高温下SiO2-KNO3-KReO4混合物中铼的挥发

IF 2.5 3区 工程技术 Q1 NUCLEAR SCIENCE & TECHNOLOGY Nuclear Engineering and Design Pub Date : 2025-02-01 Epub Date: 2024-12-12 DOI:10.1016/j.nucengdes.2024.113758
Chenchen Niu , Aiqing Chen , Kaiwen Hu , Kai Xu
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引用次数: 0

摘要

由于其半衰期长、裂变产率高、在地下水中的高迁移率,锝-99 (Tc-99)是核废料中的一种麻烦的核素。此外,主要关注的是核废料玻璃化过程中Tc的高挥发性。已有研究表明,硝酸盐对含Tc废物玻璃化过程中Tc的挥发有显著影响。然而,由于核废料组成的复杂性,确定硝酸盐如何影响Tc挥发是具有挑战性的。本研究采用简化的SiO2-KNO3-KReO4进料,以铼(Re)为Tc非放射性替代物,研究硝酸盐对高温下Re挥发的影响。结果表明,当KNO3-KReO4二元体系中KNO3的摩尔分数超过60 mol%时,在800℃以下的温度下,KNO3可以促进Re挥发,这是由于在310℃时,KReO4与KNO3发生了共晶反应。而在1200℃以上的温度下,增加KNO3含量可以抑制Re的挥发,因为加入KNO3可以增加非晶相的含量,Re被包裹在非晶相中,几乎不挥发。
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Rhenium volatilization in SiO2-KNO3-KReO4 mixtures at elevated temperatures
Due to its long half-life, high fission yield, and high mobility in the groundwater, Technetium-99 (Tc-99) is a troublesome nuclide in nuclear waste. Moreover, the primary concern is the high volatility of Tc during nuclear waste vitrification. Previous studies demonstrated that nitrate significantly affected the Tc volatilization during the vitrification of Tc-containing waste. However, identifying how nitrate affects Tc volatilization is challenging due to the complexity of the composition of nuclear waste. This study used a simplified SiO2-KNO3-KReO4 feed with rhenium (Re) as a Tc non-radioactive surrogate to study the nitrate effect on the Re volatilization at elevated temperatures. The results showed that KNO3 could facilitate Re volatilization at temperatures below 800 °C when the molar percentage of KNO3 in the KNO3-KReO4 binary system exceeded 60 mol%, which was attributed to the eutectic reaction between KReO4 and KNO3 at 310 °C. However, the increased KNO3 content could inhibit the Re volatilization at temperature above 1200 °C since adding KNO3 could increase the amorphous phase content, where Re was encapsulated and hardly evaporated.
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来源期刊
Nuclear Engineering and Design
Nuclear Engineering and Design 工程技术-核科学技术
CiteScore
3.40
自引率
11.80%
发文量
377
审稿时长
5 months
期刊介绍: Nuclear Engineering and Design covers the wide range of disciplines involved in the engineering, design, safety and construction of nuclear fission reactors. The Editors welcome papers both on applied and innovative aspects and developments in nuclear science and technology. Fundamentals of Reactor Design include: • Thermal-Hydraulics and Core Physics • Safety Analysis, Risk Assessment (PSA) • Structural and Mechanical Engineering • Materials Science • Fuel Behavior and Design • Structural Plant Design • Engineering of Reactor Components • Experiments Aspects beyond fundamentals of Reactor Design covered: • Accident Mitigation Measures • Reactor Control Systems • Licensing Issues • Safeguard Engineering • Economy of Plants • Reprocessing / Waste Disposal • Applications of Nuclear Energy • Maintenance • Decommissioning Papers on new reactor ideas and developments (Generation IV reactors) such as inherently safe modular HTRs, High Performance LWRs/HWRs and LMFBs/GFR will be considered; Actinide Burners, Accelerator Driven Systems, Energy Amplifiers and other special designs of power and research reactors and their applications are also encouraged.
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