In this study,an integrated technology is proposed for the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3)in a high-gravity environment.The effects of absorbent type,high-g...In this study,an integrated technology is proposed for the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3)in a high-gravity environment.The effects of absorbent type,high-gravity factor,gas/liquid ratio,and initial BaCl2concentration on the absorption rate and amount of CO_(2)and the preparation of BaCO_(3)are investigated.The results reveal that the absorption rate and amount of CO_(2)follow the order of ethyl alkanolamine(MEA)>diethanol amine(DEA)>N-methyldiethanolamine(MDEA),and thus MEA is the most effective absorbent for CO_(2)absorption.The absorption rate and amount of CO_(2)under high gravity are higher than that under normal gravity.Notably,the absorption rate at 75 min under high gravity is approximately 2 times that under normal gravity.This is because the centrifugal force resulting from the high-speed rotation of the packing can greatly increase gas-liquid mass transfer and micromixing.The particle size of BaCO_(3)prepared in the rotating packed bed is in the range of 57.2—89 nm,which is much smaller than that prepared in the bubbling reactor(>100.3 nm),and it also has higher purity(99.6%)and larger specific surface area(14.119 m^(2)·g^(-1)).It is concluded that the high-gravity technology has the potential to increase the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3).This study provides new insights into carbon emissions reduction and carbon utilization.展开更多
To date,the primary industrial carbon capture approach is still absorption using aqueous solutions of alkanolamines.Here,to pursue a substitute for the amine-based approach to improve the CO_(2) capture efficiency and...To date,the primary industrial carbon capture approach is still absorption using aqueous solutions of alkanolamines.Here,to pursue a substitute for the amine-based approach to improve the CO_(2) capture efficiency and decrease the energy cost further,we report a new carbon capture approach using a 2-methylimidazole(mIm)aqueous solution.The properties and sorption behaviors of this approach have been experimentally investigated.The results show that the mIm solution has higher CO_(2) absorption capacity under relatively higher equilibrium pressure(>130 kPa)and lower desorption heat than the methyldiethanolamine solution.91.6%sorption capacity of mIm solution can be recovered at 353.15 K and 80 kPa.The selectivity for CO_(2)/N_(2) and CO_(2)/CH_(4) can reach an exceptional 7609 and 4324,respectively.Furthermore,the pilot-scale tests were also performed,and the results demonstrate that more than 98%of CO_(2) in the feed gas could be removed and cyclic absorption capacity can reach 1 mol·L^(-1).This work indicates that mIm is an excellent alternative to alkanolamines for carbon capture in the industry.展开更多
This work systematically reviews the complex mechanisms of CO_(2)-water-rock interactions,microscopic simulations of reactive transport(dissolution,precipitation and precipitate migration)in porous media,and microscop...This work systematically reviews the complex mechanisms of CO_(2)-water-rock interactions,microscopic simulations of reactive transport(dissolution,precipitation and precipitate migration)in porous media,and microscopic simulations of CO_(2)-water-rock system.The work points out the key issues in current research and provides suggestions for future research.After injection of CO_(2) into underground reservoirs,not only conventional pressure-driven flow and mass transfer processes occur,but also special physicochemical phenomena like dissolution,precipitation,and precipitate migration.The coupling of these processes causes complex changes in permeability and porosity parameters of the porous media.Pore-scale microscopic flow simulations can provide detailed information within the three-dimensional pore and throat space and explicitly observe changes in the fluid-solid interfaces of porous media during reactions.At present,the research has limitations in the decoupling of complex mechanisms,characterization of differential multi-mineral reactions,precipitation generation mechanisms and characterization(crystal nucleation and mineral detachment),simulation methods for precipitation-fluid interaction,and coupling mechanisms of multiple physicochemical processes.In future studies,it is essential to innovate experimental methods to decouple“dissolution-precipitation-precipitate migration”processes,improve the accuracy of experimental testing of minerals geochemical reaction-related parameters,build reliable characterization of various precipitation types,establish precipitation-fluid interaction simulation methods,coordinate the boundary conditions of different physicochemical processes,and,finally,achieve coupled flow simulation of“dissolution-precipitation-precipitate migration”within CO_(2)-water-rock systems.展开更多
