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1.
Climate change is being caused by greenhouse gases such as carbon dioxide (CO2). Carbon capture and storage (CCS) is of interest to the scientific community as one way of achieving significant global reductions of atmospheric CO2 emissions in the medium term. CO2 would be captured from large stationary sources such as power plants and transported via pipelines under high pressure conditions to underground storage. If a downward leakage from a surface transportation system module occurs, the CO2 would undergo a large temperature reduction and form a bank of “dry ice” on the ground surface; the sublimation of the gas from this bank represents an area source term for subsequent atmospheric dispersion, with an emission rate dependent on the energy balance at the bank surface. Gaseous CO2 is denser than air and tends to remain close to the surface; it is an asphyxiant, a cerebral vasodilator and at high concentrations causes rapid circulatory insufficiency leading to coma and death. Hence a subliming bank of dry ice represents safety hazard. A model is presented for evaluating the energy balance and sublimation rate at the surface of a solid frozen CO2 bank under different environmental conditions. The results suggest that subliming gas behaves as a proper dense gas (i.e. it remains close to the ground surface) only for low ambient wind speeds.  相似文献   

2.
Emissions from electricity generation will have to be reduced to near-zero to meet targets for reducing overall greenhouse gas emissions. Variable renewable energy sources such as wind will help to achieve this goal but they will have to be used in conjunction with other flexible power plants with low-CO2 emissions. A process which would be well suited to this role would be coal gasification hydrogen production with CCS, underground buffer storage of hydrogen and independent gas turbine power generation. The gasification hydrogen production and CO2 capture and storage equipment could operate at full load and only the power plants would need to operate flexibly and at low load, which would result in substantial practical and economic advantages. This paper analyses the performances and costs of such plants in scenarios with various amounts of wind generation, based on data for power demand and wind energy variability in the UK. In a scenario with 35% wind generation, overall emissions of CO2 could be reduced by 98–99%. The cost of abating CO2 emissions from the non-wind residual generation using the technique proposed in this paper would be less than 40% of the cost of using coal-fired power plants with integrated CCS.  相似文献   

3.
ABSTRACT: The projected increase in the concentration of CO2 and other greenhouse gases in the atmosphere is likely to result in a global temperature increase. This paper reports on the probable effects of a temperature increase and changes in transpiration on basin discharge in two different mountain snowmelt regions of the western United States. The hydrological effects of the climate changes are modeled with a relatively simple conceptual, semi-distributed snowmelt runoff model. Based on the model results, it may be concluded that increased air temperatures will result in a shift of snowmelt runoff to earlier in the snowmelt season. Furthermore, it is shown that it is very important to include the expected change in climate-related basin conditions resulting from the modeled temperature increase in the runoff simulation. The effect of adapting the model parameters to reflect the changed basin conditions resulted in a further shift of streamflow to April and an even more significant decrease of snowmelt runoff in June and July. If the air temperatures increase by approximately 5°C and precipitation and accumulated snow amounts remain about the same, runoff in April and May, averaged for the two basins, is expected to increase by 185 percent and 26 percent, respectively. The runoff in June and July will decrease by about 60 percent each month. Overall, the total seasonal runoff decreases by about 6 percent. If increased CO2 concentrations further change basin conditions by reducing transpiration by the maximum amounts reported in the literature, then, combined with the 5°C temperature increase, the April, May, June, and July changes would average +230 percent, +40 percent, ?55 percent, and ?45 percent, respectively. The total seasonal runoff change would be +11 percent.  相似文献   

4.
The National Oceanic and Atmospheric Administration (NOAA) provides daily reference evapotranspiration (ETref) maps for the contiguous United States using climatic data from North American Land Data Assimilation System (NLDAS). This data provides large‐scale spatial representation of ETref, which is essential for regional scale water resources management. Data used in the development of NOAA daily ETref maps are derived from observations over surfaces that are different from short (grass — ETos) or tall (alfalfa — ETrs) reference crops, often in nonagricultural settings, which carries an unknown discrepancy between assumed and actual conditions. In this study, NOAA daily ETos and ETrs maps were evaluated for accuracy, using observed data from the Texas High Plains Evapotranspiration (TXHPET) network. Daily ETos, ETrs and the climatic data (air temperature, wind speed, and solar radiation) used for calculating ETref were extracted from the NOAA maps for TXHPET locations and compared against ground measurements on reference grass surfaces. NOAA ETref maps generally overestimated the TXHPET observations (1.4 and 2.2 mm/day ETos and ETrs, respectively), which may be attributed to errors in the NLDAS modeled air temperature and wind speed, to which reference ETref is most sensitive. Therefore, a bias correction to NLDAS modeled air temperature and wind speed data, or adjustment to the resulting NOAA ETref, may be needed to improve the accuracy of NOAA ETref maps.  相似文献   

