Graphene has enormous potential to capture CO_(2)due to its unique properties and cost-effectiveness.However,graphene-based adsorbents have drawbacks of lower CO_(2)adsorption capacity and poor selectivity.This work d...Graphene has enormous potential to capture CO_(2)due to its unique properties and cost-effectiveness.However,graphene-based adsorbents have drawbacks of lower CO_(2)adsorption capacity and poor selectivity.This work demonstrates a one-step rapid and sustainable N_(2)/H_(2)plasma treatment process to prepare graphene-based sorbent material with enhanced CO_(2)adsorption performance.Plasma treatment directly enriches amine species,increases surface area,and improves textural properties.The CO_(2)adsorption capacity increases from 1.6 to 3.3 mmol/g for capturing flue gas,and from 0.14 to 1.3 mmol/g for direct air capture (DAC).Importantly,the electrothermal property of the plasma-modified aerogels has been significantly improved,resulting in faster heating rates and significantly reducing energy consumption compared to conventional external heating for regeneration of sorbents.Modified aerogels display improved selectivity of 42 and 87 after plasma modification for 5 and 10 min,respectively.The plasma-treated aerogels display minimal loss between 17%and 19% in capacity after 40 adsorption/desorption cycles,rendering excellent stability.The N_(2)/H_(2)plasma treatment of adsorbent materials would lower energy expenses and prevent negative effects on the global economy caused by climate change.展开更多
Membrane gas absorption and solar-assisted absorbent regeneration offer a sustainable approach to reduce the energy penalty of post-combustion CO_(2) capture.This study introduces a novel system integrating solar ther...Membrane gas absorption and solar-assisted absorbent regeneration offer a sustainable approach to reduce the energy penalty of post-combustion CO_(2) capture.This study introduces a novel system integrating solar thermal energy with membrane gas absorption to capture CO_(2) from a 580 MWe pulverized coal power plant.The environmental impacts across six scenarios at varying solar fractions are evaluated via life cycle assessment.Results show a 7.61%–13.04%reduction in global warming potential compared to a steam-driven CO_(2) capture system.Electricity and steam consumption dominate the operational phase,contributing 15%–64%and 18%–61%to environmental impacts in non-TES scenarios,respectively.While TES reduces most impacts,it increases stratospheric ozone depletion and marine eutrophication due to nitrate-based phase change materials and monoethanolamine.Higher solar fractions lower impacts in non-TES scenarios but elevate specific impacts in TES scenarios,highlighting trade-offs for sustainable CO_(2) capture deployment.展开更多
Among the current technologies for post-combustion CO2 capture,amine-based chemical absorption appears to be the most technologically mature and commercially viable method.This review highlights the opportunities and ...Among the current technologies for post-combustion CO2 capture,amine-based chemical absorption appears to be the most technologically mature and commercially viable method.This review highlights the opportunities and challenges in post-combustion CO2 capture using amine-based chemical absorption technologies.In addition,this review provides current types and emerging trends for chemical solvents.The issues and performance of amine solvents are reviewed and addressed in terms of thermodynamics,kinetics,mass transfer,regeneration and solvent management.This review also looks at emerging and future trends in post-combustion CO2 capture using chemical solvents in the near to mid-term.展开更多
CO_(2) capture and utilization(CCU)technologies have been recognized as crucial strategies for mitigating global warming,reducing carbon emission,and promoting resource circularity.As such,the design and development o...CO_(2) capture and utilization(CCU)technologies have been recognized as crucial strategies for mitigating global warming,reducing carbon emission,and promoting resource circularity.As such,the design and development of related materials have attracted considerable research attention.Carbon-based materials,characterized by tunable pore structures,abundant active sites,high specific surface area,and excellent chemical stability,demonstrate significant potential for applications in CO_(2) capture and utilization.This review systematically analyzes the adsorption behaviors and performance variations of typical carbon materials,including activated carbon,porous carbon,graphene,and carbon nanotubes during CO_(2) capture processes.Concerning CO_(2) utilization,emphasis is placed on recent advances in the catalytic applications of carbon-based materials in key reactions such as methanation,reverse water-gas shift,dry reforming of methane,and alcohol synthesis.Moreover,the benefits and drawbacks of carbon materials in terms of CO_(2) adsorption capacity,catalytic activity,and stability are thoroughly evaluated,and their potential applications in integrated CO_(2) capture and utilization technologies are discussed.Finally,key strategies for enhancing the performance of carbonaceous materials through structural modulation and surface modification are elucidated.This review aims to provide theoretical guidance for the future development and large-scale implementation of carbon-based materials in CCU technologies.展开更多
Benzylamine(BZA) has been identified as a promising candidate for CO_2 capture process; however the evaluation of BZA in the packed column was very few. Thus, in this work, the absorption and regeneration performance ...Benzylamine(BZA) has been identified as a promising candidate for CO_2 capture process; however the evaluation of BZA in the packed column was very few. Thus, in this work, the absorption and regeneration performance of unblended BZA solvent as well as a series of amine concentrations and ratios in the formulations were studied using a semibatch bubbling reactor. And due to the formation of ivory-white precipitates in solvents containing higher BZA ratios, a 4:1 molar ratio of MEA/BZA mixed solvent was used to study its performance in a pilot-scale test bed. The results showed that a higher BZA ratio in the MEA/BZA mixed solvent resulted in a faster absorption rate, a higher mass transfer and heat transfer rate and a better cyclic performance, but the mass transfer rate of BZA decreased more quickly than MEA with the increase of CO_2 loading of the solvents. In addition, at high CO_2 loading in the MEA/ BZA mixed solvent with a molar ratio of 4:1, the ivory-white precipitates were generated which could cause blockage of the packing in the absorber, the stripper and the liquid pipelines.展开更多
Aqueous ammonia(NH3) is a promising alternative solvent for the capture of industrial CO_2 emissions, given its high chemical stability and CO_2 removal capacity, and low material costs and regeneration energy. NH3 al...Aqueous ammonia(NH3) is a promising alternative solvent for the capture of industrial CO_2 emissions, given its high chemical stability and CO_2 removal capacity, and low material costs and regeneration energy. NH3 also has potential for capturing multiple flue gas components, including NOx, SOxand CO_2, and producing value-added chemicals. However, its high volatility and low reactivity towards CO_2 limit its economic viability. Considerable efforts have been made to advance aqueous NH3-based post-combustion capture technologies in the last few years: in particular, General Electric's chilled NH3 process, CSIRO's mild-temperature aqueous NH3 process and SRI International's mixed-salts(NH3 and potassium carbonate) technology. Here, we review these research activities and other developments in the field, and outline future research needed to further improve aqueous NH3-based CO_2 capture technologies.展开更多
