Temperature-swing adsorption(TSA)is an effective technique for CO_(2) capture,but the temperature swing procedure is energy-intensive.Herein,we report a low-energy-consumption system by combining passive radiative coo...Temperature-swing adsorption(TSA)is an effective technique for CO_(2) capture,but the temperature swing procedure is energy-intensive.Herein,we report a low-energy-consumption system by combining passive radiative cooling and solar heating for the uptake of CO_(2) on commercial activated carbons(CACs).During adsorption,the adsorbents are coated with a layer of hierarchically porous poly(vinylidene fluoride-co-hexafluoropropene)[P(VdF-HFP)HP],which cools the adsorbents to a low temperature under sunlight through radiative cooling.For desorption,CACs with broad absorption of the solar spectrum are exposed to light irradiation for heating.The heating and cooling processes are completely driven by solar energy.Adsorption tests under mimicked sunlight using the CACs show that the performance of this system is comparable to that of the traditional ones.Furthermore,under real sunlight irradiation,the adsorption capacity of the CACs can be well maintained after multiple cycles.The present work may inspire the development of new temperature swing procedures with little energy consumption.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
Carbon capture,utilization and storage(CCUS) is widely recognized as a vital strategy for mitigating the impact of human induced climate change.Among various CO_(2) adsorbents,intermediate-temperature solid adsorbents...Carbon capture,utilization and storage(CCUS) is widely recognized as a vital strategy for mitigating the impact of human induced climate change.Among various CO_(2) adsorbents,intermediate-temperature solid adsorbents have garnered significant attention due to their potential applications in hydrogen utilization,specifically in the water gas shift,steam reforming and gasification processes.These processes are crucial for achieving carbon neutrality.While laboratory-level studies have showcased the high adsorption capacity of these materials via various synthesis and modification methods,their practical application in complex industrial environments remains challenging,impeding the commercialization process.This review aims to critically summarize the recent research progress made in intermediatetemperature(200-400℃) solid CO_(2) adsorbents,particularly focusing on indicators such as cyclability,gas selectivity,and formability,which play vital roles in industrial application scenarios.Additionally,we provide an overview of laboratory-level advanced technologies specifically tailored for industrial applications.Furthermore,we highlight several industrial-ready advanced technologies that can pave the way for overcoming the challenges associated with large-scale implementation.The insights provided by this review aim to assist researchers in identifying the most relevant research directions for industrial applications.By promoting advances in the application of solid adsorbents,we strive to facilitate the ultimate goal of achieving carbon neutrality.展开更多
The capture,regeneration,and conversion of CO_(2) from ambient air and flue gas streams are critical aspects of mitigating global warming.Solid sorbents for CO_(2) absorption are very promising as they have high mass ...The capture,regeneration,and conversion of CO_(2) from ambient air and flue gas streams are critical aspects of mitigating global warming.Solid sorbents for CO_(2) absorption are very promising as they have high mass transfer areas without energy input and reduce emissions and minimize corrosion as compared to liquid sorbents.However,precisely tunable solid CO_(2) sorbents are difficult to produce.Here,we demonstrate the high-throughput production of hydrogel-based CO_(2)-absorbing particles via liquid jetting.By wrapping a liquid jet consisting of an aqueous solution of cross-linkable branched polyethylenimine(PEI)with a layer of suspension containing hydrophobic silica nanoparticles,monodisperse droplets with a silica nanoparticle coating layer was formed in the air.A stable Pickering emulsion containing PEI droplets was obtained after these ejected droplets were collected in a heated oil bath.The droplets turn into mm-sized particles after thermal curing in the bath.The diameter,PEI content,and silica content of the particles were systematically varied,and their CO_(2) absorption was measured as a function of time.Steam regeneration of the particles enabled cyclic testing,revealing a CO_(2) absorption capacity of 6.5±0.5 mol kg^(−1)solid PEI in pure CO_(2) environments and 0.7±0.3 mol kg^(−1)solid PEI for direct air capture.Several thousands of particles were produced per second at a rate of around 0.5 kg per hour,with a single nozzle.This process can be further scaled by parallelization.The complete toolbox for the design,fabrication,testing,and regeneration of functional hydrogel particles provides a powerful route toward novel solid sorbents for regenerative CO_(2) capture.展开更多
