Multi-scale modeling of CO2 dispersion leaked from seafloor off the Japanese coast

A numerical simulation was conducted to predict the change of pCO₂ in the ocean caused by CO₂ leaked from an underground aquifer, in which CO₂ is purposefully stored. The target space of the present model was the ocean above the seafloor. The behavior of CO₂ bubbles, their dissolution, and the advection-diffusion of dissolved CO₂ were numerically simulated. Here, two cases for the leakage rate were studied: an extreme case, 94,600 t/y, which assumed that a large fault accidentally connects the CO₂ reservoir and the seafloor; and a reasonable case, 3800 t/y, based on the seepage rate of an existing EOR site. In the extreme case, the calculated increase in ΔpCO₂ experienced by floating organisms was less than 300 ppm, while that for immobile organisms directly over the fault surface periodically exceeded 1000 ppm, if momentarily. In the reasonable case, the calculated ΔpCO₂ and pH were within the range of natural fluctuation.     

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.     

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.     

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.     

High-resolution simulation and characterization of density-driven flow in CO2 storage in saline aquifers

Simulations are routinely used to study the process of carbon dioxide (CO₂) sequestration in saline aquifers. In this paper, we describe the modeling and simulation of the dissolution–diffusion–convection process based on a total velocity splitting formulation for a variable-density incompressible single-phase model. A second-order accurate sequential algorithm, implemented within a block-structured adaptive mesh refinement (AMR) framework, is used to perform high-resolution studies of the process. We study both the short-term and long-term behaviors of the process. It is found that the onset time of convection follows closely the prediction of linear stability analysis. In addition, the CO₂ flux at the top boundary, which gives the rate at which CO₂ gas dissolves into a negatively buoyant aqueous phase, will reach a stabilized state at the space and time scales we are interested in. This flux is found to be proportional to permeability, and independent of porosity and effective diffusivity, indicative of a convection-dominated flow. A 3D simulation further shows that the added degrees of freedom shorten the onset time and increase the magnitude of the stabilized CO₂ flux by about 25%. Finally, our results are found to be comparable to results obtained from TOUGH2-MP.     

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...     

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.     

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.     

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.     

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.     

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.     

Modelled effect of changes in the CO2 concentration on the middle and upper atmosphere: Sensitivity to gravity wave parameterization

We have studied the temperature response to changes in the CO₂ concentration in the middle and upper atmosphere using the Coupled Middle Atmosphere–Thermosphere Model 2 (CMAT2). We have performed simulations with a range of CO₂ concentrations and three different ways of accounting for the effects of gravity waves, to allow for comparison with previous studies and sensitivity analyses. We initially find that the response of the model to the changes in CO₂ concentration which took place between 1965 and 1995 (320–360 ppm) is strongly dependent on the gravity wave parameterization that is used, but this is to a large degree due to steps or kinks in an otherwise nearly linear curve describing the temperature as a function of CO₂ concentration. We have not been able to identify the cause of these steps as part of the present study, which is a limitation and must be studied in future work. Here we treated the steps as model noise and rather focused on correcting for their effects by fitting straight lines to the temperature–CO₂ curves to estimate the overall slope of the curves. From these slopes we were able to obtain more robust trend estimates than can be obtained by comparing only two model simulations, as is normally done in other, similar studies. The corrected temperature responses to a 40 ppm change in CO₂ concentration still show up to 15–17% sensitivity to the gravity wave parameterization in the mesosphere and thermosphere. This remaining sensitivity is likely to be related to the fundamental differences in the way a change in temperature modifies the propagation and dissipation characteristics of gravity waves in each parameterization, which is particularly different for linear and non-linear schemes. The corrected trends we find are largely in agreement with other modelling studies, and therefore do not fully explain observed trends, which are typically larger than those predicted by modelling studies. However, modelling results could be similarly sensitive to other model parameters and settings, for example to gravity wave characteristics or solar activity level, and this should be further investigated as well.     

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.     

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.     

CO2浓度升高对浮游藻类元素化学计量值的影响

通过梅梁湾和东太湖的四季原位实验,研究CO_2浓度升高对不同营养水平淡水生态系统中浮游藻类C、N、P元素计量值的影响.实验设置了270、380和750 ppm共3个CO_2浓度,分别代表工业革命前、当前和IPCC预测的21世纪末的CO_2浓度.结果表明梅梁湾水体营养盐浓度在四季均高于东太湖水体营养盐浓度,但梅梁湾原位实验中浮游藻类C、N、P含量却普遍低于东太湖原位实验中浮游藻类营养元素含量,并且前者在季节上变化更大.CO_2浓度升高使梅梁湾原位实验中浮游藻类C∶P比明显增加,N∶P比略有增加,这种增加归因于藻细胞内C、N含量的升高,而东太湖浮游藻类化学计量值对CO_2浓度变化的响应不显著.因此浮游藻类元素化学计量值对CO_2浓度变化的响应程度与水体营养盐的绝对浓度无关,而与浮游藻类的生长是否受营养盐限制有关,只有当藻类生长受到水体营养盐浓度限制时,CO_2浓度升高才会显著改变其元素组成.     

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.     

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.     

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。     

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.     

水-气界面CO_2通量监测的静态箱法与薄边界层模型估算法比较

模型估算法与静态箱法是水-气界面气体通量监测的主要方法,因原理不同监测结果通常存在一定差异.目前对引起上述差异的主要环境因素仍不清晰.本研究使用自行设计的静态箱对三峡支流澎溪河水-气界面CO2通量进行监测,并与同步开展的CO2通量薄边界层模型估算法结果相比较,探讨该水域引起这两种监测方法结果产生差异的主要环境因素.结果表明,瞬时风速、水汽温差及水深均会对静态箱法及模型估算法的监测结果产生影响.风速越强、水汽温差越大、水深越大,这两种方法监测结果的差异就越小;而水域面积对两种方法的差异没有影响.比较发现,两种方法所获通量数据呈显著正相关,但静态箱法所获通量数据离散性显著高于薄边界层模型估算法.从方法的稳定性角度,在峡谷河道型水库水体温室气体监测中薄边界层模型估算法可能更为适宜.