Life cycle modelling of fossil fuel power generation with post-combustion CO2 capture

Due to its compatibility with the current energy infrastructures and the potential to reduce CO₂ emissions significantly, CO₂ capture and geological storage is recognised as one of the main options in the portfolio of greenhouse gas mitigation technologies being developed worldwide. The CO₂ capture technologies offer a number of alternatives, which involve different energy consumption rates and subsequent environmental impacts. While the main objective of this technology is to minimise the atmospheric greenhouse gas emissions, it is also important to ensure that CO₂ capture and storage does not aggravate other environmental concerns. This requires a holistic and system-wide environmental assessment rather than focusing on the greenhouse gases only. Life Cycle Assessment meets this criteria as it not only tracks energy and non-energy-related greenhouse gas releases but also tracks various other environmental releases, such as solid wastes, toxic substances and common air pollutants, as well as the consumption of other resources, such as water, minerals and land use. This paper presents the principles of the CO₂ capture and storage LCA model developed at Imperial College and uses the pulverised coal post-combustion capture example to demonstrate the methodology in detail. At first, the LCA models developed for the coal combustion system and the chemical absorption CO₂ capture system are presented together with examples of relevant model applications. Next, the two models are applied to a plant with post-combustion CO₂ capture, in order to compare the life cycle environmental performance of systems with and without CO₂ capture. The LCA results for the alternative post-combustion CO₂ capture methods (including MEA, K⁺/PZ, and KS-1) have shown that, compared to plants without capture, the alternative CO₂ capture methods can achieve approximately 80% reduction in global warming potential without a significant increase in other life cycle impact categories. The results have also shown that, of all the solvent options modelled, KS-1 performed the best in most impact categories.     

Conceptual design of a three fluidised beds combustion system capturing CO2 with CaO

In this work, the Aspen Hysys conceptual design of a new process for energy generation at large scale with implicit CO₂ capture is presented. This process makes use of the CaO capability for CO₂ capture at high temperature and the possibility of regenerating this sorbent working in interconnected fluidised bed reactors operating at different temperatures. The proposed process has the advantage of producing power with minimum CO₂ emissions and very low energy penalties compared with similar air-based combustion power plants. In this system, five main parts can be distinguished: the combustor where coal is burnt with air, the calciner where the fresh and the recycled CaCO₃ is calcined, the carbonator where the CO₂ produced in the combustor is captured, the supercritical steam cycle and the CO₂ compression system. In this arrangement, the three fluidised bed reactors are interconnected in such a way that it is possible to perform the CaCO₃ calcination at a temperature of 950 °C with the energy transported by a hot solid stream produced in the circulating fluidised bed combustor operating at 1030 °C. The stream rich in CaO produced in the calciner is split into three parts. One of them is transported to the carbonator operating at 650 °C where most of the CO₂ in the flue gas produced in the combustor is captured. The second one is sent to the combustor, where it is heated up and used as energy carrier. The third solid stream that leaves the calciner is a purge in order to maintain the capture system activity and to avoid inert material accumulation. Because of the high temperatures involved in all the system, it is possible to recover most of the energy in the fuel and to produce power in a supercritical steam cycle. A case study is presented and it is demonstrated that under these operating conditions, 90% CO₂ capture efficiency can be achieved with no energy penalty further than the one originated in the CO₂ compression system.     

Multi-stage chemical looping combustion (CLC) for combined cycles with CO2 capture

This paper presents application of the chemical looping combustion (CLC) method in natural gas-fired combined cycles for power generation with CO₂ capture. A CLC combined cycle consisting of single CLC-reactor system, an air turbine, a CO₂-turbine and a steam cycle has been designated as the base-case cycle. The base-case cycle can achieve net plant efficiency of about 52% at an oxidation temperature of 1200 °C. In order to achieve a reasonable efficiency at lower oxidation temperatures, reheat is introduced into the air turbine by employing multi CLC-reactors. The results show that the single reheat CLC-combined cycle can achieve net plant efficiency of above 51% at oxidation temperature of 1000 °C and above 53% at the oxidation temperature of 1200 °C including CO₂ compression to 110 bar. The double reheat cycle results in marginal efficiency improvement as compared to the single reheat cycle. The CLC-cycles are also compared with a conventional combined cycle with and without post-combustion capture in amine solution. All the CLC-cycles show higher net plant efficiencies with close to 100% CO₂ capture as compared to a conventional combined cycle with post-combustion capture, which is very promising.     

