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1.
The goal of this paper is to find methodologies for removing a selection of impurities (H2O, O2, Ar, N2, SOx and NOx) from CO2 present in the flue gas of two oxy-combustion power plants fired with either natural gas (467 MW) or pulverized fuel (596 MW). The resulting purified stream, containing mainly CO2, is assumed to be stored in an aquifer or utilized for enhanced oil recovery (EOR) purposes. Focus has been given to power cycle efficiency i.e.: work and heat requirements for the purification process, CO2 purity and recovery factor (kg of CO2 that is sent to storage per kg of CO2 in the flue gas). Two different methodologies (here called Case I and Case II) for flue gas purification have been developed, both based on phase separation using simple flash units (Case I) or a distillation column (Case II). In both cases purified flue gas is liquefied and its pressure brought to 110 atm prior to storage.Case I: A simple flue gas separation takes place by means of two flash units integrated in the CO2 compression process. Heat in the process is removed by evaporating the purified liquid CO2 streams coming out from both flashes. Case I shows a good performance when dealing with flue gases with low concentration of impurities. CO2 fraction after purification is over 96% with a CO2 recovery factor of 96.2% for the NG-fired flue gas and 88.1% for the PF-fired flue gas. Impurities removal together with flue gas compression and liquefaction reduces power plant output of 4.8% for the NG-fired flue gas and 11.6% for the PF-fired flue gas. The total amount of work requirement per kg stored CO2 is 453 kJ for the NG-fired flue gas and 586 kJ for the PF-fired flue gas.Case II: Impurities are removed from the flue gas in a distillation column. Two refrigeration loops (ethane and propane) have been used in order to partially liquefy the flue gas and for heat removal from a partial condenser. Case II can remove higher amounts of impurities than Case I. CO2 purity prior to storage is over 99%; CO2 recovery factor is somewhat lower than in Case I: 95.4% for the NG-fired flue gas and 86.9% for the PF-fired flue gas, reduction in the power plant output is similar to Case I.Due to the lower CO2 recovery factor the total amount of work per kg stored CO2 is somewhat higher for Case II: 457 kJ for the NG-fired flue gas and 603 kJ for the PF-fired flue gas.  相似文献   

2.
Acid gas geological disposal is a promising process to reduce CO2 atmospheric emissions and an environment-friendly and economic alternative to the transformation of H2S into sulphur by the Claus process. Acid gas confinement in geological formations is to a large extent controlled by the capillary properties of the water/acid–gas/caprock system, because a significant fraction of the injected gas rises buoyantly and accumulates beneath the caprock. These properties include the water/acid gas interfacial tension (IFT), to which the so-called capillary entry pressure of the gas in the water-saturated caprock is proportional. In this paper we present the first ever systematic water/acid gas IFT measurements carried out by the pendant drop technique under geological storage conditions. We performed IFT measurements for water/H2S systems over a large range of pressure (up to P = 15 MPa) and temperature (up to T = 120 °C). Water/H2S IFT decreases with increasing P and levels off at around 9–10 mN/m at high T (≥70 °C) and P (>12 MPa). The latter values are around 30–40% of water/CO2 IFTs, and around 20% of water/CH4 IFTs at similar T and P conditions. The IFT between water and a CO2 + H2S mixture at T = 77 °C and P > 7.5 MPa is observed to be approximately equal to the molar average IFT of the water/CO2 and water/H2S binary mixtures. Thus, when the H2S content in the stored acid gas increases the capillary entry pressure decreases, together with the maximum height of acid gas column and potential storage capacity of a given geological formation. Hence, considerable attention should be exercised when refilling with a H2S-rich acid gas a depleted gas reservoir, or a depleted oil reservoir with a gas cap: in the case of hydrocarbon reservoirs that were initially (i.e., at the time of their discovery) close to capillary leakage, acid gas leakage through the caprock will inevitably occur if the refilling pressure approaches the initial reservoir pressure.  相似文献   

