混合型缓冲回填材料膨胀特性研究
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摘要
高放废物是一种含有强放射性核素的特殊废物,它具有毒性大、核素半衰期长、发热量大的特点,需要与人类生存环境长期可靠地隔离。高放性废物的处置难度极大,目前认为最可行的处置方法是深部地质处置法,即将废物深埋在地下。埋藏高放废物的地下工程称为地质处置库,处置库一般采用“多重屏障体系”的概念模型进行设计。多重屏障体系中,缓冲回填材料是阻隔放射性核素向地下水环境迁移的最主要包封设施。
近二十多年来,我国就缓冲回填材料的选择进行了大量的研究工作。高庙子膨润土因其优越的吸附性能、膨胀自愈性能以及极低的渗透性被确认为我国理想的缓冲回填材料。但是仅用纯膨润土做缓冲材料存在热传导性能低和可施工性差两个难以克服的弊端,纯膨润土过高的塑性使得加水制样过程中“团粒化”及不均匀湿化现象非常明显,土的可调理性差,试样难以压实到所需的干密度。纯膨润土较低的热传导性不利于将放射性核素衰变产生的热量散发到周围的洞室围岩中去,可能导致缓冲层温度升高超过100℃,液态水气化后产生过大的水汽压力,还有可能导致膨润土的性质改变。膨润土中添加一定量的辅料,比如石英砂或者碎石,既能满足力学强度、热传导性能和防渗阻隔能力,又能优化回填设计与施工性能。开发膨润土-砂混合物作为缓冲回填材料,是世界高放废物地质处置领域的主流方向。在国内,开发膨润土-砂混合型缓冲回填材料,是兰州大学的创新研究方向,也是世界高放废物地质处置领域的主流方向。
混合型缓冲回填材料研究的根本目标,是确定最优掺砂率,使膨润土-砂混合物的的化学吸附性能、力学性能、防渗性能、膨胀自愈性能等尽最大可能地同时得到满足。本研究的具体目标是从膨胀性质方面,研究高庙子(GMZ)膨润土-砂混合物的膨胀性质与掺砂率、干密度以及孔隙液的关系,为最终的掺砂率和干密度优化提供基础数据。
孔隙液为蒸馏水时,对掺砂率分别为0、10、15、20、25、30、35、40和50%的膨润土-砂混合物进行液塑限试验,研究液塑限随掺砂率的变化规律；对掺砂率分别为0、10、20、30、40和50%的膨润土-砂混合物采用动力击实和静力压实两种方法制成的初始干密度不同的一系列试样进行膨胀试验,研究掺砂率和初始干密度对膨胀特性的影响规律。
孔隙液为NaCl-Na2SO4溶液(NaCl与Na2SO4按干质量比2：1配置)时,对掺砂率分别为0、10、15、20、25、30、35、40和50%的膨润土-砂混合物在溶液的总溶解性固体(TDS)分别是0.5、1.0、3.0、6.0和12.0g/L(pH=7.1)进行液塑限试验,研究孔隙液浓度对液塑限的影响规律。对掺砂率为0、20、30和50%,初始干密度为1.50-1.90g/cm3的一系列膨润土-砂混合物的静力压实试样进行膨胀试验,研究孔隙液浓度对混合物膨胀特性的影响规律。
所得试验结果如下：
混合物的液限、塑限随掺砂率的增大线性降低,塑性指数线性降低；膨胀的发生分为三个阶段：孔隙间膨胀,初始膨胀和二次膨胀,膨胀力和膨胀率随时间的曲线都呈S型。当初始含水率一定时,随着初始干密度的增大,最大膨胀力指数增长,最大膨胀率线性增长。随着掺砂率的增大,最大膨胀力指数降低,最大膨胀率呈二次函数降低。
随着NaCl-Na2SO4溶液总溶解性固体(TDS)的增大,GMZ膨润土-砂混合物的液限、塑限、塑性指数、膨胀时间、最大膨胀力和最大膨胀率均降低。其中,随着溶液TDS的增大,液限,塑性指数和最大膨胀率均呈指数降低：当TDS<3.0g/L时,各参数值降低速率都很大；当TDS=3.0-6.0g/L时,各参数值降低速率减慢；当TDS>6.0g/L时,随着TDS的增大,各参数值降低缓慢,基本保持不变。随着溶液TDS的增大,膨润土-砂混合物和纯膨润土的最大膨胀力均线性降低,但是纯膨润土比掺砂30%的膨润土-砂混合物对溶液的敏感性更高。与纯膨润土相比,膨润土-砂混合物中一部分具有膨胀性质的粘土被不具膨胀性的石英砂替代了,从而导致膨润土-砂混合物对地下水化学溶液的侵蚀具有更好的耐受性,
根据中国预选处置库甘肃北山的地下水水文资料并综合考虑之前试验结果,以NaCl-Na2SO4(TDS=0.5g/L)作为孔隙液,对于初始干密度为1.70g/cm3的试样,随着掺砂率的增大,最大膨胀力指数降低最大膨胀率线性降低；对于掺砂率30%的试验,随着初始干密度的增大,最大膨胀力指数增长最大膨胀率线性增长。说明增大掺砂率会抑制膨润土的膨胀性质而增大初始干密度会提高其膨胀性质。
引入了有效粘土的密度的概念,ρb。有效粘土密度可以将初始干密度和掺砂率两个参数统一起来,并且通过对试验数据的分析回归,建立了一定初始含水率条件下,任意掺砂率和初始干密度的GMZ膨润土-砂混合物最大膨胀力／最大膨胀率与有效粘土密度一一对应的归一化模型,从而实现了膨胀性质同时与初始干密度和掺砂率对应的函数关系式,通过数据验证,该方程式与试验数据能够很好的吻合。在一定的掺砂率和初始干密度方位内,利用这些方程式可以实现对GMZ膨润土-砂混合物膨胀行为的预测和人为控制。
结合实际处置情况和要求,通过对试验数据的分析,综合考虑膨胀力和膨胀率,本研究认为基于满足膨胀性质的要求,GMZ膨润土-砂混合物的最优掺砂率范围为20-30%,初始干密度范围为1.60-1.80g/cm3。
High-Level Radioactive Waste (HLW) is a waste very difficult to be disposed, which contains strong radioactive, heat, toxicity, and long half-life nuclides. It must be long-term and reliably isolated with the living environment of the human. The deep geological disposal is currently believed to be the best feasible disposition way, which means that the waste was deeply buried in the ground. A multiple barrier system was accepted as the repository conceptual, in which the buffer/backfill material is the most important barrier to prevent the migration of radionuclides by groundwater.
