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利用xSiO₂-yAl₂O₃-zP₂O₅(SAP)材料在熔盐状态下对放射性盐废物进行稳定化/固化处理。

Stabilization/solidification of radioactive salt waste by using xSiO2-yAl2O3-zP2O5 (SAP) material at molten salt state.

作者信息

Park Hwan-Seo, Kim In-Tae, Cho Yong-Zun, Eun Hee-Chul, Lee Han-Soo

机构信息

Advanced Fuel Cycle Development, Korea Atomic Energy Research Institute, 150 Deokjin-dong, Yuseong-gu, Daejeon 305-353, Korea.

出版信息

Environ Sci Technol. 2008 Dec 15;42(24):9357-62. doi: 10.1021/es802012x.

Abstract

The molten salt waste from the pyroprocess is one of the problematic wastes to directly apply a conventional process such as vitrification or ceramization. This study suggested a novel method using a reactive material for metal chlorides at a molten temperature of salt waste, and then converting them into manageable product at a high temperature. The inorganic composite, SAP (SiO2-Al2O3-P2O5), synthesized by a conventional sol-gel process has three or four distinctive domains that are bonded sequentially, Si-O-Si-O-A-O-P-O-P. The P-rich phase in the SAP composite is unstable for producing a series of reactive sites when in contact with a molten LiCl salt. After the reaction, metal aluminosilicate, metal aluminophosphate, metal phosphates and gaseous chlorines are generated. From this process, the volatile salt waste is stabilized and it is possible to apply a high temperature process. The reaction products were fabricated successfully by using a borosilicate glass with an arbitrary composition as a chemical binder. There was a low possibility for the valorization of radionuclides up to 1200 degrees C, based on the result of the thermo gravimetric analysis. The Cs and Sr leach rates by the PCT-A method were about 1 x 10(-3) g/(m2 day). For the final disposal of the problematic salt waste, this approach suggested the design concept of an effective stabilizer for metal chlorides and revealed the chemical route to the fabrication of monolithic wasteform by using a composite as an example. Using this method, we could obtain a higher disposal efficiency and lower waste volume, compared with the present immobilization methods.

摘要

热法后处理产生的熔盐废物是难以直接采用诸如玻璃固化或陶瓷化等传统工艺处理的废物之一。本研究提出了一种新颖的方法,即在熔盐废物的熔融温度下使用一种针对金属氯化物的反应性材料,然后在高温下将它们转化为易于处理的产物。通过传统溶胶 - 凝胶法合成的无机复合材料SAP(SiO₂ - Al₂O₃ - P₂O₅)具有三到四个依次键合的独特区域,即Si - O - Si - O - A - O - P - O - P。当SAP复合材料中富含P的相与熔融LiCl盐接触时,对于产生一系列反应位点而言是不稳定的。反应后,会生成金属铝硅酸盐、金属铝磷酸盐、金属磷酸盐和气态氯。通过这个过程,挥发性盐废物得以稳定,并且可以应用高温工艺。使用任意组成的硼硅酸盐玻璃作为化学粘结剂成功制备了反应产物。基于热重分析结果,在高达1200℃的温度下,放射性核素增值的可能性较低。采用PCT - A法测得的Cs和Sr浸出率约为1×10⁻³ g/(m²·天)。对于这种有问题的盐废物的最终处置,该方法提出了一种针对金属氯化物的有效稳定剂的设计理念,并以一种复合材料为例揭示了制备整体式废物固化体的化学途径。与目前的固定方法相比,使用这种方法我们可以获得更高的处置效率和更低的废物体积。

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