Carbon nanotubes(CNTs)have garnered significant attention in the fields of science,engineering,and medicine due to their numerous advantages.The initial step towards harnessing the potential of CNTs involves their mac...Carbon nanotubes(CNTs)have garnered significant attention in the fields of science,engineering,and medicine due to their numerous advantages.The initial step towards harnessing the potential of CNTs involves their macroscopic assembly.The present study employed a gentle and direct self-assembly technique,wherein controlled growth of CNT sheaths occurred on the metal wire’s surface,followed by etching of the remaining metal to obtain the hollow tubes composed of CNTs.By controlling the growth time and temperature,it is possible to alter the thickness of the CNTs sheath.After immersing in a solution containing 1 g/L of CNTs at 60℃ for 24 h,the resulting CNTs layer achieved a thickness of up to 60μm.These hollow CNTs tubes with varying inner diameters were prepared through surface reinforcement using polymers and sacrificing metal wires,thereby exhibiting exceptional attributes such as robustness,flexibility,air tightness,and high adsorption capacity that effectively capture CO_(2) from the gas mixture.展开更多
For the application of carbon capture by membrane process,it is crucial to develop a highly permeable CO_(2)-selective membrane.In this work,we reported an ultra-thin polyether-block-amide(Pebax)mixedmatrix membranes(...For the application of carbon capture by membrane process,it is crucial to develop a highly permeable CO_(2)-selective membrane.In this work,we reported an ultra-thin polyether-block-amide(Pebax)mixedmatrix membranes(MMMs)incorporated by graphene oxide(GO),in which the interlayer channels were regulated to optimize the CO_(2)/N_(2) separation performance.Various membrane preparation conditions were systematically investigated on the influence of the membrane structure and separation performance,including the lateral size of GO nanosheets,GO loading,thermal reduction temperature,and time.The results demonstrated that the precisely regulated interlayer channel of GO nanosheets can rapidly provide CO_(2)-selective transport channels due to the synergetic effects of size sieving and preferential adsorption.The GO/Pebax ultra-thin MMMs exhibited CO_(2)/N_(2) selectivity of 72 and CO_(2) permeance of 400 GPU(1 GPU=106 cm^(3)(STP)·cm^(2)·s^(-1)·cmHg^(-1)),providing a promising candidate for CO_(2) capture.展开更多
Dendritic mesoporous silica nanoparticles own three-dimensional center-radial channels and hierarchical pores,which endows themselves with super-high specific surface area,extremely large pore volumes,especially acces...Dendritic mesoporous silica nanoparticles own three-dimensional center-radial channels and hierarchical pores,which endows themselves with super-high specific surface area,extremely large pore volumes,especially accessible internal spaces,and so forth.Dissimilar guest species(such as organic groups or metal nanoparticles)could be readily decorated onto the interfaces of the channels and pores,realizing the functionalization of dendritic mesoporous silica nanoparticles for targeted applications.As adsorbents and catalysts,dendritic mesoporous silica nanoparticles-based materials have experienced nonignorable development in CO_(2)capture and catalytic conversion.This comprehensive review provides a critical survey on this pregnant subject,summarizing the designed construction of novel dendritic mesoporous silica nanoparticles-based materials,the involved chemical reactions(such as CO_(2)methanation,dry reforming of CH_(4)),the value-added chemicals from CO_(2)(such as cyclic carbonates,2-oxazolidinones,quinazoline-2,4(1H,3H)-diones),and so on.The adsorptive and catalytic performances have been compared with traditional silica mesoporous materials(such as SBA-15 or MCM-41),and the corresponding reaction mechanisms have been thoroughly revealed.It is sincerely expected that the in-depth discussion could give materials scientists certain inspiration to design brand-new dendritic mesoporous silica nanoparticles-based materials with superior capabilities towards CO_(2)capture,utilization,and storage.展开更多
