Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode ...Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode cannot match the capacitor-type cathode, restricting the development of LICs. Herein, hierarchical carbon framework(HCF) anode material composed of 0D carbon nanocage bridged with 2D graphene network are developed via a template-confined synthesis process. The HCF with nanocage structure reduces the Li^(+) transport path and benefits the rapid Li^(+) migration, while 2D graphene network can promote the electron interconnecting of carbon nanocages. In addition, the doped N atoms in HCF facilitate to the adsorption of ions and enhance the pseudo contribution, thus accelerate the kinetics of the anode. The HCF anode delivers high specific capacity, remarkable rate capability. The LIC pouch-cell based on HCF anode and active HCF(a-HCF) cathode can provide a high energy density of 162 Wh kg^(-1) and a superior power density of 15.8 kW kg^(-1), as well as a long cycling life exceeding 15,000cycles. This study demonstrates that the well-defined design of hierarchical carbon framework by incorporating 0D carbon nanocages and 2D graphene network is an effective strategy to promote LIC anode kinetics and hence boost the LIC electrochemical performance.展开更多
Solid physical properties are vital for the design, optimization, and scale-up of gas–liquid–solid multiphase reactors. The complex and interactional effects of the solid physical properties, including particle diam...Solid physical properties are vital for the design, optimization, and scale-up of gas–liquid–solid multiphase reactors. The complex and interactional effects of the solid physical properties, including particle diameter, density, wettability, and sphericity, on the hydrodynamic behaviors in a new external airlift loop reactor(EALR) integrating mixing and separation are decoupled in this work. Two semi-empirical equations are proposed and validated to predict the overall gas holdup and liquid circulating velocity satisfactorily, and then the individual influence of such solid physical properties is further investigated. The results demonstrate that both the overall gas holdup in the riser and the liquid circulating velocity in the downcomer increase with the contact angle, but decrease with particle size, density, and sphericity.Additionally, the impact of the particle size on the liquid circulating velocity is also profoundly revealed on a micro-level considering the particle size distribution. Moreover, the axial solid concentration distribution is discussed, and the uniformity of the slurry is described by the mixing index of the solid particles. The results show that a more homogeneous mixture can be achieved by adding finer particles other than attaining violent turbulence. Therefore, this work lays a foundation for the design, scale-up, and industrialization of the EALRs.展开更多
CO_(2) electroreduction(CO_(2) ER)to high value-added chemicals is considered as a promising technology to achieve sustainable carbon neutralization.By virtue of the progressive research in recent years aiming at desi...CO_(2) electroreduction(CO_(2) ER)to high value-added chemicals is considered as a promising technology to achieve sustainable carbon neutralization.By virtue of the progressive research in recent years aiming at design and understanding of catalytic materials and electrolyte systems,the CO_(2) ER performance(such as current density,selectivity,stability,CO_(2) conversion,etc.)has been continually increased.Unfortunately,there has been relatively little attention paid to the large-scale CO 2 electrolyzers,which stand just as one obstacle,alongside series-parallel integration,challenging the practical application of this infant technology.In this review,the latest progress on the structures of low-temperature CO_(2) electrolyzers and scale-up studies was systematically overviewed.The influence of the CO_(2) electrolyzer configurations,such as the flow channel design,gas diffusion electrode(GDE)and ion exchange membrane(IEM),on the CO_(2) ER performance was further discussed.The review could provide inspiration for the design of large-scale CO_(2) electrolyzers so as to accelerate the industrial application of CO_(2) ER technology.展开更多
A type of calcium coke was developed for use in the oxy-thermal process of calcium carbide production.The calcium coke was prepared by the co-pyrolysis of coking coal and calcium carbide slag, which is a solid waste g...A type of calcium coke was developed for use in the oxy-thermal process of calcium carbide production.The calcium coke was prepared by the co-pyrolysis of coking coal and calcium carbide slag, which is a solid waste generated from the chlor-alkali industry.The characteristics of the calcium cokes under different conditions were analyzed experimentally and theoretically.The results show that the thermal strength of calcium coke increased with the increase in the coking coal proportion, and the waterproof property of calcium coke also increased with increased carbonation time.The calcium coke can increase the contact area of calcium and carbon in the calcium carbide production process.Furthermore, the pore structure of the calcium coke can enhance the diffusion of gas inside the furnace, thus improving the efficiency of the oxy-thermal technology.展开更多