5.
Carbon dioxide contents of coals in the Sydney Basin vary both aerially and stratigraphically. In places, the coal seam gas is almost pure CO2 that was introduced from deep magmatic sources via faults and replaced pre-existing CH4. In some respects this process is analogous to sequestration of anthropogenic CO2. Laboratory studies indicate that CO2:CH4 storage capacity ratios for Sydney Basin coals are up to ∼2 and gas diffusivity is greater for CO2 by a factor of up to 1.5.Present-day distribution of CO2 in the coals is controlled by geological structure, depth and a combination of hydrostatic and capillary pressures. Under present-day PT conditions, most of the CO2 occurs in solution at depths greater than about 650 m; at shallower depths, larger volumes of CO2 occur in gaseous form and as adsorbed molecules in the coal due to rapidly decreasing CO2 solubility. The CO2 has apparently migrated up to structural highs and is concentrated in anticlines and in up-dip sections of monoclines and sealing faults. CO2 sequestered in coal measure sequences similar to those of the Sydney Basin may behave in a similar way and, in the long term, equilibrate according to the prevailing PT conditions.In situ CO2 contents of Sydney Basin coals range up to 20 m3/t. Comparisons of adsorption isotherm data measured on ground coal particles with in situ gas contents of Sydney Basin coals indicate that the volumes of CO2 stored do not exceed ∼60% of the total CO2 storage capacity. Therefore, the maximum CO2 saturation that may be achieved during sequestration in analogous coals is likely to be considerably lower than the theoretical values indicated by adsorption isotherms.  相似文献   

6.
Modeling of air pollutant dispersion has been undertaken for emissions of sulfur dioxide (SO2) at the Mina Al-Fahal refinery in the Sultanate of Oman. The study was conducted during the period of November 1999 to October 2000. The Industrial Source Complex Short-Term (ISCST32) air pollution model was adopted to predict the ground level concentration of SO2 in and around the refinery. The modeling results were validated against measured data during the study period. The comparison, based on the monthly average measurements, showed that the model underestimates the observed SO2 concentrations. However, the predicted ground level concentrations of SO2 during the months of September, October, November, and June were in better agreement with the observations. The predicted SO2 values are presented in the form of concentration contours to determine the spatial distribution of SO2 and to assess the impact on air quality over the survey area. Predicted SO2 concentrations were found lower than the World Health Organisation (WHO) guideline value of 365 μg/m3, with the maximum ground level concentrations being found to occur relatively close to the sources of emission. Moreover, concentration contour patterns for the modeled area vary with changes in meteorological conditions. On the basis of this study, the refinery is not likely to cause any significant deterioration in air quality, and predicted concentrations of SO2 are well below those likely to influence health.  相似文献   

7.
A novel concept for capturing CO2 from biomass combustion using CaO as an active solid sorbent of CO2 is discussed and experimentally tested. According to the CaO/CaCO3 equilibrium, if a fuel could be burned at a sufficiently low temperature (below 700 °C) it would be possible to capture CO2in situ” with the CaO particles at atmospheric pressure. A subsequent step involving the regeneration of CaCO3 in a calciner operating at typical conditions of oxyfired-circulating fluidized combustion would deliver the CO2 ready for purification, compression and permanent geological storage. Several series of experiments to prove this concept have been conducted in a 30 kW interconnected fluidized bed test facility at INCAR-CSIC, made up of two interconnected circulating fluidized bed reactors, one acting as biomass combustor-carbonator and the other as air-fired calciner (which is considered to yield similar sorbent properties than those of an oxyfired calciner). CO2 capture efficiencies in dynamic tests in the combustor-carbonator reactor were measured over a wide range of operating conditions, including different superficial gas velocities, solids circulation rates, excess air above stoichiometric, and biomass type (olive pits, saw dust and pellets). Biomass combustion in air is effective at temperatures even below the 700 °C, necessary for the effective capture of CO2 by carbonation of CaO. Overall CO2 capture efficiencies in the combustor-carbonator higher than 70% can be achieved with sufficiently high solids circulation rates of CaO and solids inventories. The application of a simple reactor model for the combined combustion and CO2 capture reactions allows an efficiency factor to be obtained from the dynamic experimental test that could be valuable for scaling up purposes.  相似文献   

