The development of dual functional material for cyclic CO_(2)capture and hydrogenation is of great significance for converting diluted CO_(2)into valuable fuels,but suffers from kinetic limitation and deactivation of ...The development of dual functional material for cyclic CO_(2)capture and hydrogenation is of great significance for converting diluted CO_(2)into valuable fuels,but suffers from kinetic limitation and deactivation of adsorbent and catalyst.Herein,we engineered a series of RuNa/γ-Al_(2)O_(3)materials,varying the size of ruthenium from single atoms to clusters/nanoparticles.The coordination environment and structure sensitivity of ruthenium were quantitatively investigated at atomic scale.Our findings reveal that the reduced Ru nanoparticles,approximately 7.1 nm in diameter with a Ru-Ru coordination number of 5.9,exhibit high methane formation activity and selectivity at 340°C.The Ru-Na interfacial sites facilitate CO_(2)migration through a deoxygenation pathway,involving carbonate dissociation,carbonyl formation,and hydrogenation.In-situ experiments and theoretical calculations show that stable carbonyl intermediates on metallic Ru nanoparticles facilitate heterolytic C–O scission and C–H bonding,significantly lowering the energy barrier for activating stored CO_(2).展开更多
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
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
Ammonia(NH3)is a carbon-free,hydrogen-rich chemical related to global food safety,clean energy,and environmental protection.As an essential technology for meeting the requirements raised by such issues,NH3 capture has...Ammonia(NH3)is a carbon-free,hydrogen-rich chemical related to global food safety,clean energy,and environmental protection.As an essential technology for meeting the requirements raised by such issues,NH3 capture has been intensively explored by researchers in both fundamental and applied fields.The four typical methods used are(1)solvent absorption by ionic liquids and their derivatives,(2)adsorption by porous solids,(3)abadsorption by porous liquids,and(4)membrane separation.Rooted in the development of advanced materials for NH3 capture,we conducted a coherent review of the design of different materials,mainly in the past 5 years,their interactions with NH3 molecules and construction of transport pathways,as well as the structure–property relationship,with specific examples discussed.Finally,the challenges in current research and future worthwhile directions for NH3 capture materials are proposed.展开更多
Industrial thin-film composite(TFC)membranes achieve superior gas separation properties from high-performance selective layer materials,while the success of membrane technology relies on high-performance gutter layers...Industrial thin-film composite(TFC)membranes achieve superior gas separation properties from high-performance selective layer materials,while the success of membrane technology relies on high-performance gutter layers to achieve production scalability and low-cost manufacturing.However,the current literature predominantly focuses on the design of polymer architectures to obtain high permeability and selectivity,while the art of fabricating gutter layers is usually safeguarded by industrial manufacturers and appears lackluster to academic researchers.This is the first report aiming to provide a comprehensive and critical review of state-of-the-art gutter layer materials and their design and modification to enable TFC membranes with superior separation performance.We first elucidate the importance of the gutter layer on membrane performance through modeling and experimental results.Then various gutter layer materials used to obtain high-performance composite membranes are critically reviewed,and the strategies to improve their compatibility with the selective layer are highlighted,such as oxygen plasma treatment,polydopamine deposition,and surface grafting.Finally,we present the opportunities of the gutter layer design for practical applications.展开更多
As a prominent contributor to air pollution,nitric oxide(NO)has emerged as a critical agent causing detrimental environmental and health ramifications.To mitigate emissions and facilitate downstream utilization,adsorp...As a prominent contributor to air pollution,nitric oxide(NO)has emerged as a critical agent causing detrimental environmental and health ramifications.To mitigate emissions and facilitate downstream utilization,adsorption-based techniques offer a compelling approach for direct NO capture from both stationary and mobile sources.In this study,a comprehensive exploration of NO capture under oxygen-lean and oxygenrich conditions was conducted,employing Ni ion-exchanged chabazite(CHA-type)zeolites as the adsorbents.Remarkably,Ni/Na-CHA zeolites,with Ni loadings ranging from 3 to 4 wt%,demonstrate remarkable dynamic uptake capacities and exhibit exceptional NO capture efficiencies(NO-to-Ni ratio)for both oxygen-lean(0.17-0.31 mmol/g,0.32-0.43 of NO/Ni)and oxygen-rich(1.64-1.18 mmol/g)under ambient conditions.An NH3 reduction methodology was designed for the regeneration of absorbents at a relatively low temperature of 673 K.Comprehensive insights into the NO_(x) adsorption mechanism were obtained through temperature-programmed desorption experiments,in situ Fourier transform infrared spectroscopy,and density functional theory calculations.It is unveiled that NO and NO_(2) exhibit propensity to coordinate with Ni^(2+) via N-terminal or O-terminal,yielding thermally stable complexes and metastable species,respectively,while the low-temperature desorption substances are generated in close proximity to Na^(+).This study not only offers micro-level perspectives but imparts crucial insights for the advancement of capture and reduction technologies utilizing precious-metal-free materials.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