In the past20years, many researches have been done on the select of backfill/buffer materials in China, and GMZ bentonite is considered to be a reliable buffer/backfill material in HLW repositories because of its high absorption and high swelling properties and low permeability. However, because the plasticity of pure bentonite is very high, a tendency of "pelletization" will present during the process of water-soil mixed, this will cause an obvious inhomogeneous wetting of bentonite, and then give trouble to the block making process of buffer/backfill material. In addition, the heat conductivity of pure bentonite is very low, if the heat produced by radioactive waste can not be sent out to the surrounding rock promptly and effectively, the temperature of the buffer layer will rise. When the temperature exceeds100℃, liquid gasification will produce too much water vapor pressure and affect the stability of the repository. Moreover, montmorillonite in bentonite will be converted into illite when the temperature exceeds100℃, so that the function of the buffer/backfill material changes. For bentonite-and, bentonite-crushed rock or bentonite-ballast mixtures possess higher structural integrity, thermal conductivity. As a modern trend in backfill/buffer material development, bentonite is optimized by addition of certain content of quart sand to improve the strength and heat conductivity without obvious lowering of permeability. Following the recent development trend in deep geological disposal of HLW, compacted bentonite-sand mixtures is recommended by Lanzhou University, China as an innovative buffer/backfill material for its enhanced thermal conductivity and workability.
The final research aim to the compacted bentonite-sand mixtures is to investigate the optimum sand addition, under which the mixtures will provide a best adsorption to radionuclides, impermeability, swelling sealing at same time. As a specific research, objectives of this study is to reveal the swelling characteristics, study on the swelling behavious of compacted GMZ bentonite-sand mixtures with different initial dry density and sand content with different pore water, providing a basal data for final optimum ratio of sand content of the mixtures.
GMZ bentonite-sand mixtures as backfill/buffer material in China for high level radioactive waste (HLW) were mixed with quartz sand in a ratio of0,10,20,30,40and50%(w/w) and compacted to a series of specimens in different dry density. By distilled water as pore water, liquid limit,,plastic limit and swelling tests were conduced on bentonite-sand mixtures pressure and the influence of sand content, initial dry density on the characteriscice of compacted mixtures were analyzed and reported. Liquid limit, plastic limit and the swelling behaviors of compacted GMZ bentonite-sand mixtures inundated in NaCl-Na2SO4solutions are investigated and the influence of chemical solutions on the swelling behaviors of GMZ bentonite-sand mixtures is investigated. The sand content ratios of the bentonite-sand mixtures are0,20,30and50%, and the total dissolved solids (TDS) of the NaCl-Na2SO4(NaCl:Na2SO4=2:1by mass) solution are0.5,1.0,3.0,6.0and12.0g/L (pH=7.1). The specimens of bentonite-sand mixtures for swelling tests are prepared by static-compaction to various dry densities, ranging from1.50-1.90g/cm3.
