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The objective of this work is to improve the process for CO2 capture by alkanolamine absorption/stripping by developing an alternative solvent, aqueous K2CO3 promoted by piperazine. The pilot plant data have been reconciled using 17% inlet CO2. A rate-based model demonstrates that the stripper is primarily controlled by liquid film mast transfer resistance, with kinetics at vacuum and diffusion of reactants and products at normal pressure. An additional major unknown ion, probably glyoxylate, has been observed in MEA degradation. Precipitation of gypsum may be a feasible approach to removing sulphate from amine solutions and providing for simultaneous removal of CO2 and SO2. Corrosion of carbon steel in uninhibited MEA solution is increased by increased amine concentration, by addition of piperazine, and by greater CO2 loading.
The objective of this work is to improve the process for CO{sub 2} capture by alkanolamine absorption/stripping by developing an alternative solvent, aqueous K{sub 2}CO{sub 3} promoted by piperazine. Ethylenediamine was detected in a degraded solution of MEA/PZ solution, suggesting that piperazine is subject to oxidation. Stripper modeling has demonstrated that vacuum strippers will be more energy efficient if constructed short and fat rather than tall and skinny. The matrix stripper has been identified as a configuration that will significantly reduce energy use. Extensive measurements of CO{sub 2} solubility in 7 m MEA at 40 and 60 C have confirmed the work by Jou and Mather. Corrosion of carbon steel without inhibitors increases from 19 to 181 mpy in lean solutions of 6.2 m MEA/PZ as piperazine increases from 0 to 3.1 m.
Absorption-Based Post-Combustion Capture of Carbon Dioxide provides a comprehensive and authoritative review of the use of absorbents for post-combustion capture of carbon dioxide. As fossil fuel-based power generation technologies are likely to remain key in the future, at least in the short- and medium-term, carbon capture and storage will be a critical greenhouse gas reduction technique. Post-combustion capture involves the removal of carbon dioxide from flue gases after fuel combustion, meaning that carbon dioxide can then be compressed and cooled to form a safely transportable liquid that can be stored underground. Provides researchers in academia and industry with an authoritative overview of the amine-based methods for carbon dioxide capture from flue gases and related processes Editors and contributors are well known experts in the field Presents the first book on this specific topic
According to the Intergovernmental Panel on Climate Change (IPCC), carbon dioxide (CO2) concentration in the atmosphere has increased from its pre-industrial value of 280 parts per million by volume (ppmv) to 384 ppmv. IPCC predicts that CO2 concentration in the atmosphere will rise to 550 ppmv by the year 2100, if anthropogenic emissions continue to increase. The average temperature at the Earth's surface could increase 1.8-4.0K above the 1990 levels by the end of this century. Such warming is anticipated to cause sea level rise, increased intensity and frequency of extreme weather events, ice shelf disruption, and changes in rainfall patterns. As a result, reducing CO2 emissions from anthropogenic sources is a high priority. Combustion of fossil fuels for power generation is the major contributors of CO2 emission into the environment. Currently, CO2 chemical absorption using monoethanolamine (MEA) as a solvent is the best available option for CO2 capture from flue gas streams. The issue with this technology is the high capture cost which ranges from $50/metric ton to $70/metric ton CO2 avoided. Energy consumption by the process contributes to 60% of the cost. Thus, use of solvents with lower heats of absorption is preferable. A novel process called Integrated Vacuum Carbonate Absorption Process (IVCAP), which employs potassium carbonate (PC) as a solvent, has been proposed. Since chemical affinity of CO2 to K2CO3 is weak compared to MEA, the regeneration of CO2-rich solution can be operated under vacuum at a lower temperature. Hence, a low quality steam from the power plant steam cycle can be used as the heat source for the regeneration. IVCAP process is expected to have 25-30% lower energy requirements as compared to an MEA-based process. However, compared with the MEA solution, PC solutions with low heats of absorption generally exhibit much slower CO2 absorption rates. Hence, a biological catalyst, carbonic anhydrase (CA) was investigated to promote the rate of CO2 absorption into select PC solutions. Experiments were performed in a stirred-tank reactor to evaluate the activity of the CA enzyme under IVCAP conditions. Results revealed that addition of up to 300 mg/l CA enzyme to the PC solutions at 25oC increases the absorption rate by a factor of 6-20 when compared with the same solution without the CA. It was also observed that, the CO2 absorption rates into the aqueous PC solutions with different initial conversion levels of PC to potassium bicarbonate are similar, with differences no larger than 20%, when the concentration of CA enzyme is 300 mg/l. It was also observed that, at the 300 mg/l CA concentration, increasing the temperature from 25oC to 50oC reduces the rate of CO2 absorption, by up to 20%. A mathematical model based on Higbie's penetration theory was developed to simulate the absorption of CO2 into the PC solutions. A comparison of modeled to experimental absorption rates of CO2 provided agreement within 30%. The modeling results revealed that at CA concentrations > 3,000 mg/l, the absorption rate of CO2 is independent of CA concentration. Compared to the enzyme concentration (300 mg/l) used in this study, a further increase of enzyme concentration to a level not larger than 3,000 mg/l could further increase the absorption rate of CO2. Based on the experimental and modeling results obtained in this research, it is recommended that the CO2 absorption rate into PC-CA be further enhanced by improving other parameters such as the activity of CA enzyme and design optimization of the absorption column including the type of packing material. Further work is required to investigate the stability of the CA enzyme at longer test duration and use of immobilized CA enzyme. Effectiveness of the regeneration cycle also needs to be investigated. Further work should also include the test of an integrated absorption/ regeneration system for CO2 capture at a real flue gas condition. 0́3
This book reviews and characterises promising single-compound solvents, solvent blends and advanced solvent systems suitable for CO2 capture applications using gas-liquid absorption. Focusing on energy efficient solvents with minimal adverse environmental impact, the contributions included analyse the major technological advantages, as well as research and development challenges of promising solvents and solvent systems in various sustainable CO2 capture applications. It provides a valuable source of information for undergraduate and postgraduate students, as well as for chemical engineers and energy specialists.
