高压实膨润土与孔隙溶液化学作用机制研究进展

廖饶平; 陈永贵; 刘聪; 叶为民; 乌东北; 王琼

doi:10.11779/CJGE20240208

高压实膨润土与孔隙溶液化学作用机制研究进展 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项目

土木工程Ⅰ类高峰学科建设经费项目 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: 2024-02-03
- 网络出版日期: 2024-06-05
- 刊出日期: 2025-04-30

Research advances in chemical 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: 高压实膨润土作为高放废物深地质处置首选缓冲/回填材料，在处置库近场热-水-力-化多场耦合环境中必然会与孔隙溶液发生化学作用，使蒙脱石溶解甚至相变，导致工程屏障缓冲性能衰减失效。在全面阐述孔隙溶液化学作用对高压实膨润土缓冲性能影响规律的基础上，系统总结了高压实膨润土与孔隙溶液化学作用机制的最新研究成果。分析表明，层状蒙脱石溶解相变为架状矿物是导致膨润土比表面积、相对质量密度、持水性能、膨胀性能、防渗性能等发生衰减的关键因素。孔隙溶液对高压实膨润土的化学作用机制包括矿物化学相变和化学胶结作用。其中，矿物化学相变与孔隙溶液化学组成、pH、温度和活性催化离子有关，可分为同晶相变和溶解重结晶两种机制；化学胶结与膨润土干湿循环产生盐渍沉淀填充和硅铝酸盐胶凝物胶结作用密切相关。膨润土中矿物的溶解速率不仅与自身反应表面积、所受应力和溶解平衡有关，还与孔隙溶液的化学组成、pH、温度和活性催化离子等环境因素密切相关。针对膨润土内的反应体系，进一步明确化学反应参数、胶结作用影响和多场耦合反应模型仍是今后膨润土化学演化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 /
- 化学作用机制 /
- 进展
Abstract: The highly compacted bentonite, as the preferred buffer/backfill materials, is inevitably subjected to chemical erosion in the T-H-M-C environment of the high-level radioactive waste repositories, leading to dissolution or phase transition of smectite, and diminishing the buffer performance. The latest researches on the chemical mechanism are summarized on the basis of reviewing the effects of the solution on the buffer performance of the compacted bentonite. The analysis indicates that the dissolution or phase transformation of layered smectite into a framework mineral is the key factor leading to the attenuation of the specific surface area, density, water retention, swelling and permeation resistance of bentonite. The chemical interaction mechanisms include mineral phase transformation and chemical cementation. The phase transformation of minerals is influenced by chemical composition, pH, temperature and catalytic ions of the pore solution, and can be divided into isomorphous phase transformation and recrystallization. The chemical cementation associates with saline precipitate filling and the cementation of aluminosilicate gelation during wetting-drying cycles. The dissolution rate of minerals in bentonite is influenced by both the intrinsic factors like surface area and stress, and the extrinsic factors including pore solution. Further clarification of chemical reaction parameters, cementation effects and multi-field coupling reaction model within the bentonite reaction system remains the focus of further researches on the chemical evolution of bentonite in the future.
- deep geological repository /
- high-level radioactive waste /
- compacted bentonite /
- pore solution /
- chemical interaction mechanism /
- advance

HTML全文

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 蒙脱石晶体结构示意图

Figure 2. Crystal structure diagram of smectite

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图 3 碱-热作用下膨润土基本性能变化规律^[30]

Figure 3. Basic properties of bentonite under alkali-heat action

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图 4 碱-热作用下膨润土持水性能随时间变化^[31]

Figure 4. Water retention curves of bentonite under alkali-heat action

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图 5 不同离子类型对膨润土膨胀变形的影响^[32]

Figure 5. Effects of ion types on swelling deformation of bentonite

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图 6 碱-热作用下膨润土最终膨胀力随时间变化^[31]

Figure 6. Final swelling pressures of bentonite under alkali-heat action

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图 7 pH和温度对压实膨润土饱和渗透系数的影响^{[33, 35]}

Figure 7. Effects of pH and temperature on permeability of bentonite

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图 8 碱溶液饱和下压实膨润土孔径分布^[34]

