COcapture with ionic liquids(ILs) has attracted many attentions, and most works focused on absorption ability at ambient temperatures, while seldom research was concerned at elevated temperatures.This not only limit...COcapture with ionic liquids(ILs) has attracted many attentions, and most works focused on absorption ability at ambient temperatures, while seldom research was concerned at elevated temperatures.This not only limits the COabsorption application at elevated temperature, but also the determination of the operation condition of the COdesorption generally occurring at higher temperature. This work mainly reported COsolubilities in ILs at elevated temperatures and related properties were also provided. 1-alkyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide([CnMIm][TfN]) ILs were selected as physical absorbents for COcapture in this work due to their relative higher COabsorption capacities and good thermal stabilities. The long-term stability tests showed that [CnMIm][TfN] is thermally stable at 393.15 K for long time. COsolubilities in [CnMIm][TfN] were systematically determined at temperatures from 353.15 K to 393.15 K. It demonstrated that COsolubility obviously increases with the increase of pressure while slightly decreases with increase of temperature. As the length of alkyl chain on the cation increases, COsolubility in ILs increases. Additionally, the thermodynamic properties including the Gibbs free energy, enthalpy, and entropy of COwere also calculated.展开更多
The development of multilayer composite membranes for CO_2 separation has gained increasing attention due to the desire for energy efficient technologies. Multilayer composite membranes have many advantages, including...The development of multilayer composite membranes for CO_2 separation has gained increasing attention due to the desire for energy efficient technologies. Multilayer composite membranes have many advantages, including the possibility to optimize membrane materials independently by layers according to their different functions and to reduce the overall transport resistance by using ultrathin selective layers, and less limitations on the material mechanical properties and processability. A comprehensive review is required to capture details of the progresses that have already been achieved in developing multilayer composite membranes with improved CO_2 separation performance in the past 15-20 years.In this review, various composite membrane preparation methods were compared, advances in composite membranes for CO_2/CH_4 separation,CO_2/N_2 and CO_2/H_2 separation were summarized with detailed data, and challenges facing for the CO_2 separation using composite membranes,such as aging, plasticization and long-term stability, were discussed. Finally the perspectives and future research directions for composite membranes were presented.展开更多
CO2 separation performance in facilitated transport membranes has been reported depended not only on the CO2 carrier properties but also to a great extent on the polymeric matrix regarding the capacity of retaining wa...CO2 separation performance in facilitated transport membranes has been reported depended not only on the CO2 carrier properties but also to a great extent on the polymeric matrix regarding the capacity of retaining water and carriers as well as the processability for coating defect-free ultra-thin films. In this study, the blends of hydrophilic polymers polyvinyl pyrrolidone(PVP) and polyvinyl alcohol(PVA) were studied to find an optimal polymer matrix to host carriers in facilitated transport membranes for enhanced CO2 separation. It is found out that the optimized blend is 50/50 PVA/PVP by weight, which shows a significant increase in the water uptake(from 63 to 84%) at equilibrium state compared to the neat PVA. Polyethyleneimine(PEI) was employed to provide sample carriers to evaluate the synergistic effect of PVA and PVP on the CO2 separation performance. A thin film composite(TFC) membrane of the optimized blend(50/50 PVA/PVP with 50 wt% PEI) was fabricated on polysulfone(PSf) porous support. The fabrication of the TFC membranes is simple and low cost, and CO2 permeance of the optimized blend membrane is nearly doubled with the CO2/N2 selectivity remained unchanged, showing great potential for industrial applications of the resulted membranes.展开更多
