A contribution to risk analysis for leakage through abandoned wells in geological CO2 storage

The selection and the subsequent design of a subsurface CO₂ storage system are subject to considerable uncertainty. It is therefore important to assess the potential risks for health, safety and environment. This study contributes to the development of methods for quantitative risk assessment of CO₂ leakage from subsurface reservoirs. The amounts of leaking CO₂ are estimated by evaluating the extent of CO₂ plumes after numerically simulating a large number of reservoir realizations with a radially symmetric, homogeneous model. To conduct the computationally very expensive simulations, the ‘CO₂ Community Grid’ was used, which allows the execution of many parallel simulations simultaneously. The individual realizations are set up by randomly choosing reservoir properties from statistical distributions. The statistical characteristics of these distributions have been calculated from a large reservoir database, holding data from over 1200 reservoirs. An analytical risk equation is given, allowing the calculation of average risk due to multiple leaky wells with varying distance in the surrounding of the injection well. The reservoir parameters most affecting risk are identified. Using these results, the placement of an injection well can be optimized with respect to risk and uncertainty of leakage. The risk and uncertainty assessment can be used to determine whether a site, compared to others, should be considered for further investigations or rejected for CO₂ storage.     

CO2/CaCl2 solution interfacial tensions under CO2 geological storage conditions: Influence of cation valence on interfacial tension

The effectiveness of CO₂ storage in deep saline aquifers and hydrocarbon reservoirs is governed, among other factors, by the interfacial tension between the injected CO₂ and formation water (brine). Experimental data on CO₂/water and CO₂/NaCl solution have revealed that the interfacial tension depends on the pressure, temperature and water salinity. However, there is still a lack of data for other salts (such as MgCl₂ and CaCl₂) which are also present in aquifers and carbonate reservoirs.     

A stochastic model for daily subsurface CO2 concentration and related soil respiration

Near-surface soil CO₂ gas-phase concentration (C) and concomitant incident rainfall (P_i) and through-fall (P_t) depths were collected at different locations in a temperate pine forest every 30 min during the 2005 and 2006 growing seasons (and then averaged to the daily timescale). At the daily scale, C temporal variations were well described by a sequence of monotonically decreasing functions interrupted by large positive jumps induced by rainfall events. A stochastic model was developed to link rainfall statistics responsible for these jumps to near-surface C dynamics. The model accounted for the effect of daily rainfall variability, both in terms of timing and amount of water, and permitted an analytical derivation of the C probability density function (pdf) using the parameters of the rainfall pdf. Given the observed positive correlation between daily C and soil CO₂ fluxes to the atmosphere (F_s), the effects of various rainfall regimes on the statistics of F_s can be deduced from the behavior of C under different climatic conditions. The predictions from this analytical model are consistent with flux measurements reported in manipulative experiments that varied rainfall amount and frequency.     

Geochemical features of the geothermal CO2-watercarbonate rock system and analysis on its CO2 sources

Taking Huanglong Ravine and Kangding, Sichuan, and Xiage, Zhongdian, Yunnan, as examples, the authors summarize the hydrogeochemical and carbon stable isotopic features of the geothermal CO₂-water-carbonate rock system and analyze the CO₂ sources of the system. It was found that the hydrogeochemical and carbon stable isotopic features of such a system are different from those of shallow CO₂-water-carbonate rock system, which is strongly influenced by biosphere. The former has higher CO₂ partial pressure, and is rich in heavy carbon stable isotope. In addition, such a geothermal system is also different from that developed in igneous rock. The water in the latter system lacks Ca²⁺, and thus, there are few tufa deposits on ground surface, but it is rich in light carbon stable isotope. Further analysis shows that CO₂ of the geothermal CO₂-water-carbonate rock system is a mixture of metamorphic CO₂ and magmatic CO₂.     