A qualitative reliability and operability analysis of an integrated reforming combined cycle plant with CO2 capture

Most of the current CO₂ capture technologies are associated with large energy penalties that reduce their economic viability. Efficiency has therefore become the most important issue when designing and selecting power plants with CO₂ capture. Other aspects, like reliability and operability, have been given less importance, if any at all, in the literature.This article deals with qualitative reliability and operability analyses of an integrated reforming combined cycle concept. The plant reforms natural gas into a syngas, the carbon is separated out as CO₂ after a water-gas shift section, and the hydrogen-rich fuel is used for a gas turbine. The qualitative reliability analysis in the article consists of a functional analysis followed by a failure mode, effects, and criticality analysis (FMECA). The operability analysis introduces the comparative complexity indicator (CCI) concept.Functional analysis and FMECA are important steps in a system reliability analysis, as they can serve as a platform and basis for further analysis. Also, the results from the FMECA can be interesting for determining how the failures propagate through the system and their effects on the operation of the process. The CCI is a helpful tool in choosing the level of integration and to investigate whether or not to include a certain process feature. Incorporating the analytical approach presented in the article during the design stage of a plant can be advantageous for the overall plant performance.     

Experimental validation of in situ CO2 capture with CaO during the low temperature combustion of biomass in a fluidized bed reactor

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 CO₂ “in 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.     

Design and off-design analyses of a pre-combustion CO2 capture process in a natural gas combined cycle power plant

In this study, a cycle designed for capturing the greenhouse gas CO₂ in a natural gas combined cycle power plant has been analyzed. The process is a pre-combustion CO₂ capture cycle utilizing reforming of natural gas and removal of the carbon in the fuel prior to combustion in the gas turbine. The power cycle consists of a H₂-fired gas turbine and a triple pressure steam cycle. Nitrogen is used as fuel diluent and steam is injected into the flame for additional NO_x control. The heat recovery steam generator includes pre-heating for the various process streams. The pre-combustion cycle consists of an air-blown auto-thermal reformer, water–gas shift reactors, an amine absorption system to separate out the CO₂, as well as a CO₂ compression block. Included in the thermodynamic analysis are design calculations, as well as steady-state off-design calculations. Even though the aim is to operate a plant, as the one in this study, at full load there is also a need to be able to operate at part load, meaning off-design analysis is important. A reference case which excludes the pre-combustion cycle and only consists of the power cycle without CO₂ capture was analyzed at both design and off-design conditions for comparison. A high degree of process integration is present in the cycle studied. This can be advantageous from an efficiency stand-point but the complexity of the plant increases. The part load calculations is one way of investigating how flexible the plant is to off-design conditions. In the analysis performed, part load behavior is rather good with efficiency reductions from base load operation comparable to the reference combined cycle plant.     

CO2 capture from combined cycles integrated with Molten Carbonate Fuel Cells

In this paper Molten Carbonate Fuel Cells (MCFCs) are considered for their potential application in carbon dioxide separation when integrated into natural gas fired combined cycles. The MCFC performs on the anode side an electrochemical oxidation of natural gas by means of CO₃^2? ions which, as far as carbon capture is concerned, results in a twofold advantage: the cell removes CO₂ fed at the cathode to promote carbonate ion transport across the electrolyte and any dilution of the oxidized products is avoided.The MCFC can be “retrofitted” into a combined cycle, giving the opportunity to remove most of the CO₂ contained in the gas turbine exhaust gases before they enter the heat recovery steam generator (HRSG), and allowing to exploit the heat recovery steam cycle in an efficient “hybrid” fuel cell + steam turbine configuration. The carbon dioxide can be easily recovered from the cell anode exhaust after combustion with pure oxygen (supplied by an air separation unit) of the residual fuel, cooling of the combustion products in the HRSG and water separation. The resulting power cycle has the potential to keep the overall cycle electrical efficiency approximately unchanged with respect to the original combined cycle, while separating 80% of the CO₂ otherwise vented and limiting the size of the fuel cell, which contributes to about 17% of the total power output so that most of the power capacity relies on conventional low cost turbo-machinery. The calculated specific energy for CO₂ avoided is about 4 times lower than average values for conventional post-combustion capture technology. A sensitivity analysis shows that positive results hold also changing significantly a number of MCFC and plant design parameters.     

