高压实膨润土与孔隙溶液物理作用机制研究进展

廖饶平; 陈永贵; 刘聪; 叶为民; 乌东北; 王琼

doi:10.11779/CJGE20230811

高压实膨润土与孔隙溶液物理作用机制研究进展 English Version

廖饶平^1,,
陈永贵^{1, 2, ,},
刘聪¹,
叶为民^{1, 2},
乌东北³,
王琼^{1, 2}

1.
同济大学土木工程学院地下建筑与工程系, 上海 200092
2.
土木工程防灾减灾全国重点实验室(同济大学), 上海 200092
3.
同济大学化学科学与工程学院, 上海 200092

基金项目:

国家自然科学基金项目 42125701

国家自然科学基金项目 41977232

国家自然科学基金项目 42030714

上海市教委科研创新计划项目 2023ZKZD26

中央高校基本科研业务费

土木工程Ⅰ类高峰学科建设经费 2022-3-ZD-08

详细信息

作者简介:
廖饶平(1993—)，男，博士研究生，主要从事环境地质与非饱和土力学研究。E-mail: lrp_liao@tongji.edu.cn

通讯作者:
陈永贵, E-mail: cyg@tongji.edu.cn

中图分类号: TU413
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出版历程
- 收稿日期: 2023-08-21
- 网络出版日期: 2024-03-24
- 刊出日期: 2024-11-30

Advances in physical interaction mechanism between highly compacted bentonite and pore solution

LIAO Raoping^1,,
CHEN Yonggui^{1, 2, ,},
LIU Cong¹,
YE Weimin^{1, 2},
WU Dongbei³,
WANG Qiong^{1, 2}

1.
Department of Geotechnical Engineering, College of Civil Engineering, Tongji University, Shanghai 200092, China
2.
State Key Laboratory of Disaster Reduction in Civil Engineering, Tongji University, Shanghai 200092, China
3.
School of Chemical Science and Engineering, Tongji University, Shanghai 200092, China

摘要

摘要: 作为高放废物处置库的工程屏障，高压实膨润土在长期服役过程中将受到围岩地下水及其化学成分的渗入作用，膨胀性能不断衰减，最终威胁处置安全。在阐述孔隙溶液对高压实膨润土水化膨胀过程影响规律的基础上，总结了高压实膨润土与孔隙溶液物理作用机制的最新研究成果。结果表明，孔隙溶液对高压实膨润土的物理作用机制包括晶层膨胀、扩散双电层膨胀和吸附作用等3种。其中，孔隙溶液对晶层膨胀的作用与浓度有关，低浓度时表现为促进作用，高浓度时表现为抑制作用，取决于孔隙溶质吸力与临界吸力的差；孔隙溶液对扩散双电层的抑制作用是导致有效孔隙通道扩大、渗透和扩散系数增大的主要原因；pH对膨润土表面活性位点和核素水解的影响是引起吸附特性变化的主要原因，背景离子的竞争吸附作用致使膨润土对核素离子的吸附量显著减少。目前，孔隙溶液作用的参数概化、有效孔隙量化和吸附化学模型的研究仍有不足。因此，进一步优化本构模型中孔隙溶液作用的化学参数，明确不同尺度孔隙的等效量化研究，构建约束条件下压实膨润土多组分竞争吸附模型仍是今后需要深入研究的重点方向。
- 深地质处置库 /
- 高放射性废物 /
- 高压实膨润土 /
- 孔隙溶液 /
- 作用机制 /
- 进展
Abstract: The swelling performance of highly compacted bentonite deteriorates due to infiltrating rock groundwater and chemical components during its long-term operation, ultimately posing a threat to disposal safety. The recent researches on the physical interaction between compacted bentonite and pore solution are reviewed based on the phenomena related to the influences of the pore solution on buffering properties. The results show that the physical mechanism of the pore solution on highly compacted bentonite includes swelling of crystal layer, swelling of diffusion double layers and adsorption effects. The effects of the pore solution on the swelling of crystal layer are related to its concentration, and they are promoted at low concentration and inhibited at high concentration, which depends on the difference between the suction and the critical suction of the poresolution. The inhibition of the pore solution on the swelling of double layers is the main factor for the enlarged pore channels, higher permeability and diffusion coefficients. The pH change and nuclide hydrolysis alter the adsorption characteristics, while the competitive background ion adsorption reduces the nuclide capacity of bentonite. The current shortcomings include parameter generalization for pore solution effects, effective porosity quantification and adsorption models. Therefore, the further optimization of chemical parameters of pore solution in the constitutive model, the clarification of the equivalent quantification of the pores at different scales, and the establishment of a multi-component competitive adsorption model under the constraint of compacted bentonite are still the key directions for the further researches in the future.
- deep geological repository /
- high-level radioactive waste /
- highly compacted bentonite /
- pore solution /
- physical interaction mechanism /
- advance

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图 1 高放废物深地质处置库及多重屏障缓冲示意图

Figure 1. Schematic diagram of deep geological repository and multiple barrier buffer for high-level waste

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图 2 高压实膨润土微观结构组成^[24]