A membrane contactor using ionic liquids(ILs) as solvent for pre-combustion capture CO_2 at elevated temperature(303-393 K) and pressure(20 bar) has been studied using mathematic model in the present work. A comprehen...A membrane contactor using ionic liquids(ILs) as solvent for pre-combustion capture CO_2 at elevated temperature(303-393 K) and pressure(20 bar) has been studied using mathematic model in the present work. A comprehensive two-dimensional(2 D) mass-transfer model was developed based on finite element method. The effects of liquid properties, membrane configurations, as well as operation parameters on the CO_2 removal efficiency were systematically studied. The simulation results show that CO_2 can be effectively removed in this process. In addition, it is found that the liquid phase mass transfer dominated the overall mass transfer. Membranes with high porosity and small thickness could apparently reduce the membrane resistance and thus increase the separation efficiency. On the other hand, the membrane diameter and membrane length have a relatively small influence on separation performance within the operation range.展开更多
In this study,cellulose nanofibrils(CNF)of high charge(H-P-CNF)and screened size(H-P-CNF-S)were fabricated by increasing the charge of phosphorylated cellulose nanofibrils(P-CNFs)during the pre-treatment step of CNF p...In this study,cellulose nanofibrils(CNF)of high charge(H-P-CNF)and screened size(H-P-CNF-S)were fabricated by increasing the charge of phosphorylated cellulose nanofibrils(P-CNFs)during the pre-treatment step of CNF production.Results show that the H-P-CNF have a significantly higher charge(3.41 mmol g^(-1))compared with P-CNF(1.86 mmol g^(-1)).Centrifugation of H-P-CNF gave a supernatant with higher charge(5.4 mmol g^(-1))and a reduced size(H-P-CNF-S).These tailored nanocelluloses were added to polyvinyl alcohol(PVA)solutions and the suspensions were successfully coated on porous polysulfone(PSf)supports to produce thin-film nanocomposite membranes.The humid mixed gas permeation tests show that CO_(2)permeability increases for membranes with the addition of H-P-CNF-S by 52%and 160%,compared with the P-CNF/PVA membrane and neat PVA membrane,respectively.展开更多
Although not everybody wants to admit,climate change has been happening with irreversible consequences.It is getting worse and worse and becoming more and more influential to not only the environment but also to all k...Although not everybody wants to admit,climate change has been happening with irreversible consequences.It is getting worse and worse and becoming more and more influential to not only the environment but also to all kinds of beings;our earth is now seriously threatened by climate change.It is a critical issue the whole society must face and actions must展开更多
In this study a thin film composite (TFC) membrane with a Pebax/Task-specific ionic liquid (TSIL) blend selective layer was prepared. Defect-flee Pebax/TSIL layers were coated successfully on a polysulfone ultrafi...In this study a thin film composite (TFC) membrane with a Pebax/Task-specific ionic liquid (TSIL) blend selective layer was prepared. Defect-flee Pebax/TSIL layers were coated successfully on a polysulfone ultrafiltration porous support with a poly- dimethylsiloxane (PDMS) gutter layer. Different parameters in the membrane preparation (e.g. concentration, coating time) were investigated and optimized. The morphology of the membranes was studied by scanning electron microscopy (SEM), while the thermal properties and chemical structures of the membrane materials were investigated by thermo-gravimetric ana- lyzer (TGA), differential scanning calorimetry (DSC) and Fourier transform infrared spectroscopy (FTIR). The CO2 separation performance of the membrane was evaluated using a mixed gas permeation test. Experimental results show that the incorpora- tion of TSIL into the Pebax matrix can significantly increase both C02 permeance and CO2/N2 selectivity. With the presence of water vapor, the membrane exhibits the best CO2/N2 selectivity at a relative humidity of around 75%, where a CO2 permeance of around 500 GPU and a CO2/N2 selectivity of 46 were documented. A further increase in the relative humidity resulted in higher CO: permeance but decreased COIN2 selectivity. Experiments also show that CO2 permeance decreases with a CO2 partial pressure increase, which is considered a characteristic in facilitated transport membranes.展开更多
In a sharp contrast to tropical cyclone(TC) genesis over the main development region of the western North Pacific(WNP), near-equatorial(0°-5°N) TCs exhibit a distinctive annual cycle, peaking in boreal winte...In a sharp contrast to tropical cyclone(TC) genesis over the main development region of the western North Pacific(WNP), near-equatorial(0°-5°N) TCs exhibit a distinctive annual cycle, peaking in boreal winter and being inactive in boreal summer. The relative roles of dynamic and thermodynamic background states on near-equatorial TCs formation were investigated based on the observational diagnosis of the genesis potential index(GPI) and high-resolution model simulations. It is found that the background vorticity makes a major contribution to the distinctive annual cycle, while mean temperature and specific humidity fields are not critical. Numerical simulations further indicate that seasonal mean cyclonic vorticity in boreal winter has three effects on TC genesis near the equator. First, the environmental cyclonic vorticity interacts with TC vortex to promote a mid-level outflow, which strengthens boundary layer friction induced ascending motion and thus condensational heating. Second, it produces an equivalent Coriolis effect(via enhanced absolute vorticity), which strengthens positive feedback between primary and secondary circulation. Third, it helps to merge small-scale vortical hot towers(VHTs) into a mesoscale core through vorticity segregation process. However, background vorticity in boreal summer has an opposite effect on TC development near the equator.展开更多