Numerical modeling of formation damage by two-phase particulate transport processes during CO2 injection in deep heterogeneous porous media

Prediction of CO₂ injection performance in deep subsurface porous media relies on the ability of the well to maintain high flow rates of carbon dioxide during several decades typically without fracturing the host formation or damaging the well. Dynamics of solid particulate suspensions in permeable media are recognized as one major factor leading to injection well plugging in sandstones. The invading supercritical liquid-like fluid can contain exogenous fine suspensions or endogenous particles generated in situ by physical and chemical interactions or hydrodynamic release mechanisms. Suspended solids can plug the pores possibly leading to formation damage and permeability reduction in the vicinity of the injector. In this study we developed a finite volume simulator to predict the injectivity decline near CO₂ injection wells and also for production wells in the context of enhanced oil recovery. The numerical model solves a system of two coupled sets of finite volume equations corresponding to the pressure-saturation two-phase flow, and a second subsystem of solute and particle convection-diffusion equations. Particle transport equations are subject to mechanistic rate laws of colloidal, hydrodynamic release from pore surfaces, blocking in pore bodies and pore throats, and interphase particle transfer. The model was validated against available laboratory experiments at the core scale. Example results reveal that lower CO₂ residual saturation and formation porosity enhance CO₂-wet particle mobility and clogging around sinks and production wells. We conclude from more realistic simulations with heterogeneous permeability spanning several orders of magnitude that the control mode of mobilization, capture of particles, and permeability reduction processes strongly depends on the type of permeability distribution and connectivity between injection and production wells.     

Upscaling of CO2 vertical migration through a periodic layered porous medium: The capillary-free and capillary-dominant cases

We present an upscaled model for the vertical migration of a CO₂ plume through a vertical column filled with a periodic layered porous medium. This model may describe the vertical migration of a CO₂ plume in a perfectly layered horizontal aquifer. Capillarity and buoyancy are taken into account and semi-explicit upscaled flux functions are proposed in the two following cases: (i) capillarity is the main driving force and (ii) buoyancy is the only driving force. In both cases, we show that the upscaled buoyant flux is a bell-shaped function of the saturation, as in the case of a homogeneous porous medium. In the capillary-dominant case, we show that the upscaled buoyant flux is the harmonic mean of the buoyant fluxes in each layer. The upscaled saturation is governed by the continuity of the capillary pressure at the interface between layers. In the capillary-free case, the upscaled buoyant flux and upscaled saturation are determined by the flux continuity condition at the interface. As the flux is not continuous over the entire range of saturation, the upscaled saturation is only defined where continuity is verified, i.e. in two saturation domains. As a consequence, the upscaled buoyant flux is described by a piecewise continuous function. Two analytical approximations of this flux are proposed and this capillary-free upscaled model is validated for two cases of heterogeneity. Upscaled and cell averaged saturations are in good agreement. Furthermore, the proposed analytical upscaled fluxes provide satisfactory approximations as long as the saturation set at the inlet of the column is in a range where analytical and numerical upscaled fluxes are close.     

The oxygen minimum zone (OMZ) off Chile as intense source of CO2 and N2O

The oxygen minimum zones (OMZs) are recognized as intense sources of N₂O greenhouse gas (GHG) and could also be potential sources of CO₂, the most important GHG for the present climate change. This study evaluates, for one of the most intense and shallow OMZ, the Chilean East South Pacific OMZ, the simultaneous N₂O and CO₂ fluxes at the air–sea interface. Four cruises (2000–2002) and 1 year of monitoring (21°–30°–36°S) off Chile allowed the determination of the CO₂ and N₂O concentrations at the sea surface and the analysis of fluxes variations associated with different OMZ configurations. The Chilean OMZ area can be an intense GHG oceanic local source of both N₂O and CO₂. The mean N₂O fluxes are 5–10 times higher than the maximal previous historical source in an OMZ open area as in the Pacific and Indian Oceans. For CO₂, the mean fluxes are also positive and correspond to very high oceanic sources. Even if different coupling and decoupling between N₂O and CO₂ are observed along the Chilean OMZ, 65% of the situations represent high CO₂ and/or N₂O sources. The high GHG sources are associated with coastal upwelling transport of OMZ waters rich in N₂O and probably also in CO₂, located at a shallow depth. The integrated OMZ role on GHG should be better considered to improve our understanding of the past and future atmospheric CO₂ and N₂O evolutions.     

微囊藻CO2-浓缩机制基因型的动态变化及其对CO2的竞争效应

由于具有高效的CO₂-浓缩机制,蓝藻在低CO₂浓度条件下具有竞争优势。然而,随着大气中CO₂浓度急剧增加,蓝藻CO₂-浓缩机制如何响应的研究较少。因此,本文以常见水华蓝藻——微囊藻为研究对象,通过对滇池微囊藻水华动态及不同CO₂-浓缩机制基因型进行监测,探讨蓝藻CO₂-浓缩机制基因的微进化特征及其动态变化。同时,设置高(0.08%)、中(0.04%)、低(0.02%)CO₂浓度(V/V)进一步揭示微囊藻不同CO₂-浓缩机制基因微进化对CO₂的竞争效应。结果表明:滇池无机碳浓度在4个采样点存在空间差异性,均呈现先降低后升高的趋势,并以HCO₃^-为主要无机碳存在形式。调查期间,东大河、观音山、洛龙河和生态所4个采样点的微囊藻均以sbtA基因型占绝对优势,相对丰度远高于bicA基因型。在不同水华时期,bicA基因型和sbtA基因型呈现相反的变化趋势,即从...     