Chemical looping combustion has the potential to be an efficient and low-cost technology capable of contributing to the reduction of the atmospheric concentration of CO_(2) in order to reach the 1.5/2°C goal and ...Chemical looping combustion has the potential to be an efficient and low-cost technology capable of contributing to the reduction of the atmospheric concentration of CO_(2) in order to reach the 1.5/2°C goal and mitigate climate change.In this process,a metal oxide is used as oxygen carrier in a dual fluidized bed to generate clean CO_(2) via combustion of biomass.Most commonly,natural ores or synthetic materials are used as oxygen carrier whereas both must meet special requirements for the conversion of solid fuels.Synthetic oxygen carriers are characterized by higher reactivity at the expense of higher costs versus the lower-cost natural ores.To determine the viability of both possibilities,a techno-economic comparison of a synthetic material based on manganese,iron,and copper to the natural ore ilmenite was conducted.The synthetic oxygen carrier was characterized and tested in a pilot plant,where high combustion efficiencies up to 98.4%and carbon capture rates up to 98.5%were reached.The techno-economic assessment resulted in CO_(2) capture costs of 75 and 40€/tCO_(2) for the synthetic and natural ore route respectively,whereas a sensitivity analysis showed the high impact of production costs and attrition rates of the synthetic material.The synthetic oxygen carrier could break even with the natural ore in case of lower production costs and attrition rates,which could be reached by adapting the production process and recycling material.By comparison to state-of-the-art technologies,it is demonstrated that both routes are viable and the capture cost of CO_(2) could be reduced by implementing the chemical looping combustion technology.展开更多
Emerging excessive greenhouse gas emissions pose great threats to the ecosystem,which thus requires efficient CO_(2)capture to mitigate the disastrous issue.In this report,large molecular size bisphenol A ethoxylate d...Emerging excessive greenhouse gas emissions pose great threats to the ecosystem,which thus requires efficient CO_(2)capture to mitigate the disastrous issue.In this report,large molecular size bisphenol A ethoxylate diacrylate(BPA)was employed to crosslink poly(ethylene glycol)methyl ether acrylate(PEGMEA)via the green and rapid UV polymerization strategy.The microstructure of such-prepared membrane could be conveniently tailored by tuning the ratio of the two prepolymers,aiming at obtaining the optimized microstructures with suitable mesh size and PEO sol content,which was approved by a novel low-field nuclear magnetic resonance technique.The optimum membrane overcomes the tradeoff challenge:dense microstructures lower the gas permeability while loose microstructures lower high-pressure-resistance capacity,realizing a high CO_(2)permeability of 1711 Barrer and 100-h long-term running stability under 15 atm.The proposed membrane fabrication approach,hence,opens a novel gate for developing high-performance robust membranes for CO_(2)capture.展开更多
An integrated vacuum pressure swing adsorption(VPSA) and Rectisol process is proposed for CO_(2) capture from underground coal gasification(UCG) syngas. A ten-bed VPSA process with silica gel adsorbent is firstly desi...An integrated vacuum pressure swing adsorption(VPSA) and Rectisol process is proposed for CO_(2) capture from underground coal gasification(UCG) syngas. A ten-bed VPSA process with silica gel adsorbent is firstly designed to pre-separate and capture 74.57% CO_(2) with a CO_(2) purity of 98.35% from UCG syngas(CH_(4)/CO/CO_(2)/H_(2)/N_(2)= 30.77%/6.15%/44.10%/18.46%/0.52%, mole fraction, from Shaar Lake Mine Field,Xinjiang Province, China) with a feed pressure of 3.5 MPa. Subsequently, the Rectisol process is constructed to furtherly remove and capture the residual CO_(2)remained in light product gas from the VPSA process using cryogenic methanol(233.15 K, 100%(mass)) as absorbent. A final purified gas with CO_(2) concentration lower than 3% and a regenerated CO_(2) product with CO_(2) purity higher than 95% were achieved by using the Rectisol process. Comparisons indicate that the energy consumption is deceased from 2.143 MJ·kg^(-1) of the single Rectisol process to 1.008 MJ·kg^(-1) of the integrated VPSA & Rectisol process, which demonstrated that the deployed VPSA was an energy conservation process for CO_(2) capture from UCG syngas. Additionally, the high-value gas(e.g., CH_(4)) loss can be decreased and the effects of key operating parameters on the process performances were detailed.展开更多
