Two-dimensional reactive transport modeling of the alteration of a fractured limestone by hyperalkaline solutions at Maqarin (Jordan)

Two-dimensional reactive transport modeling of the Maqarin Eastern Springs site, a natural analogue for the alteration of a fractured limestone by high-pH Portland cement waters, has been performed using the CrunchFlow code. These 2D calculations included transport by advection–dispersion–diffusion along a single fracture and diffusion in the wall rock. Solute transport was coupled to mineral dissolution and precipitation. A limited sensitivity analysis evaluated the effect of different values of primary mineral surface areas, flow velocity and sulfate concentration of the inflowing high-pH solution.Major secondary minerals include ettringite–thaumasite, C–S–H/C–A–S–H and calcite. C–S–H/C–A–S–H precipitation is controlled by the dissolution of primary silicates. Ettringite precipitation is controlled by diffusion of sulfate and aluminum from the wall rock to the fracture, with aluminum provided by the dissolution of albite. Calcite precipitation is controlled by diffusion of carbonate from the wall rock. Extents of porosity sealing along the fracture and in the fracture-wall rock interface depend on assumptions regarding flow velocity and composition of the high-pH solution. The multiple episodes of fracture sealing and reactivation evidenced in the fracture infills were not included in the simulations. Results can qualitatively reproduce the reported decrease in porosity in the fractures and in the wall rock next to the fractures. Instances of porosity increase next to fractures caused by carbonate dissolution were not reproduced by the calculations.     

Reactive transport modeling of the interaction between water and a cementitious grout in a fractured rock. Application to ONKALO (Finland)

Grouting of water-conducting fractures with low-alkali cement is foreseen for the potential future repository for spent nuclear fuel in Finland (ONKALO). A possible consequence of the interaction between groundwater and grout is the formation of high-pH solutions which will be able to react with the host rock (gneisses) and alter its mineralogy and porosity. A reactive transport modeling study of this possible alteration has been conducted. First, the hydration of the low-alkali cementitious grout has been modeled, using results from the literature as a guide. The hydrated cement is characterized by the absence of portlandite and the presence of a C-S-H gel with a Ca/Si ratio about 0.8 after tens of years (Ca/Si is about 1.7 in Ordinary Portland Cement). Second, calculations have simulated the interaction between flowing water and grout and the formation of an alkalinity plume, which flows beyond the grouted section of the fracture. The calculations include the hydration and simultaneous leaching of the grout through diffusive exchange between the porewater in the grout and the flowing water in the fracture. The formation of an alkaline plume is extremely limited when the low-pH grout is used. Even when using a grout with a lower silica fume content, the extent and magnitude of the alkaline plume is quite minor. These results are in qualitative agreement with monitoring at ONKALO.     

Mineralogical alteration and associated permeability changes induced by a high-pH plume: Modeling of a granite core infiltration experiment

Within the framework of the HPF project (Hyperalkaline Plume in Fractured Rock) at the Grimsel Test Site (Switzerland), a small scale core infiltration experiment was performed at the University of Bern. A high-pH solution was continuously injected, under a constant pressure gradient, into a cylindrical core of granite containing a fracture. This high-pH solution was a synthetic version of solutions characteristic of early stages in the degradation of cement. The interaction between the rock and the solutions was reflected by significant changes in the composition of the injected solution and a decrease in the permeability of the rock. Changes in the mineralogy and porosity of the fault gouge filling the fracture were only minor. One-dimensional reactive transport modeling, using a modified version of the GIMRT code, was used to interpret the results of the experiment. Dispersive and advective solute transport, mineral reaction kinetics and a coupling between porosity and permeability changes were taken into account. In order to obtain a reasonable agreement between models and experimental results, reactive surface areas of the order of 10⁵ m²/m³ rock had to be used. These values are much smaller than the values measured for the fault gouge filling the fracture, which are in the order of 10⁶–10⁷ m²/m³ rock. However, the results could be improved by adding a small fraction of fine grained mineral, which could explain the high initial peaks in Al and Si concentration. With the inclusion of this fine grained fraction, the initial surface areas in the model were within the range of the measured specific surface areas of the fault gouge. The fact that the decrease in permeability was significant despite the minor changes in mineralogy, suggests that permeability may be controlled by changes in the structure of the rock (pore geometries) rather than by only the bulk volumetric (porosity) changes.     

