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1.
Predicting the fate of the injected CO2 is crucial for the safety of carbon storage operations in deep saline aquifers: especially the evolution of the position, the spreading and the quantity of the mobile CO2 plume during and after the injection has to be understood to prevent any loss of containment. Fluid flow modelling is challenging not only given the uncertainties on subsurface formation intrinsic properties (parameter uncertainty) but also on the modelling choices/assumptions for representing and numerically implementing the processes occurring when CO2 displaces the native brine (model uncertainty). Sensitivity analysis is needed to identify the group of factors which contributes the most to the uncertainties in the predictions. In this paper, we present an approach for assessing the importance of model and parameter uncertainties regarding post-injection trapping of mobile CO2. This approach includes the representation of input parameters, the choice of relevant simulation outputs, the assessment of the mobile plume evolution with a flow simulator and the importance ranking for input parameters. A variance-based sensitivity analysis is proposed, associated with the ACOSSO-like meta-modelling technique to tackle the issues linked with the computational burden posed by the use of long-running simulations and with the different types of uncertainties to be accounted for (model and parameter). The approach is tested on a potential site for CO2 storage in the Paris basin (France) representative of a project in preliminary stage of development. The approach provides physically sound outcomes despite the challenging context of the case study. In addition, these outcomes appear very helpful for prioritizing the future characterisation efforts and monitoring requirements, and for simplifying the modelling exercise.  相似文献   

2.
Practical geologic CO2 sequestration will require long-term monitoring for detection of possible leakage back into the atmosphere. One potential monitoring method is multi-spectral imaging of vegetation reflectance to detect leakage through CO2-induced plant stress. A multi-spectral imaging system was used to simultaneously record green, red, and near-infrared (NIR) images with a real-time reflectance calibration from a 3-m tall platform, viewing vegetation near shallow subsurface CO2 releases during summers 2007 and 2008 at the Zero Emissions Research and Technology field site in Bozeman, Montana. Regression analysis of the band reflectances and the Normalized Difference Vegetation Index with time shows significant correlation with distance from the CO2 well, indicating the viability of this method to monitor for CO2 leakage. The 2007 data show rapid plant vigor degradation at high CO2 levels next to the well and slight nourishment at lower, but above-background CO2 concentrations. Results from the second year also show that the stress response of vegetation is strongly linked to the CO2 sink–source relationship and vegetation density. The data also show short-term effects of rain and hail. The real-time calibrated imaging system successfully obtained data in an autonomous mode during all sky and daytime illumination conditions.  相似文献   

3.
Simulation of carbon dioxide (CO2) at hourly/weekly intervals and fine vertical resolution at the continental or coastal sites is challenging because of coarse horizontal resolution of global transport models. Here the regional Weather Research and Forecasting (WRF) model coupled with atmospheric chemistry is adopted for simulating atmospheric CO2 (hereinafter WRF-CO2) in nonreactive chemical tracer mode. Model results at horizontal resolution of 27 × 27 km and 31 vertical levels are compared with hourly CO2 measurements from Tsukuba, Japan (36.05°N, 140.13 oE) at tower heights of 25 and 200 m for the entire year 2002. Using the wind rose analysis, we find that the fossil fuel emission signal from the megacity Tokyo dominates the diurnal, synoptic and seasonal variations observed at Tsukuba. Contribution of terrestrial biosphere fluxes is of secondary importance for CO2 concentration variability. The phase of synoptic scale variability in CO2 at both heights are remarkably well simulated the observed data (correlation coefficient >0.70) for the entire year. The simulations of monthly mean diurnal cycles are in better agreement with the measurements at lower height compared to that at the upper height. The modelled vertical CO2 gradients are generally greater than the observed vertical gradient. Sensitivity studies show that the simulation of observed vertical gradient can be improved by increasing the number of vertical levels from 31 in the model WRF to 37 (4 below 200 m) and using the Mellor–Yamada–Janjic planetary boundary scheme. These results have large implications for improving transport model simulation of CO2 over the continental sites.  相似文献   