High-quality standard oil synthetic zeolite-13(SSZ-13) membranes with thickness only ~ 1.0 μm were prepared on tubular supports by the new seeded-gel approach. Seeded-gel approach is simpler than the normal secondary...High-quality standard oil synthetic zeolite-13(SSZ-13) membranes with thickness only ~ 1.0 μm were prepared on tubular supports by the new seeded-gel approach. Seeded-gel approach is simpler than the normal secondary-growth one since adding seeds in the gel is simpler than seeding on the support surface. The synthesis time was greatly reduced from 3.0 to 1.0 d after synthesis modification of gel aging and seed sizes. Low temperature ozone calcination was used for the removal of the organic structural directing agent. The best SSZ-13 membrane displayed CO_(2)permeances of 1.3 × 10^(-6) and 1.5 × 10^(-6) mol·m^(-2)·s^(-1)·Pa^(-1) and CO_(2)/CH_(4) and CO_(2)/N_(2) selectivities of 125 and 27 for equimolar CO_(2)/CH_(4) and CO_(2)/N2mixtures at 0.2 MPa pressure drop and 298 K, respectively. Separation performance of the membrane in the two binary mixtures is higher than that of most zeolite membranes. Three SSZ-13 membranes were reproducibly prepared on tubular supports by seeded-gel approach and the standard deviation ratios of CO_(2) permeance and CO_(2)/CH_(4) selectivity are 12.5% and 7%, respectively. It suggests that this new synthesis approach is creditable. The effects of temperature and pressure on separation performance of the thin SSZ-13 membranes were studied in the two binary mixtures. The tubular SSZ-13 membranes displayed great potentials for CO_(2) capture from natural gas, biogas and flue gas.展开更多
Developing metal-organic framework(MOF)materials with the moisture-resistant feature is highly desirable for CO_(2)capture from highly humid flue gas.In this work,a new core-shell MOF@MOF composite using Mg-MOF-74 wit...Developing metal-organic framework(MOF)materials with the moisture-resistant feature is highly desirable for CO_(2)capture from highly humid flue gas.In this work,a new core-shell MOF@MOF composite using Mg-MOF-74 with high CO_(2)capture capacity as a functional core and hydrophobic zeolitic imidazolate framework-8(ZIF-8)as a protective shell is fabricated by the epitaxial growth method.Experimental results show that the CO_(2)adsorption performance of the core-shell structured Mg-MOF-74@ZIF-8 composites from water-containing flue gas is enhanced along with their improved hydrophobicity.The dynamic breakthrough results show that the Mg-MOF-74@ZIF-8 with three assembled layers(Mg-MOF-74@ZIF-8-3)can capture 3.56 mmol-g^(-1)CO_(2)from wet CO_(2)/N_(2)(VCO_(2):V_(N_(2))=15:85)mixtures,which outperforms Mg-MOF-74(0.37 mmol·g^(-1))and most of the reported physisorbents.展开更多
The absorber is the key unit in the post-combustion monoethanolamine(MEA)-based carbon dioxide(CO_(2))capture process.A rate-based dynamic model for the absorber is developed and validated using steady-state experimen...The absorber is the key unit in the post-combustion monoethanolamine(MEA)-based carbon dioxide(CO_(2))capture process.A rate-based dynamic model for the absorber is developed and validated using steady-state experimental data reported in open literature.Sensitivity analysis is performed with respect to important model parameters associated with the reaction,mass transport and phy-sical property relationships.Then,a singular value decomposition(SVD)-based subspace parameter estimation method is proposed to improve the model accu-racy.Finally,dynamic simulations are carried out to investigate the effects of the feed rate of lean MEA solution and the flue inlet conditions.Simulation results indicate that the established dynamic model can reasonably reflect the physical behavior of the absorber.Some new insights are gained from the simulation results.展开更多
基金supported by the National Science Fund for Distinguished Young Scholars(22125804)the National Natural Science Foundation of China(21808110,22078155,and 21878149).
