The emission of large amounts of carbon dioxide is of major concern with regard to increasing the risk of climate change. Carbon capture, utilisation and storage (CCUS) has been proposed as an important pathway for sl...The emission of large amounts of carbon dioxide is of major concern with regard to increasing the risk of climate change. Carbon capture, utilisation and storage (CCUS) has been proposed as an important pathway for slowing the rate of these emissions. Solvent absorption of CO_2 using amino acid solvents has drawn much attention over the last few years due to advantages including their ionic nature, low evaporation rate, low toxicity, high absorption rate and high biodegradation potential, compared to traditional amine solvents. In this review, recent progress on the absorption kinetics of amino acids is summarised, and the engineering potential of using amino acids as carbon capture solvents is discussed. The reaction orders between amino acids and carbon dioxide are typ- ically between 1 and 2. Glycine exhibits a reaction order of 1, whilst, by comparison, lysine, proline and sarcosine have the largest reaction constants with carbon dioxide which is much larger than that of the benchmark solvent monoethanolamine (MEA). Ionic strength, p H and cations such as sodium and potassium have been shown to be important factors influencing the reactivity of amino acids. Corrosivity and reactivity with impurities such as SOx and NOxare not considered to be significant problems for amino acids solvents. The precipitation of CO_2 loaded amino acid salts is thought to be a good pathway for increasing CO_2loading capacity and cutting desorption energy costs if well-controlled. It is recommended that more detailed research on amino acid degradation and overall process energy costs is conducted. Overall, amino acid solvents are recognised as promising potential solvents for car- bon dioxide capture.展开更多
The process models for an equilibrium CO_2 absorber and a rate based CO_2 absorber using potassium carbonate(K2 CO3) solvents were developed in Aspen Custom Modeller(ACM) to remove CO_2 from a flue gas. The process mo...The process models for an equilibrium CO_2 absorber and a rate based CO_2 absorber using potassium carbonate(K2 CO3) solvents were developed in Aspen Custom Modeller(ACM) to remove CO_2 from a flue gas. The process model utilised the Electrolyte Non-Random Two Liquid(ENRTL) thermodynamic model and various packing correlations. The results from the ACM equilibrium model shows good agreement with an inbuilt Aspen Plus?model when using the same input conditions. By further introducing a Murphree efficiency which is related to mass transfer and packing hydraulics, the equilibrium model can validate the experimental results from a pilot plant within a deviation of 10%. A more rigorous rate based model included mass and energy flux across the interface and the enhancement effect resulting from chemical reactions. The rate based model was validated using experimental data from pilot plants and was shown to predict the results to within 10%. A parametric sensitivity analysis showed that inlet flue gas flowrate and K2 CO3 concentration in the lean solvent has significant impact on CO_2 recovery. Although both models can provide reasonable predictions based on pilot plant results, the rate based model is more advanced as it can explain mass and heat transfer, transport phenomena and chemical reactions occurring inside the absorber without introducing an empirical Murphree efficiency.展开更多
Aqueous solutions of tertiary amines are promising absorbents for CO2 capture,as they are typically characterized by a high absorption capacity,low heat of reaction,and low corrosivity.However,tertiary amines also exh...Aqueous solutions of tertiary amines are promising absorbents for CO2 capture,as they are typically characterized by a high absorption capacity,low heat of reaction,and low corrosivity.However,tertiary amines also exhibit very low kinetics of CO2 absorption,which has made them unattractive options for large-scale utilization.Here,a series of novel nanoporous carbonaceous promoters(NCPs)with different properties were synthesized,characterized,and used as rate promoters for CO2 absorption in aqueous N,N-diethylethanolamine(DEEA)solutions.To prepare a DEEA–NCP nanofluid,NCPs were dispersed into aqueous 3 mol∙L1 DEEA solution using ultrasonication.The results revealed that among microporous(GC)and mesoporous(GS)carbonaceous structures functionalized with ethylenediamine(EDA)and polyethyleneimine(PEI)molecules,the GC–EDA promoter exhibited the best performance.A comparison between DEEA–GC–EDA nanofluid and typical aqueous DEEA solutions highlighted that the GC-EDA promoter enhances the rate of CO2 absorption at 40C by 38.6%(36.8–50.7 kPamin1)and improves the equilibrium CO2 absorption capacity(15 kPa;40C)by 13.2%(0.69–0.78 mol of CO2 per mole of DEEA).Moreover,the recyclability of DEEA–GC–EDA nanofluid was determined and a promotion mechanism is suggested.The outcomes demonstrate that NCP–GC–EDA in tertiary amines is a promising strategy to enhance the rate of CO2 absorption and facilitate their large-scale deployment.展开更多