The addition of dispersed-phase nanoparticles in the liquid phase can enhance the gas-liquid transfer process as the suspended nanoparticles affect the transfer process inside the fluid through microdisturbance or mic...The addition of dispersed-phase nanoparticles in the liquid phase can enhance the gas-liquid transfer process as the suspended nanoparticles affect the transfer process inside the fluid through microdisturbance or micro-convection effects.In this article,a high-speed digital camera was used to visualize the bubble behavior of CO_(2) in pure water and nanofluids to examine the effects of CO_(2) gas flow rate,nanoparticle solid content and type on the bubble behavior in the fluids.The CO_(2) absorption performance in three water-based nanofluids were compared in a bubbler.And the mass transfer characteristics during CO_(2) bubble absorption and the reasons for the enhanced gas-liquid mass transfer effect of nanoparticles were analyzed.The results showed that the presence of nanoparticles affected the formation process of bubbles in the fluid,shortened the bubble detachment time,reduced the detachment diameter,effectively increased the gas-liquid contact area,and improved the bubbles detachment frequency.The system with MCM-41 corresponded to a higher overall mass transfer coefficient.Uncalined MCM-41 contained surfactant that enhanced foaming behavior in water.This prevented the transfer of CO_(2) to some extent,and the CO_(2) absorption by uncalined MCM-41/H_(2)O was 5.34%higher than that by pure water.Compared with SiO_(2) nanoparticles with the same particle size and the same composition,MCM-41 had a higher adsorption capacity and better hydrophilicity due to its larger specific surface area and rich porous structure,which was more favorable to accelerate the collision between nanoparticles and CO_(2) bubbles to cause micro-convection.Under the condition of 0.1%(mass)solid content,the enhancement of CO_(2) absorption process by MCM-41 nanoparticles was more significant and improved by 16.9%compared with pure water.展开更多
The conversion of CO2 into H+ and is a relatively slow reaction. Hence, its kinetics may be rate determining in carbonate rock dissolution. Carbonic anhydrase (CA), which is widespread in nature, was used to catalyze ...The conversion of CO2 into H+ and is a relatively slow reaction. Hence, its kinetics may be rate determining in carbonate rock dissolution. Carbonic anhydrase (CA), which is widespread in nature, was used to catalyze the CO2 conversion process in dissolution experiments of limestone and dolomite. It was found that the rate of dissolution increases by a factor of about 10 after the addition of CA at a high CO2 partial pressure (Pco2) for limestone and about 3 at low Pco2 for dolomite. This shows that reappraisal is necessary for the importance of chemical weathering (including carbonate rock dissolution and silicate weathering) in the atmospheric CO2 sink and the mysterious missing sink in carbon cycling. It is doubtless that previous studies of weathering underestimated weathering rates due to the ignorance of CA as an activator in weathering, thus the contribution of weathering to the atmospheric CO2 sink is also underestimated. This finding also shows the need to examine the situ distribution and activity of CA in different waters and to investigate the role of CA in weathering.展开更多
CO_(2)capture with a low energy consumption is of important application significance for reducing CO_(2)emission.The phase-change absorbent developed in recent years shows its potential for low-energy CO_(2)capture.Th...CO_(2)capture with a low energy consumption is of important application significance for reducing CO_(2)emission.The phase-change absorbent developed in recent years shows its potential for low-energy CO_(2)capture.The unclear phase-splitting rule hinders the efficient development of CO_(2)phase-change absorbents.To predict phase-splitting behaviors of mono/poly-amine-organic solvent-water system with various concentrations,a quasi-activity coefficient was developed based on Debye&Mc Aulay equation and some Density function theory descriptors.Six models based on Debye&Mc Aulay equation were developed with different ion radius,descriptors or poly-amine-CO_(2)products.The phase-splitting boundary was drawn on the model with the best predictability.This quasi-activity coefficient would provide guidance for the phase-splitting systems development,especially for polyamines.展开更多
Intermetallic complexes of rare-earth and 3d transition metals with core-shell structures are commonly employed as microwave absorbing materials due to their high saturation magnetizations and natural resonance in GHz...Intermetallic complexes of rare-earth and 3d transition metals with core-shell structures are commonly employed as microwave absorbing materials due to their high saturation magnetizations and natural resonance in GHz. Hence, we synthesized Y_2Co_(17)alloy via the co-precipitation reduction-diffusion technique, then coated the Y_2Co_(17)magnetic powders with SiO_(2)to create Y_2Co_(17)@SiO_(2) core-shell structures. The formation of Y_2Co_(17)@SiO_(2)/polyurethane(PU) at various volume fractions and their magnetic, electromagnetic properties were investigated using x-ray diffraction, scanning electron microscopy, energy dispersive spectroscopy, and vector network analyzer. The microwave absorption characteristics of Y_2Co_(17)@SiO_(2)/PU were also investigated at various volume fractions. We not only investigate the zero-reflection conditions of the samples with different volume fractions, but also show that every absorber has a strong reflection loss value(RL ≤-65.00 d B) and excellent microwave absorption properties with an average RL of Y_2Co_(17)@SiO_(2)/PU being below-10 d B at 8 GHz–18 GHz under different thicknesses, showing that the enhancement of microwave absorption performance arises from the balance between permeability and permittivity of absorber.展开更多