3.
With thermogravimetric apparatus (TGA), X-ray diffraction (XRD) and barium sulfate gravimetric methods, the carbonation reactivities of K2CO3 and K2CO3/Al2O3 in the simulated flue gases with SO2 are investigated and the reaction equations are inferred. Results show that there are KHCO3 and K2SO3 generated. The generation K2SO3 reduces the utilization ratio of the sorbent. H2O may accelerates the sulfation reaction of AR K2CO3 as K4H2(CO3)3·1.5H2O is generated in the reaction among K2CO3, SO2 and H2O. K2SO3 is directly generated from sulfation reaction of K2CO3/Al2O3, because there are K2CO3·1.5H2O and K2SO3 generated in the reaction among K2CO3/Al2O3, SO2 and H2O. K2CO3·1.5H2O does not react with SO2, and K2CO3·1.5H2O/Al2O3 reacts with SO2 slowly. Compare with the reaction process without H2O pretreatment, the reaction rates of KAl30 increased after H2O pretreatment and the failure ratio is about a half of that without H2O pretreatment. So, K2CO3/Al2O3 shows good carbonation and anti-sulfation characteristic after H2O pretreatment.  相似文献   

4.
A method is presented here by which the actual numbers of individuals in the U.S. population who would be expected to suffer respiratory illness as a result of exposure to ambient nitrogen dioxide (NO2) concentrations in excess of the Federally-designated ambient air quality standard can be estimated. At the same time we have attempted to quantify how these adverse health effects would be alleviated by various degrees of reductions in current ambient concentrations. In addition, the health benefit expected to be derived by various NOx emission control strategies will be examined utilizing the health benefit estimation method presented.It is estimated that there were approximately 33.2×106 excess cases of respiratory illnesses in the U.S. in 1973 associated with ambient NO2 concentrations in excess of the national ambient standard. A reduction of approximately 50 to 60 percent below 1973 NO2 levels is needed to essentially eliminate excess respiratory illness associated with ambient NO2 concentration.  相似文献   

5.
FeSO4·xH2O is generated in large amounts in galvanizing workshops. It can be reutilized by conversion to Fe2O3. In this study, the recovery of Fe2O3 from FeSO4·xH2O formed in the galvanizing process has been examined. The experimental work was carried out at various temperatures and times in the oxidizing medium. The reaction temperatures and times were selected as 450, 500, 550, 600, 650, 700, 800 and 900°C, and 15, 30, 45, 60, 90 and 120 minutes, respectively. In order to determine the amount of Fe2O3, a titrimetric method was applied. The reaction products were characterized by means of IR and XRD techniques.The extent of conversion is low at temperatures below 650°C. Almost all of the iron (II) sulfate in the original sample was converted to iron(III) oxide at 650°C (120 min), 700°C (90 min), 800°C (60 min) and 900°C (45 min).  相似文献   

6.
The degradation of polyacrylamide (PAM) in simulate wastewater was studied in UV/Fenton/C4H4O62? system. The factors such as molecular ratio of H2O2/Fe2+/C4H4O62?, pH, and the dosage of Fenton reagent that could affect the PAM degradation in the UV/Fenton/C4H4O62? system were investigated. The experimental results showed that adding C4H4O62? to UV/Fenton system could form photosensitive ferrous complexes, which led to higher degradation efficiency of PAM. The degradation rate of PAM could be up to 95.2% under the following conditions: the concentration of H2O2, Fe2+, and C4H4O62? were 22.5, 2.25, and 2.25 mmol/L, respectively (i.e., molecular ratio of H2O2/Fe2+/C4H4O62? was 10:1:1), the pH value was 3.0.  相似文献   

7.
本研究利用2010年污染源普查数据和MEIC排放清单建立全国大气污染物高时空分辨率排放清单,在此基础上利用2012年环境统计数据对其进行修订建立2012年全国大气污染物高时空分辨率排放清单;结合《大气污染防治行动计划》(以下简称《计划》)研究工作,测算了《计划》实施后在污染源综合治理、落后产能淘汰、能源结构调整方面对SO2、NOx、颗粒物、VOCs的减排量,同时对污染物新增量进行了预测,建立了《计划》实施后全国大气污染物高时空分辨率排放清单;利用CMAQ空气质量模型模拟分析了《计划》实施的空气质量改善效果。结果表明:《计划》实施后,将可以减少641万吨SO2、859万吨NOx、547万吨颗粒物(不含扬尘污染控制)、627万吨VOCs,全国、京津冀、长三角及珠三角区域PM2.5年均浓度将分别比2012年下降22.08%、33.99%、23.98%、24.04%。如果《计划》要求全部落实,可以实现空气质量改善目标。  相似文献   