This paper presented a comparative study of monoethanolamine （MEA） and diethanolamine （DEA） for post- combustion CO2 capture （PCC） process with different process configurations to study the interaction effect be...This paper presented a comparative study of monoethanolamine （MEA） and diethanolamine （DEA） for post- combustion CO2 capture （PCC） process with different process configurations to study the interaction effect between solvent and process. The steady state process model of the conventional MEA-based PCC process was developed in Pro/II and was validated with the experimental data. Then ten different process configurations were simulated for both MEA and DEA. Their performances in energy consumption were compared in terms of reboiler duty and total equivalent work. The results show that DEA generally has better thermal performances than MEA for all these ten process configurations. Seven process configurations provide 0.38%-4.61% total energy saving compared with the conventional PCC process for MEA, and other two configurations are not favourable. For DEA, except one configuration, other process configurations have 0.27%-4.50% total energy saving. This work also analyzed the sensitivities of three key parameters （amine concentration, stripper pressure and lean solvent loading） in conventional process and five process modifications to show optimization strategy.展开更多
Global warming and associated global climate change have led to serious efforts towards reducing CO_(2)emissions through the CO_(2)capture from the major emission sources.CO_(2)capture using the amine functionalized a...Global warming and associated global climate change have led to serious efforts towards reducing CO_(2)emissions through the CO_(2)capture from the major emission sources.CO_(2)capture using the amine functionalized adsorbents is regard as a direct and effective way to reducing CO_(2)emissions due to their large CO_(2)adsorption amount,excellent CO_(2)adsorption selectivity and lower energy requirements for adsorbent regeneration.Moreover,large number of achievements on the amine functionalized solid adsorbent have been recorded for the enhanced CO_(2)capture in the past few years.In view of this,we review and analyze the recent advances in amine functionalized solid adsorbents prepared with different supporting materials including mesoporous silica,zeolite,porous carbon materials,metal organic frameworks(MOF)and other composite porous materials.In addition,amine functionalized solid adsorbents derived from waste resources are also reviewed because of the large number demand for cost-effective carbon dioxide adsorbents and the processing needs of waste resources.Considering the importance of the stability of the adsorbent in practical applications,advanced research in the capture cycle stability has also been summarized and analyzed.Finally,we summarize the review and offer the recommendations for the development of amine-based solid adsorbents for carbon dioxide capture.展开更多
In the current work five different solvent blends are experimentally studied and the reboiler duties are calculated using the so-called short-cut method.Tertiary amines,2-(diethylamino)ethanol(DEEA),3-(Diethylamino)-1...In the current work five different solvent blends are experimentally studied and the reboiler duties are calculated using the so-called short-cut method.Tertiary amines,2-(diethylamino)ethanol(DEEA),3-(Diethylamino)-1,2-propanediol(DEA-12PD),2-[2-(Diethylamino)ethoxy]ethanol(DEA-EO),1-(2-Hydroxyethyl)piperidine(12HE-PP)are blended with 3-(Methylamino)propylamine(MAPA)and ethanolamine(MEA).The first results from simple solvent screening are given and the cyclic capacities are calculated based data at 40℃ and 80℃.Then,five solvent systems are chosen for vapor–liquid equilibrium characterization.The vapor–liquid equilibrium data are then used to estimate cyclic capacities at more realistic temperatures,between 40℃ and 120℃ and by using a short-cut method proposed in the literature the reboiler duties of the characterized solvents are estimated.Finally,the potential of the studied systems is discussed.Several of the characterized blends showed reboiler duties around 2.5 MJ kgCO2^-1.展开更多
Carbon dioxide(CO_(2))capture by gas-separation membranes has become increasingly attractive due to its high energy efficiency,relatively low cost,and environmental impact.Polyvinylamine(PVAm)-based facilitated transp...Carbon dioxide(CO_(2))capture by gas-separation membranes has become increasingly attractive due to its high energy efficiency,relatively low cost,and environmental impact.Polyvinylamine(PVAm)-based facilitated transport(FT)membranes were developed in the last decade for CO_(2) capture.This work discusses the challenges of applying PVAm-based FT membranes from materials to processes for postcombustion CO_(2) capture in power plants and cement factories.Experiences learned from a pilot demonstration system can be used to guide the design of other membranes for CO_(2) capture.The importance of module and process design is emphasized in the achievement of a high-performance membrane system.Moreover,the results from process simulation and cost estimation indicate that a three-stage membrane system is feasible for achieving a high CO_(2) purity of 95 vol%.The specific CO_(2) capture cost was found to significantly depend on the required CO_(2) capture ratio,and a moderate CO_(2) capture ratio of 50%presented a cost of 63.7USD per tonne CO_(2) captured.Thus,FT membrane systems were found to be more competitive for partial CO_(2) capture.展开更多
This work presents a simulation study of several Ca-Cu looping variants with CO(2)capture,aiming at both parameter optimization and exergy analysis of these Ca-Cu looping systems.Three kinds of Ca-Cu looping are consi...This work presents a simulation study of several Ca-Cu looping variants with CO(2)capture,aiming at both parameter optimization and exergy analysis of these Ca-Cu looping systems.Three kinds of Ca-Cu looping are considered:(1)carbonation-calcination/reduction-oxidation;(2)carbonation-oxidation-calcination/reduction and (3)carbona tion/oxidation-calcination/reduction.A conventional Ca looping is also simulated for comparison.The influences of the calcination temperature on the mole fractions of CO(2)and CaO at the calciner outlet,the CaCO3 flow rate on the carbonator performance and the Cu/Ca ratio on the calciner performance are analyzed.The second kind of Ca-Cu looping has the highest carbonation conversion.At 1×10^5 Pa and 820℃,complete decomposition of CaCO3 can be achieved in three Ca-Cu looping systems,while the operation condition of 1×10^5 Pa,840℃is required for the conventional Ca looping system.Furthermore,the Cu/Ca molar ratio of 5.13-5.19 is required for the Ca-Cu looping.Exergy analyses show that the maximum exergy destruction occurs in the calciner for the four modes and the second Ca-Cu looping system(i.e.,carbonation-oxidation-calcination/reduction)performs the highest exergy efficiency,up to 65.04%,which is about 30%higher than that of the conventional Ca looping.展开更多