Results received by these tests were as follows:
Liquid limit and plastic limit of the mixture decrease linearly with the increase of sand addition percentage. Swell occurs in three distinct phases:inter-void swelling, primary swelling and secondary swelling, both swelling pressure and swelling strain follow a sigmoid relationship with time. With constant initial water content, the maximum swelling pressure presents an exponential increase with increased initial dry density, and the maximum swelling strain increases linearly. With the increase of sand content ratio, the maximum swelling pressure decreases exponentially and the maximum swelling strain follow a quadratic decrease.
Liquid limit (wL), plasticity limit (wP), swell time, maximum swelling pressure and maximum swelling strain decrease with the increase of TDS for GMZ bentonite-sand mixtures. All of the LL, PI and maximum swelling strain are decreased exponentially with TDS increase:very quickly as TDS<3.0g/L, slowly as TDS=3.0-6.0g/L and almost stabilized as TDS>6.0g/L. The maximum swelling pressure shows a linear reduction with the TDS increasing, but the pure bentonite indicates a high sensitivity than the bentonite-sand mixtures with30%sand content ratio. Compared with the pure bentonite, bentonite-sand mixtures show a better tolerance withstanding the chemical attack to ground water chemistry because of the replacement of some quantity of expansive clay by quartz sand in the mixtures.
As NaCl-NaoSO4(TDS=0.5g/L) solution was used according to the ground water, with initial dry density of1.70g/cm3, the maximum swelling pressure of specimens decrease exponentially while the maximum strain decrease linearly with the increase of sand addition. With30%sand addition in0.5g/L NaCl-Na2SO4solution, the maximum swelling pressure increase exponentially while the maximum strain increase linearly with the increase of initial dry density. This means that the increase of sand would restrain the swelling properties of bentonite while the increase of initial dry density can enhance that.
By the introduction of the concept, effective clay density pb, equations include both initial dry density and sand content ratio are proposed, they produce a good satisfaction with the experimental data. And these equations can predict the swelling characteristics of GMZ bentonite-sand mixtures with sand content ratio and initial dry density designed in certain range.
Based on the data obtained from experimental tests, considering both swelling pressure and swelling strain comprehensively, the optimal sand content ratio and initial dry density are20-30%and1.60-1.80g/cm3.