8.
长三角地区作为我国大气污染较为严重区域之一,如何在保持经济增长的同时减少CO2与大气污染物的排放已成为一个重要挑战。本研究基于2007年与2012年长三角区域间投入产出表,定量分析了长三角地区省市间贸易引致的二氧化碳和大气污染物排放转移特征和变化趋势。同时,运用产业关联系数法,从前向关联与后向关联双重视角分析了长三角地区减缓CO2和大气污染物排放的关键行业。研究结果表明,长三角的SO2、PM2.5排放总量表现为消费端大于生产端,CO2、NOx排放总量表现为生产端大于消费端。安徽省总体呈现为长三角地区贸易的SO2、NOx与PM2.5排放净调出地,而上海与浙江表现为多数污染物排放净调入地。CO2与大气污染物协同前向减排的关键行业为江苏省、浙江省和安徽省的电力、热力的生产和供应业,安徽省的煤炭开采和洗选业等,可以通过生产端技术革新和能源结构优化来促进减排;CO2与大气污染物后向协同减排的关键行业为江苏省、浙江省和安徽省的建筑业等,对于这些行业,调整消费结构是有效的减排措施。为更好地制定长三角地区减排与污染防治政策,应当综合考虑行业减排、协同减排等,以确保经济持续增长的同时达到减排目标。  相似文献   

9.
Elevated levels of CO2 in the atmosphere have been linked to the rise in land and sea temperature [Climate Change, 2001. In: Houghton, J.T., Ding, Y., Griggs, D.J., Noguer, M., van der Linden, P.J., Xiaosu, D. (Eds.), The Scientific Basis Contribution of Working Group I to the Third Assessment Report of the Intergovernmental Panel on Climate Change (IPCC). Cambridge University Press, UK, p. 944]. To demonstrate geological carbon sequestration as a mitigation technique, a carbon dioxide injection experiment was conducted in East Texas. The target – Frio formation – is a highly porous, permeable and unconsolidated sandstone. The specific interval is the Frio C sand, which originally was saturated with saline formation water. At the injection location, the Frio C sand dips 18° to the south. To monitor the injected CO2 spreading in the formation, an old well from 1956 drilled into the deeper Yegua formation was selected as the observation well. The injection well was drilled at a distance of 100 ft downdip from the monitoring well. Several borehole measurement methods were available to monitor the CO2 injection, but the most suitable technology was thought to be the pulsed neutron logging. This logging is used widely in cased hole, and the measured macroscopic thermal absorption cross-section (Σ) is sensitive to CO2 saturation in high porosity saline water environments. Several log examples are given demonstrating successful the monitoring of the CO2 plume moving through the two boreholes and the resulting saturation changes.  相似文献   

10.
Chemical looping combustion (CLC) is a process in which oxygen required for combustion of a fuel is supplied by the metal oxide. Metal oxide plays the role of an oxygen carrier by providing oxygen for combustion when being reduced and is then re-oxidized by air in a separate reactor. Combustion is thus without any direct contact between air and fuel: as a consequence flue gas does not contain nitrogen of air which simplifies flue gas treatment prior to sequestration. In the present study, biogas combustion was analyzed in a chemical looping combustion fluidized bed reactor. NiAl0.44O1.67 and Cu0.95Fe1.05AlO4 metal oxide particles were used as oxygen carriers. The experiments have shown the feasibility of biogas combustion in chemical looping combustion: CH4 of the biogas was completely converted to CO2 and H2O with a small fraction of CO and H2. The outlet flue gas distribution profile was not affected by ageing during the cycles of reduction and oxidation, indicating the chemical stability of the oxygen carriers. There was limited formation of carbon on the oxygen carriers during reduction.  相似文献   

