Electric Swing Adsorption for CO2 removal from flue gases

One of the most important sources of CO₂ emissions are the fossil-fuel fired plants for production of electricity. Removal of CO₂ from flue gas streams for further sequestration has been proposed by the International Panel on Climate Change experts as one of the most reliable solutions to mitigate anthropogenic greenhouse emissions. When natural gas is employed as fuel, the molar fraction of CO₂ in the flue gas is lower than 5% causing serious problems for capture. The purpose of this work is to present experimental validation of an Electric Swing Adsorption (ESA) technology that may be employed for carbon capture for low molar fractions of CO₂ in the flue gas streams. To improve energy utilization, an activated carbon honeycomb monolith with low electrical resistivity was employed as selective adsorbent. A mathematical model for this honeycomb is proposed as well as different ESA cycles for CO₂ capture.     

Effect of steam hydration on performance of lime sorbent for CO2 capture

Lime is considered a feasible sorbent for the capture of CO₂ from large stationary sources. The positive attributes of a natural source material, low cost and lack of harmful by-products are offset by rapid deterioration in performance and high regeneration temperature. Performance can be improved by hydrating the lime using steam. We investigate a steam hydration process wherein lime is hydrated for 5 min at 300 °C and atmospheric pressure in a mixture of steam and CO₂. The experiments consisted of 10 capture cycles with 60% of the lime active at the end. Extrapolation using a decay model suggests a residual carbonation level of 48%, significantly higher than the 8% achieved by dry lime cycles. The cost of replacement sorbent under these conditions is less than $1/t of CO₂ captured. The hydrated lime process also reduces the thermal load, for heating and cooling, by half as well as the inventory, and therefore solids handling, by a factor 5 over dry lime. The introduction of the hydration reaction provides another exothermic reaction for heat management.     

An engineering-economic model of pipeline transport of CO2 with application to carbon capture and storage

Carbon dioxide capture and storage (CCS) involves the capture of CO₂ at a large industrial facility, such as a power plant, and its transport to a geological (or other) storage site where CO₂ is sequestered. Previous work has identified pipeline transport of liquid CO₂ as the most economical method of transport for large volumes of CO₂. However, there is little published work on the economics of CO₂ pipeline transport. The objective of this paper is to estimate total cost and the cost per tonne of transporting varying amounts of CO₂ over a range of distances for different regions of the continental United States. An engineering-economic model of pipeline CO₂ transport is developed for this purpose. The model incorporates a probabilistic analysis capability that can be used to quantify the sensitivity of transport cost to variability and uncertainty in the model input parameters. The results of a case study show a pipeline cost of US$ 1.16 per tonne of CO₂ transported for a 100 km pipeline constructed in the Midwest handling 5 million tonnes of CO₂ per year (the approximate output of an 800 MW coal-fired power plant with carbon capture). For the same set of assumptions, the cost of transport is US$ 0.39 per tonne lower in the Central US and US$ 0.20 per tonne higher in the Northeast US. Costs are sensitive to the design capacity of the pipeline and the pipeline length. For example, decreasing the design capacity of the Midwest US pipeline to 2 million tonnes per year increases the cost to US$ 2.23 per tonne of CO₂ for a 100 km pipeline, and US$ 4.06 per tonne CO₂ for a 200 km pipeline. An illustrative probabilistic analysis assigns uncertainty distributions to the pipeline capacity factor, pipeline inlet pressure, capital recovery factor, annual O&M cost, and escalation factors for capital cost components. The result indicates a 90% probability that the cost per tonne of CO₂ is between US$ 1.03 and US$ 2.63 per tonne of CO₂ transported in the Midwest US. In this case, the transport cost is shown to be most sensitive to the pipeline capacity factor and the capital recovery factor. The analytical model elaborated in this paper can be used to estimate pipeline costs for a broad range of potential CCS projects. It can also be used in conjunction with models producing more detailed estimates for specific projects, which requires substantially more information on site-specific factors affecting pipeline routing.     