4.
A screening and ranking framework (SRF) has been developed to evaluate potential geologic carbon dioxide (CO2) storage sites on the basis of health, safety, and environmental (HSE) risk arising from CO2 leakage. The approach is based on the assumption that CO2 leakage risk is dependent on three basic characteristics of a geologic CO2 storage site: (1) the potential for primary containment by the target formation; (2) the potential for secondary containment if the primary formation leaks; and (3) the potential for attenuation and dispersion of leaking CO2 if the primary formation leaks and secondary containment fails. The framework is implemented in a spreadsheet in which users enter numerical scores representing expert opinions or published information along with estimates of uncertainty. Applications to three sites in California demonstrate the approach. Refinements and extensions are possible through the use of more detailed data or model results in place of property proxies.  相似文献   

5.
Fossil energy consumption is one of the main reasons for the deterioration of environmental pollution and decline in public health. This paper tests for the long-run and short-run relationship among energy consumption, environment pollution and public health using the autoregressive-distributed lag approach in China for the period 1985–2014. The study used energy consumption variables (i.e., the proportion of coal consumption, that of oil and clean energy, abbreviated as PCC, POIL and PCE, respectively), environmental pollution ones (i.e., SO2 emissions, abbreviated SO2, soot and dust emissions,), two health proxies (i.e., the proportion of cardiovascular and respiratory diseases mortality, abbreviated as PCD and PRD, respectively). These variables were selected due to vital importance in China. The overall results indicate that there was co-integration relationship under the study with statistically significantly positive relationship between environmental pollution and energy consumption, public health and environmental pollution in the short and long run. Comparing the long-run and short-run coefficients of energy use variable with respect to SO2 and soot indicates that the long-run coefficients are the same as the short-run. The long-run coefficients of soot and dust emissions with respect to PCD and PRD, respectively, are higher than the short-run coefficients. This implies that environment pollution level is found to worsen with respect to fossil energy use presently and over time, while public health level descending with reference to soot and dust emission over time in China. The Granger causality results suggested a unidirectional Granger causality between energy use and environment pollution, environment pollution and public health. The results emphasized the importance of energy transformation and sustainable development policies that help to adjust the structure of energy consumption and to improve public health level.  相似文献   

6.
This paper explores China’s strategies for addressing climate change on the industrial level. Focusing on six energy-intensive industries, this paper applies gray relational analysis theory to the affecting factors to CO2 emissions of each industry after calculating each industry’s CO2 emissions during 2001–2010. Further research based on GM(1, 1) model is conducted to forecast the trend of the factors, the energy consumption and each industry’s CO2 emissions during the 12th Five-Year Plan period. As a breakthrough in previous conclusions, energy consumption structure was divided into the respective proportion of coal, oil, natural gas and electricity in the primary energy consumption, with which industrial output and energy intensity are combined to analyze each of their impacts on the energy-intensive industries. It turns out that all the factors’ impacts on emissions of the six major energy-intensive industries are significant, despite their differentiated extents. It is worth noting that, contrary to previous findings, industrial output is not the leading affecting factor to CO2 emissions of the energy-intensive industries compared with the proportion of coal and electricity in the primary energy consumption. The GM(1, 1) forecast results of energy consumption and CO2 emissions by the end of 2015 show that coal and electricity will remain a large proportion in primary energy consumption. This research may shed some light on China’s adjustment of energy structure under the pressure of addressing climate change and hence provide decision support for the acceleration of renewable energy utilization in the industrial departments.  相似文献   

7.
Carbon dioxide (CO2) has been injected in the subsurface permeable formations as a means to cut atmospheric CO2 emissions and/or enhance oil recovery (EOR). It is important to constrain the boundaries of the CO2 plume in the target formation and/or other formations hosting the CO2 migrated from the target formation. Monitoring methods and technologies to assess the CO2 plume boundaries over time within a reservoir of interest are required. Previously introduced methods and technologies on pressure monitoring to detect the extent of the CO2 plume require at least two wells, i.e. pulser and observation wells. We introduce pressure transient technique requiring single well only. Single well pressure transient testing (drawdown/buildup/injection/falloff) is widely used to determine reservoir properties and wellbore conditions. Pressure diagnostic plots are used to identify different flow regimes and determine the reservoir/well characteristics. We propose a method to determine the plume extent for a constant rate pressure transient test at a single well outside the CO2 plume. Due to the significant contrast between mobility and storativity of the CO2 and native fluids (oil or brine), the CO2 boundary causes deviation in the pressure diagnostic response from that corresponding to previously identified heterogeneities. Using the superposition principle, we develop a relationship between the deviation time and the plume boundary. We demonstrate the applicability of the proposed method using numerically generated synthetic data corresponding to homogeneous, heterogeneous, and anisotropic cases to evaluate its potential and limitations. We discuss ways to identify and overcome the potential limitations for application of the method in the field.  相似文献   

