, and biological, medicinal and environmental chemistry. Articles describing original research are welcomed.
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