Power generation with CO2 capture: Technology for CO2 purification

The goal of this paper is to find methodologies for removing a selection of impurities (H₂O, O₂, Ar, N₂, SO_x and NO_x) 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.     

Anticipating public attitudes toward underground CO2 storage

Carbon capture and storage (CCS) may play a central role in managing carbon emissions from the power sector and industry, but public support for the technology is unclear. To address this knowledge gap, and to test the use of discrete choice analysis for determining public attitudes, two focus groups and a national survey were conducted in Canada to investigate the public's perceptions of the benefits and risks of CCS, the likely determinants of public opinion, and overall support for the use of CCS.The results showed slight support for CCS development in Canada, and a belief that CCS is less risky than normal oil and gas industry operations, nuclear power, or coal-burning power plants. A majority of respondents indicate that they would support the use of CCS as part of a greenhouse gas reduction strategy, although it would likely have to be used in combination with energy efficiency and alternative energy technologies in order to retain public support.     

对一次高炉煤气燃烧放散过程可吸入颗粒物浓度变化情况的分析

通过对环境空气中可吸入颗粒物浓度监测数据在一次高炉煤气燃烧放散过程中变化情况的分析,得出特殊的局地地形条件和局部地面气象条件可能造成污染物汇集和积累的结论,并就此提出高炉煤气燃烧放散时污染控制的建议。     

A DFT study on the carbamates formation through the absorption of CO2 by AMP

DFT calculations in gas and aqueous solution phases have been performed to study the mechanism of carbamate formation by the absorption of CO₂ in 2-amino-2-methyl-1-propanol (AMP). The results reveal the importance of considering the effect of water as solvent for the reaction to proceed. Furthermore water molecules play an important role as a basic reactant leading to stable intermediates formation. These results point at a single-step, third order reaction as the most probable mechanism for the formation of carbamate by the absorption process.     

CO2 capture and storage from a bioethanol plant: Carbon and energy footprint and economic assessment

Biomass energy and carbon capture and storage (BECCS) can lead to a net removal of atmospheric CO₂. This paper investigates environmental and economic performances of CCS retrofit applied to two mid-sized refineries producing ethanol from sugar beets. Located in the Region Centre France, each refinery has two major CO₂ sources: fermentation and cogeneration units. “carbon and energy footprint” (CEF) and “discounted cash flow” (DCF) analyses show that such a project could be a good opportunity for CCS early deployment. CCS retrofit on fermentation only with natural gas fired cogeneration improves CEF of ethanol production and consumption by 60% without increasing much the non renewable energy consumption. CCS retrofit on fermentation and natural gas fired cogeneration is even more appealing by decreasing of 115% CO₂ emissions, while increasing non renewable energy consumption by 40%. DCF shows that significant project rates of return can be achieved for such small sources if both a stringent carbon policy and direct subsidies corresponding to 25% of necessary investment are assumed. We also underlined that transport and storage cost dilution can be realistically achieved by clustering emissions from various plants located in the same area. On a single plant basis, increasing ethanol production can also produce strong economies of scale.     

Highly siliceous MCM-48 from rice husk ash for CO2 adsorption

Mesoporous MCM-48 silica was synthesized using a cationic-neutral surfactant mixture as the structure-directing template and rice husk ash (RHA) as the silica source. The MCM-48 samples were characterized by X-ray powder diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), N₂ physisorption and SEM. X-ray diffraction pattern of the resulting MCM-48 revealed typical pattern of cubic Ia3d mesophase. BET results showed the MCM-48 to have a surface area of 1024 m²/g and FT-IR revealed a silanol functional group at about 3460 cm⁻¹. Breakthrough experiments in the presence of MCM-48 were also carried out to test the material's CO₂ adsorption capacity. The breakthrough time for CO₂ was found to decrease as the temperature increased from 298 K to 348 K. The steep slopes observed shows the CO₂ adsorption occurred very quickly, with only a minimal mass transfer effect and very fast kinetics. In addition, amine grafted MCM-48, APTS-MCM-48 (RHA), was prepared with the 3-aminopropyltriethoxysilane (APTS) to investigate the effect of amine functional group in CO₂ separation. An order of magnitude higher CO₂ adsorption capacity was obtained in the presence of APTS-MCM-48 (RHA) compared to that with MCM-48 (RHA). These results suggest that MCM-48 synthesized from rice husk ash could be usefully applied for CO₂ removal.     