裂隙岩体渗透系数确定方法研究

裂隙岩体渗透系数以及渗透主方向的确定对研究岩体渗透性大小及各向异性具有重要意义。高放废物地质处置库介质岩体的渗透性能将直接影响其使用安全性。本文运用离散裂隙网络模拟的方法对我国高放废物处置库甘肃北山预选区3#钻孔附近裂隙岩体进行了渗透性质分析。通过对3#钻孔171.5~178.0m段压水试验数据的反演,标定了离散裂隙网络渗流模型中的裂隙渗透参数(导水系数T)。利用标定的离散裂隙网络模型对场区裂隙岩体进行了渗流模拟,确定了该区域裂隙岩体的渗流表征单元体(REV)的尺寸大小以及渗透主值和主渗透方向。运用离散裂隙网络模型计算得出的渗透主值的几何均值与现场压水试验计算结果较接近,证明了计算结果的有效性。     

Scoping analyses of the coupled thermal-hydrological-mechanical behaviour of the rock mass around a nuclear fuel waste repository

Scoping calculations were performed in order to assess the influence of radiogenic heat on the performance of the rock mass around a nuclear fuel waste repository. The full coupling between the thermal, mechanical and hydrological processes involved was considered by using the finite element code, FRACON, developed through an extension of Biot's classical theory of soil consolidation. By considering the full T---H---M coupling, several important safety features, which would otherwise be omitted in uncoupled analyses, were detected in the present study. In particular, it was shown that the heat-induced pore pressure increase around the repository has the potential to significantly increase the rate of groundwater flow, and affect the structural integrity of the rock mass.     

Methodology for bounding calculations of nuclear criticality of fissile material accumulations external to a waste container at Yucca Mountain, Nevada

The possibility of nuclear criticality, however remote, in the vicinity of the proposed repository at Yucca Mountain, Nevada generates justified concerns and may impact the performance of the repository. A heuristic approach is presented here for determining the amount, spatial distribution and other characteristics of fissile material accumulation in the rock beneath a waste package that could contribute to such an event. This study is concerned primarily with waste packages containing special spent fuel from the Department of Energy and high-level nuclear waste glass. Mixing with less alkaline waters and the subsequent drop in pH is the mechanism that is most efficient for precipitating fissile material from the waste package internal leachate, in contrast to natural deposits in which redox changes are the main precipitation driver. External accumulation size is determined by (1) computing the chemical composition of the leachate leaving a package as its internal materials degrade (with the batch geochemical code EQ3/6), (2) determining precipitation of fissile material into mineral phases (using the 1D geochemical code PHREEQC) as the effluent mixes with percolation water, and (3) heuristically scaling results to a 3D volume and computing the criticality coefficient (using the code MCNP). Loci for accumulation are the multiple lithophysal cavities and the fracture system. A bounding conservative approach is used by necessity in Step 3. Nuclear criticality is sensitive to small variations in the distribution of fissile material and parameters of natural systems vary by orders of magnitude. Because the most likely combinations of parameters are not conducive to nuclear criticality, this study focuses on extreme values of parameter probabilistic distributions, such as limited flow into the package associated with a large percolation rate, combinations of material degradation rates favoring actinide release, and very high host-rock porosity values. By considering these combinations, most favorable to criticality but unlikely, it was concluded that external nuclear criticality is not a concern at the proposed repository.     