文摘The emission of large amounts of carbon dioxide is of major concern with regard to increasing the risk of climate change. Carbon capture, utilisation and storage (CCUS) has been proposed as an important pathway for slowing the rate of these emissions. Solvent absorption of CO_2 using amino acid solvents has drawn much attention over the last few years due to advantages including their ionic nature, low evaporation rate, low toxicity, high absorption rate and high biodegradation potential, compared to traditional amine solvents. In this review, recent progress on the absorption kinetics of amino acids is summarised, and the engineering potential of using amino acids as carbon capture solvents is discussed. The reaction orders between amino acids and carbon dioxide are typ- ically between 1 and 2. Glycine exhibits a reaction order of 1, whilst, by comparison, lysine, proline and sarcosine have the largest reaction constants with carbon dioxide which is much larger than that of the benchmark solvent monoethanolamine (MEA). Ionic strength, p H and cations such as sodium and potassium have been shown to be important factors influencing the reactivity of amino acids. Corrosivity and reactivity with impurities such as SOx and NOxare not considered to be significant problems for amino acids solvents. The precipitation of CO_2 loaded amino acid salts is thought to be a good pathway for increasing CO_2loading capacity and cutting desorption energy costs if well-controlled. It is recommended that more detailed research on amino acid degradation and overall process energy costs is conducted. Overall, amino acid solvents are recognised as promising potential solvents for car- bon dioxide capture.
基金financial support from Peter Cook Centre for CCS Research
文摘The process models for an equilibrium CO_2 absorber and a rate based CO_2 absorber using potassium carbonate(K2 CO3) solvents were developed in Aspen Custom Modeller(ACM) to remove CO_2 from a flue gas. The process model utilised the Electrolyte Non-Random Two Liquid(ENRTL) thermodynamic model and various packing correlations. The results from the ACM equilibrium model shows good agreement with an inbuilt Aspen Plus?model when using the same input conditions. By further introducing a Murphree efficiency which is related to mass transfer and packing hydraulics, the equilibrium model can validate the experimental results from a pilot plant within a deviation of 10%. A more rigorous rate based model included mass and energy flux across the interface and the enhancement effect resulting from chemical reactions. The rate based model was validated using experimental data from pilot plants and was shown to predict the results to within 10%. A parametric sensitivity analysis showed that inlet flue gas flowrate and K2 CO3 concentration in the lean solvent has significant impact on CO_2 recovery. Although both models can provide reasonable predictions based on pilot plant results, the rate based model is more advanced as it can explain mass and heat transfer, transport phenomena and chemical reactions occurring inside the absorber without introducing an empirical Murphree efficiency.
基金University of Melbourne for the Melbourne Research Scholarship,infrastructural support,and financial resources provided for this project.
文摘Aqueous solutions of tertiary amines are promising absorbents for CO2 capture,as they are typically characterized by a high absorption capacity,low heat of reaction,and low corrosivity.However,tertiary amines also exhibit very low kinetics of CO2 absorption,which has made them unattractive options for large-scale utilization.Here,a series of novel nanoporous carbonaceous promoters(NCPs)with different properties were synthesized,characterized,and used as rate promoters for CO2 absorption in aqueous N,N-diethylethanolamine(DEEA)solutions.To prepare a DEEA–NCP nanofluid,NCPs were dispersed into aqueous 3 mol∙L1 DEEA solution using ultrasonication.The results revealed that among microporous(GC)and mesoporous(GS)carbonaceous structures functionalized with ethylenediamine(EDA)and polyethyleneimine(PEI)molecules,the GC–EDA promoter exhibited the best performance.A comparison between DEEA–GC–EDA nanofluid and typical aqueous DEEA solutions highlighted that the GC-EDA promoter enhances the rate of CO2 absorption at 40C by 38.6%(36.8–50.7 kPamin1)and improves the equilibrium CO2 absorption capacity(15 kPa;40C)by 13.2%(0.69–0.78 mol of CO2 per mole of DEEA).Moreover,the recyclability of DEEA–GC–EDA nanofluid was determined and a promotion mechanism is suggested.The outcomes demonstrate that NCP–GC–EDA in tertiary amines is a promising strategy to enhance the rate of CO2 absorption and facilitate their large-scale deployment.