三峡水库澎溪河消落区土-气界面CO2和CH4通量初探

水库近岸湿地(消落区)温室气体(CO₂、CH₄)产汇是水库温室气体效应问题的重要组成部分.本文以三峡水库支流澎溪河的白家溪、养鹿两处大面积消落区为研究对象,于2010年6 9月水库低水位运行期间,对近岸消落区土-气界面CO₂、CH₄通量进行监测.白家溪消落区土-气界面CO₂通量均值为12.38±2.42 mmol/(m²·h);CH₄通量均值为0.0112±0.0064 mmol/(m²·h).养鹿消落区CO₂、CH₄通量均值分别为10.54±5.17、0.14±0.16 mmol/(m²·h).总体上,6 9月土-气界面CO₂通量呈增加趋势,而CH₄通量水平呈现显著的递减趋势.消落区土地出露后植被恢复,在一定程度上促进了土壤有机质含量的增加,使得6 9月CO₂释放通量的总体趋势有所增加.消落区退耕后,其甲烷氧化菌的活性得到恢复,加之在土地出露曝晒过程中土壤透气性增强,使得消落区土壤对大气中CH₄吸收氧化潜势增强.尽管如此,仍需进一步的研究以明晰消落区土-气界面CO₂、CH₄产汇的主要影响因素.     

Effects of CO2 on benthic biota: An in situ benthic chamber experiment in Storfjorden (Norway)

Carbon capture and storage (CCS) methods, either sub-seabed or in ocean depths, introduces risk of CO₂ leakage and subsequent interaction with the ecosystem. It is therefore important to obtain information on possible effects of CO₂. In situ CO₂ exposure experiments were carried out twice for 10 days during 2005 using a Benthic Chamber system at 400 m depth in Storfjorden, Norway. pCO₂ in the water above the sediment in the chambers was controlled at approximately 500, 5000 and 20,000 μatm, respectively. This article describes the experiment and the results from measured the biological responses within the chamber sediments. The results show effects of elevated CO₂ concentrations on biological processes such as increased nanobenthos density. Methane production and sulphate reduction was enhanced in the approximately 5000 μatm chamber.     

Modeling vertical stratification of CO2 injected into a deep layered aquifer

The vertical stratification of carbon dioxide (CO₂) injected into a deep layered aquifer made up of high-permeability and low-permeability layers, such as Utsira aquifer at Sleipner site in Norway, is investigated with a Buckley–Leverett equation including gravity effects. In a first step, we study both by theory and simulation the application of this equation to the vertical migration of a light phase (CO₂), in a denser phase (water), in 1D vertical columns filled with different types of porous media: homogeneous, piecewise homogeneous, layered periodic and finally heterogeneous. For each case, we solve the associated Riemann problems and propose semi-analytical solutions describing the spatial and temporal evolution of the light phase saturation. These solutions agree well with simulation results. We show that the flux continuity condition at interfaces between high-permeability and low-permeability layers leads to CO₂ saturation discontinuities at these interfaces and, in particular, to a saturation increase beneath low-permeability layers. In a second step, we analyze the vertical migration of a CO₂ plume injected into a 2D layered aquifer. We show that the CO₂ vertical stratification under each low-permeability layer is induced, as in 1D columns, by the flux continuity condition at interfaces. As the injection takes place at the bottom of the aquifer the velocity and the flux function decrease with elevation and this phenomenon is proposed to explain the stratification under each mudstone layer as observed at Sleipner site.     