松辽盆地营城组火山岩储层流动单元特征和控制因素

根据孔隙度、渗透率、储层品质指数(RQI)、流动层带指数(FZI)4个参数对XS1井区白垩系营城组火山岩的388个样品进行聚类分析,通过对聚类结果与各井产气情况的对比将储层流动单元划分为4类,所占比例依次为39.2%(Ⅲ类)、33.2%(Ⅱ类)、25.0%(Ⅰ类)、2.6%(Ⅳ类)。Ⅰ类储层流动单元多为高孔高渗、高孔中渗和中孔高渗储层,厚度范围为10～20m;Ⅱ类储层流动单元多为中孔高渗、高孔中渗和低孔高渗储层,厚度范围为10～47m;Ⅲ类储层流动单元多为中孔高渗、中孔低渗和低孔中渗储层,厚度范围为11～86m;Ⅳ类储层流动单元为低孔低渗和特低孔特低渗储层,厚度小于10m。火山岩储层流动单元发育和分布受火山机构相带和火山岩亚相的控制,表现为火山口-近火山口相带成为Ⅰ、Ⅱ类储层流动单元的机率最大,近源相带成为Ⅱ、Ⅲ类储层流动单元的机率最大,远源相带成为Ⅲ类和Ⅳ类储层流动单元的机率最大。原生气孔发育的上部亚相和粒间孔发育的热碎屑流亚相形成Ⅰ类储层流动单元的机率最大,原生孔隙不发育的空落亚相和下部亚相形成Ⅲ类储层流动单元的机率大。实现了火山岩储层流动单元的单井识别,为其三维模型的建立提供依据。     

应力腐蚀和压力溶解作用下双重孔隙岩体中 THMM耦合过程的有限元分析

在使用Yasuhara等建立的裂隙开度的应力腐蚀和压力溶解模型的基础上,将溶质浓度场引入笔者已开发的双重孔隙-裂隙介质热-水-应力耦合的二维有限元分析程序中,针对一个假设的位于非饱和岩体中且有核素泄漏的高放废物地质处置库,拟定2种计算工况：（1）裂隙开度随应力腐蚀和压力溶解而变化（基岩的孔隙率亦是应力的函数）;（2）裂隙开度和基岩的孔隙率均为常数,进行热-水-应力-迁移耦合的数值模拟,考察了岩体中的温度、裂隙开度的闭合速率、闭合量、孔（裂）隙水压力、地下水流速、核素浓度和应力的变化、分布等情况。结果主要显示：应力腐蚀引起的闭合速率要高于压力溶解引起的闭合速率6个数量级,且两种因素产生的闭合速率随时间先增加后减小,并趋于稳定;当考虑应力腐蚀和压力溶解时,近场的负裂隙水压力上升很高;工况1中裂隙开度和孔隙率减小,使得相应的渗透系数降低,故该工况的裂隙和孔隙中核素浓度较工况2为高;由于不计入负的孔（裂）隙水压力对应力平衡的影响,2种工况的岩体中的应力量值及分布基本相同。     

鄂尔多斯盆地南部上古生界低孔低渗砂岩储层成岩作用特征研究

对鄂尔多斯盆地南部山西组二段—下石盒子组八段储层砂岩的岩石学特征、孔隙类型与物性特征、胶结物种类及成岩作用特点的详细研究表明:山西组二段—下石盒子组八段砂岩的主要孔隙类型大部分是与胶结物和泥质杂基有关的微孔隙,也是造成研究区砂岩储层低孔低渗的内在原因之一。砂岩主要的成岩作用包括机械压实作用、胶结作用、溶蚀溶解作用。压实作用是成岩早期导致砂岩储层质量变差的主要原因之一;胶结作用包括硅质胶结、钙质胶结和粘土矿物胶结,硅质胶结对储层物性的贡献大于其他胶结类型,方解石是造成储层物性降低的主要胶结物;煤系地层埋藏后提供的酸性孔隙流体造成早期长石和方解石的溶蚀溶解,形成次生孔隙,对早期储层物性起到了一定的改善作用,但由于后期强烈的方解石胶结作用而消失殆尽。     

High-pH plume from low-alkali-cement fracture grouting: Reactive transport modeling and comparison with pH monitoring at ONKALO (Finland)