The quantitative understanding of how atomic-level catalyst structural changes affect the reactivity of the electrochemical CO_(2)reduction reaction is challenging.Due to the complexity of catalytic systems,convention...The quantitative understanding of how atomic-level catalyst structural changes affect the reactivity of the electrochemical CO_(2)reduction reaction is challenging.Due to the complexity of catalytic systems,conventional in situ X-ray spectroscopy plays a limited role in tracing the underlying dynamic structural changes in catalysts active sites.Herein,operando high-energy resolution fluorescence-detected X-ray absorption spectroscopy was used to precisely identify the dynamic structural transformation of well-defined active sites of a representative model copper(Ⅱ)phthalocyanine catalyst which is of guiding significance in studying single-atom catalysis system.Comprehensive X-ray spectroscopy analyses,including surface sensitive△μspectra which isolates the surface changes by subtracting the disturb of bulk base and X-ray absorption near-edge structure spectroscopy simulation,were used to discover that Cu species aggregated with increasing applied potential,which is responsible for the observed evolution of C_(2)H_(4).The approach developed in this work,characterizing the active-site geometry and dynamic structural change,is a novel and powerful technique to elucidate complex catalytic mechanisms and is expected to con tribute to the rational design of highly effective catalysts.展开更多
Lithium slurry flow cell(LSFC)is a novel energy storage device that combines the concept of both lithium ion batteries(LIBs)and flow batteries(FBs).Although it is hoped to inherit the advantages of both LIBs and FBs,s...Lithium slurry flow cell(LSFC)is a novel energy storage device that combines the concept of both lithium ion batteries(LIBs)and flow batteries(FBs).Although it is hoped to inherit the advantages of both LIBs and FBs,such as high energy density,ease of fabrication,environmental friendly,independent energy and power density,to name but a few.While unfortunately,it still has many challenges to overcome before it becoming the future star in energy storage area.Here in this paper,we briefly recall its history and try to illustrate the main issues that hindering its research as well as application.As a typical interdisciplinary product,LSFC is definitely a promising candidate for large scale energy storage application,while obviously it still has a long way to go.展开更多
The Ru-catalyzed carbonylation of alkenes with CO_(2)as a C1 surrogate and imidazole chlorides as the promotor is investigated by a combination of computational and experimental study.The conversion rate of CO_(2)to C...The Ru-catalyzed carbonylation of alkenes with CO_(2)as a C1 surrogate and imidazole chlorides as the promotor is investigated by a combination of computational and experimental study.The conversion rate of CO_(2)to CO is positively correlated with the efficiency of both hydroesterification and hydroformylation,which is found facilitated in the presence of chloride additives with a decreasing order of BmimCl~B3MimCl>BmmimCl~LiCl.Taking the hydroesterification with MeOH as a representative example,BmimCl bearing C-H functionality at the C^(2)site of the cation assists the reduction of CO_(2)to CO as a hydrogen donor medium,with the anion and cation acting in a synergistic fashion.Subsequent insertion of CO_(2)into the formed Ru-H bond with the assistance of chloride anion produces the Ru-COOH species,which ultimately accelerates the activation of CO_(2).展开更多
Efficient and low-cost recycling of spent lithium iron phosphate(LiFePO_(4),LFP)batteries has become an inevitable trend.In this study,an integrated closed-loop recycling strategy including isomorphic substitution lea...Efficient and low-cost recycling of spent lithium iron phosphate(LiFePO_(4),LFP)batteries has become an inevitable trend.In this study,an integrated closed-loop recycling strategy including isomorphic substitution leaching and solvent extraction process for spent LFP was proposed.An inexpensive FeCl_(3)was used as leaching agent to directly substitute Fe^(2+)from LFP.99%of Li can be rapidly leached in just 30 min,accompanied by 98%of FePO_(4)precipitated in lixivium.The tri-n-butyl phosphate(TBP)-sulfonated kerosene(SK)system was applied to extract Li from lixivium through a twelve-stage countercurrent process containing synchronous extraction and stepwise stripping of Li^(+)and Fe^(3+).80.81%of Li can be selectively enriched in stripping liquor containing 3.059 mol·L^(-1)of Li^(+)under optimal conditions.And the Fe stripping liquor was recovered for LFP re-leaching,of which,Fe^(2+)was oxidized to Fe^(3+)by appropriate H_(2)O_(2).Raffinate and lixivium were concentrated and entered into extraction process to accomplished closeloop recycling process.Overall,the results suggest that more than 99%of Li was recovered.FeCl_(3)holding in solution was directly regenerated without any pollutant emission.The sustainable mothed would be an alternative candidate for total element recycling of spent LFP batteries with industrial potential.展开更多