Figure 8. PSD of bentonite in high alkal isolution

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图 9 高压实膨润土近场化学作用机制示意图

Figure 9. Schematic diagram of near field chemical action mechanism of compacted bentonite

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图 10 pH、温度和应力对石英矿物溶解速率的影响^[37]

Figure 10. Effects of pH, temperature and stress on dissolution rate of quartz minerals

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图 11 蒙脱石同晶矿物溶解速率随pH的变化^{[7, 39-43]}

Figure 11. Variation of dissolution rate of smectite isomorphous minerals with pH

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图 12 蒙脱石溶解速率随pH的变化^[7]

Figure 12. Variation of dissolution rate of smectite with pH

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图 13 不同碱溶液中蒙脱石d₀₀₁衍射峰的变化^[21]

Figure 13. Reflection peaks of smectite d₀₀₁ under alkali solutions

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图 14 硅/铝四面体重结晶转化示意图

Figure 14. Schematic diagram of Si/Al tetrahedral crystallization

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表 1 各国处置库所选膨润土的矿物成分对比

Table 1 Mineral composition of bentonite in disposal repositories of various countries

国家	名称	主要矿物含量/%	文献
中国	GMZ-Na基	蒙脱石（75.4），石英（11.7），方英石（7.3），长石（4.3），高岭石（0.8），方解石（0.5）	文献[17]
西班牙	FEBEX-Ca基	蒙脱石（92），石英（2），斜长石（2）	文献[18]
法国	MX80-Na基	蒙脱石（75.5），石英（15），方解石（1.4），斜长石（5~8）	文献[19]
日本	Kunigel-Na基	蒙脱石（73.2），石英（37.6）斜长石（4）	文献[20]

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表 2 各国处置库地下水离子成分

Table 2 Main ion components of groundwater of disposal repositories in various countries

国家	地下水类型	TDS/(g·L^-1)	主要离子组成/(mmol·L^-1)	文献
中国	花岗岩裂隙水	7.1	Na⁺（74）, Ca²⁺（7）, Cl^-（53）, SO₄^2-（30）	文献[12]
西班牙	花岗岩裂隙水	0.3	Na⁺（0.6）, Ca²⁺（1.0）, Cl^-（0.4）, HCO₃^-（2.5）	文献[21]
法国	黏土岩孔隙水	5.7	Na⁺（45）, Ca²⁺（7）, Cl（40）, SO₄^2-（16）	文献[22，23]
日本	沉积岩（海水）	42.4	Na⁺（480）, Ca²⁺（11）, Cl^-（691）, SO₄^2-（29）	文献[24]
韩国	花岗岩裂隙水	0.2	Na⁺（0.8）, Ca²⁺（0.4）, HCO₃^-（1.3）, SO₄^2-（0.1）	文献[25]

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表 3 常见离子在水溶液中的直径^[44]

Table 3 Diameters of common ions in aqueous solution

离子类型	D_c (Å）	D_s (Å）	D_H (Å）
H⁺	—	(0.56）	(4.56）
Na⁺	1.90	3.68	7.16
K⁺	2.66	2.50	6.62
NH₄⁺	2.96	2.50	6.62
Mg²⁺	1.30	6.94	8.56
Ca²⁺	1.98	6.20	8.24
Fe²⁺	1.50	6.88	8.56
Fe³⁺	1.20	8.12	9.14
Al³⁺	1.00	8.78	9.50
OH^-	3.52	(0.92）	(6.00）
Cl^-	3.62	2.42	6.64
NO^3-	5.28	2.58	6.70
CO₃^2-	5.32	5.32	7.88
SO₄^2-	5.80	4.60	7.58
注：D_c为晶体直径；D_s为斯托克斯直径；D_H为水化离子直径。

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表 4 2︰1型二八面体层状黏土矿物对比^[45]

Table 4 Comparison of stratified clay minerals of type 2︰1 dioctahedral

层间物质	单位晶胞携带的负电荷量X	矿物种类
无	X=0	叶腊石，滑石
阳离子或水化阳离子	0.2<X<0.6	蒙脱石，贝德石，绿脱石
	0.6<X<0.9	黏粒蛭石
	0.6<X<1	伊利石，水白云母水钠云母
	X=1	白云母，钠云母
	X=2	珍珠云母
氢氧化物	X不定	绿泥石

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