近二十多年来,我国就缓冲回填材料的选择进行了大量的研究工作。高庙子膨润土因其优越的吸附性能、膨胀自愈性能以及极低的渗透性被确认为我国理想的缓冲回填材料。但是仅用纯膨润土做缓冲材料存在热传导性能低和可施工性差两个难以克服的弊端,纯膨润土过高的塑性使得加水制样过程中“团粒化”及不均匀湿化现象非常明显,土的可调理性差,试样难以压实到所需的干密度。纯膨润土较低的热传导性不利于将放射性核素衰变产生的热量散发到周围的洞室围岩中去,可能导致缓冲层温度升高超过100℃,液态水气化后产生过大的水汽压力,还有可能导致膨润土的性质改变。膨润土中添加一定量的辅料,比如石英砂或者碎石,既能满足力学强度、热传导性能和防渗阻隔能力,又能优化回填设计与施工性能。开发膨润土-砂混合物作为缓冲回填材料,是世界高放废物地质处置领域的主流方向。在国内,开发膨润土-砂混合型缓冲回填材料,是兰州大学的创新研究方向,也是世界高放废物地质处置领域的主流方向。
混合型缓冲回填材料研究的根本目标,是确定最优掺砂率,使膨润土-砂混合物的的化学吸附性能、力学性能、防渗性能、膨胀自愈性能等尽最大可能地同时得到满足。本研究的具体目标是从膨胀性质方面,研究高庙子(GMZ)膨润土-砂混合物的膨胀性质与掺砂率、干密度以及孔隙液的关系,为最终的掺砂率和干密度优化提供基础数据。
孔隙液为蒸馏水时,对掺砂率分别为0、10、15、20、25、30、35、40和50%的膨润土-砂混合物进行液塑限试验,研究液塑限随掺砂率的变化规律；对掺砂率分别为0、10、20、30、40和50%的膨润土-砂混合物采用动力击实和静力压实两种方法制成的初始干密度不同的一系列试样进行膨胀试验,研究掺砂率和初始干密度对膨胀特性的影响规律。
孔隙液为NaCl-Na2SO4溶液(NaCl与Na2SO4按干质量比2：1配置)时,对掺砂率分别为0、10、15、20、25、30、35、40和50%的膨润土-砂混合物在溶液的总溶解性固体(TDS)分别是0.5、1.0、3.0、6.0和12.0g/L(pH=7.1)进行液塑限试验,研究孔隙液浓度对液塑限的影响规律。对掺砂率为0、20、30和50%,初始干密度为1.50-1.90g/cm3的一系列膨润土-砂混合物的静力压实试样进行膨胀试验,研究孔隙液浓度对混合物膨胀特性的影响规律。
所得试验结果如下：
混合物的液限、塑限随掺砂率的增大线性降低,塑性指数线性降低；膨胀的发生分为三个阶段：孔隙间膨胀,初始膨胀和二次膨胀,膨胀力和膨胀率随时间的曲线都呈S型。当初始含水率一定时,随着初始干密度的增大,最大膨胀力指数增长,最大膨胀率线性增长。随着掺砂率的增大,最大膨胀力指数降低,最大膨胀率呈二次函数降低。
随着NaCl-Na2SO4溶液总溶解性固体(TDS)的增大,GMZ膨润土-砂混合物的液限、塑限、塑性指数、膨胀时间、最大膨胀力和最大膨胀率均降低。其中,随着溶液TDS的增大,液限,塑性指数和最大膨胀率均呈指数降低：当TDS<3.0g/L时,各参数值降低速率都很大；当TDS=3.0-6.0g/L时,各参数值降低速率减慢；当TDS>6.0g/L时,随着TDS的增大,各参数值降低缓慢,基本保持不变。随着溶液TDS的增大,膨润土-砂混合物和纯膨润土的最大膨胀力均线性降低,但是纯膨润土比掺砂30%的膨润土-砂混合物对溶液的敏感性更高。与纯膨润土相比,膨润土-砂混合物中一部分具有膨胀性质的粘土被不具膨胀性的石英砂替代了,从而导致膨润土-砂混合物对地下水化学溶液的侵蚀具有更好的耐受性,
根据中国预选处置库甘肃北山的地下水水文资料并综合考虑之前试验结果,以NaCl-Na2SO4(TDS=0.5g/L)作为孔隙液,对于初始干密度为1.70g/cm3的试样,随着掺砂率的增大,最大膨胀力指数降低最大膨胀率线性降低；对于掺砂率30%的试验,随着初始干密度的增大,最大膨胀力指数增长最大膨胀率线性增长。说明增大掺砂率会抑制膨润土的膨胀性质而增大初始干密度会提高其膨胀性质。
引入了有效粘土的密度的概念,ρb。有效粘土密度可以将初始干密度和掺砂率两个参数统一起来,并且通过对试验数据的分析回归,建立了一定初始含水率条件下,任意掺砂率和初始干密度的GMZ膨润土-砂混合物最大膨胀力／最大膨胀率与有效粘土密度一一对应的归一化模型,从而实现了膨胀性质同时与初始干密度和掺砂率对应的函数关系式,通过数据验证,该方程式与试验数据能够很好的吻合。在一定的掺砂率和初始干密度方位内,利用这些方程式可以实现对GMZ膨润土-砂混合物膨胀行为的预测和人为控制。
结合实际处置情况和要求,通过对试验数据的分析,综合考虑膨胀力和膨胀率,本研究认为基于满足膨胀性质的要求,GMZ膨润土-砂混合物的最优掺砂率范围为20-30%,初始干密度范围为1.60-1.80g/cm3。
High-Level Radioactive Waste (HLW) is a waste very difficult to be disposed, which contains strong radioactive, heat, toxicity, and long half-life nuclides. It must be long-term and reliably isolated with the living environment of the human. The deep geological disposal is currently believed to be the best feasible disposition way, which means that the waste was deeply buried in the ground. A multiple barrier system was accepted as the repository conceptual, in which the buffer/backfill material is the most important barrier to prevent the migration of radionuclides by groundwater.