8.
Chemical-looping combustion (CLC) is a promising technology for the combustion of gas or solid fuel with efficient use of energy and inherent separation of CO2. The technique involves the use of an oxygen carrier which transfers oxygen from combustion air to the fuel, and hence a direct contact between air and fuel is avoided. A chemical-looping combustion system consists of a fuel reactor and an air reactor. A metal oxide is used as oxygen carrier that circulates between the two reactors. The air reactor is a high velocity fluidized bed where the oxygen carrier particles are transported together with the air stream to the top of the air reactor, where they are then transferred to the fuel reactor using a cyclone. The fuel reactor is a bubbling fluidized bed reactor where oxygen carrier particles react with hydrocarbon fuel and get reduced. The reduced oxygen carrier particles are transported back to the air reactor where they react with oxygen in the air and are oxidized back to metal oxide. The exhaust from the fuel reactor mainly consists of CO2 and water vapor. After condensation of the water in the exit gas from the fuel reactor, the remaining CO2 gas is compressed and cooled to yield liquid CO2, which can be disposed of in various ways.With the improvement of numerical methods and more advanced hardware technology, the time needed to run CFD (Computational fluid dynamics) codes is decreasing. Hence multiphase CFD-based models for dealing with complex gas-solid hydrodynamics and chemical reactions are becoming more accessible. Until now there were a few literatures about mathematical modeling of chemical-looping combustion using CFD approach. In this work, the reaction kinetics model of the fuel reactor (CaSO4 + H2) was developed by means of the commercial code FLUENT. The bubble formation and the relation between bubble formation and molar fraction of products in gas phase were well captured by CFD simulation. Computational results from the simulation also showed low fuel conversion rate. The conversion of H2 was about 34% partially due to fast, large bubbles rising through the reactor, low bed temperature and large particles diameter.  相似文献   

9.
To reduce the risks of climate change, atmospheric concentrations of greenhouse gases must be lowered. Direct capture of CO2 from ambient air, “air capture”, might be one of the few methods capable of systematically managing dispersed emissions. The most commonly proposed method for air capture is a wet scrubbing technique which absorbs CO2 in an alkaline absorbent, i.e. sodium hydroxide producing an aqueous solution of sodium hydroxide and sodium carbonate. In most of the previous works it was assumed that the absorbent would be regenerated and CO2 liberated from the alkaline carbonate solution using a lime and calcium carbonate causticization cycle.We describe a novel technique for recovering sodium hydroxide from an aqueous alkaline solution of sodium carbonate and present an end-to-end energy and exergy analysis. In the first step of the recovery process, anhydrous sodium carbonate is separated from the concentrated sodium hydroxide solution using a two-step precipitation and crystallization process. The anhydrous sodium carbonate is then causticized using sodium tri-titanate. The titanate direct causticization process has been of interest for the pulp and paper industry and has been tested at lab- and pilot-scale. In the causticization process, sodium hydroxide is regenerated and carbon dioxide is liberated as a pure stream, which is compressed for use or disposal. The technique requires ~50% less high-grade heat than conventional causticization and the maximum temperature required is reduced by at least 50 °C. This titanate cycle may allow a substantial reduction in the overall cost of direct air capture.  相似文献   

10.
Use of amines is one of the leading technologies for post-combustion carbon dioxide capture from gas and coal-fired power plants. This study assesses the potential environmental impact of emissions to air that result from use of monoethanol amine (MEA) as an absorption solvent for the capture of carbon dioxide (CO2). Depending on operation conditions and installed reduction technology, emissions of MEA to the air due to solvent volatility losses are expected to be in the range of 0.01–0.8 kg/tonne CO2 captured. Literature data for human and environmental toxicity, together with atmospheric dispersion model calculations, were used to derive maximum tolerable emissions of amines from CO2 capture. To reflect operating conditions with typical and with elevated emissions, we defined a scenario MEA-LOW, with emissions of 40 t/year MEA and 5 t/year diethyl amine (DEYA), and a scenario MEA-HIGH, with emissions of 80 t/year MEA and 15 t/year DEYA. Maximum MEA deposition fluxes would exceed toxicity limits for aquatic organisms by about a factor of 3–7 depending on the scenario. Due to the formation of nitrosamines and nitramines, the estimated emissions of DEYA are close to or exceed safety limits for drinking water and aquatic ecosystems. The “worst case” scenario approach to determine maximum tolerable emissions of MEA and other amines is in particular useful when both expected environmental loads and the toxic effects are associated with high uncertainties.  相似文献   