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
This paper presented a novel tinny motion capture system for measuring bird posture based on inertial and magnetic measurement units that are made up of micromachined gyroscopes, accelerometers, and magnetometers. Mul...This paper presented a novel tinny motion capture system for measuring bird posture based on inertial and magnetic measurement units that are made up of micromachined gyroscopes, accelerometers, and magnetometers. Multiple quaternion-based extended Kalman filters were implemented to estimate the absolute orientations to achieve high accuracy.Under the guidance of ornithology experts, the extending/contracting motions and flapping cycles were recorded using the developed motion capture system, and the orientation of each bone was also analyzed. The captured flapping gesture of the Falco peregrinus is crucial to the motion database of raptors as well as the bionic design.展开更多
Direct air capture(DAC)of CO_(2)plays an indispensable role in achieving carbon-neutral goals as one of the key negative emission technologies.Since large air flows are required to capture the ultradilute CO_(2)from t...Direct air capture(DAC)of CO_(2)plays an indispensable role in achieving carbon-neutral goals as one of the key negative emission technologies.Since large air flows are required to capture the ultradilute CO_(2)from the air,lab-synthesized adsorbents in powder form may cause unacceptable gas pressure drops and poor heat and mass transfer efficiencies.A structured adsorbent is essential for the implementation of gas-solid contactors for cost-and energy-efficient DAC systems.In this study,efficient adsorbent poly(ethyleneimine)(PEI)-functionalized Mg-Al-CO_(3)layered double hydroxide(LDH)-derived mixed metal oxides(MMOs)are three-dimensional(3D)printed into monoliths for the first time with more than 90%adsorbent loadings.The printing process has been optimized by initially printing the LDH powder into monoliths followed by calcination into MMO monoliths.This structure exhibits a 32.7%higher specific surface area and a 46.1%higher pore volume,as compared to the direct printing of the MMO powder into a monolith.After impregnation of PEI,the monolith demonstrates a large adsorption capacity(1.82 mmol/g)and fast kinetics(0.7 mmol/g/h)using a CO_(2)feed gas at 400 ppm at 25℃,one of the highest values among the shaped DAC adsorbents.Smearing of the amino-polymers during the post-printing process affects the diffusion of CO_(2),resulting in slower adsorption kinetics of pre-impregnation monoliths compared to post-impregnation monoliths.The optimal PEI/MeOH ratio for the post-impregnation solution prevents pores clogging that would affect both adsorption capacity and kinetics.展开更多
This work demonstrates a micron-sized nanosecond current pulse probe using a quantum diamond magnetometer.A micron-sized diamond crystal affixed to a fiber tip is integrated on the end of a conical waveguide.We demons...This work demonstrates a micron-sized nanosecond current pulse probe using a quantum diamond magnetometer.A micron-sized diamond crystal affixed to a fiber tip is integrated on the end of a conical waveguide.We demonstrate real-time visualization of a single 100 nanosecond pulse and discrimination of two pulse trains of different frequencies with a coplanar waveguide and a home-made PCB circuit.This technique finds promising applications in the display of electronic stream and can be used as a pulse discriminator to simultaneously receive and demodulate multiple pulse frequencies.This method of detecting pulse current is expected to provide further detailed analysis of the internal working state of the chip.展开更多
To ensure project safety and secure public support, an integrated and comprehensive monitoring program is needed within a carbon capture and storage(CCS) project. Monitoring can be done using many well-established tec...To ensure project safety and secure public support, an integrated and comprehensive monitoring program is needed within a carbon capture and storage(CCS) project. Monitoring can be done using many well-established techniques from various fields, and the seismic method proves to be the crucial one. This method is widely used to determine the CO_(2) distribution, image the plume development, and quantitatively estimate the concentration. Because both the CO_(2) distribution and the potential migration pathway can be spatially small scale, high resolution for seismic imaging is demanded. However, obtaining a high-resolution image of a subsurface structure in marine settings is difficult. Herein, we introduce the novel Hcable(Harrow-like cable system) technique, which may be applied to offshore CCS monitoring. This technique uses a highfrequency source(the dominant frequency>100 Hz) to generate seismic waves and a combination of a long cable and several short streamers to receive seismic waves. Ultrahigh-frequency seismic images are achieved through the processing of Hcable seismic data. Hcable is then applied in a case study to demonstrate its detailed characterization for small-scale structures. This work reveals that Hcable is a promising tool for timelapse seismic monitoring of oceanic CCS.展开更多