Grouting of water-conducting fractures with low-alkali cement is foreseen for the potential future repository for spent nuclear fuel in Finland (ONKALO site). A possible consequence is the formation of high-pH solutions which will be able to react with the host rock. Calculations have been performed including the hydration and simultaneous leaching of the grout. The effect of different possible groundwater compositions has been studied. The results show that after grouting, the duration of the initial high-pH peak is short (<0.5 a), which compares well with observations at a test borehole. Magnesium in the groundwater induces the precipitation of brucite at the grout–fracture interface, which consumes OH⁻. In the longer term, the results show a gradually decaying pH tail (pH < 9) controlled by the precipitation of calcite at the grout–fracture interface. The duration of this tail correlates inversely with the carbonate content of the inflowing groundwater.     

甘肃酒泉盆地青西油田裂缝特征及成因分析

甘肃酒泉盆地青西油田泥砾岩相和泥云岩相储层中发育两种裂缝系统。采用多种方法,系统研究了不同岩相区裂缝的产状特征、电性响应特征和物性特征,并重点分析了控制裂缝形成的成岩演化成因。研究结果表明:泥砾岩相中发育有砾缘缝、粒内溶蚀缝和构造裂缝;泥云岩相中发育层面溶蚀缝、泄水裂缝及构造裂缝。裂缝系统不但对储层渗流能力有较大程度的改善,而且也具有一定程度的储集能力。母岩矿物的选择性（差异）溶蚀是控制本区裂缝和次生孔隙发育的主要因素：泥砾岩成分复杂,各种碎屑物及胶结物之间的交代、溶蚀以及不稳定碎屑颗粒的选择性（差异）溶蚀是砾缘缝、成岩溶蚀缝及大量次生孔隙在泥砾岩储层中形成的主要原因;泥云岩中存在的二元和三元纹层结构从根本上决定了裂缝的发育程度,碳酸钙的白云岩化和沸石化是层面溶蚀缝形成的主要成岩作用。     

稀疏不规则裂隙岩体模型三维水流-传热对温度和应力影响的试验研究

选取高放射核废物处置库重要预选场区甘肃北山地区的花岗岩,制作750 mm（宽）×300 mm（厚）×1 000 mm（高）的稀疏不规则裂隙岩体模型,该模型由18块花岗岩和竖向与斜向各两条裂隙组成,在裂隙及岩石内部埋置温度传感器、水压计、直角应变花,并在模型一侧设置局部热源,研究热源温度和裂隙水流速对岩石温度和应力的影响。结果表明,竖裂隙水主要从顶部进水口流向底部出水口,斜裂隙水主要从侧部进水口流向侧部出水口,竖裂隙与斜裂隙在交汇处存在微小流量交换;由于热源处在两条斜裂隙进水口之间,并且斜裂隙长度小于竖裂隙,岩石热传导与斜裂隙水流对岩石温度分布起控制作用,竖裂隙水流对岩石横向热传导起阻滞作用;由于热传导和水流传热的不规则性,上层岩石形成从左向右为主的传热路径,中层和下层岩石形成从上向下为主的传热路径;由于上、下层岩石温度梯度较小,岩石收缩受热拉应力,而中层岩石温度梯度较大,岩石膨胀受热压应力,大主应力的方向大致垂直于斜裂隙面与竖裂隙面的交线,岩石应力增量随斜平面方向的温度梯度增大而增大;热源温度越高,裂隙水流速越低,岩石温度越高、岩石应力越大,系统达到稳态需要的时间越长。     

Simulating Oxygen Intrusion into Highly Heterogeneous Fractured Media Using High Performance Computing