文摘Temperature-swing adsorption(TSA)is an effective technique for CO_(2) capture,but the temperature swing procedure is energy-intensive.Herein,we report a low-energy-consumption system by combining passive radiative cooling and solar heating for the uptake of CO_(2) on commercial activated carbons(CACs).During adsorption,the adsorbents are coated with a layer of hierarchically porous poly(vinylidene fluoride-co-hexafluoropropene)[P(VdF-HFP)HP],which cools the adsorbents to a low temperature under sunlight through radiative cooling.For desorption,CACs with broad absorption of the solar spectrum are exposed to light irradiation for heating.The heating and cooling processes are completely driven by solar energy.Adsorption tests under mimicked sunlight using the CACs show that the performance of this system is comparable to that of the traditional ones.Furthermore,under real sunlight irradiation,the adsorption capacity of the CACs can be well maintained after multiple cycles.The present work may inspire the development of new temperature swing procedures with little energy consumption.
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funded by the National Key R&D Program of China(2022YFB4101702)the National Natural Science Foundation of China(52106072 and 52225003)the Fundamental Research Funds for Central Universities(2019JQ03015)。
文摘Carbon capture,utilization and storage(CCUS) is widely recognized as a vital strategy for mitigating the impact of human induced climate change.Among various CO_(2) adsorbents,intermediate-temperature solid adsorbents have garnered significant attention due to their potential applications in hydrogen utilization,specifically in the water gas shift,steam reforming and gasification processes.These processes are crucial for achieving carbon neutrality.While laboratory-level studies have showcased the high adsorption capacity of these materials via various synthesis and modification methods,their practical application in complex industrial environments remains challenging,impeding the commercialization process.This review aims to critically summarize the recent research progress made in intermediatetemperature(200-400℃) solid CO_(2) adsorbents,particularly focusing on indicators such as cyclability,gas selectivity,and formability,which play vital roles in industrial application scenarios.Additionally,we provide an overview of laboratory-level advanced technologies specifically tailored for industrial applications.Furthermore,we highlight several industrial-ready advanced technologies that can pave the way for overcoming the challenges associated with large-scale implementation.The insights provided by this review aim to assist researchers in identifying the most relevant research directions for industrial applications.By promoting advances in the application of solid adsorbents,we strive to facilitate the ultimate goal of achieving carbon neutrality.
基金supported by the European Regional Development Fund(CONTROL,EFRO#00943).
文摘The capture,regeneration,and conversion of CO_(2) from ambient air and flue gas streams are critical aspects of mitigating global warming.Solid sorbents for CO_(2) absorption are very promising as they have high mass transfer areas without energy input and reduce emissions and minimize corrosion as compared to liquid sorbents.However,precisely tunable solid CO_(2) sorbents are difficult to produce.Here,we demonstrate the high-throughput production of hydrogel-based CO_(2)-absorbing particles via liquid jetting.By wrapping a liquid jet consisting of an aqueous solution of cross-linkable branched polyethylenimine(PEI)with a layer of suspension containing hydrophobic silica nanoparticles,monodisperse droplets with a silica nanoparticle coating layer was formed in the air.A stable Pickering emulsion containing PEI droplets was obtained after these ejected droplets were collected in a heated oil bath.The droplets turn into mm-sized particles after thermal curing in the bath.The diameter,PEI content,and silica content of the particles were systematically varied,and their CO_(2) absorption was measured as a function of time.Steam regeneration of the particles enabled cyclic testing,revealing a CO_(2) absorption capacity of 6.5±0.5 mol kg^(−1)solid PEI in pure CO_(2) environments and 0.7±0.3 mol kg^(−1)solid PEI for direct air capture.Several thousands of particles were produced per second at a rate of around 0.5 kg per hour,with a single nozzle.This process can be further scaled by parallelization.The complete toolbox for the design,fabrication,testing,and regeneration of functional hydrogel particles provides a powerful route toward novel solid sorbents for regenerative CO_(2) capture.