Magnetization roasting is one of the most effective way of utilizing low-grade refractory iron ore.However,the reduction roasting of siderite(FeCO3)generates weakly magnetic wüstite,thus reducing iron recovery vi...Magnetization roasting is one of the most effective way of utilizing low-grade refractory iron ore.However,the reduction roasting of siderite(FeCO3)generates weakly magnetic wüstite,thus reducing iron recovery via weak magnetic separation.We systematically studied and proposed the fluidized preoxidation-low-temperature reduction magnetization roasting process for siderite.We found that the maghemite generated during the air oxidation roasting of siderite would be further reduced into wüstite at 500 and 550℃due to the unstable intermediate product magnetite(Fe_(3)O_(4)).Stable magnetite can be obtained through maghemite reduction only at low temperature.The optimal fluidized magnetization roasting parameters included preoxidation at 610℃for 2.5 min,followed by reduction at 450℃for 5 min.For roasted ore,weak magnetic separation yielded an iron ore concentrate grade of 62.0wt%and an iron recovery rate of 88.36%.Compared with that of conventional direct reduction magnetization roasting,the iron recovery rate of weak magnetic separation had greatly improved by 34.33%.The proposed fluidized preoxidation-low-temperature reduction magnetization roasting process can realize the efficient magnetization roasting utilization of low-grade refractory siderite-containing iron ore without wüstite generation and is unlimited by the proportion of siderite and hematite in iron ore.展开更多
As the largest steel-producing country,China’s steel industry has experienced rapid development in terms of production level and quality.Owing to the high consumption of coal in the iron and steel industry,air pollut...As the largest steel-producing country,China’s steel industry has experienced rapid development in terms of production level and quality.Owing to the high consumption of coal in the iron and steel industry,air pollutants and carbon dioxide(CO_(2))show similar emission properties in flue gas.In view of the collaborative reduction of pollution and carbon emissions,the emission standards for pollutants and carbon were first analyzed,suggesting that carbon emission standards for the iron and steel industry should be accelerated.A collaborative technology system for the reduction of pollution and carbon emissions from the iron and steel industry in China is demonstrated,consisting of(1)optimization of present ultra-low emission technology,(2)low-carbon innovation for present production processes,(3)steel production process reengineering,and(4)carbon capture,utilization,and storage(CCUS).Finally,the technical prospect for collaborative reduction of pollution and carbon emissions from the iron and steel industry in China is suggested to support high-quality green development in this industry.展开更多
Chitin is a widely used important industrial polymer mainly from shrimp shells, but its commercial preparation is under the great challenge of serious pollution due to the requirement of HCl and Na OH.Herein, we demon...Chitin is a widely used important industrial polymer mainly from shrimp shells, but its commercial preparation is under the great challenge of serious pollution due to the requirement of HCl and Na OH.Herein, we demonstrated that high purity chitin can be obtained from waste shrimp shells(WSSs) by cascade separation with transition metal salt aqueous solution and ionic liquid(IL). Firstly, calcium carbonate of WSSs was effectively removed in the metal salt aqueous solution driven by the ion exchange interaction. Subsequently, 1-butyl-3-methylimidazolium chloride([Bmim]Cl) had bifunctional abilities to remove residual protein and introduced metal salts simultaneously by hydrogen bonding and coordination interactions. The key experimental factors affecting the separation process were systematically studied, including the type of metal salts, temperature, and [Bmim]Cl loading. After sequential treatment with a 20%(mass) Ni SO4aqueous solution at 130 ℃ and [Bmim]Cl at 150 ℃, the purity of a-chitin can be up to 96.5%(mass) that meets commercial requirements. The use of metal salts with higher coordination ability makes the preparation of chitin no longer depend on the commonly acid-base reaction, which is conducive to the preservation of chitin structure.展开更多