Computer simulations are utilized to investigate the dynamic behavior of self-propelled particles(SPPs)within a complex obstacle environment.The findings reveal that SPPs exhibit three distinct aggregation states with...Computer simulations are utilized to investigate the dynamic behavior of self-propelled particles(SPPs)within a complex obstacle environment.The findings reveal that SPPs exhibit three distinct aggregation states within the obstacle,each contingent on specific conditions.A phase diagram outlining the aggregation states concerning self-propulsion conditions is presented.The results illustrate a transition of SPPs from a dispersion state to a transition state as persistence time increases within the obstacle.Conversely,as the driving strength increases,self-propelled particles shift towards a cluster state.A systematic exploration of the interplay between driving strength,persistence time,and matching degree on the dynamic behavior of self-propelled particles is conducted.Furthermore,an analysis is performed on the spatial distribution of SPPs along the y-axis,capture rate,maximum capture probability,and mean-square displacement.The insights gained from this research make valuable contributions to understanding the capture and collection of active particles.展开更多
Climate change, resulting from human-caused CO_(2) and other greenhouse gas emissions, is an urgent problem that demands immediate action from everyone. The need to decrease emissions has sparked a renewed emphasis on...Climate change, resulting from human-caused CO_(2) and other greenhouse gas emissions, is an urgent problem that demands immediate action from everyone. The need to decrease emissions has sparked a renewed emphasis on developing and utilizing offshore Carbon Capture,Utilization,and Storage(CCUS) technologies.While these technologies offer potential solutions to mitigate greenhouse gas emissions,many challenges must be addressed to ensure successful implementation.展开更多
The semiclassical non-perturbative atomic orbital close-coupling approach has been employed to study the electron capture and excitation processes in He^(2+)-H(1s)and He^(2+)-H(2s)collision systems.In order to ensure ...The semiclassical non-perturbative atomic orbital close-coupling approach has been employed to study the electron capture and excitation processes in He^(2+)-H(1s)and He^(2+)-H(2s)collision systems.In order to ensure the accuracy of our calculated cross sections,a large number of high excited states and pseudostates are included in the expansion basis sets which are centered on the target and projectile,respectively.The total and partial charge transfer and excitation cross sections are obtained for a wide-energy domain ranging from 1 keV/amu to 200 keV/amu.The present calculations are also compared with the results from other theoretical methods.These cross section data are useful for the investigation of astrophysics and laboratory plasma.展开更多
Boron neutron capture therapy(BNCT)is recognized as a precise binary targeted radiotherapy technique that effectively eliminates tumors through the^(10)B(n,α)^(7)Li nuclear reaction.Among various neutron sources,acce...Boron neutron capture therapy(BNCT)is recognized as a precise binary targeted radiotherapy technique that effectively eliminates tumors through the^(10)B(n,α)^(7)Li nuclear reaction.Among various neutron sources,accelerator-based sources have emerged as particularly promising for BNCT applications.The^(7)Li(p,n)^(7)Be reaction is highly regarded as a potential neutron source for BNCT,owing to its low threshold energy for the reaction,significant neutron yield,appropriate average neutron energy,and additional benefits.This study utilized Monte Carlo simulations to model the physical interactions within a lithium target subjected to proton bombardment,including neutron moderation by an MgF_(2)moderator and subsequent BNCT dose analysis using a Snyder head phantom.The study focused on calculating the yields of epithermal neutrons for various incident proton energies,finding an optimal energy at 2.7 MeV.Furthermore,the Snyder head phantom was employed in dose simulations to validate the effectiveness of this specific incident energy when utilizing a^(7)Li(p,n)^(7)Be neutron source for BNCT purposes.展开更多