A comprehensive computational fluid dynamics（CFD） model is developed based on the gas-liquid two-phase hydrodynamics,gas-liquid mass-transfer theory and chemical reaction kinetics,and the ammonia-based CO2 absorptio...A comprehensive computational fluid dynamics（CFD） model is developed based on the gas-liquid two-phase hydrodynamics,gas-liquid mass-transfer theory and chemical reaction kinetics,and the ammonia-based CO2 absorption in a spray column is numerically studied.The Euler-Lagrange model is applied to describe the behavior of gas-liquid twophase flowand heat transfer.The dual-film theory and related correlations are adopted to model the gas-liquid mass transfer and chemical absorption process.The volatilization model of multi-component droplet is utilized to account for ammonia slippage.The effect of operation parameters on CO2 removal efficiency is numerically studied.The results showa good agreement with the previous experimental data,proving the validity of the proposed model.The profile studies of gasphase velocity and CO2 concentration suggest that the flowfield has a significant impact on the CO2 concentration field.Also,the local CO2 absorption rate is influenced by both local turbulence and the local liquid-gas ratio.Furthermore,the velocity field of gas phase is optimized by the method of adjusting the orifice plate,and the results showthat the CO2 removal efficiency is improved by approximately 4%.展开更多
基金supported by Research Project Supported by Horizon Europe Framework Programme(101183092)Shanxi Scholarship Council of China(2023-128)+2 种基金National Natural Science Foundation of China(22208328)Fundamental Research Program of Shanxi Province(20210302124618)Small and mediumsized oriented scientific and technological enterprises innovation ability improvement project of Shandong Province(2023TSGC0004)。
文摘In this study,an integrated technology is proposed for the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3)in a high-gravity environment.The effects of absorbent type,high-gravity factor,gas/liquid ratio,and initial BaCl2concentration on the absorption rate and amount of CO_(2)and the preparation of BaCO_(3)are investigated.The results reveal that the absorption rate and amount of CO_(2)follow the order of ethyl alkanolamine(MEA)>diethanol amine(DEA)>N-methyldiethanolamine(MDEA),and thus MEA is the most effective absorbent for CO_(2)absorption.The absorption rate and amount of CO_(2)under high gravity are higher than that under normal gravity.Notably,the absorption rate at 75 min under high gravity is approximately 2 times that under normal gravity.This is because the centrifugal force resulting from the high-speed rotation of the packing can greatly increase gas-liquid mass transfer and micromixing.The particle size of BaCO_(3)prepared in the rotating packed bed is in the range of 57.2—89 nm,which is much smaller than that prepared in the bubbling reactor(>100.3 nm),and it also has higher purity(99.6%)and larger specific surface area(14.119 m^(2)·g^(-1)).It is concluded that the high-gravity technology has the potential to increase the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3).This study provides new insights into carbon emissions reduction and carbon utilization.
基金The financial supports received from National Natural Science Foundation of China (U20B6005, 22178378, and 22127812)
文摘To date,the primary industrial carbon capture approach is still absorption using aqueous solutions of alkanolamines.Here,to pursue a substitute for the amine-based approach to improve the CO_(2) capture efficiency and decrease the energy cost further,we report a new carbon capture approach using a 2-methylimidazole(mIm)aqueous solution.The properties and sorption behaviors of this approach have been experimentally investigated.The results show that the mIm solution has higher CO_(2) absorption capacity under relatively higher equilibrium pressure(>130 kPa)and lower desorption heat than the methyldiethanolamine solution.91.6%sorption capacity of mIm solution can be recovered at 353.15 K and 80 kPa.The selectivity for CO_(2)/N_(2) and CO_(2)/CH_(4) can reach an exceptional 7609 and 4324,respectively.Furthermore,the pilot-scale tests were also performed,and the results demonstrate that more than 98%of CO_(2) in the feed gas could be removed and cyclic absorption capacity can reach 1 mol·L^(-1).This work indicates that mIm is an excellent alternative to alkanolamines for carbon capture in the industry.