Carbon dioxide(CO_(2))emissions from the cement industry account for 26%of the total industrial emissions,and the need to develop low-carbon techniques within the cement industry is extremely urgent.Low-carbon project...Carbon dioxide(CO_(2))emissions from the cement industry account for 26%of the total industrial emissions,and the need to develop low-carbon techniques within the cement industry is extremely urgent.Low-carbon projects and technologies for the cement industry in different regions and countries have been thoroughly reviewed in this manuscript,and the low-carbon development concept for each county has been analyzed.For developing countries such as China and India,energy saving and efficiency enhancement are currently the key points,while for developed countries and regions such as Europe,more efforts have been focused on carbon capture,utilization,and storage(CCUS).Global CCUS projects have been previously conducted,and the majority of CCUS projects are currently performed in Europe where major projects such as the CEMCAP,CLEANKER,and IEILAC projects represent the latest research progress in cement production technologies and low-carbon technologies for the global cement industry.The development of low-carbon cement technologies has changed from focusing on the end point to instead focusing on the source and process through the exploration of hydrogen and solar energies,and more disruptive and original technologies are expected to be developed,particularly in the cement industry in China.展开更多
By modeling a group of neighboring real particles as a single coarse-grained particle(CGP),discrete particle method(DPM)is now capable of simulating industrial-scale particle-fluid systems.However,a systematic approac...By modeling a group of neighboring real particles as a single coarse-grained particle(CGP),discrete particle method(DPM)is now capable of simulating industrial-scale particle-fluid systems.However,a systematic approach to determine the CGP properties and develop their interaction models is still lacking,which casts uncertainty on the predictivity of the method.In this study,collisions between predefined particle groups are analyzed to construct kernel functions for modeling the CGPs and then the model parameters are determined by equating the statistical properties of the CGPs and the real particles in the physical process studied.This approach is implemented for homogeneous cooling of granular gas,then demonstrated effective in simulating experimental fluidized beds.展开更多
The sustainability of the coking industry is supported by reasonable production profit and environmental quality requirements.The traditional measures substantially increased the related costs for enterprises to reach...The sustainability of the coking industry is supported by reasonable production profit and environmental quality requirements.The traditional measures substantially increased the related costs for enterprises to reach standards.This paper aims to develop a comprehensive cost combined environmental impact assessment method that is necessary for the analysis of wastewater treatment systems.Typical three coking wastewater treatment processes in China were evaluated.Results showed that eutrophication dominantly contributed to the overall environmental effect.Improving effluent quality could significantly reduce the total environmental impact.In terms of an economic perspective,the price of raw materials was the main factor that affected the operating cost of comprehensive treatment.Based on subsystem analysis,the pretreatment stage accounted for the majority of environmental and cost burdens,respectively reaching 64%-78%and 64%-86%.Optimizing the pretreatment process by enhancing the efficiency of high concentration raw material recovery and substituting toxic raw materials for extractant could reduce the environmental impact and economic cost by 43.8%and 57%,respectively,which was an effective way to improve the potential performance of coking wastewater treatment plants(WWTPs).展开更多
MXenes have aroused intensive enthusiasm because of their exotic properties and promising applications.However,to date,they are usually synthesized by etching technologies.Developing synthetic technologies provides mo...MXenes have aroused intensive enthusiasm because of their exotic properties and promising applications.However,to date,they are usually synthesized by etching technologies.Developing synthetic technologies provides more opportunities for innovation and may extend unexplored applications.Here,we report a bottom-up gas-phase synthesis of Cl-terminated MXene(Ti_(2)CCl_(2)).The gas-phase synthesis endows Ti_(2)CCl_(2) with unique surface chemistry,high phase purity,and excellent metallic conductivity,which can be used to accelerate polysulfide conversion kinetics and dramatically prolong the cyclability of Li-S batteries.In-depth mechanistic analysis deciphers the origin of the formation of Ti_(2)CCl_(2) and offers a paradigm for tuning MXene chemical vapor deposition.In brief,the gas-phase synthesis transforms the synthesis of MXenes and unlocks the hardly achieved potentials of MXenes.展开更多
