Dissolution experiments with surrogate treated organic wastes immobilized by hot isostatic pressing

IF 2.1 3区 工程技术 Q1 NUCLEAR SCIENCE & TECHNOLOGY
Karine Ferrand, Pieter Schroeders, Sébastien Caes, Karel Lemmens
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Abstract

The presence of organic compounds in radioactive wastes might be incompatible with long-term waste management options. Consequently, as part of the H2020-PREDIS project, different thermal treatment routes and conditioning techniques were first used to process surrogates of solid organic wastes. Then, the chemical durability of the conditioned wastes was investigated performing dissolution experiments in a synthetic cementitious water at pH 12.7, 22 °C and in diluted conditions. These tests were conducted with a glass–ceramic, produced by hot isostatic pressing using a mixture of ashes and sodium tetraborate (95/5 wt%). The results showed that glass–ceramic dissolution was incongruent and controlled by diffusion. SEM–EDX analysis showed the presence of an altered zone of about 45  µm after 730  days of alteration, with amorphous and crystalline phases (spinel and chlorapatite), and containing voids due to the dissolution of the glass matrix. The average diffusion coefficients were in the range of (4.26 ± 1.36) × 10−15  (2.88 ± 0.59) × 10−13 m2/s, with the lowest and highest values for Zn and B, respectively. This corresponds to leachability indexes in the range of 10.40 ± 0.14 and 8.54 ± 0.07. The maximum dissolution rate of the glass matrix based on the B release between the start of the tests and 28  days was similar to that found when borosilicate glass was corroded by a KOH solution at pH 12.5. Hot isostatic pressing was thus successfully used to immobilize ashes, and the resulting glass–ceramic exhibited good chemical durability under alkaline conditions.
热等静压固定化有机废物的溶解实验
放射性废物中存在有机化合物可能与长期废物管理办法不相容。因此,作为H2020-PREDIS项目的一部分,首先使用不同的热处理路线和调理技术来处理固体有机废物的替代品。然后,在pH值为12.7、22°C和稀释条件下的合成胶凝水中进行溶解实验,研究了条件废物的化学耐久性。这些测试是用玻璃陶瓷进行的,玻璃陶瓷是用灰烬和四硼酸钠的混合物(95/5 wt%)通过热等静压制成的。结果表明,微晶玻璃的溶解不一致,受扩散控制。SEM-EDX分析显示,经过730天的蚀变后,存在一个约45µm的蚀变区,其中有非晶态和结晶相(尖晶石和绿磷灰石),并且由于玻璃基体的溶解而含有空洞。平均扩散系数为(4.26±1.36)× 10−15 -(2.88±0.59)× 10−13 m2/s, Zn和B的扩散系数最小,B的扩散系数最高。对应的浸出性指标范围为10.40±0.14和8.54±0.07。基于从试验开始到28天的B释放量,玻璃基体的最大溶解速率与硼硅酸盐玻璃被pH为12.5的KOH溶液腐蚀时的溶解速率相似。因此,热等静压成功地固定了灰,得到的玻璃陶瓷在碱性条件下表现出良好的化学耐久性。
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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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