Modeling CO2 capture with aqueous monoethanolamine

Hilliard completed several thermodynamic models in Aspen Plus^® for modeling CO₂ removal with amine solvents, including MEA–H₂O–CO₂. This solvent was selected to make a system model for CO₂ removal by absorption/stripping. Both the absorber and the stripper used RateSep? to rigorously calculate mass transfer rates. The accuracy of the new model was assessed using a recent pilot plant run with 35 wt.% (9 m) MEA. Absorber loading and removal were predicted within 6%, and the temperature profile was approached within 5 °C. An average 3.8% difference between measured and calculated values was achieved in the stripper. A three-stage flash configuration which efficiently utilizes solar energy was developed. It reduces energy use by 6% relative to a simple stripper. Intercooling was used to reach 90% removal in the absorber at these optimized conditions.     

Co-production of hydrogen and electricity with CO2 capture

Electricity and hydrogen can be used as energy carriers to reduce emissions of CO₂ from small and mobile energy users. One of the most promising technologies for the production of electricity and hydrogen with low CO₂ emissions is coal gasification with CO₂ capture and storage. Performance and cost data are presented for plants which produce electricity and hydrogen alone and plants which co-produce both of these energy carriers. The co-production plants include plants which produce a fixed ratio of hydrogen to electricity and plants which are able to vary the ratio while continuing to operate the gasification and CO₂ capture parts of the plant at full load. The paper also assesses the ability of these types of plants to satisfy the varying demands for hydrogen and electricity in future energy supply systems. The lowest cost option for the scenarios assessed in the paper is the use of flexible co-production plants with underground buffer storage of hydrogen.     

Integration and evaluation of a power plant with a CaO-based CO2 capture system

This paper explores the integration and evaluation of a power plant with a CaO-based CO₂ capture system. There is a great amount of recoverable heat in the CaO-based CO₂ capture process. Five cases for the possible integration of a 600 MW power plant with CaO-based CO₂ capture process are considered in this paper. When the system is configured so that recovered heat is used to replace part of the boiler heat load (Case 2), modelling not only shows that this is the system recovering the most heat of 1008.8 MW but also results in the system with the lowest net power output of 446 MW and the second lowest of efficiency of 34.1%. It is indicated that system performance depends both on the amount of heat recovery and the type of heat utilization. When the system is configured so that a 400 MW power plant is built using the recovered heat (Case 4), modelling shows that this is the system with the most net power output of 846 MW, the highest efficiency of 36.8%, the lowest cost of electricity of 54.3 €/MWh and the lowest cost of CO₂ avoided of 28.9 €/tCO₂. This new built steam cycle will not affect the operation of the reference plant which vents its CO₂ to the atmosphere, highly reducing the connection between the CO₂ capture process and the reference plant which vents its CO₂ to the atmosphere. The average cost of electricity and the cost of CO₂ avoided of the five cases are about 58.9 €/kWh and 35.9 €/tCO₂, respectively.     

Estimation of annual CH4 and N2O emissions from fluidised bed combustion: An advanced measurement-based method and its application to Finland

The aim of this study was to develop and apply an advanced, measurement based method for the estimation of annual CH₄ and N₂O emissions and thus gain improved understanding on the actual greenhouse gas (GHG) balances of combustion of fossil fuels, peat, biofuels and REF. CH₄ and N₂O emissions depend strongly on combustion conditions, and therefore the emission factors used in the calculation of annual emissions contain significant uncertainties. Fluidised bed combustion (FBC) has many good properties for combustion of different types of fuels and fuels of varying quality, e.g., biofuels and wastes. Therefore, it is currently increasing its market share. In this study, long term measurements (up to 50 days) were carried out at seven FBC boilers representing different size classes, loadings and fuel mixes. Both decreasing load and increasing share of coal in fuel mix increased N₂O emissions. Measurement results from different loading levels were combined with the common loading curves of similar plants in Finland to estimate annual emissions. Based on the results, recommendations for emission factors for the Finnish GHG emission inventory are given. The role of FBC as a potential technology for the utilisation of biofuels and wastes with future GHG reduction requirements is discussed.     

CO2 capture for refineries,a practical approach

This paper evaluates the opportunities and associated costs for post-combustion capture at a world-scale complex refinery. It is concluded that it is technically feasible to apply post-combustion capture at such a refinery. The costs for capture and sequestration from a gasifier are calculated to be lowest at about 30 Euro per ton; this process currently already produces a concentrated CO₂ stream. Next, the CO₂ source most suited for capture appears to be a combined stack, but there are a number of other sources that may be targeted at comparable costs. In total these sources may form about 40% of the overall refinery emissions. Our evaluations show the costs of capture from such sources based on available amine technology will be in the range of 90–120 Euro per ton, which is about 3–4 times higher than the current carbon trading values. The capture of CO₂ from a large amount of smaller CO₂ sources will bring along even much higher costs. A high-level study of the CO₂ emissions profile of a number of Shell refineries shows that, typically, up to 50% of the emitted CO₂ may be captured at similar costs. About 10–20% of concentrated CO₂ associated with hydrogen manufacturing may be captured at lower costs. The remainder of emitted dilute CO₂ will bring along significantly higher costs. Based on this study, it is concluded for the justification of the implementation of post-combustion capture at refineries, either a significant increase in carbon trading values, mandatory regulations, or a major technological break-through is required.     