This paper presents modelling of a post-combustion CO2 capture process using bootstrap aggregated extreme learning machine （ELM）. ELM randomly assigns the weights between input and hidden layers and obtains the weig...This paper presents modelling of a post-combustion CO2 capture process using bootstrap aggregated extreme learning machine （ELM）. ELM randomly assigns the weights between input and hidden layers and obtains the weights between the hidden layer and output layer using regression type approach in one step. This feature allows an ELM model being developed very quickly. This paper proposes using principal component regression to obtain the weights between the hidden and output layers to address the collinearity issue among hidden neuron outputs. Due to the weights between input and hidden layers are randomly assigned, ELM models could have variations in performance. This paper proposes combining multiple ELM models to enhance model prediction accuracy and reliability. To predict the CO2 production rate and CO2 capture level, eight parameters in the process were utilized as model input variables： inlet gas flow rate, CO2 concentration in inlet flow gas, inlet gas temperature, inlet gas pressure, lean solvent flow rate, Jean solvent temperature, lean loading and reboiler duty. The bootstrap re-sampling of training data was applied for building each single ELM and then the individual ELMs are stacked, thereby enhancing the model accuracy and reliability. The bootstrap aggregated extreme learning machine can provide fast learning speed and good generalization performance, which will be used to optimize the CO2 capture process.展开更多
Abstract： Two Canadian limestones with different properties were tested to determine the effect of SO2 during the carbonation of sorbent on the CO2 capture performance in Ca- looping. When the reaction gas is mixed w...Abstract： Two Canadian limestones with different properties were tested to determine the effect of SO2 during the carbonation of sorbent on the CO2 capture performance in Ca- looping. When the reaction gas is mixed with SO2, the carbonation ratio of the sorbent is always lower than that without SO2 for each cycle under the same conditions, and the sulfation ratio increases almost linearly with the increase in the cycle times. At 650 ℃, there is little difference in the carbonation ratio of the sorbent during the first four cycles for the two carbonation time, 5 and 10 rain at 0. 18% SO2. The indirect sulfation reaction that occurs simultaneously with the carbonation of CaO is responsible for the degradation of the sorbent for CO2 capture, and the carbonation duration is not the main factor that affects the ability of the sorbent. 680℃ is the best carbonation temperature among the three tested temperatures and the highest carbonation ratio can be obtained. Also, the sulfation ratio is the highest. The probable cause is the different effects of temperature on the carbonation rate and sulfation rate. A higher SO2 concentration will decrease the carbonation ratio clearly, but the decrease in the carbonation capability of the sorbent is not proportional to the increase of the SO2 concentration in flue gases.展开更多
A kind of industrial solid waste, i.e., carbide slag, was used as CaO precursor to synthesize CO2 sorbent. The highly reactive synthetic sorbent was prepared from carbide slag, aluminum nitrate hydrate and glycerol wa...A kind of industrial solid waste, i.e., carbide slag, was used as CaO precursor to synthesize CO2 sorbent. The highly reactive synthetic sorbent was prepared from carbide slag, aluminum nitrate hydrate and glycerol water solution by the combustion synthesis method. The results show that the synthetic sorbent exhibits a much higher CO2 capture capacity compared with carbide slag. The CO2 capture capacity and the carbonation conversion of the synthetic sorbent are 0. 38 g/g and 0. 70 after 50 cycles, which are 1.8 and 2. 1 times those of carbide slag. The average carbonation conversion and the CO2 capture efficiency of the synthetic sorbent are higher than those of carbide slag with the same sorbent flow ratios. The required sorbent flow ratios are lower for synthetic sorbent to achieve the same CO2 capture efficiency compared with carbide slag. With the same sorbent flow ratio and CO2 capture efficiency, the energy requirement in calciner for the synthetic sorbent is less than that for carbide slag.展开更多
Abstract： In order to improve the reactivity of Na2CO3/Al2O3 sorbent with CO2, a new sorbent showing high reactivity was developed by doping Na2CO3/Al2O3 with TiO2 using impregnation. Fourteen multi-cycle carbonation...Abstract： In order to improve the reactivity of Na2CO3/Al2O3 sorbent with CO2, a new sorbent showing high reactivity was developed by doping Na2CO3/Al2O3 with TiO2 using impregnation. Fourteen multi-cycle carbonation/regeneration tests of the sorbent were carried out in a fluidized-bed reactor and the sorbent was characterized by X-ray diffraction and nitrogen adsorption. It is confirmed that TiO2 shows a positive effect on the adsorption process of Na2CO3 and the reaction rate is observed to increase significantly, especially in the first 10 min. Moreover, TiO2 is stable within the temperature range of the process and no other Ti-compounds are detected. The carbonation products are NaHCO3 and Na5H3 （CO3 ）4. The surface area and the pore volume of the sorbent keep stable after 14 cycles. The Fourier transform infrared spectroscopy and the X-ray photoelectron spectroscopy are used to analyze the effect mechanism of TiO2 on CO2 adsorption process of Na2CO3/Al2O3.展开更多
Currently,the solid adsorbents with porous structure have been widely applied in CO_(2)capture.However,the unmodified MgO-ZrO_(2)adsorbents appeared to be low adsorption capacity of CO_(2).The solid adsorbent material...Currently,the solid adsorbents with porous structure have been widely applied in CO_(2)capture.However,the unmodified MgO-ZrO_(2)adsorbents appeared to be low adsorption capacity of CO_(2).The solid adsorbent materials were successfully synthesized by loading TEPA onto the pore MgO/ZrO_(2)carriers in the paper.The pore structure and surface characteristic of the samples were analyzed by using XRD,BET,FT-IR and SEM.The adsorbent materials exhibited microcrystalline state,and the crystallinity of all samples gradually decreased as the increase of TEPA content.The pore structure analysis indicated that the modification of MgO-ZrO_(2)adsorbents with TEPA led to the decrease of the specific surface areas,but the narrow micro-mesopore size distributions ranging from 1.8-12 nm in the adsorbents still were maintained.FT-IR spectrum results further verified the successful loading of TEPA.The adsorption capacity of the adsorbents for CO_(2)were tested by using an adsorption apparatus equipped with gas chromatography.The results indicated that when the TEPA loading reached 50%,the sample exhibited the maximum adsorption value for CO_(2),reaching 4.07 mmol/g under the operation condition of 75℃and atmospheric pressure.This result could be assigned to not only the base active sites but also the coexistence of both micropore and mesopore in the adsorbent.After three cycles tests for CO_(2)capture,the adsorption value of the sample for CO_(2)can also reached 95%of its original adsorption capacity,which verified the excellent cyclic operation stability.展开更多