Interfacial tension measurements and wettability evaluation for geological CO2 storage

Interfacial interactions, namely interfacial tension, wettability, capillarity and interfacial mass transfer are known to govern fluid distribution and behavior in porous media. Therefore the interfacial interactions between CO₂, brine and oil and/or gas reservoirs have a significant influence on the effectiveness of any CO₂ storage operations. However, data and knowledge of interfacial properties in storage conditions are scarce. This issue becomes particularly true in the case of deep saline aquifers where limited, economically driven, data collection and archiving are available. In this paper, we present a complete set of brine–CO₂ interfacial tension data at pressure, temperature and salinity conditions, representative of a CO₂ storage operation. A semi-empirical correlation is proposed to calculate the interfacial tension from the experimental data. Wettability is studied at pore scale, using glass micromodels in order to track fluids distribution as a function of the thermodynamic properties and wettability conditions for water–CO₂ systems. With this approach, we show that, in strongly hydrophilic porous media, the CO₂ does not wet the solid surface whereas; if the porous media has less hydrophilic properties the CO₂ significantly wets the surface.     

夏季金沙江下游水-气界面CO2、CH4通量特征初探

河流是连接大陆和海洋两大碳库的桥梁,在全球碳循环中的作用举足轻重.金沙江作为长江的上游段,对区域碳循环及区域化学风化的影响非常重要.于2015年8月8-18日对金沙江下游水-气界面CO_2与CH_4通量特征进行监测与分析.采用顶空平衡法结合薄边界层模型估算法计算表层水体CO_2与CH_4的分压以及水-气界面的交换通量,并分析环境变量与其之间的相关性.研究发现,金沙江下游表层水体p(CO_2)平均值为2724.84±477.18μatm,表层水体p(CH_4)平均值为59.96±6.74μatm;水-气界面CO_2通量平均值为2.24±0.50 mmol/(m2·h),CH_4通量平均值为0.000163±0.00009 mmol/(m2·h),通量与分压趋势基本保持一致.表层水体p(CO_2)与溶解性无机碳浓度、碱度均呈显著正相关,而p(CH_4)与水温、叶绿素a浓度均呈显著正相关,CO_2通量与p(CO_2)、溶解性无机碳浓度、碱度均呈正相关,CH_4通量与p(CH_4)、风速均呈正相关,其他环境因素对通量的影响不明显,仍需进一步研究.金沙江下游水-气界面CH_4扩散通量较低,而CO_2扩散通量在世界主要河流中属于中等水平.     

Variations of near-surface atmospheric CO2 and H2O concentrations during summer on Muztagata

Expeditions during the summers of 2002 and 2003 implemented continuous monitoring of near-surface (2 m height) atmospheric CO₂ and H₂O concentrations at the 4500 m elevation on Muztagata. The resultant data sets reveal a slight decrease of CO₂ concentrations (of about 5 μmol·mol^-1) and changes in the diurnal variations from the end of June to the middle August. The daily maximum CO₂ concentrations occur between 02:30-05:30 AM (local time) and the minimum levels occur between 12:00-15:30 PM. The atmospheric CO₂ concentrations in the summer of 2002 were around 5 μmol·mol^-1 lower than those during the same period of 2003, whereas the diurnal amplitude was higher. In contrast, we found that the daily mean atmospheric H₂O content in 2003 was much lower than that in 2002 and there exists a striking negative correlation between CO₂ and H₂O concentrations. We therefore suggest that the near-surface atmospheric CO₂ concentration is affected not only by photosynthesis and respiration, but also by the air H₂O content in the glaciated region around Muztagata.     

Diffuse CO2 emission rate from Pululahua and the lake-filled Cuicocha calderas,Ecuador

We report herein the first results of two soil CO₂ efflux surveys carried out at Cuicocha lake-filled and Pululahua caldera volcanic systems, Ecuador. A total of 172 and 217 soil CO₂ efflux measurements were taken at the surface environment of Pululahua and Cuicocha calderas respectively, by means of the “accumulation chamber” method during the summer of 2006 to constrain the total CO₂ output from the studied area. Soil CO₂ efflux values ranged from non-detectable up to 48.5 and 141.7 g m^{− 2} d^{− 1} for Cuicocha and Pululahua calderas respectively. In addition, probability graphs were used to distinguish the existence of different geochemical populations. Sequential Gaussian Simulation was used to construct an average map for 100 simulations and to compute the total CO₂ emission at each studied area: 106 and 270 t d^{− 1} (metric tons per day) for Cuicocha (13.3 km²) and Pululahua (27.6 km²) volcanoes respectively.     