8.
The CO2 migrated from deeper to shallower layers may change its phase state from supercritical state to gaseous state (called phase transition). This phase transition makes both viscosity and density of CO2 experience a sharp variation, which may induce the CO2 further penetration into shallow layers. This is a critical and dangerous situation for the security of CO2 geological storage. However, the assessment of caprock sealing efficiency with a fully coupled multi-physical model is still missing on this phase transition effect. This study extends our previous fully coupled multi-physical model to include this phase transition effect. The dramatic changes of CO2 viscosity and density are incorporated into the model. The impacts of temperature and pressure on caprock sealing efficiency (expressed by CO2 penetration depth) are then numerically investigated for a caprock layer at the depth of 800 m. The changes of CO2 physical properties with gas partial pressure and formation temperature in the phase transition zone are explored. It is observed that phase transition revises the linear relationship of CO2 penetration depth and time square root as well as penetration depth. The real physical properties of CO2 in the phase transition zone are critical to the safety of CO2 sequestration. Pressure and temperature have different impact mechanisms on the security of CO2 geological storage.  相似文献   

9.
Cave air CO2 is a vital part of the cave environment. Most studies about cave air CO2 variations are performed in caves with no streams; there are few studies to date regarding the relationship of cave air CO2 variations and drip water hydrochemistry in underground stream–developed caves. To study the relationship of underground stream, drip water, and cave air CO2, monthly and daily monitoring of air CO2 and of underground stream and drip water was performed in Xueyu Cave from 2012 to 2013. The results revealed that there was marked seasonal variation of air CO2 and stream hydrochemistry in the cave. Daily variations of cave air CO2, and of stream and drip water hydrochemistry, were notable during continuous monitoring. A dilution effect was observed by analyzing hydrochemical variations in underground stream and drip water after rainfall. High cave air CO2 along with low pH and low δ13CDIC in stream and drip water indicated that air CO2 was one of the dominant factors controlling stream and drip water hydrochemistry on a daily scale. On a seasonal scale, stream flows may promote increased cave air CO2 in summer; in turn, the higher cave air CO2 could inhibit degassing of drip water and make calcite δ13C more negative. Variation of calcite δ13C (precipitated from drip water) was in reverse of monthly temperature, soil CO2, and cave air CO2. Therefore, calcite δ13C in Xueyu Cave could be used to determine monthly changes outside the cave. However, considering the different precipitation rate of sediment in different seasons, it was difficult to use stalagmites to reconstruct environmental change on a seasonal scale.  相似文献   

10.
The discovery of Hadean to Paleoarchean zircons in a metaconglomerate from Jack Hills, Western Australia, has catalyzed intensive study of these zircons and their mineral inclusions, as they represent unique geochemical archives that can be used to unravel the geological evolution of early Earth. Here, we report the occurrence and physical properties of previously undetected CO2 inclusions that were identified in 3.36–3.47 Ga and 3.80–4.13 Ga zircon grains by confocal micro-Raman spectroscopy. Minimum P–T conditions of zircon formation were determined from the highest density of the inclusions, determined from the density-dependence of the Fermi diad splitting in the Raman spectrum and Ti-in-zircon thermometry. For both age periods, the CO2 densities and Ti-in-zircon temperatures correspond to high-grade metamorphic conditions (≥5 to ≥7 kbar/~670 to 770 °C) that are typical of mid-crustal regional metamorphism throughout Earth’s history. In addition, fully enclosed, highly disordered graphitic carbon inclusions were identified in two zircon grains from the older population that also contained CO2 inclusions. Transmission electron microscopy on one of these inclusions revealed that carbon forms a thin amorphous film on the inclusion wall, whereas the rest of the volume was probably occupied by CO2 prior to analysis. This indicates a close relationship between CO2 and the reduced carbon inclusions and, in particular that the carbon precipitated from a CO2-rich fluid, which is inconsistent with the recently proposed biogenic origin of carbon inclusions found in Hadean zircons from Jack Hills.  相似文献   