Carbon capture is an important strategy and is implemented to achieve the goals of CO_(2)reduction and carbon neutrality.As a high energy-efficient technology,membrane-based separation plays a crucial role in CO_(2)ca...Carbon capture is an important strategy and is implemented to achieve the goals of CO_(2)reduction and carbon neutrality.As a high energy-efficient technology,membrane-based separation plays a crucial role in CO_(2)capture.It is urgently needed for membrane-based CO_(2)capture to develop the high-performance membrane materials with high permeability,selectivity,and stability.Herein,ultrapermeable carbon molecular sieve(CMS)membranes are fabricated by py roly zing a finely-engineered benzoxazole-containing copolyimide precursor for efficient CO_(2)capture.The microstructure of CMS membrane has been optimized by initially engineering the precursor-chemistry and subsequently tuning the pyrolysis process.Deep insights into the structure-property relationship of CMSs are provided in detail by a combination of experimental characterization and molecular simulations.We demonstrate that the intrinsically high free volume environment of the precursor,coupled with the steric hindrance of thermostable contorted fragments,promotes the formation of loosely packed and ultramicroporous carbon structures within the resultant CMS membrane,thereby enabling efficient CO_(2)discrimination via size sieving and affinity.The membrane achieves an ultrahigh CO_(2)permeability,good selectivity,and excellent stability.After one month of long-term operation,the CO_(2)permeability in the mixed gas is maintained at 11,800 Barrer,with a CO_(2)/N_(2)selectivity exceeding 60.This study provides insights into the relationship between precursor-chemistry and CMS performance,and our ultrapermeable CMS membrane,which is scalable using thin film manufacturing,holds great potential for industrial CO_(2)capture.展开更多
Due to the significant impact of carbon dioxide on global ecology,more efforts have been put into the exploration on CO_(2)capture and utilization.Porous organic framework materials,as a kind of materials with high po...Due to the significant impact of carbon dioxide on global ecology,more efforts have been put into the exploration on CO_(2)capture and utilization.Porous organic framework materials,as a kind of materials with high porosity and designable structure,have been considered as effective host materials for adsorbing carbon dioxide or separating it from other gases.This review gives a deep insight into the applications of metal-organic frameworks,covalent-organic frameworks,and other porous frameworks on CO_(2)capture,focusing on the enhanced capture performances originated from their high surface area with abundant porous structure,functional groups with specific heteroatoms modification,or other building unit interactions.Besides,the main challenges associated with porous frameworks for CO_(2)capture and proposed strategies to address these obstacles,including the structural design strategy or the capture mechanism exploration,have been demonstrated and emphasized.This review can contribute to further investigation on porous frameworks for gas capture and separation with enhanced performance and efficiency.展开更多
Catalyst-aided regeneration is a promising method for reducing the high regeneration energy consumption of amine-based CO_(2)capture technologies.However,the intrinsic relationship between the properties of the acidic...Catalyst-aided regeneration is a promising method for reducing the high regeneration energy consumption of amine-based CO_(2)capture technologies.However,the intrinsic relationship between the properties of the acidic sites and their catalytic activity is controversial.In this study,a series of W-based catalysts supported by ZrTiO_(x)were synthesised,and the effects of the intensity,distribution,and type of acid sites were systematically investigated by quantitatively regulating the acidic site properties.The results indicate stronger acidic sites play a more important role in the catalytic reaction.Moreover,the catalysts showed excellent performance only if the Br?nsted acid sites(BASs)and Lewis acid sites(LASs)coexisted.During the catalytic reaction,the BASs facilitated deprotonation,and the LASs promoted the decomposition of carbamates.The ratio of BASs to LASs(B/L)was a critical factor for catalytic activity,wherein optimal performance was achieved when the B/L ratio was close to 1.The 10%HPW/ZrTiO_(x)composite performed better than WO_(3)/ZrTiO_(x)and HSiW/ZrTiO_(x)because it had a stronger acid intensity and a suitable B/L ratio.As a result,the relative heat duty was reduced by 47%compared to 30%aqueous MEA,and the maximum CO_(2)desorption rate was increased by 83%.The Bader charge indicated that the W atoms of HPW/ZrTiO_(x)lost more electrons(0.18)than those of WO_(3)/ZrTiO_(x),which can weaken the O±H bond energy.Consequently,the calculated deprotonation energy is as low as 257 kJ mol^(-1)for HPW/ZrTiO_(x).展开更多
The non-aqueous solid-liquid biphasic solvent of 2-amino-2-methyl-1-propanol(AMP)/piperazine(PZ)/dipropylene glycol dimethyl ether(DME)features a high CO_(2)absorption loading,favorable phase separation behavior and h...The non-aqueous solid-liquid biphasic solvent of 2-amino-2-methyl-1-propanol(AMP)/piperazine(PZ)/dipropylene glycol dimethyl ether(DME)features a high CO_(2)absorption loading,favorable phase separation behavior and high regeneration efficiency.Different with the liquid-liquid phase change solvent,the reaction kinetics of CO_(2)capture into solid-liquid biphasic solvent was rarely studied.In the present work,the reaction kinetics of CO_(2)absorption into AMP/PZ/DME solid-liquid biphasic solvent was investigated into the double stirred kettle reactor.The absorption reaction followed a pseudo-first-order kinetic model according to the zwitterion mechanism.The overall reaction rate constant(kov)and the enhancement factor(E)of CO_(2)absorption both increased with increasing temperature.The total mass transfer resistance of the absorbent decreased with increasing temperature and increased with increasing absorption loading,so the higher reaction temperature was conducive to the absorption,and the liquid phase mass transfer resistance was the main factor affecting the absorption rate.展开更多
基金Guangzhou (China) government postdoctoral program for providing financial support to conduct this worksupport from the National Natural Science Foundation of China (No. 72140008)funding from the European Union’s Horizon 2020 Research and Innovation program under grant agreement No. 101022484。
文摘Graphene has enormous potential to capture CO_(2)due to its unique properties and cost-effectiveness.However,graphene-based adsorbents have drawbacks of lower CO_(2)adsorption capacity and poor selectivity.This work demonstrates a one-step rapid and sustainable N_(2)/H_(2)plasma treatment process to prepare graphene-based sorbent material with enhanced CO_(2)adsorption performance.Plasma treatment directly enriches amine species,increases surface area,and improves textural properties.The CO_(2)adsorption capacity increases from 1.6 to 3.3 mmol/g for capturing flue gas,and from 0.14 to 1.3 mmol/g for direct air capture (DAC).Importantly,the electrothermal property of the plasma-modified aerogels has been significantly improved,resulting in faster heating rates and significantly reducing energy consumption compared to conventional external heating for regeneration of sorbents.Modified aerogels display improved selectivity of 42 and 87 after plasma modification for 5 and 10 min,respectively.The plasma-treated aerogels display minimal loss between 17%and 19% in capacity after 40 adsorption/desorption cycles,rendering excellent stability.The N_(2)/H_(2)plasma treatment of adsorbent materials would lower energy expenses and prevent negative effects on the global economy caused by climate change.