基金Project(ZCLTGS24B0101)supported by Zhejiang Provincial Natural Science Foundation of ChinaProject(Y202250501)supported by Scientific Research Fund of Zhejiang Provincial Education Department,ChinaProject supported by SRT Research Project of Jiaxing Nanhu University,China。
文摘Carbon nanotubes(CNTs)have garnered significant attention in the fields of science,engineering,and medicine due to their numerous advantages.The initial step towards harnessing the potential of CNTs involves their macroscopic assembly.The present study employed a gentle and direct self-assembly technique,wherein controlled growth of CNT sheaths occurred on the metal wire’s surface,followed by etching of the remaining metal to obtain the hollow tubes composed of CNTs.By controlling the growth time and temperature,it is possible to alter the thickness of the CNTs sheath.After immersing in a solution containing 1 g/L of CNTs at 60℃ for 24 h,the resulting CNTs layer achieved a thickness of up to 60μm.These hollow CNTs tubes with varying inner diameters were prepared through surface reinforcement using polymers and sacrificing metal wires,thereby exhibiting exceptional attributes such as robustness,flexibility,air tightness,and high adsorption capacity that effectively capture CO_(2) from the gas mixture.
基金financially supported by The Natural Science Foundation of the Jiangsu Higher Education Institutions of China(22KJB530007,22KJA530001)National Natural Science Foundation of China(22208151)+1 种基金the Natural Science Foundation of Jiangsu Province(BK20220002)the State Key Laboratory of MaterialsOriented Chemical Engineering(SKL-MCE-22B07).
文摘For the application of carbon capture by membrane process,it is crucial to develop a highly permeable CO_(2)-selective membrane.In this work,we reported an ultra-thin polyether-block-amide(Pebax)mixedmatrix membranes(MMMs)incorporated by graphene oxide(GO),in which the interlayer channels were regulated to optimize the CO_(2)/N_(2) separation performance.Various membrane preparation conditions were systematically investigated on the influence of the membrane structure and separation performance,including the lateral size of GO nanosheets,GO loading,thermal reduction temperature,and time.The results demonstrated that the precisely regulated interlayer channel of GO nanosheets can rapidly provide CO_(2)-selective transport channels due to the synergetic effects of size sieving and preferential adsorption.The GO/Pebax ultra-thin MMMs exhibited CO_(2)/N_(2) selectivity of 72 and CO_(2) permeance of 400 GPU(1 GPU=106 cm^(3)(STP)·cm^(2)·s^(-1)·cmHg^(-1)),providing a promising candidate for CO_(2) capture.
基金supported by the National Key R&D program of China(2019YFA0706802)National Natural Science Foundation of China(52063029)+2 种基金Natural Science Basic Research Program of Shaanxi(2022JM-200,2021JQ-716)China Postdoctoral Science Foundation(2020M672269)Doctoral Research Program of Yan’an University(YDBK2019-02)
文摘Dendritic mesoporous silica nanoparticles own three-dimensional center-radial channels and hierarchical pores,which endows themselves with super-high specific surface area,extremely large pore volumes,especially accessible internal spaces,and so forth.Dissimilar guest species(such as organic groups or metal nanoparticles)could be readily decorated onto the interfaces of the channels and pores,realizing the functionalization of dendritic mesoporous silica nanoparticles for targeted applications.As adsorbents and catalysts,dendritic mesoporous silica nanoparticles-based materials have experienced nonignorable development in CO_(2)capture and catalytic conversion.This comprehensive review provides a critical survey on this pregnant subject,summarizing the designed construction of novel dendritic mesoporous silica nanoparticles-based materials,the involved chemical reactions(such as CO_(2)methanation,dry reforming of CH_(4)),the value-added chemicals from CO_(2)(such as cyclic carbonates,2-oxazolidinones,quinazoline-2,4(1H,3H)-diones),and so on.The adsorptive and catalytic performances have been compared with traditional silica mesoporous materials(such as SBA-15 or MCM-41),and the corresponding reaction mechanisms have been thoroughly revealed.It is sincerely expected that the in-depth discussion could give materials scientists certain inspiration to design brand-new dendritic mesoporous silica nanoparticles-based materials with superior capabilities towards CO_(2)capture,utilization,and storage.