Methodology for CO2 chain analysis

The paper presents a methodology for CO₂ chain analysis with particular focus on the impact of technology development on the total system economy. The methodology includes the whole CO₂ chain; CO₂ source, CO₂ capture, transport and storage in aquifers or in oil reservoirs for enhanced oil recovery. It aims at supporting the identification of feasible solutions and assisting the selection of the most cost-effective options for carbon capture and storage. To demonstrate the applicability of the methodology a case study has been carried out to illustrate the possible impact of technology improvements and market development. The case study confirms that the CO₂-quota price to a large extent influence the project economy and dominates over potential technology improvements. To be economic feasible, the studied chains injecting the CO₂ in oil reservoirs for increased oil production require a CO₂-quota price in the range of 20–27 €/tonne CO₂, depending on the technology breakthrough. For the chains based on CO₂ storage in saline aquifers, the corresponding CO₂-quota price varies up to about 40 €/tonne CO₂.     

Separation and recovery of carbon dioxide by a membrane flash process

A novel process for carbon dioxide (CO₂) separation, which was named a membrane flash process, was developed to realize an energy-saving technology and to substitute it for a conventional regenerator. The electric energy for CO₂ recovery in a membrane flash process using aluminum oxide and diethanolamine was lower than the thermal energy of the conventional chemical absorption process. Flashing at elevated temperature by the low temperature energy significantly reduced the electric energy and required much less membrane area. This process has potentiality of low cost capture of CO₂ when the low temperature energy, which is not available for other purposes, can be utilized to elevate flashing temperature.     

Corrosion and polarization behavior of carbon steel in MEA-based CO2 capture process

This work reveals levels of corrosion rate and polarization behavior of carbon steel immersed in aqueous solutions of monoethanolamine (MEA) used in the absorption-based carbon dioxide (CO₂) capture process for greenhouse gas reduction from industrial flue gas streams. Such information was obtained from electrochemical-based corrosion experiments under a wide range of the CO₂ capture process conditions. The corrosion of carbon steel was evaluated in respect to process parameters including partial pressure of oxygen (O₂), CO₂ loading in solution, solution velocity, solution temperature, MEA concentration and metal surface condition. Results show that the aqueous MEA solution containing CO₂ provides a favorable condition for the corrosion of carbon steel to proceed. Corrosion rate is increased by all tested process parameters. These parametric effects were explained by the electrochemical kinetic data obtained from polarization curves and by the thermodynamic data obtained from Pourbaix diagram.     

Evaluation of large-scale CO2 storage on fresh-water sections of aquifers: An example from the Texas Gulf Coast Basin

Large-scale injections of CO₂ into subsurface saline aquifers have been proposed to remediate climate change related to buildup of green house gases in the atmosphere. The pressure buildup caused by such injections may impact a volume of the basin significantly larger than the CO₂ plume itself. In areas with hydrological settings similar to the Gulf Coast Basin, the perturbation of the flow-field in deep parts of the basin could result in brines or brackish water being pushed up-dip into unconfined sections of the same formations or into the capture zone of fresh-water wells. The premise of the current study is that the details of multiple-phase flow processes necessary to model the near field evolution of the CO₂ plume are not necessary to describe the impact of the pressure anomaly on up-dip aquifers. This paper quantitatively explores conditions under which shallow groundwater would be impacted by up-dip displacement of brines, utilizing an existing carefully calibrated flow model. Modeling an injection of water, arguably equivalent to 50 million tons of CO₂/year for 50 years resulted in an average water-table rise of 1 m, with minor increase in stream baseflow and larger increase in ground water evapotranspiration, but no significant change in salinity.     