Parametric investigation of the calcium looping process for CO2 capture in a 10 kWth dual fluidized bed

Calcium looping (CaL) is a promising post-combustion CO₂ capture technology which is carried out in a dual fluidized bed (DFB) system with continuous looping of CaO, the CO₂ carrier, between two beds. The system consists of a carbonator, where flue gas CO₂ is adsorbed by CaO and a regenerator, where captured CO₂ is released. The CO₂-rich regenerator flue gas can be sequestered after gas processing and compression. A parametric study was conducted on the 10 kW_th DFB facility at the University of Stuttgart, which consists of a bubbling fluidized bed carbonator and a riser regenerator. The effect of the following parameters on CO₂ capture efficiency was investigated: carbonator space time, carbonator temperature and calcium looping ratio. The active space time in the carbonator, which is a function of the space time and the calcium looping ratio, was found to strongly correlate with the CO₂ capture efficiency. BET and BJH techniques provided surface area and pore volume distribution data, respectively, for collected sorbent samples. The rate of sorbent attrition was found to be 2 wt.%/h which is below the expected sorbent make-up rate required to maintain sufficient sorbent activity. Steady-state CO₂ capture efficiencies greater than 90% were achieved for different combinations of operational parameters. Moreover, the experimental results obtained were briefly compared with results derived from reactor modeling studies. Finally, the implications of the experimental results with respect to commercialization of the CaL process have been assessed.     

Life cycle assessment of natural gas combined cycle power plant with post-combustion carbon capture,transport and storage

Hybrid life cycle assessment has been used to assess the environmental impacts of natural gas combined cycle (NGCC) electricity generation with carbon dioxide capture and storage (CCS). The CCS chain modeled in this study consists of carbon dioxide (CO₂) capture from flue gas using monoethanolamine (MEA), pipeline transport and storage in a saline aquifer.Results show that the sequestration of 90% CO₂ from the flue gas results in avoiding 70% of CO₂ emissions to the atmosphere per kWh and reduces global warming potential (GWP) by 64%. Calculation of other environmental impacts shows the trade-offs: an increase of 43% in acidification, 35% in eutrophication, and 120–170% in various toxicity impacts. Given the assumptions employed in this analysis, emissions of MEA and formaldehyde during capture process and generation of reclaimer wastes contributes to various toxicity potentials and cause many-fold increase in the on-site direct freshwater ecotoxicity and terrestrial ecotoxicity impacts. NO_x from fuel combustion is still the dominant contributor to most direct impacts, other than toxicity potentials and GWP. It is found that the direct emission of MEA contribute little to human toxicity (HT < 1%), however it makes 16% of terrestrial ecotoxicity impact. Hazardous reclaimer waste causes significant freshwater and marine ecotoxicity impacts. Most increases in impact are due to increased fuel requirements or increased investments and operating inputs.The reductions in GWP range from 58% to 68% for the worst-case to best-case CCS system. Acidification, eutrophication and toxicity potentials show an even large range of variation in the sensitivity analysis. Decreases in energy use and solvent degradation will significantly reduce the impact in all categories.     

Gas conditioning—The interface between CO2 capture and transport

Gas conditioning is commonly referred to as the required processing for a produced natural gas to achieve transport and sales specifications. In this paper, gas conditioning as the processing required in the interface between CO₂ capture and transport is studied for nine different natural gas fired power plant concepts and three different CO₂ transport processes. Conditioning processes for both pipeline and ship transport are described and an enhanced process for volatile removal is developed. The energy requirement for the conditioning processes is normally between 90 and 120 kWh/tonne CO₂; however, this depends on the pressure and composition of the captured CO₂-rich stream. The loss of CO₂ in the water purge is small for most capture processes. The waste streams from the gas conditioning processes can contain large amounts of CO₂ and should therefore be further processed or reintroduced at an appropriate point upstream in the capture or gas conditioning process if possible. The integration benefit may vary depending on the composition of the CO₂-rich stream. It could be particularly interesting for processes with “innovative reactors” (membranes, sorbents, chemical looping) to integrate CO₂ capture and gas conditioning.     