11.
Fluid inclusions have recorded the history of degassing in basalt. Some fluid inclusions in olivine and pyroxene phenocrysts of basalt were analyzed by micro-thermometry and Raman spectroscopy in this paper. The experimental results showed that many inclusions are present almost in a pure CO2 system. The densities of some CO2 inclusions were computed in terms of Raman spectroscopic characteristics of CO2 Fermi resonance at room temperature. Their densities change over a wide range, but mainly between 0.044 g/cm3 and 0.289 g/cm3. Their micro-thermometric measurements showed that the CO2 inclusions examined reached homogenization between 1145.5℃ and 1265℃ . The mean value of homogenization temperatures of CO2 inclusions in basalts is near 1210℃. The trap pressures (depths) of inclusions were computed with the equation of state and computer program. Distribution of the trap depths makes it know that the degassing of magma can happen over a wide pressure (depth) range, but mainly at the depth of 0.48 km to 3.85 km. This implicates that basalt magma experienced intensive degassing and the CO2 gas reservoir from the basalt magma also may be formed in this range of depths. The results of this study showed that the depth of basalt magma degassing can be forecasted from CO2 fluid inclusions, and it is meaningful for understanding the process of magma degassing and constraining the inorganogenic CO2 gas reservoir.  相似文献   

12.
13.
Spring wheat (Triticum aestivum Linn.) is an important crop for food security in the desert-oasis farmland in the middle reaches of the Heihe River in northwestern China. We measured fluxes using eddy covariance and meteorological parameters to explore the energy fluxes and the relationship between CO2 flux and climate change in this region during the wheat growing seasons in 2013 and 2014. The energy balance closures were 70.5% and 72.7% in the 2013 and 2014 growing season, respectively. The wheat ecosystem had distinct seasonal and diurnal dynamics of CO2 fluxes with U-shaped curves. The accumulated net ecosystemic CO2 exchanges (NEE) were -111.6 and -142.2 g C/m2 in 2013 and 2014 growing season, respectively. The ecosystem generally acted as a CO2 sink during the growing season but became a CO2 source after the wheat harvest. A correlation analysis indicated that night-time CO2 fluxes were exponentially dependent on air temperature and soil temperature at a depth of 5 cm but were not correlated with soil-water content, water-vapour pressure, or vapour-pressure deficit. CO2 flux was not correlated with the meteorological parameters during daytime. However, irrigation and precipitation, may complicate the response of CO2 fluxes to other meteorological parameters.  相似文献   

14.
In this work 3-[2-(2-aminoethylamino)ethylamino]propyl trimethoxysilane (TRI) was employed to functionalize MWCNT containing hydroxyl groups (OH-MWCNT), and the XRD, FTIR, TGA and CHNS elemental analysis techniques were used to characterize the resulted adsorbents. The characterization results for amine-MWCNT showed amine groups effectively attached to the surface of the MWCNT. The equilibrium adsorption capacity of pure CO2 and CH4 and their binary mixture on the pristine MWCNT, OH-MWCNT and amine-MWCNT was measured through a set of equilibrium adsorption experiments at 303.2 and 318.2 K. Capacities of all three types of adsorbents for CO2 adsorption were higher than those for methane adsorption. Also, amine-MWCNT demonstrated better performance on CO2 adsorption than the other two adsorbents, especially at low partial pressures. The capacity of amine-MWCNT for pure CO2 adsorption was 2.5 and 4 times as much as those for pristine MWCNT and OH-MWCNT, respectively, at the temperature of 303.2 K and the pressure of 0.2 bar. The binary adsorption experiment revealed that CO2/CH4 selectivity for pristine MWCNT and amine-MWCNT in all molar fractions of CO2 is about 1.77 and 7, respectively.  相似文献   