11.
A core sample including casing, cement, and shale caprock was obtained from a 30-year old CO2-flooding operation at the SACROC Unit, located in West Texas. The core was investigated as part of a program to evaluate the integrity of Portland-cement based wellbore systems in CO2-sequestration environments. The recovered cement had air permeabilities in the tenth of a milliDarcy range and thus retained its capacity to prevent significant flow of CO2. There was evidence, however, for CO2 migration along both the casing–cement and cement–shale interfaces. A 0.1–0.3 cm thick carbonate precipitate occurs adjacent to the casing. The CO2 producing this deposit may have traveled up the casing wall or may have infiltrated through the casing threads or points of corrosion. The cement in contact with the shale (0.1–1 cm thick) was heavily carbonated to an assemblage of calcite, aragonite, vaterite, and amorphous alumino-silica residue and was transformed to a distinctive orange color. The CO2 causing this reaction originated by migration along the cement–shale interface where the presence of shale fragments (filter cake) may have provided a fluid pathway. The integrity of the casing–cement and cement–shale interfaces appears to be the most important issue in the performance of wellbore systems in a CO2 sequestration reservoir.  相似文献   

12.
Capturing and storing carbon dioxide (CO2) underground for thousands of years is one way to reduce atmospheric greenhouse gases, often associated with global warming. Leakage through wells is one of the major issues when storing CO2 in depleted oil or gas reservoirs. CO2-injection candidates may be new wells, or old wells that are active, closed or abandoned. In all cases, it is critical to ensure that the long-term integrity of the storage wells is not compromised. The loss of well integrity may often be explained by the geochemical alteration of hydrated cement that is used to isolate the annulus across the producing/injection intervals in CO2-related wells. However, even before any chemical degradation, changes in downhole conditions due to supercritical CO2 injections can also be responsible for cement debonding from the casing and/or from the formation, leading to rapid CO2 leakage. A new cement with better CO2 resistance is compared with conventional cement using experimental procedure and methodology simulating the interaction of set cement with injected, supercritical CO2 under downhole conditions. Geochemical experimental data and a mechanical modeling approach are presented. The use of adding expanding property to this new cement to avoid microannulus development during the CO2 injection is discussed.  相似文献   

13.
In Salah Gas Project in Algeria has been injecting 0.5–1 million tonnes CO2 per year over the past 5 years into a water-filled strata at a depth of about 1800–1900 m. Unlike most CO2 storage sites, the permeability of the storage formation is relatively low and comparatively thin with a thickness of about 20 m. To ensure adequate CO2 flow-rates across the low-permeability sand-face, the In Salah Gas Project decided to use long-reach (about 1–1.5 km) horizontal injection wells. In an ongoing research project we use field data and coupled reservoir-geomechanical numerical modeling to assess the effectiveness of this approach and to investigate monitoring techniques to evaluate the performance of a CO2 injection operation in relatively low-permeability formations. Among the field data used are ground surface deformations evaluated from recently acquired satellite-based inferrometry (InSAR). The InSAR data shows a surface uplift on the order of 5 mm per year above active CO2 injection wells and the uplift pattern extends several km from the injection wells. In this paper we use the observed surface uplift to constrain our coupled reservoir-geomechanical model and conduct sensitivity studies to investigate potential causes and mechanisms of the observed uplift. The results of our analysis indicate that most of the observed uplift magnitude can be explained by pressure-induced, poro-elastic expansion of the 20-m-thick injection zone, but there could also be a significant contribution from pressure-induced deformations within a 100-m-thick zone of shaly sands immediately above the injection zone.  相似文献   