基金Supported by the National Natural Science Foundation of China(52234003,52222402,52304044).
文摘This work systematically reviews the complex mechanisms of CO_(2)-water-rock interactions,microscopic simulations of reactive transport(dissolution,precipitation and precipitate migration)in porous media,and microscopic simulations of CO_(2)-water-rock system.The work points out the key issues in current research and provides suggestions for future research.After injection of CO_(2) into underground reservoirs,not only conventional pressure-driven flow and mass transfer processes occur,but also special physicochemical phenomena like dissolution,precipitation,and precipitate migration.The coupling of these processes causes complex changes in permeability and porosity parameters of the porous media.Pore-scale microscopic flow simulations can provide detailed information within the three-dimensional pore and throat space and explicitly observe changes in the fluid-solid interfaces of porous media during reactions.At present,the research has limitations in the decoupling of complex mechanisms,characterization of differential multi-mineral reactions,precipitation generation mechanisms and characterization(crystal nucleation and mineral detachment),simulation methods for precipitation-fluid interaction,and coupling mechanisms of multiple physicochemical processes.In future studies,it is essential to innovate experimental methods to decouple“dissolution-precipitation-precipitate migration”processes,improve the accuracy of experimental testing of minerals geochemical reaction-related parameters,build reliable characterization of various precipitation types,establish precipitation-fluid interaction simulation methods,coordinate the boundary conditions of different physicochemical processes,and,finally,achieve coupled flow simulation of“dissolution-precipitation-precipitate migration”within CO_(2)-water-rock systems.
基金financial support from National Natural Science Foundation of China(22108263)Shanxi Province Basic Research Program Project(20210302124060)the 18th Graduate Student Technology Project of North University of China(20221824).
文摘The addition of dispersed-phase nanoparticles in the liquid phase can enhance the gas-liquid transfer process as the suspended nanoparticles affect the transfer process inside the fluid through microdisturbance or micro-convection effects.In this article,a high-speed digital camera was used to visualize the bubble behavior of CO_(2) in pure water and nanofluids to examine the effects of CO_(2) gas flow rate,nanoparticle solid content and type on the bubble behavior in the fluids.The CO_(2) absorption performance in three water-based nanofluids were compared in a bubbler.And the mass transfer characteristics during CO_(2) bubble absorption and the reasons for the enhanced gas-liquid mass transfer effect of nanoparticles were analyzed.The results showed that the presence of nanoparticles affected the formation process of bubbles in the fluid,shortened the bubble detachment time,reduced the detachment diameter,effectively increased the gas-liquid contact area,and improved the bubbles detachment frequency.The system with MCM-41 corresponded to a higher overall mass transfer coefficient.Uncalined MCM-41 contained surfactant that enhanced foaming behavior in water.This prevented the transfer of CO_(2) to some extent,and the CO_(2) absorption by uncalined MCM-41/H_(2)O was 5.34%higher than that by pure water.Compared with SiO_(2) nanoparticles with the same particle size and the same composition,MCM-41 had a higher adsorption capacity and better hydrophilicity due to its larger specific surface area and rich porous structure,which was more favorable to accelerate the collision between nanoparticles and CO_(2) bubbles to cause micro-convection.Under the condition of 0.1%(mass)solid content,the enhancement of CO_(2) absorption process by MCM-41 nanoparticles was more significant and improved by 16.9%compared with pure water.
基金Financial supports for this research was provided by the National Nature Science Foundation of China(Grant 40073026)Ministry of Science and Technology of China(Grant 164)+1 种基金Natural Science Foundation of Guangxi(Grant 9824021)Ministry of Land and Resources of China(Grant 9806)and Bremen University of Germany.