15.
Field experiments on the CO2 flux of alpine meadow soil in the Qilian Mountain were conducted along the elevation gradient during the growing season of 2004 and 2005. The soil CO2 flux was measured using the Li-6400-09 soil respiration chamber attached to the Li-6400 portable photosynthesis system. The effects of water and heat and roots on the soil CO2 flux were statistically analyzed. The results show that soil CO2 flux along the elevation gradient gradually decreases. The soil CO2 flux was low at night, with lowest value occurring between 0200 and 0600 hours, started to rise rapidly during 0700–0830 hours, and then descend during 1600–1830 hours. The peak CO2 efflux appears during 1100–1600 hours. The diurnal average of soil CO2 efflux was between 0.56 ± 0.32 and 2.53 ± 0.76 μmol m−2 s−1. Seasonally, soil CO2 fluxes are relatively high in summer and autumn and low in spring and winter. The soil CO2 efflux, from the highest to the lowest in the ranking order, occurred in July and August (4.736 μmol m−2 s−1), June and September, and May and October, respectively. The soil CO2 efflux during the growing season is positively correlated with soil temperature, root biomass and soil water content.  相似文献   

16.
Coal gasification with CO2 has emerged as a cleaner and more efficient way for the production of energy, and it offers the advantages of CO2 mitigation policies through simultaneous CO2 sequestration. In the present investigation, a feasibility study on the gasification of three low-quality, high-sulphur coals from the north-eastern region (NER) of India in a CO2 atmosphere using thermogravimetric analysis (TGA-DTA) has been made in order to have a better understanding of the physical and chemical characteristics in the process of gasification of coal. Model-free kinetics was applied to determine the activation energies (E) and pre-exponential factors (A) of the CO2 gasification process of the coals. Multivariate non-linear regression analyses were performed to find out the formal mechanisms, kinetic model, and the corresponding kinetic triplets. The results revealed that coal gasification with CO2 mainly occurs in the temperature range of 800°–1400°C and a maximum of at around 1100°C. The reaction mechanisms responsible for CO2 gasification of the coals were observed to be of the ‘nth order with autocatalysis (CnB)’ and ‘nth order (Fn) mechanism’. The activation energy of the CO2 gasification was found to be in the range 129.07–146.81 kJ mol?1.  相似文献   

17.
Hyperspectral plant signatures can be used as a short-term, as well as long-term (100-year timescale) monitoring technique to verify that CO2 sequestration fields have not been compromised. An influx of CO2 gas into the soil can stress vegetation, which causes changes in the visible to near-infrared reflectance spectral signature of the vegetation. For 29 days, beginning on July 9, 2008, pure carbon dioxide gas was released through a 100-m long horizontal injection well, at a flow rate of 300 kg day−1. Spectral signatures were recorded almost daily from an unmown patch of plants over the injection with a “FieldSpec Pro” spectrometer by Analytical Spectral Devices, Inc. Measurements were taken both inside and outside of the CO2 leak zone to normalize observations for other environmental factors affecting the plants. Four to five days after the injection began, stress was observed in the spectral signatures of plants within 1 m of the well. After approximately 10 days, moderate to high amounts of stress were measured out to 2.5 m from the well. This spatial distribution corresponded to areas of high CO2 flux from the injection. Airborne hyperspectral imagery, acquired by Resonon, Inc. of Bozeman, MT using their hyperspectral camera, also showed the same pattern of plant stress. Spectral signatures of the plants were also compared to the CO2 concentrations in the soil, which indicated that the lower limit of soil CO2 needed to stress vegetation is between 4 and 8% by volume.  相似文献   