This work presents the development of molecular-based mathematical model for the prediction of CO_(2) solubility in deep eutectic solvents(DESs).First,a comprehensive database containing 1011 CO_(2) solubility data in...This work presents the development of molecular-based mathematical model for the prediction of CO_(2) solubility in deep eutectic solvents(DESs).First,a comprehensive database containing 1011 CO_(2) solubility data in various DESs at different temperatures and pressures is established,and the COSMO-RS-derived descriptors of involved hydrogen bond acceptors and hydrogen bond donors of DESs are calculated.Afterwards,the efficiency of the input variables,i.e.,temperature,pressure,COSMO-RS-derived descriptors of HBA and HBD as well as their molar ratio,is explored by a qualitative analysis of CO_(2) solubility in DESs using a simple multiple linear regression model.A machine learning method namely random forest is then employed to develop more accurate nonlinear quantitative structure-property relationship(QSPR)model.Combining the QSPR validation and comparisons with literature-reported models(i.e.,COSMO-RS model,traditional thermodynamic models and equations of state methods),the developed QSPR model with COSMO-RS-derived parameters as molecular descriptors is suggested to be able to give reliable predictions of CO_(2) solubility in DESs and could be used as a useful tool in selecting DESs for CO_(2) capture processes.展开更多
基金supported by the National Natural Science Foundation of China (21606233, 21436010)the National Natural Science Fund for Distinguished Young Scholars (21425625)the Research Council of Norway through the CLIMIT program (215732)
文摘COcapture with ionic liquids(ILs) has attracted many attentions, and most works focused on absorption ability at ambient temperatures, while seldom research was concerned at elevated temperatures.This not only limits the COabsorption application at elevated temperature, but also the determination of the operation condition of the COdesorption generally occurring at higher temperature. This work mainly reported COsolubilities in ILs at elevated temperatures and related properties were also provided. 1-alkyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide([CnMIm][TfN]) ILs were selected as physical absorbents for COcapture in this work due to their relative higher COabsorption capacities and good thermal stabilities. The long-term stability tests showed that [CnMIm][TfN] is thermally stable at 393.15 K for long time. COsolubilities in [CnMIm][TfN] were systematically determined at temperatures from 353.15 K to 393.15 K. It demonstrated that COsolubility obviously increases with the increase of pressure while slightly decreases with increase of temperature. As the length of alkyl chain on the cation increases, COsolubility in ILs increases. Additionally, the thermodynamic properties including the Gibbs free energy, enthalpy, and entropy of COwere also calculated.
基金supported by the Research Council of Norway through the CLIMIT program(MCIL-CO_2 project,215732)the European Union Seventh Framework Programme(FP7/2007-2013)in HiPerCap project under grant agreement n°608555
文摘The development of multilayer composite membranes for CO_2 separation has gained increasing attention due to the desire for energy efficient technologies. Multilayer composite membranes have many advantages, including the possibility to optimize membrane materials independently by layers according to their different functions and to reduce the overall transport resistance by using ultrathin selective layers, and less limitations on the material mechanical properties and processability. A comprehensive review is required to capture details of the progresses that have already been achieved in developing multilayer composite membranes with improved CO_2 separation performance in the past 15-20 years.In this review, various composite membrane preparation methods were compared, advances in composite membranes for CO_2/CH_4 separation,CO_2/N_2 and CO_2/H_2 separation were summarized with detailed data, and challenges facing for the CO_2 separation using composite membranes,such as aging, plasticization and long-term stability, were discussed. Finally the perspectives and future research directions for composite membranes were presented.