11.
A numerical study was conducted to predict pCO2 change in the ocean on a continental shelf by the leakage of CO2, which is originally stored in the aquifer under the seabed, in the case that a large fault connects the CO2 reservoir and the seabed by an earthquake or other diastrophism. The leakage rate was set to be 6.025 × 10−4 kg/m2/sec from 2 m × 100 m fault band, which corresponds to 3800 t-CO2/year, referring to the monitored seepage rate from an existing EOR field. The target space in this study was limited to the ocean above the seabed, the depth of which was 200 or 500 m. The computational domain was idealistically rectangular with the seabed fault-band perpendicular to the uniform flow. The CO2 takes a form of bubbles or droplets, depending on the depth of water, and their behaviour and dissolution were numerically simulated during their rise in seawater flow. The advection–diffusion of dissolved CO2 was also simulated. As a result, it was suggested that the leaked CO2 droplets/bubbles all dissolve in the seawater before spouting up to the atmosphere, and that the increase in pCO2 in the seawater was smaller than 500 μ atm.  相似文献   

12.
The gasification reaction of Nantong inferior coal was investigated in a laboratory fixed-bed reactor under CO2 and O2/H2O atmospheres. The effects of the bed temperature and inlet-gas concentration on the yields of CO, H2, and CH4 were studied. The effects of coal ash and particle size on the fixed-carbon conversion were also investigated, and kinetic analysis was conducted with a homogeneous model. The product-gas-heating value and fixed-carbon conversion increased when the temperature was increased from 950 °C to 1100 °C under CO2 atmosphere. When the inlet-CO2 concentration was increased from 50 to 100 vol.%, the low heating value of the product gas and carbon conversion ratio slightly increased. During the gasification of inferior coal under the O2/H2O atmosphere, the CO concentration increased rapidly with increasing temperature. The H2 and CH4 concentrations increased initially and then decreased. The maximum gas heating value of 7934 kJ/m3 was obtained under the O2 concentration of 70 vol.% at a bed temperature of 1050 °C. The cold-gas efficiency increased with increasing temperature and became 40.6% and 86.4% at 1100 °C under the CO2 and O2/H2O atmospheres, respectively. The gasification reaction of the Nantong inferior coal strongly depended on the content of inherent inorganic matter. The gasification rates for both the CO2 and O2/H2O atmospheres were independent of the particle size. The activation energy for the CO2 and O2/H2O gasification reactions were 137 and 81 kJ/mol, respectively. The gasification reactions of the Nantong coal, which was performed under two different atmospheres, were compared and the reaction activity of the gasification reaction under CO2 atmosphere was found to be much lower than that under the O2/H2O atmosphere.  相似文献   

13.
Adsorption is one of the most promising technologies for reducing CO2 emissions and at present several different types of sorbents are being investigated. The use of sorbents obtained from low-cost and abundant precursors (i.e. solid wastes) appears an attractive strategy to adopt because it will contribute to a reduction not only in operational costs but also in the amount of waste that is dumped and burned in landfills every year. Following on from previous studies by the authors, in this work several carbon-based adsorbents were developed from different carpet wastes (pre-consumer and post-consumer wastes) by chemical activation with KOH at various activation temperatures (600–900 °C) and KOH:char impregnation ratios (0.5:1 to 4:1). The prepared materials were characterised by chemical analysis and gas adsorption (N2, −196 °C; CO2, 0 °C), and tested for CO2 adsorption at temperatures of 25 and 100 °C. It was found that both the type of precursor and the conditions of activation (i.e. impregnation ratios, and activation temperatures), had a huge influence on the microporosity of the resultant samples and their CO2 capture capacities. The carbon-based adsorbent that presented the maximum CO2 capture capacities at 25 and 100 °C (13.8 wt.% and 3.1 wt.%, respectively), was prepared from a pre-consumer carpet waste and was activated at 700 °C using a KOH:char impregnation ratio of 1:1. This sample showed the highest narrow microporosity volume (0.47 cm3 g−1), thus confirming that only pores of less than 1 nm are effective for CO2 adsorption at atmospheric pressure.  相似文献   