基金funded by State Key Laboratory of Intelligent Construction and Healthy Operation andMaintenance ofDeepUnderground Engineering,grant number SDGZ2524Shandong Province Science and Technology Smes Ability Improvement Project,grant number 2025TSGCCZZB0258Major Innovation Project of Qilu University of Technology(Shandong Academy of Sciences),grant number 2025ZDZX03.
文摘Membrane gas absorption and solar-assisted absorbent regeneration offer a sustainable approach to reduce the energy penalty of post-combustion CO_(2) capture.This study introduces a novel system integrating solar thermal energy with membrane gas absorption to capture CO_(2) from a 580 MWe pulverized coal power plant.The environmental impacts across six scenarios at varying solar fractions are evaluated via life cycle assessment.Results show a 7.61%–13.04%reduction in global warming potential compared to a steam-driven CO_(2) capture system.Electricity and steam consumption dominate the operational phase,contributing 15%–64%and 18%–61%to environmental impacts in non-TES scenarios,respectively.While TES reduces most impacts,it increases stratospheric ozone depletion and marine eutrophication due to nitrate-based phase change materials and monoethanolamine.Higher solar fractions lower impacts in non-TES scenarios but elevate specific impacts in TES scenarios,highlighting trade-offs for sustainable CO_(2) capture deployment.
基金Supported by the National Natural Science Foundation of China(21276068,U1362112and 21376067,21476064)the National Key Technology R&D Program(2012BAC26B01)+4 种基金Innovative Research Team Development Plan of the Ministry of Education of the People's Republic of China(IRT1238)Specialized Research Fund for the Doctoral Program of Higher Education(20130161110025)Technology Development contract(Shanyan 12-34)Innovative Research Program for Graduate Student of Hunan Province,China(CX2013B158)Key project of international®ional scientific and technological cooperation of Hunan Provincial science and technology plan(2014WK2037)
文摘Among the current technologies for post-combustion CO2 capture,amine-based chemical absorption appears to be the most technologically mature and commercially viable method.This review highlights the opportunities and challenges in post-combustion CO2 capture using amine-based chemical absorption technologies.In addition,this review provides current types and emerging trends for chemical solvents.The issues and performance of amine solvents are reviewed and addressed in terms of thermodynamics,kinetics,mass transfer,regeneration and solvent management.This review also looks at emerging and future trends in post-combustion CO2 capture using chemical solvents in the near to mid-term.
基金Supported by National Key R&D Program of China(2025YFE0109700)the National Natural Science Foundation of China(52106150)。
文摘CO_(2) capture and utilization(CCU)technologies have been recognized as crucial strategies for mitigating global warming,reducing carbon emission,and promoting resource circularity.As such,the design and development of related materials have attracted considerable research attention.Carbon-based materials,characterized by tunable pore structures,abundant active sites,high specific surface area,and excellent chemical stability,demonstrate significant potential for applications in CO_(2) capture and utilization.This review systematically analyzes the adsorption behaviors and performance variations of typical carbon materials,including activated carbon,porous carbon,graphene,and carbon nanotubes during CO_(2) capture processes.Concerning CO_(2) utilization,emphasis is placed on recent advances in the catalytic applications of carbon-based materials in key reactions such as methanation,reverse water-gas shift,dry reforming of methane,and alcohol synthesis.Moreover,the benefits and drawbacks of carbon materials in terms of CO_(2) adsorption capacity,catalytic activity,and stability are thoroughly evaluated,and their potential applications in integrated CO_(2) capture and utilization technologies are discussed.Finally,key strategies for enhancing the performance of carbonaceous materials through structural modulation and surface modification are elucidated.This review aims to provide theoretical guidance for the future development and large-scale implementation of carbon-based materials in CCU technologies.
基金supported by the Sinopec Ningbo Engineering Co. Ltd. (No.l4850000-14-ZC0609-0003,H8XY-0032)
文摘Benzylamine(BZA) has been identified as a promising candidate for CO_2 capture process; however the evaluation of BZA in the packed column was very few. Thus, in this work, the absorption and regeneration performance of unblended BZA solvent as well as a series of amine concentrations and ratios in the formulations were studied using a semibatch bubbling reactor. And due to the formation of ivory-white precipitates in solvents containing higher BZA ratios, a 4:1 molar ratio of MEA/BZA mixed solvent was used to study its performance in a pilot-scale test bed. The results showed that a higher BZA ratio in the MEA/BZA mixed solvent resulted in a faster absorption rate, a higher mass transfer and heat transfer rate and a better cyclic performance, but the mass transfer rate of BZA decreased more quickly than MEA with the increase of CO_2 loading of the solvents. In addition, at high CO_2 loading in the MEA/ BZA mixed solvent with a molar ratio of 4:1, the ivory-white precipitates were generated which could cause blockage of the packing in the absorber, the stripper and the liquid pipelines.