基金the Norwegian Research Council for the financial support to this work through the Nano2021 program (project number 239172)
文摘CO2 separation performance in facilitated transport membranes has been reported depended not only on the CO2 carrier properties but also to a great extent on the polymeric matrix regarding the capacity of retaining water and carriers as well as the processability for coating defect-free ultra-thin films. In this study, the blends of hydrophilic polymers polyvinyl pyrrolidone(PVP) and polyvinyl alcohol(PVA) were studied to find an optimal polymer matrix to host carriers in facilitated transport membranes for enhanced CO2 separation. It is found out that the optimized blend is 50/50 PVA/PVP by weight, which shows a significant increase in the water uptake(from 63 to 84%) at equilibrium state compared to the neat PVA. Polyethyleneimine(PEI) was employed to provide sample carriers to evaluate the synergistic effect of PVA and PVP on the CO2 separation performance. A thin film composite(TFC) membrane of the optimized blend(50/50 PVA/PVP with 50 wt% PEI) was fabricated on polysulfone(PSf) porous support. The fabrication of the TFC membranes is simple and low cost, and CO2 permeance of the optimized blend membrane is nearly doubled with the CO2/N2 selectivity remained unchanged, showing great potential for industrial applications of the resulted membranes.
基金partly supported by the Research Council of Norway through CLIMIT program (MCIL-CO_2 project, 215732)
文摘A membrane contactor using ionic liquids(ILs) as solvent for pre-combustion capture CO_2 at elevated temperature(303-393 K) and pressure(20 bar) has been studied using mathematic model in the present work. A comprehensive two-dimensional(2 D) mass-transfer model was developed based on finite element method. The effects of liquid properties, membrane configurations, as well as operation parameters on the CO_2 removal efficiency were systematically studied. The simulation results show that CO_2 can be effectively removed in this process. In addition, it is found that the liquid phase mass transfer dominated the overall mass transfer. Membranes with high porosity and small thickness could apparently reduce the membrane resistance and thus increase the separation efficiency. On the other hand, the membrane diameter and membrane length have a relatively small influence on separation performance within the operation range.
基金financial support to the work through the Nano 2021 program(NanoMBE project,number 239172)。
文摘In this study,cellulose nanofibrils(CNF)of high charge(H-P-CNF)and screened size(H-P-CNF-S)were fabricated by increasing the charge of phosphorylated cellulose nanofibrils(P-CNFs)during the pre-treatment step of CNF production.Results show that the H-P-CNF have a significantly higher charge(3.41 mmol g^(-1))compared with P-CNF(1.86 mmol g^(-1)).Centrifugation of H-P-CNF gave a supernatant with higher charge(5.4 mmol g^(-1))and a reduced size(H-P-CNF-S).These tailored nanocelluloses were added to polyvinyl alcohol(PVA)solutions and the suspensions were successfully coated on porous polysulfone(PSf)supports to produce thin-film nanocomposite membranes.The humid mixed gas permeation tests show that CO_(2)permeability increases for membranes with the addition of H-P-CNF-S by 52%and 160%,compared with the P-CNF/PVA membrane and neat PVA membrane,respectively.