文摘Chemical looping combustion has the potential to be an efficient and low-cost technology capable of contributing to the reduction of the atmospheric concentration of CO_(2) in order to reach the 1.5/2°C goal and mitigate climate change.In this process,a metal oxide is used as oxygen carrier in a dual fluidized bed to generate clean CO_(2) via combustion of biomass.Most commonly,natural ores or synthetic materials are used as oxygen carrier whereas both must meet special requirements for the conversion of solid fuels.Synthetic oxygen carriers are characterized by higher reactivity at the expense of higher costs versus the lower-cost natural ores.To determine the viability of both possibilities,a techno-economic comparison of a synthetic material based on manganese,iron,and copper to the natural ore ilmenite was conducted.The synthetic oxygen carrier was characterized and tested in a pilot plant,where high combustion efficiencies up to 98.4%and carbon capture rates up to 98.5%were reached.The techno-economic assessment resulted in CO_(2) capture costs of 75 and 40€/tCO_(2) for the synthetic and natural ore route respectively,whereas a sensitivity analysis showed the high impact of production costs and attrition rates of the synthetic material.The synthetic oxygen carrier could break even with the natural ore in case of lower production costs and attrition rates,which could be reached by adapting the production process and recycling material.By comparison to state-of-the-art technologies,it is demonstrated that both routes are viable and the capture cost of CO_(2) could be reduced by implementing the chemical looping combustion technology.
基金This research was financially supported by National Natural Science Foundation of China(No.22125801,21975005,21878004)Cooperative Research Project of BJUT-NTUT(No.110-03).
文摘Emerging excessive greenhouse gas emissions pose great threats to the ecosystem,which thus requires efficient CO_(2)capture to mitigate the disastrous issue.In this report,large molecular size bisphenol A ethoxylate diacrylate(BPA)was employed to crosslink poly(ethylene glycol)methyl ether acrylate(PEGMEA)via the green and rapid UV polymerization strategy.The microstructure of such-prepared membrane could be conveniently tailored by tuning the ratio of the two prepolymers,aiming at obtaining the optimized microstructures with suitable mesh size and PEO sol content,which was approved by a novel low-field nuclear magnetic resonance technique.The optimum membrane overcomes the tradeoff challenge:dense microstructures lower the gas permeability while loose microstructures lower high-pressure-resistance capacity,realizing a high CO_(2)permeability of 1711 Barrer and 100-h long-term running stability under 15 atm.The proposed membrane fabrication approach,hence,opens a novel gate for developing high-performance robust membranes for CO_(2)capture.
基金financially supported by the Renewable Energy and Hydrogen Projects in National Key Research & Development Program of China (2019YFB1505000)。
文摘An integrated vacuum pressure swing adsorption(VPSA) and Rectisol process is proposed for CO_(2) capture from underground coal gasification(UCG) syngas. A ten-bed VPSA process with silica gel adsorbent is firstly designed to pre-separate and capture 74.57% CO_(2) with a CO_(2) purity of 98.35% from UCG syngas(CH_(4)/CO/CO_(2)/H_(2)/N_(2)= 30.77%/6.15%/44.10%/18.46%/0.52%, mole fraction, from Shaar Lake Mine Field,Xinjiang Province, China) with a feed pressure of 3.5 MPa. Subsequently, the Rectisol process is constructed to furtherly remove and capture the residual CO_(2)remained in light product gas from the VPSA process using cryogenic methanol(233.15 K, 100%(mass)) as absorbent. A final purified gas with CO_(2) concentration lower than 3% and a regenerated CO_(2) product with CO_(2) purity higher than 95% were achieved by using the Rectisol process. Comparisons indicate that the energy consumption is deceased from 2.143 MJ·kg^(-1) of the single Rectisol process to 1.008 MJ·kg^(-1) of the integrated VPSA & Rectisol process, which demonstrated that the deployed VPSA was an energy conservation process for CO_(2) capture from UCG syngas. Additionally, the high-value gas(e.g., CH_(4)) loss can be decreased and the effects of key operating parameters on the process performances were detailed.