Life cycle assessment of a pulverized coal power plant with post-combustion capture, transport and storage of CO2

In this study the methodology of life cycle assessment has been used to assess the environmental impacts of three pulverized coal fired electricity supply chains with and without carbon capture and storage (CCS) on a cradle to grave basis. The chain with CCS comprises post-combustion CO₂ capture with monoethanolamine, compression, transport by pipeline and storage in a geological reservoir. The two reference chains represent sub-critical and state-of-the-art ultra supercritical pulverized coal fired electricity generation. For the three chains we have constructed a detailed greenhouse gas (GHG) balance, and disclosed environmental trade-offs and co-benefits due to CO₂ capture, transport and storage. Results show that, due to CCS, the GHG emissions per kWh are reduced substantially to 243 g/kWh. This is a reduction of 78 and 71% compared to the sub-critical and state-of-the-art power plant, respectively. The removal of CO₂ is partially offset by increased GHG emissions in up- and downstream processes, to a small extent (0.7 g/kWh) caused by the CCS infrastructure. An environmental co-benefit is expected following from the deeper reduction of hydrogen fluoride and hydrogen chloride emissions. Most notable environmental trade-offs are the increase in human toxicity, ozone layer depletion and fresh water ecotoxicity potential for which the CCS chain is outperformed by both other chains. The state-of-the-art power plant without CCS also shows a better score for the eutrophication, acidification and photochemical oxidation potential despite the deeper reduction of SO_x and NO_x in the CCS power plant. These reductions are offset by increased emissions in the life cycle due to the energy penalty and a factor five increase in NH₃ emissions.     

Performance of amine-multilayered solid sorbents for CO2 removal: Effect of fabrication variables

The emission of fossil fuel carbon dioxide (CO₂) to the atmosphere is implicated as the predominant cause of global climate change; therefore, advanced CO₂ capture technologies are of the utmost importance. In this study, innovative amine-multilayered sorbents were fabricated using layer-by-layer (LbL) nanoassembly technology via alternate deposition of a CO₂-adsorbing amine polymer (e.g. polyethylenimine or PEI) and an oppositely-charged polymer (e.g. polystyrene sulfonate or PSS). We found that the developed sorbents could be used for CO₂ capture and that LbL nanoassembly allows us to engineer their CO₂ capture performance through the fabrication variables (e.g. deposition polymers, deposition media, and number of bilayers). PEI/PSS was found to be the best polymer combination for developing sorbents with relatively high CO₂ capture capacity. The amine-multilayered solid sorbents possessed fine microstructures and may have similar polymer deposition within and on the surface of solid sorbents. These amine-multilayered sorbents had much faster CO₂ desorption rates compared to sorbents prepared using the current PEI-impregnation approach. Such fast CO₂ desorption could make sorbents a good option for CO₂ removal from power plants and even the atmosphere.     

Embodied energy and CO2 in UK dimension stone

A process based life cycle assessment of dimension stone production in the UK has been carried out according to PAS 2050. From a survey of eight production operations, on a cradle-to-site basis for UK destinations the carbon footprint of sandstone is 77 kgCO₂e/tonne, that of granite is 107 kgCO₂e/tonne and that of slate is 251 kgCO₂e/tonne. These values are considerably higher for stone imported from abroad due to the impact of transport. Reducing the reliance on imported stone will contribute to emissions reduction targets as well as furthering the goals of sustainable development.     