14.
Sequestration of carbon dioxide (CO2) in deep saline aquifers has emerged as an option for reducing greenhouse gas emissions to the atmosphere. The large amounts of supercritical CO2 that need to be injected into deep saline aquifers may cause large fluid pressure increases. The resulting overpressure may promote reactivation of sealed fractures or the creation of new ones in the caprock seal. This could lead to escape routes for CO2. In order to assess the probability of such an event, we model an axisymmetric horizontal aquifer–caprock system, including hydromechanical coupling. We study the failure mechanisms, using a viscoplastic approach. Simulations illustrate that, depending on boundary conditions, the least favorable moment takes place at the beginning of injection. Initially, fluid pressure rises sharply because of a reduction in permeability due to desaturation. Once CO2 fills the pores in the vicinity of the injection well and a capillary fringe is fully developed, the less viscous CO2 displaces the brine and the capillary fringe laterally. The overpressure caused by the permeability reduction within the capillary fringe due to desaturation decreases with distance from the injection well. This results in a drop in fluid pressure buildup with time, which leads to a safer situation. Nevertheless, in the presence of low-permeability boundaries, fluid pressure continues to rise in the whole aquifer. This occurs when the radius of influence of the injection reaches the outer boundary. Thus, caprock integrity might be compromised in the long term.  相似文献   

15.
The oxyfuel process is one of the most promising options to capture CO2 from coal fired power plants. The combustion takes place in an atmosphere of almost pure oxygen, delivered from an air separation unit (ASU), and recirculated flue gas. This provides a flue gas containing 80–90 vol% CO2 on a dry basis. Impurities are caused by the purity of the oxygen from the ASU, the combustion process and air ingress. Via liquefaction a CO2 stream with purity in the range from 85 to 99.5 vol% can be separated and stored geologically. Impurities like O2, NOX, SOX, and CO may negatively influence the transport infrastructure or the geological storage site by causing geochemical reactions. Therefore the maximum acceptable concentrations of the impurities in the separated CO2 stream must be defined regarding the requirements from transportation and storage. The main objective of the research project COORAL therefore is to define the required CO2 purity for capture and storage.  相似文献   

16.
A means of determining air emission source regions adversely influencing the city of Prince George, British Columbia, Canada from potential burning of isolated piles of mountain pine beetle-killed lodge pole pine is presented. The analysis uses the CALPUFF atmospheric dispersion model to identify safe burning regions based on atmospheric stability and wind direction. Model results show that the location and extent of influence regions is sensitive to wind speed, wind direction, atmospheric stability and a threshold used to quantify excessive concentrations. A concentration threshold based on the Canada Wide PM2.5 Standard is used to delineate the influence regions while Environment Canada's (EC) daily ventilation index (VI) is used to quantify local atmospheric stability. Results from the analysis, to be used by air quality meteorologists in assessing daily requests for burning permits, are presented as a series of maps delineating acceptable burning locations for sources placed at various distances from the city center and under different ventilation conditions. The results show that no burning should be allowed within 10 km of the city center; under poor ventilation conditions, no burning should be allowed within 20 km of the city center; under good ventilation conditions, burning can be allowed within 10–15 km of the city center; under good to fair ventilation conditions, burning can be allowed beyond 15 km of the city center; and if the wind direction can be reliably forecast, burning can be allowed between 5 and 10 km downwind of the city center under good ventilation conditions.  相似文献   

17.
The widespread use of fossil fuels within the current energy infrastructure is considered as the largest source of anthropogenic emissions of carbon dioxide, which is largely blamed for global warming and climate change. At the current state of development, the risks and costs of non-fossil energy alternatives, such as nuclear, biomass, solar, and wind energy, are so high that they cannot replace the entire share of fossil fuels in the near future timeframe. Additionally, any rapid change towards non-fossil energy sources, even if possible, would result in large disruptions to the existing energy supply infrastructure. As an alternative, the existing and new fossil fuel-based plants can be modified or designed to be either “capture” or “capture-ready” plants in order to reduce their emission intensity through the capture and permanent storage of carbon dioxide in geological formations. This would give the coal-fired power generation units the option to sustain their operations for longer time, while meeting the stringent environmental regulations on air pollutants and carbon emissions in years to come.Currently, there are three main approaches to capturing CO2 from the combustion of fossil fuels, namely, pre-combustion capture, post-combustion capture, and oxy-fuel combustion. Among these technology options, oxy-fuel combustion provides an elegant approach to CO2 capture. In this approach, by replacing air with oxygen in the combustion process, a CO2-rich flue gas stream is produced that can be readily compressed for pipeline transport and storage. In this paper, we propose a new approach that allows air to be partially used in the oxy-fired coal power plants. In this novel approach, the air can be used to carry the coal from the mills to the boiler (similar to the conventional air-fired coal power plants), while O2 is added to the secondary recycle flow as well as directly to the combustion zone (if needed). From a practical point of view, this approach eliminates problems with the primary recycle and also lessens concerns about the air leakage into the system. At the same time, it allows the boiler and its back-end piping to operate under slight suction; this avoids the potential danger to the plant operators and equipment due to possible exposure to hot combustion gases, CO2 and particulates. As well, by integrating oxy-fuel system components and optimizing the overall process over a wide range of operating conditions, an optimum or near-optimum design can be achieved that is both cost-effective and practical for large-scale implementation of oxy-fired coal power plants.  相似文献   