Hydrate formation rate and separation effect on the capture of CO2 from binary mixture via forming hydrate with 5 wt% tetra-n-butyl ammonium bromide （TBAB） solution were studied. The results showed that the inductio...Hydrate formation rate and separation effect on the capture of CO2 from binary mixture via forming hydrate with 5 wt% tetra-n-butyl ammonium bromide （TBAB） solution were studied. The results showed that the induction time was 5 min, and the hydrate formation process finished in 1 h at 4.5 ℃ and 4.01 MPa. The hydrate formation rate constant reached the maximum of 1.84× 10^-7 molZ/（s.J） with the feed pressure of 7.30 MPa. The CO2 recovery was about 45 % in the feed pressure range from 4.30 to 7.30 MPa. Under the feed pressure of 4.30 MPa, the maximum separation factor and CO2 concentration in hydrate phase were 7.3 and 38.2 mol%, respectively. The results demonstrated that TBAB accelerated hydrate formation and enriched CO2 in hydrate phase under the gentle condition.展开更多
Carbon dioxide capture,EOR-utilization and storage(CCUS-EOR)are the most practical and feasible large-scale carbon reduction technologies,and also the key technologies to greatly improve the recovery of low-permeabili...Carbon dioxide capture,EOR-utilization and storage(CCUS-EOR)are the most practical and feasible large-scale carbon reduction technologies,and also the key technologies to greatly improve the recovery of low-permeability oil fields.This paper sorts out the main course of CCUS-EOR technological development abroad and its industrialization progress.The progress of CCUS-EOR technological research and field tests in China are summarized,the development status,problems and challenges of the entire industry chain of CO_(2) capture,transportation,oil displacement,and storage are analyzed.The results show a huge potential of the large-scale application of CCUS-EOR in China in terms of carbon emission reduction and oil production increase.At present,CCUS-EOR in China is in a critical stage of development,from field pilot tests to industrialization.Aiming at the feature of continental sedimentary oil and gas reservoirs in China,and giving full play to the advantages of the abundant reserves for CO_(2) flooding,huge underground storage space,surface infrastructure,and wide distribution of wellbore injection channels,by cooperating with carbon emission enterprises,critical technological research and demonstration project construction should be accelerated,including the capture of low-concentration CO_(2) at low-cost and on large-scale,supercritical CO_(2) long-distance transportation,greatly enhancing oil recovery and storage rate,and CO_(2) large-scale and safe storage.CCUS-EOR theoretical and technical standard system should be constructed for the whole industrial chain to support and promote the industrial scale application,leading the rapid and profitable development of CCUS-EOR emerging industrial chain with innovation.展开更多
基金National Key R&D Program of China(2022YFE0105900)National Natural Science Foundation of China(52306179)+1 种基金Science and Technology Innovation Program of Hunan Province(2021RC4006)High Performance Computing Center of Central South University。
文摘The development of dual functional material for cyclic CO_(2)capture and hydrogenation is of great significance for converting diluted CO_(2)into valuable fuels,but suffers from kinetic limitation and deactivation of adsorbent and catalyst.Herein,we engineered a series of RuNa/γ-Al_(2)O_(3)materials,varying the size of ruthenium from single atoms to clusters/nanoparticles.The coordination environment and structure sensitivity of ruthenium were quantitatively investigated at atomic scale.Our findings reveal that the reduced Ru nanoparticles,approximately 7.1 nm in diameter with a Ru-Ru coordination number of 5.9,exhibit high methane formation activity and selectivity at 340°C.The Ru-Na interfacial sites facilitate CO_(2)migration through a deoxygenation pathway,involving carbonate dissociation,carbonyl formation,and hydrogenation.In-situ experiments and theoretical calculations show that stable carbonyl intermediates on metallic Ru nanoparticles facilitate heterolytic C–O scission and C–H bonding,significantly lowering the energy barrier for activating stored CO_(2).
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financially supported by the National Natural Science Foundation of China(22178357)CAS Project for Young Scientists in Basic Research(YSBR-038)+1 种基金the Youth Innovation Promotion Association of the Chinese Academy of Sciences(2020047)the research fund of State Key Laboratory of Mesoscience and Engineering(MESO-23-A07,MESO-23-T02)。
文摘Ammonia(NH3)is a carbon-free,hydrogen-rich chemical related to global food safety,clean energy,and environmental protection.As an essential technology for meeting the requirements raised by such issues,NH3 capture has been intensively explored by researchers in both fundamental and applied fields.The four typical methods used are(1)solvent absorption by ionic liquids and their derivatives,(2)adsorption by porous solids,(3)abadsorption by porous liquids,and(4)membrane separation.Rooted in the development of advanced materials for NH3 capture,we conducted a coherent review of the design of different materials,mainly in the past 5 years,their interactions with NH3 molecules and construction of transport pathways,as well as the structure–property relationship,with specific examples discussed.Finally,the challenges in current research and future worthwhile directions for NH3 capture materials are proposed.