文摘Aqueous ammonia(NH3) is a promising alternative solvent for the capture of industrial CO_2 emissions, given its high chemical stability and CO_2 removal capacity, and low material costs and regeneration energy. NH3 also has potential for capturing multiple flue gas components, including NOx, SOxand CO_2, and producing value-added chemicals. However, its high volatility and low reactivity towards CO_2 limit its economic viability. Considerable efforts have been made to advance aqueous NH3-based post-combustion capture technologies in the last few years: in particular, General Electric's chilled NH3 process, CSIRO's mild-temperature aqueous NH3 process and SRI International's mixed-salts(NH3 and potassium carbonate) technology. Here, we review these research activities and other developments in the field, and outline future research needed to further improve aqueous NH3-based CO_2 capture technologies.
文摘This paper presented a comparative study of monoethanolamine （MEA） and diethanolamine （DEA） for post- combustion CO2 capture （PCC） process with different process configurations to study the interaction effect between solvent and process. The steady state process model of the conventional MEA-based PCC process was developed in Pro/II and was validated with the experimental data. Then ten different process configurations were simulated for both MEA and DEA. Their performances in energy consumption were compared in terms of reboiler duty and total equivalent work. The results show that DEA generally has better thermal performances than MEA for all these ten process configurations. Seven process configurations provide 0.38%-4.61% total energy saving compared with the conventional PCC process for MEA, and other two configurations are not favourable. For DEA, except one configuration, other process configurations have 0.27%-4.50% total energy saving. This work also analyzed the sensitivities of three key parameters （amine concentration, stripper pressure and lean solvent loading） in conventional process and five process modifications to show optimization strategy.
基金supported by the National Natural Science Foundation of China(21878200 and 21676174)International S&T Cooperation Program of Shanxi province(201703D421038)+1 种基金Shanxi Scholarship Council of China(2017-036)Joint Fund of Shanxi Provincial Coal Seam Gas(2015012019)。
文摘Global warming and associated global climate change have led to serious efforts towards reducing CO_(2)emissions through the CO_(2)capture from the major emission sources.CO_(2)capture using the amine functionalized adsorbents is regard as a direct and effective way to reducing CO_(2)emissions due to their large CO_(2)adsorption amount,excellent CO_(2)adsorption selectivity and lower energy requirements for adsorbent regeneration.Moreover,large number of achievements on the amine functionalized solid adsorbent have been recorded for the enhanced CO_(2)capture in the past few years.In view of this,we review and analyze the recent advances in amine functionalized solid adsorbents prepared with different supporting materials including mesoporous silica,zeolite,porous carbon materials,metal organic frameworks(MOF)and other composite porous materials.In addition,amine functionalized solid adsorbents derived from waste resources are also reviewed because of the large number demand for cost-effective carbon dioxide adsorbents and the processing needs of waste resources.Considering the importance of the stability of the adsorbent in practical applications,advanced research in the capture cycle stability has also been summarized and analyzed.Finally,we summarize the review and offer the recommendations for the development of amine-based solid adsorbents for carbon dioxide capture.
基金Financial support from the Research Council of Norway through project 3GMC (3rd Generation Solvent Membrane Contactor, Project No. 239789)
文摘In the current work five different solvent blends are experimentally studied and the reboiler duties are calculated using the so-called short-cut method.Tertiary amines,2-(diethylamino)ethanol(DEEA),3-(Diethylamino)-1,2-propanediol(DEA-12PD),2-[2-(Diethylamino)ethoxy]ethanol(DEA-EO),1-(2-Hydroxyethyl)piperidine(12HE-PP)are blended with 3-(Methylamino)propylamine(MAPA)and ethanolamine(MEA).The first results from simple solvent screening are given and the cyclic capacities are calculated based data at 40℃ and 80℃.Then,five solvent systems are chosen for vapor–liquid equilibrium characterization.The vapor–liquid equilibrium data are then used to estimate cyclic capacities at more realistic temperatures,between 40℃ and 120℃ and by using a short-cut method proposed in the literature the reboiler duties of the characterized solvents are estimated.Finally,the potential of the studied systems is discussed.Several of the characterized blends showed reboiler duties around 2.5 MJ kgCO2^-1.
文摘Carbon dioxide(CO_(2))capture by gas-separation membranes has become increasingly attractive due to its high energy efficiency,relatively low cost,and environmental impact.Polyvinylamine(PVAm)-based facilitated transport(FT)membranes were developed in the last decade for CO_(2) capture.This work discusses the challenges of applying PVAm-based FT membranes from materials to processes for postcombustion CO_(2) capture in power plants and cement factories.Experiences learned from a pilot demonstration system can be used to guide the design of other membranes for CO_(2) capture.The importance of module and process design is emphasized in the achievement of a high-performance membrane system.Moreover,the results from process simulation and cost estimation indicate that a three-stage membrane system is feasible for achieving a high CO_(2) purity of 95 vol%.The specific CO_(2) capture cost was found to significantly depend on the required CO_(2) capture ratio,and a moderate CO_(2) capture ratio of 50%presented a cost of 63.7USD per tonne CO_(2) captured.Thus,FT membrane systems were found to be more competitive for partial CO_(2) capture.
基金financially supported by National Key R&D Program of China(2019YFE0100100)。
文摘This work presents a simulation study of several Ca-Cu looping variants with CO(2)capture,aiming at both parameter optimization and exergy analysis of these Ca-Cu looping systems.Three kinds of Ca-Cu looping are considered:(1)carbonation-calcination/reduction-oxidation;(2)carbonation-oxidation-calcination/reduction and (3)carbona tion/oxidation-calcination/reduction.A conventional Ca looping is also simulated for comparison.The influences of the calcination temperature on the mole fractions of CO(2)and CaO at the calciner outlet,the CaCO3 flow rate on the carbonator performance and the Cu/Ca ratio on the calciner performance are analyzed.The second kind of Ca-Cu looping has the highest carbonation conversion.At 1×10^5 Pa and 820℃,complete decomposition of CaCO3 can be achieved in three Ca-Cu looping systems,while the operation condition of 1×10^5 Pa,840℃is required for the conventional Ca looping system.Furthermore,the Cu/Ca molar ratio of 5.13-5.19 is required for the Ca-Cu looping.Exergy analyses show that the maximum exergy destruction occurs in the calciner for the four modes and the second Ca-Cu looping system(i.e.,carbonation-oxidation-calcination/reduction)performs the highest exergy efficiency,up to 65.04%,which is about 30%higher than that of the conventional Ca looping.