14.
The effects of nano-SiO2 on three ash particle sizes in mortar were studied by replacing a portion of the cement with incinerated sewage sludge ash. Results indicate that the amount of water needed at standard consistency increased as more nano-SiO2 was added. Moreover, a reduction in setting time became noticeable for smaller ash particle sizes. The compressive strength of the ash–cement mortar increased as more nano-SiO2 was added. Additionally, with 2% nano-SiO2 added and a cure length of 7 days, the compressive strength of the ash–cement mortar with 1 μm ash particle size was about 1.5 times better that of 75 μm particle size. Further, nano-SiO2 functioned to fill pores for ash–cement mortar with different ash particle sizes. However, the effects of this pore-filling varied with ash particle size. Higher amounts of nano-SiO2 better influenced the ash–cement mortar with larger ash particle sizes.  相似文献   

15.
Oxyfuel combustion in a pulverised fuel coal-fired power station produces a raw CO2 product containing contaminants such as water vapour plus oxygen, nitrogen and argon derived from the excess oxygen for combustion, impurities in the oxygen used, and any air leakage into the system. There are also acid gases present, such as SO3, SO2, HCl and NOx produced as byproducts of combustion. At GHGT8 (White and Allam, 2006) we presented reactions that gave a path-way for SO2 to be removed as H2SO4 and NO and NO2 to be removed as HNO3. In this paper we present initial results from the OxyCoal-UK project in which these reactions are being studied experimentally to provide the important reaction kinetic information that is so far missing from the literature. This experimental work is being carried out at Imperial College London with synthetic flue gas and then using actual flue gas via a sidestream at Doosan Babcock's 160 kW coal-fired oxyfuel rig. The results produced support the theory that SOx and NOx components can be removed during compression of raw oxyfuel-derived CO2 and therefore, for emissions control and CO2 product purity, traditional FGD and deNOx systems should not be required in an oxyfuel-fired coal power plant.  相似文献   

16.
Recent strategies for simultaneously reducing NOx and soot emissions have focused on achieving nearly premixed, low-temperature combustion (LTC) in diesel engines. A promising approach in this regard is to vary fuel reactivity in order to control the ignition delay and optimize the level of premixing and reduce emissions. The present study examines such a strategy by performing 3-D simulations in a single-cylinder of a diesel engine. Simulations employ the state-of-the-art two-phase models and a validated semi-detailed reaction mechanism. The fuel reactivity is varied by using a blend of n-heptane and iso-octane, which represent surrogates for gasoline and diesel fuels, respectively. Results indicate that the fuel reactivity strongly influences ignition delay and combustion phasing, whereas the start of injection (SOI) affects combustion phasing. As fuel reactivity is reduced, the ignition delay is increased and the combustion phasing is retarded. The longer ignition delay provides additional time for mixing, and reduces equivalence ratio stratification. Consequently, the premixed combustion is enhanced relative to diffusion combustion, and thus the soot emission is reduced. NOx emission is also reduced due to reduced diffusion combustion and lower peak temperatures caused by delayed combustion phasing. An operability range is observed in terms of fuel reactivity and SOI, beyond which the mixture may not be sufficiently well mixed, or compression ignited. The study demonstrates the possibility of finding an optimum range of fuel reactivity, SOI, and EGR for significantly reducing engine out emissions for a given load and speed.  相似文献   

17.
In this research, nanoporous zeolite T membranes were synthesized at three levels of synthesis temperature: 100, 120 and 140 °C and synthesis time: 15, 30 and 50 h and characterized by gas permeation. Effects of synthesis parameters on CO2 and CH4 permeances and CO2/CH4 ideal separation factors were studied. All experiments were conducted at 1 bar feed pressure and 30 °C module temperature. Normally, it is anticipated that increasing synthesis temperature and synthesis time increase gas permeances and consequently decrease ideal separation factor. This prediction was not observed in the case of synthesis temperature increase from 100 to 120 °C as well as synthesis time increase from 15 to 30 h, due to the dual effect of increasing synthesis temperature and synthesis time on gas permeances and ideal separation factor. More zeolites are deposited and larger crystals are formed at higher synthesis temperatures and times. Forming the larger crystals accelerates the rate of zeolite layer integration, which is responsible for gas separation, in one hand and reduces the density of deposited zeolite layer on the support, due to the formation of more voids, on the other hand. In terms of maximizing the CO2/CH4 ideal separation factor, medium synthesis temperature and synthesis time (120 °C and 30 h) can be selected, however, maximum gas permeances are obtained at low levels of synthesis temperature and time (100 °C and 15 h). According to the ranges of gas permeances (10−11 to 10−6 mol/m2 s Pa) and CO2/CH4 ideal separation factors (1.4–70.3), it is concluded that the zeolite T membranes synthesized at optimum conditions can be employed for membrane separation of CO2/CH4 mixtures.  相似文献   