Carbonic anhydrase-facilitated CO2 absorption with polyacrylamide buffering bead capture

A novel CO₂ separation concept is described wherein the enzyme carbonic anhydrase (CA) is used to increase the overall rate of CO₂ absorption after which hydrated CO₂ reacts with regenerable amine-bearing polyacrylamide buffering beads (PABB). Following saturation of the material's immobilized tertiary amines, CA-bearing carrier water is separated and recycled to the absorption stage while CO₂-loaded material is thermally regenerated. Process application of this concept would involve operation of two or more columns in parallel with thermal regeneration with low-pressure steam taking place after the capacity of a column of amine-bearing polymeric material was exceeded. PABB CO₂-bearing capacity was evaluated by thermogravimetric analysis (TGA) for beads of three acrylamido buffering monomer ingredient concentrations: 0 mol/kg bead, 0.857 mol/kg bead, and 2 mol/kg bead. TGA results demonstrate that CO₂-bearing capacity increases with increasing PABB buffering concentration and that up to 78% of the theoretical CO₂-bearing capacity was realized in prepared PABB samples (0.857 mol/kg recipe). The highest observed CO₂-bearing capacity of PABB was 1.37 mol of CO₂ per kg dry bead. TGA was also used to assess the regenerability of CO₂-loaded PABB. Preliminary results suggest that CO₂ is partially driven from PABB samples at temperatures as low as 55 °C, with complete regeneration occurring at 100 °C. Other physical characteristics of PABB are discussed. In addition, the effectiveness of bovine carbonic anhydrase for the catalysis of CO₂ dissolution is evaluated. Potential benefits and drawbacks of the proposed process are discussed.     

CO2 capture by adsorption: Materials and process development

Vacuum swing adsorptive (VSA) capture of CO₂ from flue gas and related process streams is a promising technology for greenhouse gas mitigation. Although early reports suggested that VSA was problematic and expensive, through the application of more logical process configurations that are appropriately coupled to the composition of the feed and product gas streams, we can now refute this early assertion. Improved cycle designs coupled with tighter temperature control are also helping to optimise performance for CO₂ separation. Simultaneously, new adsorbent materials are being developed. These separate CO₂ by selective (acid-base) reaction with surface bound amine groups (chemisorption), rather than on the basis of non-bonding interactions (physisorption). This report describes some of these recent developments from our own laboratories and points to synergies that are anticipated as a result of combining these improvements in adsorbent properties and VSA process cycles.     

Optimization of a membrane process for CO2 capture in the steelmaking industry

Three different types of membranes were experimentally evaluated for CO₂ recovery from blast furnace effluents: semi-commercial adsorption selective carbon membranes, in-house tailored carbon molecular sieving membranes, and fixed site carrier (FSC) membranes with amine groups in the polymer backbone for active transport of CO₂. In the single gas experiments the FSC membranes showed superior selectivity for CO₂ over the other relevant gases (CO, N₂ and H₂) and high CO₂ permeance (productivity). In addition, it is easy to process and handle, relatively inexpensive to produce and the water in the feed gas is an advantage rather than a problem, since the membrane must be humidified during operation. Based on these experiments a simulation study of a full scale process was performed. The technology showed notable low energy cost, even when converted to the thermal equivalent. Total costs for the CO₂ recovery unit (CO₂ prepared for pipeline transport) were estimated to be in the range 15.0–17.5 €/tonnes CO₂.     

Off-design performance analysis of a transcritical CO2 Rankine cycle with LNG as cold source

The transcritical CO₂ Rankine cycle with liquefied natural gas (LNG) as cold source is a promising power system to utilize mid- and low-temperature heat source. Most previous works focused on thermodynamic and thermoeconomic analysis or optimization for the system. In this article, an off-design performance analysis for the system is conducted. An off-design mathematical model for the system is established to examine the variation of system performance with the variations of heat source mass flow rate and temperature. A modified sliding pressure regulation control strategy, which regulates turbine inlet pressure to keep the temperature difference between heat source temperature and turbine inlet temperature constant, is applied to control the system when off-design conditions happen. The results show that when the mass flow rate or the temperature of heat source is less or lower than that of design condition, both the net power output of system and the system exergy efficiency decrease, whereas when they are more or higher than the values of design condition, the net power output of system increases but the system exergy efficiency still decreases. In addition, both CO₂ turbine and NG turbine could almost keep the designed efficiency values under the applied control strategy.