18.
Proper characterizations of background soil CO2 respiration rates are critical for interpreting CO2 leakage monitoring results at geologic sequestration sites. In this paper, a method is developed for determining temperature-dependent critical values of soil CO2 flux for preliminary leak detection inference. The method is illustrated using surface CO2 flux measurements obtained from the AmeriFlux network fit with alternative models for the soil CO2 flux versus soil temperature relationship. The models are fit first to determine pooled parameter estimates across the sites, then using a Bayesian hierarchical method to obtain both global and site-specific parameter estimates. Model comparisons are made using the deviance information criterion (DIC), which considers both goodness of fit and model complexity. The hierarchical models consistently outperform the corresponding pooled models, demonstrating the need for site-specific data and estimates when determining relationships for background soil respiration. A hierarchical model that relates the square root of the CO2 flux to a quadratic function of soil temperature is found to provide the best fit for the AmeriFlux sites among the models tested. This model also yields effective prediction intervals, consistent with the upper envelope of the flux data across the modeled sites and temperature ranges. Calculation of upper prediction intervals using the proposed method can provide a basis for setting critical values in CO2 leak detection monitoring at sequestration sites.  相似文献   

19.
Amine post-combustion carbon capture technology is based on washing the flue gas with a solvent that captures CO2. Thus, a small fraction of this solvent can be released together with the cleaned flue gas. This release may cause environmental concerns, both directly and indirectly through subsequent solvent degradation into other substances in the atmosphere. The paper presents the ammonia emission from CO2 capture pilot plant (1 tonne CO2 per day) using 40 wt% aminoethylethanolamine solvent, along with the efficiency of the water wash unit. In addition, the temperature effect of lean amine entering the absorber on ammonia emission was studied. Furthermore, the concentrations of other compounds such as SO2, SO3, NO2, CS2 and formaldehyde were monitored. The literature review on the NH3 emission from a pilot plant using aminoethylethanolamine solvent has not been published. The results show that the main source of ammonia emission is the absorber and that emission (in the range 27–50 ppm) corresponds to typical NH3 release from CO2 capture pilot plant using an amine solvent. The emission of amines and amine degradation products is a complex phenomenon which is difficult to predict in novel solvents, and for this reason the significance of new solvents testing in a pilot scale has been highlighted.  相似文献   

20.
This study focused on the target injection layers of deep saline aquifers in the Shiqianfeng Fm. in the Carbon Capture and Sequestration (CCS) Demonstration Projects in the Ordos Basin, northwestern China. The study employed a combination method of experiments and numerical simulation to investigate the dissolution mechanism and impact factors of CO2 in these saline aquifers. The results showed (1) CO2 solubility in different types of water chemistry were shown in ascending order: MgCl2-type water < CaCl2-type water < Na2SO4-type water < NaCl-type water < Na2CO3-type water < distilled water. These results were consistent with the calculated results undertaken by TOUGHREACT with about 5% margin of error. CO2 solubility of Shiqianfeng Fm. saline was 1.05 mol/L; (2) compared with distilled water, the more complex the water’s chemical composition, the greater the increase in HCO3 ?concentration. While the water’s composition was relatively simple, the tested water’s HCO3 ?concentrations were in close accord with the calculated value undertaken by the TOUGHREACT code, and the more complex the water’s composition, the poorer the agreement was, probably due to the complex and unstable HCO3 ? complicating matters when in an aqueous solution system including both tested HCO3 ?concentration and calculated HCO3 ?concentration; (3) the CO2 solubility in the saline at the temperature conditions of 55 °C and 70 °C were 1.17 and 1.02 mol/L. When compared with the calculated value of 1.20 and 1.05 mol/L, they were almost the same with only 1 and 3% margin of error; concentrations of HCO3 ? were 402.73 mg/L (0.007 mol/L) and 385.65 mg/L (0.006 mol/L), while the simulation results were 132.16 mg/L (0.002 mol/L) and 128.52 mg/L (0.002 mol/L). From the contrast between the tested data and the calculated data undertaken by the TOUGHREACT code, it was shown that TOUGHRACT code could better simulate the interaction between saline and CO2 in the dissolution sequestration capacity. Therefore, TOUGHREACT code could be used for the inter-process prediction of CO2 long-term geological storage of CO2; (4) The Ca2+ concentration and SO4 2?concentration in saline water had less effect on the solubility of CO2 and HCO3 ?concentration. In addition, TDS and pH values of saline affected not only the solubility of CO2, but also the conversion of CO2 to HCO3 ? due to that they can affect the activity and acid-base balance. So in fact, we just need to consider that the TDS and pH values are main impact factors in the dissolution sequestration capacity of CO2 geological sequestration in deep saline aquifers.  相似文献   

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