基金support from the U.S.Department of Energy National Energy Technology Laboratory(DE-FE0031736)the New York State Foundation for Science,Technology and Innovation(NYSTAR).
文摘Industrial thin-film composite(TFC)membranes achieve superior gas separation properties from high-performance selective layer materials,while the success of membrane technology relies on high-performance gutter layers to achieve production scalability and low-cost manufacturing.However,the current literature predominantly focuses on the design of polymer architectures to obtain high permeability and selectivity,while the art of fabricating gutter layers is usually safeguarded by industrial manufacturers and appears lackluster to academic researchers.This is the first report aiming to provide a comprehensive and critical review of state-of-the-art gutter layer materials and their design and modification to enable TFC membranes with superior separation performance.We first elucidate the importance of the gutter layer on membrane performance through modeling and experimental results.Then various gutter layer materials used to obtain high-performance composite membranes are critically reviewed,and the strategies to improve their compatibility with the selective layer are highlighted,such as oxygen plasma treatment,polydopamine deposition,and surface grafting.Finally,we present the opportunities of the gutter layer design for practical applications.
基金supported by the National Natural Science Foundation of China(22302100,22025203,22121005)the Fundamental Research Funds for the Central Universities(Nankai University).
文摘As a prominent contributor to air pollution,nitric oxide(NO)has emerged as a critical agent causing detrimental environmental and health ramifications.To mitigate emissions and facilitate downstream utilization,adsorption-based techniques offer a compelling approach for direct NO capture from both stationary and mobile sources.In this study,a comprehensive exploration of NO capture under oxygen-lean and oxygenrich conditions was conducted,employing Ni ion-exchanged chabazite(CHA-type)zeolites as the adsorbents.Remarkably,Ni/Na-CHA zeolites,with Ni loadings ranging from 3 to 4 wt%,demonstrate remarkable dynamic uptake capacities and exhibit exceptional NO capture efficiencies(NO-to-Ni ratio)for both oxygen-lean(0.17-0.31 mmol/g,0.32-0.43 of NO/Ni)and oxygen-rich(1.64-1.18 mmol/g)under ambient conditions.An NH3 reduction methodology was designed for the regeneration of absorbents at a relatively low temperature of 673 K.Comprehensive insights into the NO_(x) adsorption mechanism were obtained through temperature-programmed desorption experiments,in situ Fourier transform infrared spectroscopy,and density functional theory calculations.It is unveiled that NO and NO_(2) exhibit propensity to coordinate with Ni^(2+) via N-terminal or O-terminal,yielding thermally stable complexes and metastable species,respectively,while the low-temperature desorption substances are generated in close proximity to Na^(+).This study not only offers micro-level perspectives but imparts crucial insights for the advancement of capture and reduction technologies utilizing precious-metal-free materials.
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.
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Project supported by the National Natural Science Foundation of China (Grant Nos.52175279 and 51705459)the Natural Science Foundation of Zhejiang Province,China (Grant No.LY20E050022)the Key Research and Development Projects of Zhejiang Provincial Science and Technology Department (Grant No.2021C03122)。
文摘This paper presented a novel tinny motion capture system for measuring bird posture based on inertial and magnetic measurement units that are made up of micromachined gyroscopes, accelerometers, and magnetometers. Multiple quaternion-based extended Kalman filters were implemented to estimate the absolute orientations to achieve high accuracy.Under the guidance of ornithology experts, the extending/contracting motions and flapping cycles were recorded using the developed motion capture system, and the orientation of each bone was also analyzed. The captured flapping gesture of the Falco peregrinus is crucial to the motion database of raptors as well as the bionic design.