In the light of increasing fears about climate change, greenhouse gas mitigation technologies have assumed growing importance. In the United States, energy related CO2 emissions accounted for 98% of the total emissions in 2007 with electricity generation accounting for 40% of the total'. Carbon capture and sequestration (CCS) is one of the options that can enable the utilization of fossil fuels with lower CO2 emissions. Of the different technologies for CO2 capture, capture of CO2 by chemical absorption is the technology that is closest to commercialization. While a number of different solvents for use in chemical absorption of CO2 have been proposed, a systematic comparison of performance of different solvents has not been performed and claims on the performance of different solvents vary widely. This thesis focuses on developing a consistent framework for an objective comparison of the performance of different solvents. This framework has been applied to evaluate the performance of three different solvents - monoethanolamine, potassium carbonate and chilled ammonia. In this thesis, comprehensive flow-sheet models have been built for each of the solvent systems, using ASPEN Plus as the modeling tool. In order to ensure an objective and consistent comparison of the performance of different solvent systems, the representation of physical properties, thermodynamics and kinetics had to be verified and corrected as required in ASPEN Plus. The ASPEN RateSep module was used to facilitate the computation of mass transfer characteristics of the system for sizing calculations. For each solvent system, many parametric simulations were performed to identify the effect on energy consumption in the system. The overall energy consumption in the CO2 capture and compression system was calculated and an evaluation of the required equipment size for critical equipment in the system was performed. The degradation characteristics and environmental impact of the solvents were also investigated. In addition, different flow-sheet configurations were explored to optimize the energy recuperation for each system. Monoethanolamine (MEA) was evaluated as the base case system in this thesis. Simulations showed the energy penalty for CO2 capture from flue gas from coal-fired power plants to be 0.01572 kWh/gmol CO2 . The energy penalty from CO2 regeneration accounted for 60% of the energy penalty while the compression work accounted for 30%. The process flexibility in the MEA system was limited by degradation reactions. It was found that different flow-sheet configurations for energy recuperation in the MEA system did not improve energy efficiency significantly. Chilled ammonia was explored as an alternative to MEA for use in new coal-fired power plants as well as for retrofitting existing power plants. The overall energy penalty for CO2 capture in chilled ammonia was found to be higher than in the MEA system, though energy requirements for CO2 regeneration were found to be lower. The energy penalty for 85% capture of CO2 in the chilled ammonia system was estimated to be 0.021 kWh/gmol CO2. As compared to the MEA system, the breakdown of the energy requirements was different with refrigeration in the absorber accounting for 44% of the energy penalty. This illustrates the need to perform a systemwide comparison of different solvents in order to evaluate the performance of various solvent systems. The use of potassium carbonate as a solvent for CO2 capture was evaluated for use in Integrated Reforming Combined Cycle (IRCC) system. With potassium carbonate, a high partial pressure of CO2 in the flue gas is required. Different schemes for energy recuperation in the system were investigated and the energy consumption was reduced by 22% over the base case. An optimized version of the potassium carbonate flowsheet was developed for an IRCC application with a reboiler duty of 1980 kJ/kg. In conclusion, a framework for the comparison of the performance of different solvents for CO2 capture has been developed and the performance of monoethanolamine, chilled ammonia and potassium carbonate has been compared. From the standpoint of energy consumption, for existing power plants the use of MEA is found to be the best choice while for future design of power plants, potassium carbonate appears to be an attractive alternative. An economic analysis based on the technical findings in this thesis will help in identifying the optimal choices for various large, stationary sources of CO2.
Chemical Kinetics and Mechanism considers the role of rate of reaction. It begins by introducing chemical kinetics and the analysis of reaction mechanism, from basic well-established concepts to leading edge research. Organic reaction mechanisms are then discussed, encompassing curly arrows, nucleophilic substitution and E1 and E2 elimination reactions. The book concludes with a Case Study on Zeolites, which examines their structure and internal dimensions in relation to their behaviour as molecular sieves and catalysts. The accompanying CD-ROM contains the "Kinetics Toolkit", a graph-plotting application designed for manipulation and analysis of kinetic data, which is built into many of the examples, questions and exercises in the text. There are also interactive activities illustrating reaction mechanisms. The Molecular World series provides an integrated introduction to all branches of chemistry for both students wishing to specialise and those wishing to gain a broad understanding of chemistry and its relevance to the everyday world and to other areas of science. The books, with their Case Studies and accompanying multi-media interactive CD-ROMs, will also provide valuable resource material for teachers and lecturers. (The CD-ROMs are designed for use on a PC running Windows 95, 98, ME or 2000.)