Fractured crystalline rocks are under consideration by several countries as host formations for high-level nuclear waste repositories. The redox evolution in these host rock formations is an important issue for the stability and safety of these disposal sites. If, for example, during a glaciation/deglaciation event, oxygen-rich glacial meltwater penetrates to the depth of the planned repository, some of the engineered barriers would be adversely affected. Moreover, oxidizing conditions would increase the solubility and mobility of many radionuclides. Reactive transport simulations, which are typically used to assess the redox buffering capacity of these host rock formations, are computationally demanding, and thus, calculations for the evaluation of oxygen penetration are usually carried out over simplified geometries and the heterogeneity of the site, both physical (e.g., variability in the groundwater flow field and the kinematic porosity) and mineralogical (e.g., variability in the abundance of Fe(II)-bearing minerals), is usually represented in a simplified fashion. Here, it is shown how a recently developed numerical framework, combined with high performance computing technologies, allows the full geometrical, physical and mineralogical complexity of the site under study to be efficiently included in these types of reactive transport calculations. A synthetically generated realistic three-dimensional fractured medium is used to assess oxygen penetration patterns and their dependence on both the hydrogeological conditions and the availability of Fe(II)-bearing minerals. The results of the calculations point out the significant influence of both physical and mineralogical heterogeneity on the oxygen penetration patterns, thus highlighting the importance of a model parameterisation consistent with the site complexity.     

米尺度裂隙岩体模型水流-传热试验的数值模拟分析

为了研究高放射性核废物地下处置库近场的水流-传热耦合问题,采用国内高放废物地下处置库预选场址--甘肃北山地区的花岗岩石块体,加工组合成米尺度的规则裂隙岩体模型,设置边界热源和裂隙水流,试验模拟裂隙水水流与传热之间的相互作用。作为该室内模型试验的前期理论研究,采用等效孔隙介质数值模型,着重分析了裂隙开度、裂隙流量和热源功率对流场和温度场的影响。在设定条件下,计算分析表明：热传导和裂隙水水流由热源作用初期的不耦合很快转化为耦合;不流动的裂隙水主要表现为热存储和热传导,而流动的裂隙水还引起流动传热和水与岩石之间的对流换热,使岩体温度场明显不同于单纯热传导的情况;如果保持裂隙水流量不变,则裂隙开度的变化对水流-传热影响不大;如果保持裂隙水流速不变,则裂隙开度的变化对水流-传热影响显著;热源功率越大,通过裂隙水的热流量越大,裂隙水压强越大,而当温度超过100 ℃时,裂隙水会因汽化而压强显著增大;加热7 d时,热量的输入和输出几乎相等,裂隙水流带走的热量接近热源供给的热量,模型系统基本达到了热平衡。     

A natural cement analogue study to understand the long-term behaviour of cements in nuclear waste repositories: Maqarin (Jordan)

The geological storage of nuclear waste includes multibarrier engineered systems where a large amount of cement-based material is used. Predicting the long term behaviour of cement is approached by reactive transport modelling, where some of the boundary conditions can be defined through studying natural cement analogues (e.g. at the Maqarin natural analogue site). At Maqarin, pyrometamorphism of clay biomicrites and siliceous chalks, caused by the in-situ combustion of organic matter, produced various clinker minerals. The interaction of infiltrating groundwater with these clinker phases resulted in a portlandite-buffered hyperalkaline leachate plume, which migrated into the adjacent biomicrite host rock, resulting in the precipitation of hydrated cement minerals.In this study, rock samples with different degrees of interaction with the hyperalkaline plume were investigated by various methods (mostly SEM-EDS). The observations have identified a paragenetic sequence of hydrous cement minerals, and reveal how the fractures and porosity in the biomicrite have become sequentially filled. In the alkaline disturbed zone, C-A-S-H (an unstoichiometric gel of Ca, Al, Si and OH) is observed to fill the pores of the biomicrite wallrock, as a consequence of reaction with a high pH Ca-rich fluid circulating in fractures. Porosity profiles indicate that in some cases the pores of the rock adjacent to the fractures became tightly sealed, whereas in the veins some porosity is preserved. Later pulses of sulphate-rich groundwater precipitated ettringite and occasionally thaumasite in the veins, whereas downstream in the lower pH distal regions of the hyperalkaline plume, zeolite was precipitated.Comparing our observations with the reactive transport modelling results reveals two major discrepancies: firstly, the models predict that ettringite is precipitated before C-A-S-H, whereas the C-A-S-H is observed as the earlier phase in Maqarin; and, secondly, the models predict that ettringite acts as the principal pore-filling phase in contrast to the C-A-S-H observed in the natural system. These discrepancies are related to the fact that our data were not available at the time the modelling studies were performed. However, all models succeeded in reproducing the porosity reduction observed at the fracture–rock interface in the natural analogue system.     

