地学前缘 ›› 2021, Vol. 28 ›› Issue (5): 68-78.DOI: 10.13745/j.esf.sf.2021.2.19
惠淑君1(), 杨冰1,2, 郭华明1,*(), 连国玺2, 孙娟2
收稿日期:
2020-08-17
修回日期:
2021-01-15
出版日期:
2021-09-25
发布日期:
2021-10-29
通讯作者:
郭华明
作者简介:
惠淑君(1994—),女,硕士,主要从事环境科学与工程相关研究。E-mail: 1365235784@qq.com
基金资助:
HUI Shujun1(), YANG Bing1,2, GUO Huaming1,*(), LIAN Guoxi2, SUN Juan2
Received:
2020-08-17
Revised:
2021-01-15
Online:
2021-09-25
Published:
2021-10-29
Contact:
GUO Huaming
摘要:
铀矿开采过程中及井场退役后,含铀浸出液的扩散会对地下水造成一定影响,该影响范围和程度决定了铀的天然衰减特征。本文以北方某地浸铀矿区砂岩含水介质为研究对象,研究了溶液化学特征和黄铁矿含量对砂岩吸附和转化铀的影响。结果表明,砂岩颗粒对U(VI)的吸附基本在12 h可达平衡。线性等温吸附模型可以很好地描述吸附特征;砂岩颗粒对U(VI)的吸附率总体随着粒径增大而减小,当岩石粒径增大到0.200.25 mm时,吸附率趋于稳定。溶液pH值是影响吸附的主要因素,通过控制溶液中U(VI)的络合形态和岩石颗粒表面带电荷情况,在库仑力的作用下促进或者抑制吸附,在pH=6时,达到最佳吸附状态。共存离子对U(VI)吸附的抑制程度是:
中图分类号:
惠淑君, 杨冰, 郭华明, 连国玺, 孙娟. 不同因素对砂岩含水层介质吸附铀的影响[J]. 地学前缘, 2021, 28(5): 68-78.
HUI Shujun, YANG Bing, GUO Huaming, LIAN Guoxi, SUN Juan. Factors affecting uranium adsorption on aquifer sandstone[J]. Earth Science Frontiers, 2021, 28(5): 68-78.
粒径/mm | R2 | Kd/(L·g-1) |
---|---|---|
<0.10 | 0.995 1 | 0.030 |
0.10<0.15 | 0.994 3 | 0.038 |
0.15<0.20 | 0.997 9 | 0.032 |
0.20<0.25 | 0.993 6 | 0.029 |
0.250.50 | 0.997 8 | 0.029 |
表1 不同粒径砂岩样品等温吸附曲线拟合系数和吸附分配系数
Table 1 Fitting coefficients and adsorption partition coefficients of isothermal adsorption curves for sandstone samples with different particle sizes
粒径/mm | R2 | Kd/(L·g-1) |
---|---|---|
<0.10 | 0.995 1 | 0.030 |
0.10<0.15 | 0.994 3 | 0.038 |
0.15<0.20 | 0.997 9 | 0.032 |
0.20<0.25 | 0.993 6 | 0.029 |
0.250.50 | 0.997 8 | 0.029 |
因素 | 不同pH值条件下的影响因素情况 | ||
---|---|---|---|
pH<4 | pH=46 | pH>6 | |
固体表面带电荷情况 | 有正电荷也有负电荷 | 主要带负电荷 | 几乎都带负电荷 |
U的络合形态 | | (UO2)3(OH (UO2)4(OH | UO2CO3、UO2(OH (UO2)3(OH UO2(CO3 |
库仑力 | 引力为主 | 引力 | 斥力增强 |
H+竞争作用 | 较强 | 减弱 | 几乎没有 |
表2 不同pH值条件下影响U(VI)吸附的因素
Table 2 List of factors affecting U(VI) adsorption at different pH
因素 | 不同pH值条件下的影响因素情况 | ||
---|---|---|---|
pH<4 | pH=46 | pH>6 | |
固体表面带电荷情况 | 有正电荷也有负电荷 | 主要带负电荷 | 几乎都带负电荷 |
U的络合形态 | | (UO2)3(OH (UO2)4(OH | UO2CO3、UO2(OH (UO2)3(OH UO2(CO3 |
库仑力 | 引力为主 | 引力 | 斥力增强 |
H+竞争作用 | 较强 | 减弱 | 几乎没有 |
不同试验条件 | U(VI)含量占比/% | U(IV)含量占比/% | Fe(II)含量占比/% | Fe(III)含量占比/% |
---|---|---|---|---|
原始黄铁矿 | 98.9 | 1.1 | ||
近中性pH值 | 68 | 32 | 95.8 | 4.2 |
弱碱性pH值 | 100 | 0 | 98.5 | 1.5 |
表3 不同试验条件下10% FeS2组反应10 d的固体表面U(VI)、U(IV)及Fe(II)、Fe(III)含量占比
Table 3 Percentages of U (VI), U (IV), Fe(II), and Fe(III) on solid sample surface containing 10% FeS2 reacting with U(VI) for 10 d under different experimental conditions
不同试验条件 | U(VI)含量占比/% | U(IV)含量占比/% | Fe(II)含量占比/% | Fe(III)含量占比/% |
---|---|---|---|---|
原始黄铁矿 | 98.9 | 1.1 | ||
近中性pH值 | 68 | 32 | 95.8 | 4.2 |
弱碱性pH值 | 100 | 0 | 98.5 | 1.5 |
图10 不同试验条件下10% FeS2组反应10 d的固体Fe(2p)XPS光谱 a—原始黄铁矿;b—近中性pH值;c—弱碱性pH值。
Fig.10 Iron 2p XPS spectra for solid samples containing 10% FeS2 reacting with U(VI) for 10 d under different experimental conditions
图11 不同试验条件下10% FeS2组反应10 d的固体S(2p)XPS光谱 a—原始黄铁矿;b—近中性pH值;c—弱碱性pH值。
Fig.11 Sulphur 2p XPS spectra for solid samples containing 10% FeS2 reacting with U(VI) for 10 d under different experimental conditions
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