典型农业流域不同类型池塘水体CO2排放特征

内陆水体是大气CO₂收支估算的重要组成部分。农业流域分布着大量池塘景观水体,且具备蓄洪抗旱、消纳污染、水产养殖等多种功能。但是,农业流域不同功能的小型池塘CO₂排放特征尚不清楚。本研究以极具农业流域代表性的烔炀河流域为研究对象,选取流域中用于水产养殖(养殖塘)、生活污水承纳(村塘)、农业灌溉(农塘)、蓄水(水塘)的4个功能不同的景观池塘,基于为期1年的野外实地观测,以明确农业流域小型池塘CO₂排放特征。结果表明,不同功能池塘水体CO₂排放差异显著,受养殖活动、生活污水输入和农田灌溉等人类活动影响,养殖塘((80.37±100.39) mmol/(m²·d))、村塘((48.69±65.89) mmol/(m²·d))和农塘((13.50±15.81) mmol/(m²·d))是大气CO₂的热点排放源,其CO₂排放通量分别是自然蓄水塘((4.52±23.26) mmol/(m²·d))的18、11和3倍。统计分析也表明,该流域池塘CO₂排放变化总体上受溶解氧、营养盐等因素驱动。4个不同景观池塘CO₂排放通量全年均值为(37.31±67.47) mmol/(m²·d),是不容忽视的CO₂排放源,其中养殖塘和村塘具有较高的CO₂排放潜力,在未来研究中需要重点关注。     

Interfacial tension between CO2 and brine (NaCl + CaCl2) at elevated pressures and temperatures: The additive effect of different salts

An extensive laboratory study was conducted to measure the interfacial tension (IFT) between CO₂ and brine consisting in equal molal concentrations of NaCl and CaCl₂. The experiments were repeated at various pressures, temperatures and salinities that are representative of conditions prevailing during CO₂ storage in deep saline aquifers. The dependence of CO₂/brine IFT on pressure and temperature is similar to that previously reported for the systems: CO₂/NaCl solution and CO₂/CaCl₂ solution. CO₂/brine IFT increases linearly with water salinity and the magnitude of this increase was found equal to the sum of the individual CO₂/NaCl solution and CO₂/CaCl₂ solution IFT increments, indicating a strong additive effect on IFT when the brine is composed of various salts.     

CO2气体在地震孕育与发生过程中的作用及其机理研究

通过甘东南地震危险区地震宏观异常观测实例分析,系统研究CO_2气体在地震构造活动过程中的地球化学演化过程,以及发生的一系列酸碱平衡和氧化还原化学反应。结果表明地下深部CO_2气体不仅是其他微量气体Rn等向地表方向运移的载体,而且参与酸碱平衡和氧化还原反应,是地下深部生物化学反应的重要影响条件,地震前兆及宏观异常现象的发生常伴随着CO_2的异常变化。因此CO_2气体可以作为良好的示踪气体,在地震前兆观测及重大异常落实中尤其要重视对其进行监测。     

The effect of heterogeneity on the character of density-driven natural convection of CO2 overlying a brine layer

The efficiency of mixing in density-driven natural-convection is largely governed by the aquifer permeability, which is heterogeneous in practice. The character (fingering, stable mixing or channeling) of flow-driven mixing processes depends primarily on the permeability heterogeneity character of the aquifer, i.e., on its degree of permeability variance (Dykstra-Parsons coefficient) and the correlation length. Here we follow the ideas of Waggoner et al. (1992) [13] to identify different flow regimes of a density-driven natural convection flow by numerical simulation. Heterogeneous fields are generated with the spectral method of Shinozuka and Jan (1972) [13], because the method allows the use of power-law variograms. In this paper, we extended the classification of Waggoner et al. (1992) [13] for the natural convection phenomenon, which can be used as a tool in selecting optimal fields with maximum transfer rates of CO₂ into water. We observe from our simulations that the rate of mass transfer of CO₂ into water is higher for heterogeneous media.     

Capillary pressure for the sand–CO2–water system under various pressure conditions. Application to CO2 sequestration

Accurate modeling of storage of carbon dioxide (CO₂) in heterogeneous aquifers requires experiments of the capillary pressure as function of temperature and pressure. We present a method with which static drainage and imbibition capillary pressures can be measured continuously as a function of saturation at various temperature (T) and pressure (P) conditions. The measurements are carried out at (T, P) conditions of practical interest. Static conditions can be assumed as small injection rates are applied. The capillary pressure curves are obtained for the unconsolidated sand–distilled water–CO₂ system. The experimental results show a decrease of drainage and imbibition capillary pressure for increasing CO₂ pressures and pronounced dissolution rate effects for gaseous CO₂. Significant capillary pressure fluctuations and negative values during imbibition are observed at near critical conditions. The measurement procedure is validated by a numerical model that simulates the experiments.