基金The work was supported by the EU through the project ＂Research and Development in Coal-fired Supercritical Power Plant with Post-combustion Carbon Capture using Process Systems Engineering techniques＂ （Project No. PIRSES-GA-2013-612230） and National Natural Science Foundation of China （61673236）.
文摘This paper presents modelling of a post-combustion CO2 capture process using bootstrap aggregated extreme learning machine （ELM）. ELM randomly assigns the weights between input and hidden layers and obtains the weights between the hidden layer and output layer using regression type approach in one step. This feature allows an ELM model being developed very quickly. This paper proposes using principal component regression to obtain the weights between the hidden and output layers to address the collinearity issue among hidden neuron outputs. Due to the weights between input and hidden layers are randomly assigned, ELM models could have variations in performance. This paper proposes combining multiple ELM models to enhance model prediction accuracy and reliability. To predict the CO2 production rate and CO2 capture level, eight parameters in the process were utilized as model input variables： inlet gas flow rate, CO2 concentration in inlet flow gas, inlet gas temperature, inlet gas pressure, lean solvent flow rate, Jean solvent temperature, lean loading and reboiler duty. The bootstrap re-sampling of training data was applied for building each single ELM and then the individual ELMs are stacked, thereby enhancing the model accuracy and reliability. The bootstrap aggregated extreme learning machine can provide fast learning speed and good generalization performance, which will be used to optimize the CO2 capture process.
基金The National Natural Science Foundation of China(No.51276064)the Natural Science Foundation of Beijing City(No.3132028)
文摘Abstract： Two Canadian limestones with different properties were tested to determine the effect of SO2 during the carbonation of sorbent on the CO2 capture performance in Ca- looping. When the reaction gas is mixed with SO2, the carbonation ratio of the sorbent is always lower than that without SO2 for each cycle under the same conditions, and the sulfation ratio increases almost linearly with the increase in the cycle times. At 650 ℃, there is little difference in the carbonation ratio of the sorbent during the first four cycles for the two carbonation time, 5 and 10 rain at 0. 18% SO2. The indirect sulfation reaction that occurs simultaneously with the carbonation of CaO is responsible for the degradation of the sorbent for CO2 capture, and the carbonation duration is not the main factor that affects the ability of the sorbent. 680℃ is the best carbonation temperature among the three tested temperatures and the highest carbonation ratio can be obtained. Also, the sulfation ratio is the highest. The probable cause is the different effects of temperature on the carbonation rate and sulfation rate. A higher SO2 concentration will decrease the carbonation ratio clearly, but the decrease in the carbonation capability of the sorbent is not proportional to the increase of the SO2 concentration in flue gases.
基金The National Natural Science Foundation of China(No.51376003)
文摘A kind of industrial solid waste, i.e., carbide slag, was used as CaO precursor to synthesize CO2 sorbent. The highly reactive synthetic sorbent was prepared from carbide slag, aluminum nitrate hydrate and glycerol water solution by the combustion synthesis method. The results show that the synthetic sorbent exhibits a much higher CO2 capture capacity compared with carbide slag. The CO2 capture capacity and the carbonation conversion of the synthetic sorbent are 0. 38 g/g and 0. 70 after 50 cycles, which are 1.8 and 2. 1 times those of carbide slag. The average carbonation conversion and the CO2 capture efficiency of the synthetic sorbent are higher than those of carbide slag with the same sorbent flow ratios. The required sorbent flow ratios are lower for synthetic sorbent to achieve the same CO2 capture efficiency compared with carbide slag. With the same sorbent flow ratio and CO2 capture efficiency, the energy requirement in calciner for the synthetic sorbent is less than that for carbide slag.
基金The National Natural Science Foundation of China(No.51476030)the Specialized Research Fund for the Doctoral Program of Higher Education(No.20130092110006)
文摘Abstract： In order to improve the reactivity of Na2CO3/Al2O3 sorbent with CO2, a new sorbent showing high reactivity was developed by doping Na2CO3/Al2O3 with TiO2 using impregnation. Fourteen multi-cycle carbonation/regeneration tests of the sorbent were carried out in a fluidized-bed reactor and the sorbent was characterized by X-ray diffraction and nitrogen adsorption. It is confirmed that TiO2 shows a positive effect on the adsorption process of Na2CO3 and the reaction rate is observed to increase significantly, especially in the first 10 min. Moreover, TiO2 is stable within the temperature range of the process and no other Ti-compounds are detected. The carbonation products are NaHCO3 and Na5H3 （CO3 ）4. The surface area and the pore volume of the sorbent keep stable after 14 cycles. The Fourier transform infrared spectroscopy and the X-ray photoelectron spectroscopy are used to analyze the effect mechanism of TiO2 on CO2 adsorption process of Na2CO3/Al2O3.
基金supported by Shanxi Provincial Key Research and Development Project(202102090301026)Graduate Education Innovation Project of Taiyuan University of Science and Technology(SY2023024)。
文摘Currently,the solid adsorbents with porous structure have been widely applied in CO_(2)capture.However,the unmodified MgO-ZrO_(2)adsorbents appeared to be low adsorption capacity of CO_(2).The solid adsorbent materials were successfully synthesized by loading TEPA onto the pore MgO/ZrO_(2)carriers in the paper.The pore structure and surface characteristic of the samples were analyzed by using XRD,BET,FT-IR and SEM.The adsorbent materials exhibited microcrystalline state,and the crystallinity of all samples gradually decreased as the increase of TEPA content.The pore structure analysis indicated that the modification of MgO-ZrO_(2)adsorbents with TEPA led to the decrease of the specific surface areas,but the narrow micro-mesopore size distributions ranging from 1.8-12 nm in the adsorbents still were maintained.FT-IR spectrum results further verified the successful loading of TEPA.The adsorption capacity of the adsorbents for CO_(2)were tested by using an adsorption apparatus equipped with gas chromatography.The results indicated that when the TEPA loading reached 50%,the sample exhibited the maximum adsorption value for CO_(2),reaching 4.07 mmol/g under the operation condition of 75℃and atmospheric pressure.This result could be assigned to not only the base active sites but also the coexistence of both micropore and mesopore in the adsorbent.After three cycles tests for CO_(2)capture,the adsorption value of the sample for CO_(2)can also reached 95%of its original adsorption capacity,which verified the excellent cyclic operation stability.
