锡青铜在中子辐照-地下水耦合作用下的腐蚀加速机理研究

杨波; 张梦; 陈沫汝; 赵石; 魏强林; 刘义保

doi:10.3724/j.0253-3219.2025.hjs.48.240454

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锡青铜在中子辐照-地下水耦合作用下的腐蚀加速机理研究

核物理、交叉学科研究 | 更新时间：2025-11-27

- 锡青铜在中子辐照-地下水耦合作用下的腐蚀加速机理研究
- Study on the accelerated corrosion mechanisms of tin bronze under the coupled effects of neutron irradiation and groundwater
- 核技术 2025年48卷第11期文章编号：110501
- 作者机构：
  
  1.东华理工大学核物理与核技术江西省重点实验室南昌 330013
  2.东华理工大学核资源与环境国家重点实验室南昌 330013
  3.东华理工大学核科学与工程学院南昌 330013
- 作者简介：
  
  杨波，男，1982年出生，2017年于中国原子能科学研究院获博士学位，研究领域为高放废物包装容器腐蚀加速机理
  刘义保，E-mail：ybliu@ecut.edu.cn
- 基金信息：
  
  国家自然科学基金(11965001);江西省自然科学基金面上项目(20212BAB201004)
- DOI：10.3724/j.0253-3219.2025.hjs.48.240454
  中图分类号： TL942
- 收稿：2024-11-18，
  
  修回：2025-06-23，
  
  纸质出版：2025-11-15
- 稿件说明：
移动端阅览
杨波,张梦,陈沫汝等.锡青铜在中子辐照-地下水耦合作用下的腐蚀加速机理研究[J].核技术,2025,48(11):110501.

YANG Bo,ZHANG Meng,CHEN Moru,et al.Study on the accelerated corrosion mechanisms of tin bronze under the coupled effects of neutron irradiation and groundwater[J].NUCLEAR TECHNIQUES,2025,48(11):110501.
杨波,张梦,陈沫汝等.锡青铜在中子辐照-地下水耦合作用下的腐蚀加速机理研究[J].核技术,2025,48(11):110501. DOI： 10.3724/j.0253-3219.2025.hjs.48.240454. CSTR： 32193.14.hjs.CN31-1342/TL.2025.48.240454.

YANG Bo,ZHANG Meng,CHEN Moru,et al.Study on the accelerated corrosion mechanisms of tin bronze under the coupled effects of neutron irradiation and groundwater[J].NUCLEAR TECHNIQUES,2025,48(11):110501. DOI： 10.3724/j.0253-3219.2025.hjs.48.240454. CSTR： 32193.14.hjs.CN31-1342/TL.2025.48.240454.

摘要

高放废物深地质处置中包装容器材料的腐蚀行为研究具有重要意义。以锡青铜C5191为包装容器候选材料、BS03地下水为模拟液，开展中子辐照-地下水耦合作用下的锡青铜材料腐蚀加速实验，同时利用第一性原理计算了地下水中SO

在CuSn（110）完整及缺陷表面的吸附能、Bader电荷转移数和分波态密度，通过理论计算解释材料的腐蚀加速机理。结果表明：在不同实验条件下，锡青铜腐蚀速率从0.516 μm·a

-1

增长到17.9 μm·a

-1

，地下水中SO

在CuSn（110）完整及缺陷表面的吸附能分别为-5.311 eV和-5.691 eV，Bader电荷转移数分别为-0.327 1和-0.516 6，说明SO

与缺陷表面更易发生作用。共吸附时，吸附能减小至-12.391 eV，Bader电荷转移数增加到-6.063 9和-6.007 4，表明H

O的辐射分解产物促进了金属缺陷表面对SO

的吸附，实验与理论计算结果一致，证明辐照-地下水耦合作用明显加速锡青铜腐蚀速率。

Abstract

Background

The selection of disposal canister materials is crucial in the deep geological disposal of high-level radioactive waste

as metal packaging containers serve as the first engineering barrier to isolate the waste. Tin bronze C5191 is one of the most selected canister materials

hence its corrosion behavior is worthy of study.

Purpose

This study aims to investigate the accelerated corrosion mechanisms of tin bronze C5191 under the coupled effects of neutron irradiation and groundwater.

Methods

Used tin bronze C5191 as a potential material for the tin bronze C5191 and the BS03 groundwater in Beishan were used as a simulated fluid

samples were immersed in simulated fluids of varying concentrations under different irradiation conditions for 30 d. Subsequently

scanning electron microscope (SEM) was employed to analyze the micromorphology of the sample surfaces

and the mass loss and corrosion rates were analyzed. On the theoretical side

single adsorption and co-adsorption models of SO

and water irradiation decomposition products on the intact and defective surfaces of CuSn(110) were established. Subsequently

first-principles calculations were employed to compute and analyze the adsorption energy

Bader charge transfer numbers

and projected density of states (PDOS) of the adsorption models. Finally

both experimental and theoretical calculations were combined to elucidate the mechanism of material corrosion acceleration.

Results

The experimental and theoretical calculation results indicate that under varying experimental conditions

the corrosion rate of tin bronze is increased from 0.516 μm·a

-1

to 17.9 μm·a

-1

. The adsorption energies of SO

on the intact and defective CuSn(110) surfaces are -5.311 eV and -5.691 eV

respectively

with Bader charge transfer numbers of -0.327 1 and -0.516 6

suggesting that SO

interacts more readily with the defective surface. When co-adsorbed

the adsorption energy is decreased to -12.391 eV

and the Bader charge transfer numbers is increase

d to -6.063 9 and -6.007 4.

Conclusions

Results of this study demonstrates that the radiolysis products of H

O enhance the adsorption of SO

on metal defect surfaces. The experimental and theoretical results are consistent

demonstrating that the coupling of irradiation and groundwater significantly accelerates the corrosion rate of tin bronze.

关键词

Keywords

references

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