基金supported by the Shanghai Agricultural Science and Technology Program (2022-02-08-00-12-F01176)he National Natural Science Foundation of China (52006135)
文摘Direct air capture(DAC)of CO_(2)plays an indispensable role in achieving carbon-neutral goals as one of the key negative emission technologies.Since large air flows are required to capture the ultradilute CO_(2)from the air,lab-synthesized adsorbents in powder form may cause unacceptable gas pressure drops and poor heat and mass transfer efficiencies.A structured adsorbent is essential for the implementation of gas-solid contactors for cost-and energy-efficient DAC systems.In this study,efficient adsorbent poly(ethyleneimine)(PEI)-functionalized Mg-Al-CO_(3)layered double hydroxide(LDH)-derived mixed metal oxides(MMOs)are three-dimensional(3D)printed into monoliths for the first time with more than 90%adsorbent loadings.The printing process has been optimized by initially printing the LDH powder into monoliths followed by calcination into MMO monoliths.This structure exhibits a 32.7%higher specific surface area and a 46.1%higher pore volume,as compared to the direct printing of the MMO powder into a monolith.After impregnation of PEI,the monolith demonstrates a large adsorption capacity(1.82 mmol/g)and fast kinetics(0.7 mmol/g/h)using a CO_(2)feed gas at 400 ppm at 25℃,one of the highest values among the shaped DAC adsorbents.Smearing of the amino-polymers during the post-printing process affects the diffusion of CO_(2),resulting in slower adsorption kinetics of pre-impregnation monoliths compared to post-impregnation monoliths.The optimal PEI/MeOH ratio for the post-impregnation solution prevents pores clogging that would affect both adsorption capacity and kinetics.
基金Project supported by the National Key R&D Program of China(Grant No.2021YFB2012600)。
文摘This work demonstrates a micron-sized nanosecond current pulse probe using a quantum diamond magnetometer.A micron-sized diamond crystal affixed to a fiber tip is integrated on the end of a conical waveguide.We demonstrate real-time visualization of a single 100 nanosecond pulse and discrimination of two pulse trains of different frequencies with a coplanar waveguide and a home-made PCB circuit.This technique finds promising applications in the display of electronic stream and can be used as a pulse discriminator to simultaneously receive and demodulate multiple pulse frequencies.This method of detecting pulse current is expected to provide further detailed analysis of the internal working state of the chip.
基金Supported by the project of Sanya Yazhou Bay Science and Technology City (Grant No:SCKJ-JYRC-2022-14)。
文摘To ensure project safety and secure public support, an integrated and comprehensive monitoring program is needed within a carbon capture and storage(CCS) project. Monitoring can be done using many well-established techniques from various fields, and the seismic method proves to be the crucial one. This method is widely used to determine the CO_(2) distribution, image the plume development, and quantitatively estimate the concentration. Because both the CO_(2) distribution and the potential migration pathway can be spatially small scale, high resolution for seismic imaging is demanded. However, obtaining a high-resolution image of a subsurface structure in marine settings is difficult. Herein, we introduce the novel Hcable(Harrow-like cable system) technique, which may be applied to offshore CCS monitoring. This technique uses a highfrequency source(the dominant frequency>100 Hz) to generate seismic waves and a combination of a long cable and several short streamers to receive seismic waves. Ultrahigh-frequency seismic images are achieved through the processing of Hcable seismic data. Hcable is then applied in a case study to demonstrate its detailed characterization for small-scale structures. This work reveals that Hcable is a promising tool for timelapse seismic monitoring of oceanic CCS.
基金Project supported by the Natural Science Foundation of Shanxi Province,China(Grant Nos.202303021212148 and 202103021223245)。
文摘Computer simulations are utilized to investigate the dynamic behavior of self-propelled particles(SPPs)within a complex obstacle environment.The findings reveal that SPPs exhibit three distinct aggregation states within the obstacle,each contingent on specific conditions.A phase diagram outlining the aggregation states concerning self-propulsion conditions is presented.The results illustrate a transition of SPPs from a dispersion state to a transition state as persistence time increases within the obstacle.Conversely,as the driving strength increases,self-propelled particles shift towards a cluster state.A systematic exploration of the interplay between driving strength,persistence time,and matching degree on the dynamic behavior of self-propelled particles is conducted.Furthermore,an analysis is performed on the spatial distribution of SPPs along the y-axis,capture rate,maximum capture probability,and mean-square displacement.The insights gained from this research make valuable contributions to understanding the capture and collection of active particles.