基金Financial supports from the National Natural Science Foundation of China (21921006, 21938007 and 21576131)the open project of the State Key Laboratory of Materials-Oriented Chemical Engineering of China (KL21-04)。
文摘High-quality standard oil synthetic zeolite-13(SSZ-13) membranes with thickness only ~ 1.0 μm were prepared on tubular supports by the new seeded-gel approach. Seeded-gel approach is simpler than the normal secondary-growth one since adding seeds in the gel is simpler than seeding on the support surface. The synthesis time was greatly reduced from 3.0 to 1.0 d after synthesis modification of gel aging and seed sizes. Low temperature ozone calcination was used for the removal of the organic structural directing agent. The best SSZ-13 membrane displayed CO_(2)permeances of 1.3 × 10^(-6) and 1.5 × 10^(-6) mol·m^(-2)·s^(-1)·Pa^(-1) and CO_(2)/CH_(4) and CO_(2)/N_(2) selectivities of 125 and 27 for equimolar CO_(2)/CH_(4) and CO_(2)/N2mixtures at 0.2 MPa pressure drop and 298 K, respectively. Separation performance of the membrane in the two binary mixtures is higher than that of most zeolite membranes. Three SSZ-13 membranes were reproducibly prepared on tubular supports by seeded-gel approach and the standard deviation ratios of CO_(2) permeance and CO_(2)/CH_(4) selectivity are 12.5% and 7%, respectively. It suggests that this new synthesis approach is creditable. The effects of temperature and pressure on separation performance of the thin SSZ-13 membranes were studied in the two binary mixtures. The tubular SSZ-13 membranes displayed great potentials for CO_(2) capture from natural gas, biogas and flue gas.
基金supported by the National Natural Science Foundation of China(51772329,51972340,and 51825201)。
文摘Developing metal-organic framework(MOF)materials with the moisture-resistant feature is highly desirable for CO_(2)capture from highly humid flue gas.In this work,a new core-shell MOF@MOF composite using Mg-MOF-74 with high CO_(2)capture capacity as a functional core and hydrophobic zeolitic imidazolate framework-8(ZIF-8)as a protective shell is fabricated by the epitaxial growth method.Experimental results show that the CO_(2)adsorption performance of the core-shell structured Mg-MOF-74@ZIF-8 composites from water-containing flue gas is enhanced along with their improved hydrophobicity.The dynamic breakthrough results show that the Mg-MOF-74@ZIF-8 with three assembled layers(Mg-MOF-74@ZIF-8-3)can capture 3.56 mmol-g^(-1)CO_(2)from wet CO_(2)/N_(2)(VCO_(2):V_(N_(2))=15:85)mixtures,which outperforms Mg-MOF-74(0.37 mmol·g^(-1))and most of the reported physisorbents.
基金The work was financially supported by Basic Public Welfare research Plan of Zhejiang Province(LGG19F030006)Key Laboratory of Intelligent Manufacturing Quality Big Data Tracing and Analysis of Zhejiang Province,China Jiliang University(Grant No.ZNZZSZ–CJLU2022–04)the Key Research and Development Program of Ningbo(2022Z165).
文摘The absorber is the key unit in the post-combustion monoethanolamine(MEA)-based carbon dioxide(CO_(2))capture process.A rate-based dynamic model for the absorber is developed and validated using steady-state experimental data reported in open literature.Sensitivity analysis is performed with respect to important model parameters associated with the reaction,mass transport and phy-sical property relationships.Then,a singular value decomposition(SVD)-based subspace parameter estimation method is proposed to improve the model accu-racy.Finally,dynamic simulations are carried out to investigate the effects of the feed rate of lean MEA solution and the flue inlet conditions.Simulation results indicate that the established dynamic model can reasonably reflect the physical behavior of the absorber.Some new insights are gained from the simulation results.