Discharging untreated oily wastewater into the environment disrupts the ecological balance,which is a global problem that requires urgent solutions.Superhydrophilic and superoleophilic fibrous medium(FM)effectively se...Discharging untreated oily wastewater into the environment disrupts the ecological balance,which is a global problem that requires urgent solutions.Superhydrophilic and superoleophilic fibrous medium(FM)effectively separated oil–water emulsion as it was hydrophobic underwater.But its separation efficiencies(SEs)first increased to 98.9%,then dropped to 97.6%in 10 min because of oil-fouling.To tackle this problem,FM deposited with 0%–10%silica nanoparticle(NPsFMs),then coated by fluorocarbon polymer(X-[CH_(2)CH_(2)O]nCH_(2)CH_(2)O-Y-NH-COOCH_(2)C4F9)(FCNPs FMs),was used to enhance its roughness and regulate its initial wettability to improve the anti-fouling property.FCFM and FCNPs FMs were hydrophobic and oleophobic in air and oleophobic underwater.Their water contact angles,oil contact angles and oil contact angles were 115.3°–121.1°,128.8°–136.5°,and 131.6°–136.7°,respectively,meeting the requirement of 90°–140°for coalescence separation.FCNPs FM-5 had the best separation performance with a constant value of 99.8%in 10 min,while that of FCNPs FM-10 slightly decreased to 99.5%.Theoretical released droplet(TRD)diameter,calculated by the square root of the product of pore radius and fiber diameter,was used for the evaluation of coalescence performance.Analyzed by two ideal models,TRD diameter and fiber diameter showed a parabola type relationship,proving that the separation efficiency was a collaborative work of wettability,pore size and fiber diameter.Also,it explained the SEs reduction from FCNPs FM-5 to FCNPs FM-10 was revelent to the three parameters.Moreover,FCNPsFMs effectively separated emulsions stabilized by cationic surfactant CTAB(SEs:97.3%–98.4%)and anionic surfactant SDBS(SEs:91.3%–93.4%).But they had an adverse effect on nonionic surfactant Tween-80 emulsion separation(SEs:94.0%–71.76%).Emulsions made by diverse oils can be effectively separated:octane(SEs:99.4%–100%),rapeseed oil(SEs:97.3%–98.8%),and diesel(SEs:95.2%–97.0%).These findings provide new insights for designing novel materials for oil–water separation by coalescence mechanism.展开更多
The low O^(2-)diffusion rate in the electro-deoxidation of titanium containing compounds by either the OS process or the FFC process leads to a low reaction speed and a low current efficiency.In this study,Ca_(3)Ti_(2...The low O^(2-)diffusion rate in the electro-deoxidation of titanium containing compounds by either the OS process or the FFC process leads to a low reaction speed and a low current efficiency.In this study,Ca_(3)Ti_(2)O_(7) was used as a precursor to improve the reduction speed of titanium.Because of the greater number of"diffusion channels"created in cathode as Ca^(2+) liberates from Ca_(3)Ti_(2)O_(7) precursor in the electrodeoxidation process,the O^(2-)diffusion rate was improved significantly by using Ca_(3)Ti_(2)O_(7) instead of CaTiO3 as precursor.Parallel constant voltage electrolysis(3.2 V)confirms that Ca_(3)Ti_(2)O_(7) and CaTiO3 are reduced simultaneously because of their similar crystal structures.However,the reduction area of Ca_(3)Ti_(2)O_(7) spreads much faster than that of CaTiO3,indicating a difference in the O^(2-) diffusion rate.Constant voltage cyclic voltammetry(CV)and theoretical analysis of the crystal structure were also conducted to compare the differences between Ca_(3)Ti_(2)O_(7) and CaTiO3.The results indicate that using a precursor with a greater number of soluble cations,titanium reduction speed can be greatly improved in the electro-deoxidation process.Finally,a new electrolysis method for converting and recycling excess CaO from the Ca_(3)Ti_(2)O_(7) precursor was proposed.展开更多