In the past20years, many researches have been done on the select of backfill/buffer materials in China, and GMZ bentonite is considered to be a reliable buffer/backfill material in HLW repositories because of its high absorption and high swelling properties and low permeability. However, because the plasticity of pure bentonite is very high, a tendency of "pelletization" will present during the process of water-soil mixed, this will cause an obvious inhomogeneous wetting of bentonite, and then give trouble to the block making process of buffer/backfill material. In addition, the heat conductivity of pure bentonite is very low, if the heat produced by radioactive waste can not be sent out to the surrounding rock promptly and effectively, the temperature of the buffer layer will rise. When the temperature exceeds100℃, liquid gasification will produce too much water vapor pressure and affect the stability of the repository. Moreover, montmorillonite in bentonite will be converted into illite when the temperature exceeds100℃, so that the function of the buffer/backfill material changes. For bentonite-and, bentonite-crushed rock or bentonite-ballast mixtures possess higher structural integrity, thermal conductivity. As a modern trend in backfill/buffer material development, bentonite is optimized by addition of certain content of quart sand to improve the strength and heat conductivity without obvious lowering of permeability. Following the recent development trend in deep geological disposal of HLW, compacted bentonite-sand mixtures is recommended by Lanzhou University, China as an innovative buffer/backfill material for its enhanced thermal conductivity and workability.
The final research aim to the compacted bentonite-sand mixtures is to investigate the optimum sand addition, under which the mixtures will provide a best adsorption to radionuclides, impermeability, swelling sealing at same time. As a specific research, objectives of this study is to reveal the swelling characteristics, study on the swelling behavious of compacted GMZ bentonite-sand mixtures with different initial dry density and sand content with different pore water, providing a basal data for final optimum ratio of sand content of the mixtures.
GMZ bentonite-sand mixtures as backfill/buffer material in China for high level radioactive waste (HLW) were mixed with quartz sand in a ratio of0,10,20,30,40and50%(w/w) and compacted to a series of specimens in different dry density. By distilled water as pore water, liquid limit,,plastic limit and swelling tests were conduced on bentonite-sand mixtures pressure and the influence of sand content, initial dry density on the characteriscice of compacted mixtures were analyzed and reported. Liquid limit, plastic limit and the swelling behaviors of compacted GMZ bentonite-sand mixtures inundated in NaCl-Na2SO4solutions are investigated and the influence of chemical solutions on the swelling behaviors of GMZ bentonite-sand mixtures is investigated. The sand content ratios of the bentonite-sand mixtures are0,20,30and50%, and the total dissolved solids (TDS) of the NaCl-Na2SO4(NaCl:Na2SO4=2:1by mass) solution are0.5,1.0,3.0,6.0and12.0g/L (pH=7.1). The specimens of bentonite-sand mixtures for swelling tests are prepared by static-compaction to various dry densities, ranging from1.50-1.90g/cm3.
Results received by these tests were as follows:
Liquid limit and plastic limit of the mixture decrease linearly with the increase of sand addition percentage. Swell occurs in three distinct phases:inter-void swelling, primary swelling and secondary swelling, both swelling pressure and swelling strain follow a sigmoid relationship with time. With constant initial water content, the maximum swelling pressure presents an exponential increase with increased initial dry density, and the maximum swelling strain increases linearly. With the increase of sand content ratio, the maximum swelling pressure decreases exponentially and the maximum swelling strain follow a quadratic decrease.
Liquid limit (wL), plasticity limit (wP), swell time, maximum swelling pressure and maximum swelling strain decrease with the increase of TDS for GMZ bentonite-sand mixtures. All of the LL, PI and maximum swelling strain are decreased exponentially with TDS increase:very quickly as TDS<3.0g/L, slowly as TDS=3.0-6.0g/L and almost stabilized as TDS>6.0g/L. The maximum swelling pressure shows a linear reduction with the TDS increasing, but the pure bentonite indicates a high sensitivity than the bentonite-sand mixtures with30%sand content ratio. Compared with the pure bentonite, bentonite-sand mixtures show a better tolerance withstanding the chemical attack to ground water chemistry because of the replacement of some quantity of expansive clay by quartz sand in the mixtures.
As NaCl-NaoSO4(TDS=0.5g/L) solution was used according to the ground water, with initial dry density of1.70g/cm3, the maximum swelling pressure of specimens decrease exponentially while the maximum strain decrease linearly with the increase of sand addition. With30%sand addition in0.5g/L NaCl-Na2SO4solution, the maximum swelling pressure increase exponentially while the maximum strain increase linearly with the increase of initial dry density. This means that the increase of sand would restrain the swelling properties of bentonite while the increase of initial dry density can enhance that.
By the introduction of the concept, effective clay density pb, equations include both initial dry density and sand content ratio are proposed, they produce a good satisfaction with the experimental data. And these equations can predict the swelling characteristics of GMZ bentonite-sand mixtures with sand content ratio and initial dry density designed in certain range.
Based on the data obtained from experimental tests, considering both swelling pressure and swelling strain comprehensively, the optimal sand content ratio and initial dry density are20-30%and1.60-1.80g/cm3.
引文
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