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关于碳化铀在水溶液中的稳定性——碳酸氢根和氢氧根的影响

On the Stability of Uranium Carbide in Aqueous Solution-Effects of HCO and HO.

作者信息

El Jamal Sawsan, Johnsson Mats, Jonsson Mats

机构信息

School of Engineering Sciences in Chemistry, Biotechnology and Health, Department of Chemistry, KTH Royal Institute of Technology, Stockholm SE-100 44, Sweden.

Department of Materials and Environmental Chemistry, Stockholm University, Stockholm SE-106 91, Sweden.

出版信息

ACS Omega. 2021 Sep 10;6(37):24289-24295. doi: 10.1021/acsomega.1c04581. eCollection 2021 Sep 21.

Abstract

Uranium carbide (UC) is a candidate fuel material for future Generation IV nuclear reactors. As part of a general safety assessment, it is important to understand how fuel materials behave in aqueous systems in the event of accidents or upon complete barrier failure in a geological repository for spent nuclear fuel. As irradiated nuclear fuel is radioactive, it is important to consider radiolysis of water as a process where strongly oxidizing species can be produced. These species may display high reactivity toward the fuel itself and thereby influence its integrity. The most important radiolytic oxidant under repository conditions has been shown to be HO. In this work, we have studied the dissolution of uranium upon exposure of UC powder to aqueous solutions containing HCO and HO, separately and in combination. The experiments show that UC dissolves quite readily in aqueous solution containing 10 mM HCO and that the presence of HO increases the dissolution further. UC also dissolves in pure water after the addition of HO, but more slowly than in solutions containing both HCO and HO. The experimental results are discussed in view of possible mechanisms.

摘要

碳化铀(UC)是未来第四代核反应堆的候选燃料材料。作为总体安全评估的一部分,了解在事故发生时或乏核燃料地质处置库中屏障完全失效的情况下,燃料材料在水系统中的行为非常重要。由于辐照核燃料具有放射性,因此将水的辐射分解视为一种可产生强氧化性物质的过程很重要。这些物质可能对燃料本身表现出高反应性,从而影响其完整性。已表明在处置库条件下最重要的辐射分解氧化剂是HO。在这项工作中,我们分别并结合研究了UC粉末暴露于含有HCO和HO的水溶液时铀的溶解情况。实验表明,UC在含有10 mM HCO的水溶液中很容易溶解,并且HO的存在会进一步增加溶解。添加HO后UC也能溶解于纯水中,但比在同时含有HCO和HO的溶液中溶解得更慢。根据可能的机制对实验结果进行了讨论。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/9c8d/8459425/4cb59261a51b/ao1c04581_0002.jpg

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