18.
This work presents contact angle measurements for CO2–water–quartz/calcite systems at general sequestration pressure and temperature conditions (200–3000 psig and 77–122 °F). The effect of drop volume, repeated exposure of the substrates to dense water saturated CO2, pressure and temperature on the contact angles is examined. In the 1st measurement cycle, the contact angles for the quartz substrate varied from 46 to 48° and 47 to 46° for gaseous (water saturated) CO2 and liquid (water saturated) CO2 respectively, at 77 °F. For calcite substrate, these values varied from 45 to 48° and 42 to 40°, respectively. Remarkably, this work highlights a characteristic permanent shift in the contact angle data with repeated exposure to dense, water saturated, CO2. The contact angle data trends after repeated exposure to the dense, water saturated CO2 varied from 89 to 91° and 85 to 80° for the quartz substrate for gaseous (water saturated) CO2 and liquid (water saturated) CO2 respectively, at 77 °F. For calcite substrates, these values varied from 60 to 59° and 54 to 48°, respectively. This important observation has serious implications towards the design and safety issues, as a permanent positive contact angle shift indicates lower CO2 retention capabilities of sequestration sites due to a reduction in the capillary pressure. It is further confirmed that the permanent shift in the contact angle is due to surface phenomena. With an increase in temperature (from 77 to 122 °F), the contact angle shift is reduced from about 45° to about 20° for quartz substrates. Other observations in the contact angle data with respect to pressure are in good agreement with the trends reported in the literature.  相似文献   

19.
Recycling of municipal wastewater requires treatment with flocculants, such as polyacrylamide. It is unknown how polyacrylamide in sludge affects removal of polycyclic aromatic hydrocarbons (PAH) from soil. An alkaline-saline soil and an agricultural soil were contaminated with phenanthrene and anthracene. Sludge with or without polyacrylamide was added while emission of CO2 and concentrations of NH4+, NO3, NO2, phenanthrene and anthracene were monitored in an aerobic incubation experiment. Polyacrylamide in the sludge had no effect on the production of CO2, but it reduced the concentration of NH4+, increased the concentration of NO3 in the Acolman soil and NO2 in the Texcoco soil, and increased N mineralization compared to the soil amended with sludge without polyacrylamide. After 112 d, polyacrylamide accelerated the removal of anthracene from both soils and that of phenanthrene in the Acolman soil. It was found that polyacrylamide accelerated removal of phenanthrene and anthracene from soil.  相似文献   

20.
The membrane separation process for CO2 capture can be interfered by the gaseous components and the fine particles in flue gas, especially in desulfurized flue gas. In this work, the pint-sized Polyimide(PI) hollow fiber membrane contactors were self-packed to investigate the membrane CO2 separation from flue gas containing fine particles and gaseous contaminants (SO2,SO3,H2O). First, the effects of SO2, SO3, water vapor, and gypsum particles on the CO2 capture were studied independently and synergistically. The results showed that the effect of SO2 on the membrane separation properties is indistinctive; however, the membrane performance was damaged seriously with the addition of SO3. The high humidity promoted the CO2 separation initially before inhibiting the PI membrane performance. Moreover, the decrease of the CO2/N2 selectivity and the permeation rate were accelerated with the coexistence of SO2. The membrane performance showed an obvious deterioration in the presence of gypsum particles, with a 21% decrease in the CO2/N2 selectivity and 51% decrease in the permeation rate. Furthermore, the gypsum particles exerted dramatic damage. Under the WFGD conditions, the combined effects of SO2, water vapor, and the gypsum particles influenced the stability of the membrane significantly. This tendency is mainly attributed to the deposition of fine particles and aerosol on the membrane surface, which occupied the effective area and enhanced the mass transfer resistance. This study of impurities’ influence could play an important role in further industrial application of membrane CO2 capture.  相似文献   

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