文摘Climate change, resulting from human-caused CO_(2) and other greenhouse gas emissions, is an urgent problem that demands immediate action from everyone. The need to decrease emissions has sparked a renewed emphasis on developing and utilizing offshore Carbon Capture,Utilization,and Storage(CCUS) technologies.While these technologies offer potential solutions to mitigate greenhouse gas emissions,many challenges must be addressed to ensure successful implementation.
基金supported by the National Key Research and Development Program of China (Grant No.2022YFA 1602500)the National Natural Science Foundation of China (Grant Nos.11934004 and 12241410).
文摘The semiclassical non-perturbative atomic orbital close-coupling approach has been employed to study the electron capture and excitation processes in He^(2+)-H(1s)and He^(2+)-H(2s)collision systems.In order to ensure the accuracy of our calculated cross sections,a large number of high excited states and pseudostates are included in the expansion basis sets which are centered on the target and projectile,respectively.The total and partial charge transfer and excitation cross sections are obtained for a wide-energy domain ranging from 1 keV/amu to 200 keV/amu.The present calculations are also compared with the results from other theoretical methods.These cross section data are useful for the investigation of astrophysics and laboratory plasma.
文摘Boron neutron capture therapy(BNCT)is recognized as a precise binary targeted radiotherapy technique that effectively eliminates tumors through the^(10)B(n,α)^(7)Li nuclear reaction.Among various neutron sources,accelerator-based sources have emerged as particularly promising for BNCT applications.The^(7)Li(p,n)^(7)Be reaction is highly regarded as a potential neutron source for BNCT,owing to its low threshold energy for the reaction,significant neutron yield,appropriate average neutron energy,and additional benefits.This study utilized Monte Carlo simulations to model the physical interactions within a lithium target subjected to proton bombardment,including neutron moderation by an MgF_(2)moderator and subsequent BNCT dose analysis using a Snyder head phantom.The study focused on calculating the yields of epithermal neutrons for various incident proton energies,finding an optimal energy at 2.7 MeV.Furthermore,the Snyder head phantom was employed in dose simulations to validate the effectiveness of this specific incident energy when utilizing a^(7)Li(p,n)^(7)Be neutron source for BNCT purposes.
文摘Hydrate formation rate and separation effect on the capture of CO2 from binary mixture via forming hydrate with 5 wt% tetra-n-butyl ammonium bromide （TBAB） solution were studied. The results showed that the induction time was 5 min, and the hydrate formation process finished in 1 h at 4.5 ℃ and 4.01 MPa. The hydrate formation rate constant reached the maximum of 1.84× 10^-7 molZ/（s.J） with the feed pressure of 7.30 MPa. The CO2 recovery was about 45 % in the feed pressure range from 4.30 to 7.30 MPa. Under the feed pressure of 4.30 MPa, the maximum separation factor and CO2 concentration in hydrate phase were 7.3 and 38.2 mol%, respectively. The results demonstrated that TBAB accelerated hydrate formation and enriched CO2 in hydrate phase under the gentle condition.
基金Supported by the Major Science and Technology Project of PetroChina(2021ZZ01).
文摘Carbon dioxide capture,EOR-utilization and storage(CCUS-EOR)are the most practical and feasible large-scale carbon reduction technologies,and also the key technologies to greatly improve the recovery of low-permeability oil fields.This paper sorts out the main course of CCUS-EOR technological development abroad and its industrialization progress.The progress of CCUS-EOR technological research and field tests in China are summarized,the development status,problems and challenges of the entire industry chain of CO_(2) capture,transportation,oil displacement,and storage are analyzed.The results show a huge potential of the large-scale application of CCUS-EOR in China in terms of carbon emission reduction and oil production increase.At present,CCUS-EOR in China is in a critical stage of development,from field pilot tests to industrialization.Aiming at the feature of continental sedimentary oil and gas reservoirs in China,and giving full play to the advantages of the abundant reserves for CO_(2) flooding,huge underground storage space,surface infrastructure,and wide distribution of wellbore injection channels,by cooperating with carbon emission enterprises,critical technological research and demonstration project construction should be accelerated,including the capture of low-concentration CO_(2) at low-cost and on large-scale,supercritical CO_(2) long-distance transportation,greatly enhancing oil recovery and storage rate,and CO_(2) large-scale and safe storage.CCUS-EOR theoretical and technical standard system should be constructed for the whole industrial chain to support and promote the industrial scale application,leading the rapid and profitable development of CCUS-EOR emerging industrial chain with innovation.