文摘The conversion of CO2 into H+ and is a relatively slow reaction. Hence, its kinetics may be rate determining in carbonate rock dissolution. Carbonic anhydrase (CA), which is widespread in nature, was used to catalyze the CO2 conversion process in dissolution experiments of limestone and dolomite. It was found that the rate of dissolution increases by a factor of about 10 after the addition of CA at a high CO2 partial pressure (Pco2) for limestone and about 3 at low Pco2 for dolomite. This shows that reappraisal is necessary for the importance of chemical weathering (including carbonate rock dissolution and silicate weathering) in the atmospheric CO2 sink and the mysterious missing sink in carbon cycling. It is doubtless that previous studies of weathering underestimated weathering rates due to the ignorance of CA as an activator in weathering, thus the contribution of weathering to the atmospheric CO2 sink is also underestimated. This finding also shows the need to examine the situ distribution and activity of CA in different waters and to investigate the role of CA in weathering.
基金financial support from National Natural Science Foundation of China(21878190)China Petrochemical Corporation(419033-1)the Engineering Experimental Teaching Center,School of Chemical Engineering,Sichuan University for the Nuclear Magnetic Resonance(NMR,JNM-ECZ400S/L1,JEOL Ltd.)support and the compute server support。
文摘CO_(2)capture with a low energy consumption is of important application significance for reducing CO_(2)emission.The phase-change absorbent developed in recent years shows its potential for low-energy CO_(2)capture.The unclear phase-splitting rule hinders the efficient development of CO_(2)phase-change absorbents.To predict phase-splitting behaviors of mono/poly-amine-organic solvent-water system with various concentrations,a quasi-activity coefficient was developed based on Debye&Mc Aulay equation and some Density function theory descriptors.Six models based on Debye&Mc Aulay equation were developed with different ion radius,descriptors or poly-amine-CO_(2)products.The phase-splitting boundary was drawn on the model with the best predictability.This quasi-activity coefficient would provide guidance for the phase-splitting systems development,especially for polyamines.
基金the National Key Research and Development Program of China (Grant No. 2021YFB3501302)the National Natural Science Foundation of China (Grant No. 51731001)the Fund from the State Key Laboratory of Baiyunobo Rare Earth Resource Researches and Comprehensive Utilization’s Key Research and Development Projects。
文摘Intermetallic complexes of rare-earth and 3d transition metals with core-shell structures are commonly employed as microwave absorbing materials due to their high saturation magnetizations and natural resonance in GHz. Hence, we synthesized Y_2Co_(17)alloy via the co-precipitation reduction-diffusion technique, then coated the Y_2Co_(17)magnetic powders with SiO_(2)to create Y_2Co_(17)@SiO_(2) core-shell structures. The formation of Y_2Co_(17)@SiO_(2)/polyurethane(PU) at various volume fractions and their magnetic, electromagnetic properties were investigated using x-ray diffraction, scanning electron microscopy, energy dispersive spectroscopy, and vector network analyzer. The microwave absorption characteristics of Y_2Co_(17)@SiO_(2)/PU were also investigated at various volume fractions. We not only investigate the zero-reflection conditions of the samples with different volume fractions, but also show that every absorber has a strong reflection loss value(RL ≤-65.00 d B) and excellent microwave absorption properties with an average RL of Y_2Co_(17)@SiO_(2)/PU being below-10 d B at 8 GHz–18 GHz under different thicknesses, showing that the enhancement of microwave absorption performance arises from the balance between permeability and permittivity of absorber.
基金The National Natural Science Foundation of China(No.51276038)
文摘A comprehensive computational fluid dynamics（CFD） model is developed based on the gas-liquid two-phase hydrodynamics,gas-liquid mass-transfer theory and chemical reaction kinetics,and the ammonia-based CO2 absorption in a spray column is numerically studied.The Euler-Lagrange model is applied to describe the behavior of gas-liquid twophase flowand heat transfer.The dual-film theory and related correlations are adopted to model the gas-liquid mass transfer and chemical absorption process.The volatilization model of multi-component droplet is utilized to account for ammonia slippage.The effect of operation parameters on CO2 removal efficiency is numerically studied.The results showa good agreement with the previous experimental data,proving the validity of the proposed model.The profile studies of gasphase velocity and CO2 concentration suggest that the flowfield has a significant impact on the CO2 concentration field.Also,the local CO2 absorption rate is influenced by both local turbulence and the local liquid-gas ratio.Furthermore,the velocity field of gas phase is optimized by the method of adjusting the orifice plate,and the results showthat the CO2 removal efficiency is improved by approximately 4%.