Numerical parametric study on CO2 capture by indirect thermal swing adsorption

Post-combustion CO₂ capture remains one of the most-challenging issue to lower CO₂ emissions of existing power plants or heavy industry installations because of strong economy and energy efficiency aspects. The major issue comes from CO₂ dilution (4% for NGCC and 14% for PC) and the high flow rates to be treated. Furthermore, CO₂ purity has to be higher than 95% with recovery at 90%, to match the transportation/injection requirements.The MEA absorption process remains the reference today but its energy consumption (about 3 MJ/kg_CO2) and the amine consumption are still challenging drawbacks.The interest of CO₂ capture by indirect TSA (Temperature Swing Adsorption) was demonstrated experimentally in a previous work. The aim of this paper is to present the results of a numerical parametric study. Two main parameters are explored: the desorption temperature (100–200 °C) and the purge flow rate (0.1–0.5 Ndm³ min⁻¹). Four performance indicators are evaluated: CO₂ purity, recovery, productivity and specific energy consumption.Results show that purity above 95% can be achieved. Keeping the 95% target, it is possible to achieve recovery at 81% with productivity at 57.7 g_CO2/kg_ads h and a specific energy consumption of 3.23 MJ/kg_CO2, which is less than for the reference MEA process.Comparison with other adsorption processes exhibits that this process has good potential especially since some improvements are still expected from further research.     

Integration of counter-current relative permeability in the simulation of CO2 injection into saline aquifers

Carbon dioxide (CO₂) injection into saline aquifers is one of the promising options to sequester large amounts of CO₂ in geological formations. During as well as after injection of CO₂ into an aquifer, CO₂ migrates towards the top of the formation due to density differences between the formation brine and the injected CO₂. The time scales of CO₂ migration towards the top of an aquifer and the fraction of CO₂ that is trapped as residual gas depends strongly on the driving forces that are acting on the injected CO₂.When CO₂ migrates to the top of an aquifer, brine may be displaced downwards in a counter-current flow setting particularly during the injection period. A majority of the published work on counter-current flow settings have reported significant reductions in the associated relative permeability functions as compared to co-current measurements. However, this phenomenon has not yet been considered in the simulation of CO₂ storage into saline aquifers.In this paper we study the impact of changes in mobility for the two-phase brine/CO₂ system as a result of transitions between co- and counter-current flow settings. We have included this effect in a simulator and studied the impact of the related mobility reduction on the saturation distribution and residual saturation of CO₂ in aquifers over relevant time scales. We demonstrate that the reduction in relative permeability in the vertical direction changes the plume migration pattern and has an impact on the amount of gas that is trapped as a function of time. This is to our best knowledge the first attempt to integrate counter-current relative permeability into the simulation of injection and subsequent migration of CO₂ in aquifers. The results and analysis presented in this paper are directly relevant to all ongoing activities related to the design of large-scale CO₂ storage in saline aquifers.     

Pipeline design for a least-cost router application for CO2 transport in the CO2 sequestration cycle

CO₂ capture and geological storage (CCS) is considered as a viable option to mitigate greenhouse gas emissions during the transition phase towards the use of clean and renewable energy. This paper concentrates on the transport of CO₂ between source (CO₂ capture at plants) and sink (geological storage reservoirs). In the cost estimation of CO₂ transport, the pipeline diameter plays an important role. In this respect, the paper reviews equations that were used in several reports on CO₂ pipeline transport. As some parameters are not taken into account in these equations, alternative formulas are proposed which calculate the proper inner diameter size based on flow rate, pressure drop per unit length, CO₂ density, CO₂ viscosity, pipeline material roughness and topographic height differences (the Darcy–Weisbach solution) and, in addition, on the amount and type of bends (the Manning solution). Comparison between calculated diameters using the reviewed and the proposed equations demonstrate the important influence of elevation difference (which is not considered in the reviewed equations) and pipeline material roughness-related factor on the calculated diameter. Concerning the latter, it is suggested that a Darcy–Weisbach roughness height of 0.045 mm better corresponds to a Manning factor of 0.009 than higher Manning values previously proposed in literature. Comparison with the actual diameter of the Weyburn pipeline confirms the accuracy of the proposed equations. Comparison with other existing CO₂ pipelines (without pressure information) indicate that the pipelines are designed for lower pressure gradients than 25 Pa/m or for (future) higher flow rates. The proposed Manning equation is implemented in an economic least-cost route planner in order to obtain the best economic solution for pipeline trajectory and corresponding diameter.     

CO2 transportation for carbon capture and storage: Sublimation of carbon dioxide from a dry ice bank

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.