18.
Coalbed methane is an important resource of energy. Meanwhile CO2 sequestration in coal is a potential management option for greenhouse gas emissions. An attractive aspect to this process is that CO2 is adsorbed to the coal, reducing the risk of CO2 migration to the surface. Another aspect to this is that the injected CO2 could displace adsorbed methane leading to enhanced coalbed methane recovery. Therefore, in order to understand gas migration within the reservoir, mixed-gas adsorption models are required. Moreover, coal reservoir permeability will be significantly affected by adsorption-induced coal swelling during CO2 injection. Coal swelling is directly related to reservoir pressure and gas content which is calculated by adsorption models in reservoir simulation. Various models have been studied to describe the pure- and mixed-gas adsorption on coal. Nevertheless, only the Langmuir and Extended Langmuir models are usually applied in coal reservoir simulations. This paper presents simulation work using several approaches to representing gas adsorption, implemented into the coal seam gas reservoir simulator SIMED II. The adsorption models are the Extended Langmuir model (ELM), the Ideal Adsorbed Solution (IAS) model and the Two-Dimensional Equation of State (2D EOS). The simulations based on one Australian and one American coal sample demonstrated that (1) the Ideal Adsorbed Solution model, in conjunction with Langmuir model as single-component isotherm, shows similar simulation results as the ELM for both coals, with the IAS model representing the experimental adsorption data more accurately than the ELM for one coal and identically with the ELM for the other coal; (2) simulation results using the 2D EOS, however, are significantly different to the ELM or IAS model for both coal samples. The magnitude of the difference is also dependent on coal swelling and the well operating conditions, such as injection pressure.  相似文献   

19.
CO2 injection into a depleted hydrocarbon field or aquifer may give rise to a variety of coupled physical and chemical processes. During CO2 injection, the increase in pore pressure can induce reservoir expansion. As a result the in situ stress field may change in and around the reservoir. The geomechanical behaviour induced by oil production followed by CO2 injections into an oil field reservoir in the Paris Basin has been numerically modelled. This paper deals with an evaluation of the induced deformations and in situ stress changes, and their potential effects on faults, using a 3D geomechanical model. The geomechanical analysis of the reservoir–caprock system was carried out as a feasibility study using pressure information in a “one way” coupling, where pressures issued from reservoir simulations were integrated as input for a geomechanical model. The results show that under specific assumptions the mechanical effects of CO2 injection do not affect the mechanical stability of the reservoir–caprock system. The ground vertical movement at the surface ranges from ?2 mm during oil production to +2.5 mm during CO2 injection. Furthermore, the changes in in situ stresses predicted under specific assumptions by geomechanical modelling are not significant enough to jeopardize the mechanical stability of the reservoir and caprock. The stress changes issued from the 3D geomechanical modelling are also combined with a Mohr–Coulomb analysis to determine the fault slip tendency. By integrating the stress changes issued from the geomechanical modelling into the fault stability analysis, the critical pore pressure for fault reactivation is higher than calculated for the fault stability analysis considering constant horizontal stresses.  相似文献   

20.
A reaction calorimeter was used to determine the enthalpies of absorption of CO2 in aqueous ammonia and in aqueous solutions of ammonium carbonate at temperatures of 35–80 °C. The heat of absorption of CO2 with 2.5 wt% aqueous ammonia solution was found to be about 70 kJ/mol CO2, which is lower than that with MEA (around 85 kJ/mol) at 35 and 40 °C. The value decreases with increased loading, but not to as low a value as expected by the carbonate–bicarbonate reaction (26.88 kJ/mol). The enthalpy of absorption of CO2 in aqueous ammonia at 60 and 80 °C decreases with loadings at first, then increases between 0.2 mol CO2/mol NH3 and 0.6 mol CO2/mol NH3, and then decreases again. The behavior of the heat of absorption of CO2 in 10 wt% ammonium carbonate solution was found to be the same as that of aqueous ammonia at loadings above 0.6 mol CO2/mol NH3. The heat of absorption increases with increasing temperature. The heats of absorption are directly related to the extent of the various reactions with CO2 and can be assessed from the species variation in the liquid phase.  相似文献   

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