基金financial support from the National Key R&D Program of China(2021YFB3801200)the National Natural Science Foundation of China(22278051,22178044,22308043)CNPC Innovation Found(2022DQ02-0608)。
文摘Carbon capture is an important strategy and is implemented to achieve the goals of CO_(2)reduction and carbon neutrality.As a high energy-efficient technology,membrane-based separation plays a crucial role in CO_(2)capture.It is urgently needed for membrane-based CO_(2)capture to develop the high-performance membrane materials with high permeability,selectivity,and stability.Herein,ultrapermeable carbon molecular sieve(CMS)membranes are fabricated by py roly zing a finely-engineered benzoxazole-containing copolyimide precursor for efficient CO_(2)capture.The microstructure of CMS membrane has been optimized by initially engineering the precursor-chemistry and subsequently tuning the pyrolysis process.Deep insights into the structure-property relationship of CMSs are provided in detail by a combination of experimental characterization and molecular simulations.We demonstrate that the intrinsically high free volume environment of the precursor,coupled with the steric hindrance of thermostable contorted fragments,promotes the formation of loosely packed and ultramicroporous carbon structures within the resultant CMS membrane,thereby enabling efficient CO_(2)discrimination via size sieving and affinity.The membrane achieves an ultrahigh CO_(2)permeability,good selectivity,and excellent stability.After one month of long-term operation,the CO_(2)permeability in the mixed gas is maintained at 11,800 Barrer,with a CO_(2)/N_(2)selectivity exceeding 60.This study provides insights into the relationship between precursor-chemistry and CMS performance,and our ultrapermeable CMS membrane,which is scalable using thin film manufacturing,holds great potential for industrial CO_(2)capture.
基金the Natural Science Foundation of Shanghai(23ZR1422600)the Innovative research team of high-level local university in Shanghai for their financial support.
文摘Due to the significant impact of carbon dioxide on global ecology,more efforts have been put into the exploration on CO_(2)capture and utilization.Porous organic framework materials,as a kind of materials with high porosity and designable structure,have been considered as effective host materials for adsorbing carbon dioxide or separating it from other gases.This review gives a deep insight into the applications of metal-organic frameworks,covalent-organic frameworks,and other porous frameworks on CO_(2)capture,focusing on the enhanced capture performances originated from their high surface area with abundant porous structure,functional groups with specific heteroatoms modification,or other building unit interactions.Besides,the main challenges associated with porous frameworks for CO_(2)capture and proposed strategies to address these obstacles,including the structural design strategy or the capture mechanism exploration,have been demonstrated and emphasized.This review can contribute to further investigation on porous frameworks for gas capture and separation with enhanced performance and efficiency.
基金supported by the National Natural Science Foundation of China(No.52100133,No.52222005)the Key R&D Program of Yunnan Province(No.202303AC100008)。
文摘Catalyst-aided regeneration is a promising method for reducing the high regeneration energy consumption of amine-based CO_(2)capture technologies.However,the intrinsic relationship between the properties of the acidic sites and their catalytic activity is controversial.In this study,a series of W-based catalysts supported by ZrTiO_(x)were synthesised,and the effects of the intensity,distribution,and type of acid sites were systematically investigated by quantitatively regulating the acidic site properties.The results indicate stronger acidic sites play a more important role in the catalytic reaction.Moreover,the catalysts showed excellent performance only if the Br?nsted acid sites(BASs)and Lewis acid sites(LASs)coexisted.During the catalytic reaction,the BASs facilitated deprotonation,and the LASs promoted the decomposition of carbamates.The ratio of BASs to LASs(B/L)was a critical factor for catalytic activity,wherein optimal performance was achieved when the B/L ratio was close to 1.The 10%HPW/ZrTiO_(x)composite performed better than WO_(3)/ZrTiO_(x)and HSiW/ZrTiO_(x)because it had a stronger acid intensity and a suitable B/L ratio.As a result,the relative heat duty was reduced by 47%compared to 30%aqueous MEA,and the maximum CO_(2)desorption rate was increased by 83%.The Bader charge indicated that the W atoms of HPW/ZrTiO_(x)lost more electrons(0.18)than those of WO_(3)/ZrTiO_(x),which can weaken the O±H bond energy.Consequently,the calculated deprotonation energy is as low as 257 kJ mol^(-1)for HPW/ZrTiO_(x).
基金supported by the National Natural Science Foundation of China(No.22276064)the Youth Innovation Grant of Xiamen,Fujian Province(No.3502Z20206006)+1 种基金the MOE Key Laboratory of Resources and Environmental System Optimization(No.KLRE-KF202205)Fujian Science and Technology Project(No.2022Y3007).
文摘The non-aqueous solid-liquid biphasic solvent of 2-amino-2-methyl-1-propanol(AMP)/piperazine(PZ)/dipropylene glycol dimethyl ether(DME)features a high CO_(2)absorption loading,favorable phase separation behavior and high regeneration efficiency.Different with the liquid-liquid phase change solvent,the reaction kinetics of CO_(2)capture into solid-liquid biphasic solvent was rarely studied.In the present work,the reaction kinetics of CO_(2)absorption into AMP/PZ/DME solid-liquid biphasic solvent was investigated into the double stirred kettle reactor.The absorption reaction followed a pseudo-first-order kinetic model according to the zwitterion mechanism.The overall reaction rate constant(kov)and the enhancement factor(E)of CO_(2)absorption both increased with increasing temperature.The total mass transfer resistance of the absorbent decreased with increasing temperature and increased with increasing absorption loading,so the higher reaction temperature was conducive to the absorption,and the liquid phase mass transfer resistance was the main factor affecting the absorption rate.