热-水-应力耦合影响的有限元分析

为了考虑应力拉压和压力（化学）溶解对裂隙开度的综合影响,对所建立的双重孔隙-裂隙介质热-水-应力耦合模型中裂隙开度的计算模型作了改进。通过一个假定的高放废物地质处置库算例,就岩体裂隙开度变化的3种工况,分析了岩体中的温度、孔（裂）隙水压力、地下水流速和主应力的变化、分布情况。结果显示：3种工况的计算域中温度场基本相同;孔（裂）隙水渗流场形态相似,但其量值有一定差别;工况1的裂隙开度在应力和压力（化学）溶解的共同作用下闭合量最大,负孔（裂）隙水压力增值最高;核废物的释热效应明显地改变了岩体自重应力场的水平分量,但对其垂直分量影响较小。     

Erosion of bentonite particles at the interface of a compacted bentonite and a fractured granite

Compacted bentonite has been considered as a candidate buffer material in the underground repository for the disposal of high-level radioactive waste. An erosion of bentonite particles caused by a groundwater flow at the interface of a compacted bentonite and a fractured granite was studied experimentally under various geochemical conditions. The experimental results showed that bentonite particles could be eroded from a compacted bentonite buffer by a flowing groundwater depending upon the contact time, the flow rate of the groundwater, and the geochemical parameters of the groundwater such as the pH and ionic strength.

A gel formation of the bentonite was observed to be a dominant process in the erosion of bentonite particles although an intrusion of bentonite into a rock fracture also contributed to the erosion. The concentration of the eroded bentonite particles eroded by a flowing groundwater was increased with an increasing flow rate of the groundwater. It was observed from the experiments that the erosion of the bentonite particles was considerably affected by the ionic strength of a groundwater although the effect of the pH was not great within the studied pH range from 7 to 10. An erosion of the bentonite particles in a natural groundwater was also observed to be considerable and the eroded bentonite particles are expected to be stable at the given groundwater condition.

The erosion of the bentonite particles by a flowing groundwater did not significantly reduce the physical stability and thus the performance of a compacted bentonite buffer. However, it is expected that an erosion of the bentonite particles due to a groundwater flow will generate bentonite particles in a given groundwater condition, which can serve as a source of the colloids facilitating radionuclide migration through rock fractures.     

A methodology to constrain the parameters of a hydrogeological discrete fracture network model for sparsely fractured crystalline rock,exemplified by data from the proposed high-level nuclear waste repository site at Forsmark,Sweden

The large-scale geological structure of the crystalline rock at the proposed high-level nuclear waste repository site at Forsmark, Sweden, has been classified in terms of deformation zones of elevated fracture frequency. The rock between deformation zones was divided into fracture domains according to fracture frequency. A methodology to constrain the geometric and hydraulic parameters that define a discrete fracture network (DFN) model for each fracture domain is presented. The methodology is based on flow logging and down-hole imaging in cored boreholes in combination with DFN realizations, fracture connectivity analysis and pumping test simulations. The simulations suggest that a good match could be obtained for a power law size distribution where the value of the location parameter equals the borehole radius but with different values for the shape parameter, depending on fracture domain and fracture set. Fractures around 10–100 m in size are the ones that typically form the connected network, giving inflows in the simulations. The report also addresses the issue of up-scaling of DFN properties to equivalent continuous porous medium (ECPM) bulk flow properties. Comparisons with double-packer injection tests provide confidence that the derived DFN formulation of detailed flows within individual fractures is also suited to simulating mean bulk flow properties and their spatial variability.