文摘Although not everybody wants to admit,climate change has been happening with irreversible consequences.It is getting worse and worse and becoming more and more influential to not only the environment but also to all kinds of beings;our earth is now seriously threatened by climate change.It is a critical issue the whole society must face and actions must
基金supported by the Research Council of Norway through the CLIMIT program (MCIL-CO2 project, 21732)the National Natural Science Fund for Distinguished Young Scholars (21425625) from China
文摘In this study a thin film composite (TFC) membrane with a Pebax/Task-specific ionic liquid (TSIL) blend selective layer was prepared. Defect-flee Pebax/TSIL layers were coated successfully on a polysulfone ultrafiltration porous support with a poly- dimethylsiloxane (PDMS) gutter layer. Different parameters in the membrane preparation (e.g. concentration, coating time) were investigated and optimized. The morphology of the membranes was studied by scanning electron microscopy (SEM), while the thermal properties and chemical structures of the membrane materials were investigated by thermo-gravimetric ana- lyzer (TGA), differential scanning calorimetry (DSC) and Fourier transform infrared spectroscopy (FTIR). The CO2 separation performance of the membrane was evaluated using a mixed gas permeation test. Experimental results show that the incorpora- tion of TSIL into the Pebax matrix can significantly increase both C02 permeance and CO2/N2 selectivity. With the presence of water vapor, the membrane exhibits the best CO2/N2 selectivity at a relative humidity of around 75%, where a CO2 permeance of around 500 GPU and a CO2/N2 selectivity of 46 were documented. A further increase in the relative humidity resulted in higher CO: permeance but decreased COIN2 selectivity. Experiments also show that CO2 permeance decreases with a CO2 partial pressure increase, which is considered a characteristic in facilitated transport membranes.
基金Supported by the National Natural Science Foundation of China(41630423 and 41875069)NOAA of U.S.(NA18OAR4310298)+2 种基金National Science Foundation of U.S.(AGS-1643297)China Scholarship Council(CSC,N201808320286)Postgraduate Research and Practice Innovation Program of Jiangsu Province(KYCX18_1002)。
文摘In a sharp contrast to tropical cyclone(TC) genesis over the main development region of the western North Pacific(WNP), near-equatorial(0°-5°N) TCs exhibit a distinctive annual cycle, peaking in boreal winter and being inactive in boreal summer. The relative roles of dynamic and thermodynamic background states on near-equatorial TCs formation were investigated based on the observational diagnosis of the genesis potential index(GPI) and high-resolution model simulations. It is found that the background vorticity makes a major contribution to the distinctive annual cycle, while mean temperature and specific humidity fields are not critical. Numerical simulations further indicate that seasonal mean cyclonic vorticity in boreal winter has three effects on TC genesis near the equator. First, the environmental cyclonic vorticity interacts with TC vortex to promote a mid-level outflow, which strengthens boundary layer friction induced ascending motion and thus condensational heating. Second, it produces an equivalent Coriolis effect(via enhanced absolute vorticity), which strengthens positive feedback between primary and secondary circulation. Third, it helps to merge small-scale vortical hot towers(VHTs) into a mesoscale core through vorticity segregation process. However, background vorticity in boreal summer has an opposite effect on TC development near the equator.
基金support from National Natural Science Foundation of China(21861132019,21776074)is greatly acknowledged.
文摘This work presents the development of molecular-based mathematical model for the prediction of CO_(2) solubility in deep eutectic solvents(DESs).First,a comprehensive database containing 1011 CO_(2) solubility data in various DESs at different temperatures and pressures is established,and the COSMO-RS-derived descriptors of involved hydrogen bond acceptors and hydrogen bond donors of DESs are calculated.Afterwards,the efficiency of the input variables,i.e.,temperature,pressure,COSMO-RS-derived descriptors of HBA and HBD as well as their molar ratio,is explored by a qualitative analysis of CO_(2) solubility in DESs using a simple multiple linear regression model.A machine learning method namely random forest is then employed to develop more accurate nonlinear quantitative structure-property relationship(QSPR)model.Combining the QSPR validation and comparisons with literature-reported models(i.e.,COSMO-RS model,traditional thermodynamic models and equations of state methods),the developed QSPR model with COSMO-RS-derived parameters as molecular descriptors is suggested to be able to give reliable predictions of CO_(2) solubility in DESs and could be used as a useful tool in selecting DESs for CO_(2) capture processes.