γ辐照下硼锂协同与溶解氢对水辐解及材料电化学行为的影响

Synergistic Effect of Boron Lithium and Dissolved Hydrogen on Water Radiolysis and Material Electrochemical Behavior under Gamma Irradiation

  • 摘要: 水化学环境是压水堆能否安全运行的重要因素,水化学环境的改变会影响材料腐蚀行为与辐射场分布,进而威胁反应堆结构完整性和运行安全边界。本文采用原位辐照-电化学联合表征技术,探究了γ辐 射场中关键环境参数(吸收剂量、溶解氢浓度、硼酸与氢氧化锂协同浓度)对水辐射分解(辐解)行为及材料腐蚀电化学特性(腐蚀电位、腐蚀电流密度)的影响。实验结果表明,水辐射分解程度和材料腐蚀倾向随吸收剂量的增加而增强,表现为腐蚀电位负向偏移、腐蚀电流密度上升。其次,溶解氢能有效抑制水辐解,降低腐蚀电流密度,同时诱导腐蚀电位正向偏移。相较于单一的硼酸或氢氧化锂浓度增加对水辐解的加剧作用,硼锂浓度在实验范围内的协同变化对水辐解的促进作用不显著。然而,硼锂浓度的协同升高却会加剧材料腐蚀,表现为腐蚀电位下降、腐蚀电流密度上升,最终导致金属耐蚀性能减弱和整体腐蚀进程加速。研究表明,吸收剂量的增加会促进水辐解及材料腐蚀,溶解氢能有效抑制水辐解并降低腐蚀电流密度,而硼锂协同浓度对水辐解作用不显著,但浓度的协同升高却会加剧材料电化学腐蚀。本文研究可为核反应堆结构材料的抗辐照-腐蚀协同设计提供理论依据,并为核设施延寿与安全评估提供数据支撑。

     

    Abstract: This study used in-situ irradiation electrochemical joint characterization technology to investigate the effects of key environmental parameters (absorbed dose, dissolved hydrogen concentration, synergistic concentration of boric acid and lithium hydroxide) on water radiolysis behavior and material corrosion electrochemical characteristics (corrosion potential, corrosion current density) in a γ radiation field. The water radiolysis behavior was obtained by measuring the amount of hydrogen peroxide produced using a spectrophotometer, and the corrosion potential and corrosion current density of the material were obtained by measuring the polarization curve using an electrochemical workstation, which was calculated from the polarization curve. The experimental results show that the degree of water radiolysis and material corrosion tendency increase with the increase of absorbed dose, manifested as a negative shift in corrosion potential and an increase in corrosion current density. This is mainly attributed to the continuous irradiation process, where the total energy absorbed by water molecules increases with the increase of absorbed dose, leading to the intensification of water radiolysis. Secondly, dissolved hydrogen, as an effective radiation decomposition inhibitor, can effectively suppress water radiolysis and reduce corrosion current with increasing concentration. Moreover, the addition of dissolved hydrogen induces a positive shift in corrosion potential, but the effect of concentration changes on potential is relatively weak. The changes in potential and current are inconsistent with some literature, mainly due to differences in environmental parameters (low temperature vs. high temperature, irradiation vs. non-irradiation) and time scales (short-term electrochemistry vs. long-term corrosion). Compared to increasing the concentration of boric acid or lithium hydroxide alone (both of which exacerbate water radiolysis), the synergistic effect of boron lithium concentration within the experimental range on promoting water radiolysis is not significant. However, the synergistic increase in boron lithium concentration will exacerbate material corrosion, manifested as a decrease in corrosion potential and an increase in corrosion current density, ultimately leading to a weakening of metal corrosion resistance and an acceleration of overall corrosion process. The reason for the change in electrochemical results despite little change in water radiolysis is that the increase in the concentration of boric acid and lithium hydroxide increases the concentration of  hydrogen ions, hydroxide ions, and other ions in the system, promoting electrochemical reactions. Research has shown that an increase in absorbed dose promotes both water radiolysis and material corrosion. The addition of dissolved hydrogen can effectively suppress water radiolysis and reduce corrosion current density. The synergistic concentration of boron and lithium has no significant effect on water radiolysis, but the synergistic increase in concentration exacerbates material electrochemical corrosion.

     

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