A novel and high-efficiency coalescence membrane enhanced by nano-sized polyvinylidene fluoride(PVDF)nanofibers based on polyester(PET)substrate was fabricated using electrospinning method.The properties of the electr...A novel and high-efficiency coalescence membrane enhanced by nano-sized polyvinylidene fluoride(PVDF)nanofibers based on polyester(PET)substrate was fabricated using electrospinning method.The properties of the electrospun nanofibers such as roughness and surface morphology greatly affected the oil droplet interception efficiency and surface wettability of the membrane.A series of coalescence units were prepared with different layers of nanofibrous membrane and the separation efficiencies at different initial concentrations,flow rates,and oil types were tested.It is very interesting that the obtained nanofibrous membrane exhibited superoleophilicity in air but poor oleophilicity under water,which was beneficial to the coalescence process.The coalescence unit with four membrane layers had excellent performances under different initial concentrations and flow rates.The separation efficiency of the 4-layers unit remained above 98.2%when the initial concentration reached up to 2000 mg·L-1.Furthermore,the unit also exhibited good performance with the increasing oil density and viscosity,which is promising for large-scale oil wastewater treatment.展开更多
In light of the increasing demand for environmental protection and energy conservation,the recovery of highly valuable metals,such as Li,Co,and Ni,from spent lithium-ion batteries(LIBs)has attracted widespread attenti...In light of the increasing demand for environmental protection and energy conservation,the recovery of highly valuable metals,such as Li,Co,and Ni,from spent lithium-ion batteries(LIBs)has attracted widespread attention.Most conventional recycling strategies,however,suffer from a lack of lithium recycling,although they display high efficiency in the recovery of Co and Ni.In this work,we report an efficient extraction process of lithium from the spent LIBs by using a functional imidazolium ionic liquid.The extraction efficiency can be reached to 92.5%after a three-stage extraction,while the extraction efficiency of Ni-Co-Mn is less than 4.0%.The new process shows a high selectivity of lithium ion.FTIR spectroscopy and ultraviolet are utilized to characterize the variations in the functional groups during extraction to reveal that the possible extraction mechanism is cation exchange.The results of this work provide an effective and sustainable strategy of lithium recycling from spent LIBs.展开更多
Studies on the degradation process of waste polyethylene terephthalate(PET)have become increasingly mature,but there are relatively few studies on the separation of degradation products.The products contain many compo...Studies on the degradation process of waste polyethylene terephthalate(PET)have become increasingly mature,but there are relatively few studies on the separation of degradation products.The products contain many components and the separation of which is difficult.Therefore,the study on phase equilibrium thermodynamics of bis-2-hydroxyethyl terephthalate(BHET)is of great theoretical significance and practical value to provide basic data for the BHET crystallization separation.In this work,the degraded products were purified and characterized.The solubility of BHET in methanol,ethanol,ethylene glycol,water and the mixture of ethylene glycol+water were determined by static method.The experimental results were correlated with different models,such as ideal solution(IS)model,λh equation,Apelblat equation and NRTL model.Based on the van’t Hoff equation,the mixing Gibbs energy,enthalpy and entropy were calculated.From this work,the basic data which can be used to guide the crystallization process of BHET were obtained,including solubility data,correlation model and thermodynamic properties.展开更多
基金the financial support by the National Science Foundation of China(51822706 and 52107234)Beijing Natural Science Foundation(JQ19012)+2 种基金the DNL Cooperation Fund,CAS(DNL201912 and DNL201915)Innovation Academy for Green Manufacture Fund(IAGM2020C02)Youth Innovation Promotion Association,CAS(Y2021052).
文摘Lithium-ion capacitors(LICs) combining the advantages of lithium-ion batteries and supercapacitors are considered a promising nextgeneration energy storage device. However, the sluggish kinetics of battery-type anode cannot match the capacitor-type cathode, restricting the development of LICs. Herein, hierarchical carbon framework(HCF) anode material composed of 0D carbon nanocage bridged with 2D graphene network are developed via a template-confined synthesis process. The HCF with nanocage structure reduces the Li^(+) transport path and benefits the rapid Li^(+) migration, while 2D graphene network can promote the electron interconnecting of carbon nanocages. In addition, the doped N atoms in HCF facilitate to the adsorption of ions and enhance the pseudo contribution, thus accelerate the kinetics of the anode. The HCF anode delivers high specific capacity, remarkable rate capability. The LIC pouch-cell based on HCF anode and active HCF(a-HCF) cathode can provide a high energy density of 162 Wh kg^(-1) and a superior power density of 15.8 kW kg^(-1), as well as a long cycling life exceeding 15,000cycles. This study demonstrates that the well-defined design of hierarchical carbon framework by incorporating 0D carbon nanocages and 2D graphene network is an effective strategy to promote LIC anode kinetics and hence boost the LIC electrochemical performance.
