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1.北京分子科学国家实验室 放射化学与辐射化学重点学科实验室 北京大学 化学与分子工程学院 北京 100871
2.环境保护部固体废物与化学品管理技术中心 北京 100029
3.中国工程物理研究院 核物理与化学研究所 绵阳 621900
[ "周万强, 男, 1994年出生, 2016年毕业于哈尔滨工程大学, 现为博士研究生, 从事环境放射化学研究", "ZHOU Wanqiang, male, born in 1994, graduated from Harbin Engineering University in 2016, doctoral student, engaging in the study of environmental radiochemistry" ]
刘春立, E-mail:liucl@pku.edu.cn LIU Chunli, E-mail: liucl@pku.edu.cn
收稿日期:2017-03-01,
修回日期:2017-09-16,
纸质出版日期:2018-07-10
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周万强, 蒋京呈, 何建刚, 等. 计算模拟铀在北山地下水的种态分布及在两种不同材料上的吸附[J]. 核技术, 2018,41(7):070301
Wanqiang ZHOU, Jingcheng JIANG, Jiangang HE, et al. Computational simulation of the speciation distribution of uranium in Beishan groundwater and the sorption of uranium on two different materials[J]. Nuclear techniques, 2018, 41(7): 070301
周万强, 蒋京呈, 何建刚, 等. 计算模拟铀在北山地下水的种态分布及在两种不同材料上的吸附[J]. 核技术, 2018,41(7):070301 DOI: 10.11889/j.0253-3219.2018.hjs.41.070301.
Wanqiang ZHOU, Jingcheng JIANG, Jiangang HE, et al. Computational simulation of the speciation distribution of uranium in Beishan groundwater and the sorption of uranium on two different materials[J]. Nuclear techniques, 2018, 41(7): 070301 DOI: 10.11889/j.0253-3219.2018.hjs.41.070301.
为了解铀在北山地下水的存在种态和吸附行为,利用CHEMSPEC软件计算了铀在北山地下水的种态分布及其在石英和水合氧化铁两种材料上的吸附,并考察了pH、Eh和不同离子浓度的变化对铀种态分布的影响。结果显示:在酸性条件下,铀主要以U(OH)
4
(aq)形式存在;在中性和弱碱性条件下,主要以UO
2
(CO
3
)
2
2-
和UO
2
(CO
3
)
3
4-
形式存在;在强碱性条件下,主要以UO
2
(OH)
3
-
形式存在。U的价态受电位影响较大,在还原条件下,U(Ⅳ)较稳定,在氧化条件下,U(Ⅵ)较稳定。不同离子的引入会影响U的种态分布,其影响大小顺序为HCO
3
-
>
F
-
>
SO
4
2-
>
Cl
-
。U(Ⅵ)在石英上的吸附随pH同步增大,并在pH=4.3处达到最大值,U(Ⅵ)在水合氧化铁的吸附随pH增大而先增大后减小,pH在5.7~8.2内达到最大值。
Background
2
The disposal of high-level radioactive wastes is critical for sustainable development of nuclear energy. And the adsorption
diffusion and migration behaviors of radionuclides in the environment depend on the chemical species in the system.
Purpose
2
The paper aims to understand the speciation distribution of uranium and adsorption behavior on quartz and hydrous ferric oxide.
Methods
2
The speciation distribution and sorption of uranium are calculated by chemical speciation analysis software CHEMSPEC
which is developed by Peking University Nuclear Environmental Group.
Results and Conclusions
2
The calculation results indicate that uranium exists as UO
2
(CO
3
)
3
4-
and UO
2
(CO
3
)
2
2-
in the Beishan groundwater. And under acidic conditions
uranium mainly exists as U(OH)
4
(aq). While in neutral or weak alkaline conditions
the main species are UO
2
(CO
3
)
2
2-
and UO
2
(CO
3
)
3
4-
. When the solution is in strong alkaline conditions
most of uranium exists as UO
2
(OH)
3
-
. And U(Ⅳ) is stable in the redox condition
while U(Ⅵ) is stable in the oxide condition. The concentration of different ions also has influence on the speciation distribution of uranium
and in the order of HCO-3
>
F
-
>
SO
4
2-
>
Cl
-
. With the increasing number of pH
the sorption extent of U(Ⅵ) on quartz is lager. And the maximum adsorption is at pH=4.3. When it comes to U(Ⅵ) sorption on hydrous iron oxide
the greatest sorption is at pH=5.7~8.2.
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