Figure 2. Microstructural composition of highly compacted bentonite^[24]

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图 3 不同吸力下压实膨润土膨胀力时程曲线^[31]

Figure 3. Time-swelling pressure curves with increase of suction^[31]

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图 4 吸力对蒙脱石水化层间距和层叠体厚度的影响^[25-26]

Figure 4. Effects of suction on interlayer distance and laminate thickness of montmorillonite^[25-26]

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图 5 膨润土水化膨胀机制

Figure 5. Hydration swelling mechanism of bentonite

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图 6 溶液作用下膨胀力三阶段演化特征^[30]

Figure 6. Three stages of swelling pressure hydrated with salt solutions^[30]

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图 7 溶液对膨润土最终膨胀力的影响^[35-39]

Figure 7. Effects of ion species and concentration on final swelling pressure of compacted bentonite^[35-39]

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图 8 层叠体颗粒受力平衡示意图

Figure 8. Schematic diagram of stress balance of layered particles

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图 9 离子类型和浓度对膨润土膨胀指数的影响^{[15, 43]}

Figure 9. Effects of ion species and concentration on free swell index of bentonite^{[15, 44]}

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图 10 溶液浓度与渗透吸力的关系^[45]

Figure 10. Relationship between concentration of different solutions and osmotic suction^[45]

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图 11 离子类型对高压实膨润土膨胀力的影响^[16]

Figure 11. Effects of ion species on final swelling pressure of compacted bentonite^[16]

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图 12 离子类型对高压实膨润土膨胀变形的影响^[15]

Figure 12. Effects of ion species on final swelling deformation of compacted bentonite^[15]

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图 13 Stern理论扩散双电层构造^[45]

Figure 13. Diffusion double-layer structure of Stern theory^[45]

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图 14 离子类型及浓度对膨润土饱和渗透系数的影响^[46]

Figure 14. Effects of ion species and concentrations on saturation permeability coefficient of compacted bentonite^[46]

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图 15 离子强度对膨润土中核素离子扩散的影响^[47]

Figure 15. Effects of ionic strength on diffusion of nuclides^[47]

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图 16 蒙脱石表面吸附作用示意图^[49]

Figure 16. Schematic diagram of surface adsorption of montmorillonite^[49]

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图 17 pH对GMZ-Na基膨润土吸附核素的影响^[52-56]

Figure 17. Effects of pH on adsorption of nuclides by GMZ-Na bentonite^[52-56]

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图 18 不同温度中U(Ⅵ)离子形态分布随pH的变化^[49]

Figure 18. Species distribution of U(Ⅵ) ions with pH change under different temperatures^[49]

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图 19 离子强度对GMZ-Na基膨润土吸附U(Ⅵ)的影响^[54]

Figure 19. Effects of ionic strength on adsorption of U(Ⅵ) ions by GMZ-Na bentonite^[54]

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图 20 阴阳离子类型对GMZ-Na基膨润土吸附U(Ⅵ)的影响^[54]

Figure 20. Effects of cationic and anion species on adsorption of U(Ⅵ) by GMZ-Na bentonite^[54]

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图 21 背景离子类型对U(Ⅵ)吸附分配系数的影响^[60]

Figure 21. Effects of ion species on equilibrium constants of U(Ⅵ) ^[60]

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表 1 Na基膨润土表面活性位点的反应机制^[51]

Table 1 Reactions of active sites on Na-bentonite^[51]

表面活性位点反应	双层模型参数(lgK)	非静电模型参数(lgK)
$\equiv X{\text{Na}} \rightleftharpoons \equiv {X^ - } + {\text{N}}{{\text{a}}^ + }$	-1.58	-1.58
$\equiv X{\text{Na}} + {{\text{H}}^ + }f \equiv XH + {\text{N}}{{\text{a}}^ + }$	1.50	2.10
$\equiv {\text{AlOH}} + {{\text{H}}^ + }f \equiv {\text{AlOH}}_{\text{2}}^{\text{ + }}$	6.15	5.83
$\equiv {\text{AlOH}} + {\text{O}}{{\text{H}}^ - }f \equiv {\text{AlO + H}}_{\text{2}}^{}{\text{O}}$	-9.27	-7.02
$\equiv {\text{SiOH}} + {\text{O}}{{\text{H}}^ - }f \equiv {\text{Si}}{{\text{O}}^ - }{\text{ + H}}_{\text{2}}^{}{\text{O}}$	-9.06	-8.75

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表 2 GMZ-Na基膨润土表面活性位点的分布密度^[50]

Table 2 Distribution density of active sites on surface of GMZ-Na bentonite ^[50]

活性位点类型	密度
蒙脱石层间阳离子交换位点，（ $\equiv {\rm X^ - }$ ）	1.35×10^-5 mol/m², (66.5±7 cmol/kg)
铝氧八面体边缘羟基位点，（ $\rm \equiv AlOH$ ）	9.39×10^-7 mol/m², (4.61 cmol/kg)
硅氧四面体边缘羟基位点，（ $\rm \equiv SiOH$ ）	1.88×10^-6 mol/m², (9.23 cmol/kg)

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