基金supported by the National Natural Science Foundation of China (21878318, 22108285)the DNL Cooperation Fund, CAS (DNL201902)+2 种基金“Transformational Technologies for Clean Energy and Demonstration”, Strategic Priority Research Program of the Chinese Academy of Sciences (CAS) (XDA21060400)Shandong Energy Institute, Single-Cell Center Project (SCZ-16, SCZ17)Director Innovation Fund of Synthetic Biology Technology Innovation Center of Shandong Province (sdsynbio-2020-ZH-02)。
文摘Solid physical properties are vital for the design, optimization, and scale-up of gas–liquid–solid multiphase reactors. The complex and interactional effects of the solid physical properties, including particle diameter, density, wettability, and sphericity, on the hydrodynamic behaviors in a new external airlift loop reactor(EALR) integrating mixing and separation are decoupled in this work. Two semi-empirical equations are proposed and validated to predict the overall gas holdup and liquid circulating velocity satisfactorily, and then the individual influence of such solid physical properties is further investigated. The results demonstrate that both the overall gas holdup in the riser and the liquid circulating velocity in the downcomer increase with the contact angle, but decrease with particle size, density, and sphericity.Additionally, the impact of the particle size on the liquid circulating velocity is also profoundly revealed on a micro-level considering the particle size distribution. Moreover, the axial solid concentration distribution is discussed, and the uniformity of the slurry is described by the mixing index of the solid particles. The results show that a more homogeneous mixture can be achieved by adding finer particles other than attaining violent turbulence. Therefore, this work lays a foundation for the design, scale-up, and industrialization of the EALRs.
基金supported by National Key R&D Program of China(2020YFA0710200)the National Natural Science Foundation of China(21838010,22122814)+2 种基金the Youth Innovation Promotion Association of the Chinese Academy of Sciences(2018064)State Key Laboratory of Multiphase complex systems,Institute of Process Engineering,Chinese Academy of Sciences(No.MPCS-2022-A-03)Innovation Academy for Green Manufacture Institute,Chinese Academy of Science(IAGM2020C14).
文摘CO_(2) electroreduction(CO_(2) ER)to high value-added chemicals is considered as a promising technology to achieve sustainable carbon neutralization.By virtue of the progressive research in recent years aiming at design and understanding of catalytic materials and electrolyte systems,the CO_(2) ER performance(such as current density,selectivity,stability,CO_(2) conversion,etc.)has been continually increased.Unfortunately,there has been relatively little attention paid to the large-scale CO 2 electrolyzers,which stand just as one obstacle,alongside series-parallel integration,challenging the practical application of this infant technology.In this review,the latest progress on the structures of low-temperature CO_(2) electrolyzers and scale-up studies was systematically overviewed.The influence of the CO_(2) electrolyzer configurations,such as the flow channel design,gas diffusion electrode(GDE)and ion exchange membrane(IEM),on the CO_(2) ER performance was further discussed.The review could provide inspiration for the design of large-scale CO_(2) electrolyzers so as to accelerate the industrial application of CO_(2) ER technology.
基金financially supported by the Natural Science Foundation of China (Nos.U1610101 and 21776288)the Green Process Manufacturing Innovation Research Institute, Chinese Academy of Sciences (No.IAGM-2019-A09)the funding support from Vinnova (Dn: 2018-05293)。
文摘A type of calcium coke was developed for use in the oxy-thermal process of calcium carbide production.The calcium coke was prepared by the co-pyrolysis of coking coal and calcium carbide slag, which is a solid waste generated from the chlor-alkali industry.The characteristics of the calcium cokes under different conditions were analyzed experimentally and theoretically.The results show that the thermal strength of calcium coke increased with the increase in the coking coal proportion, and the waterproof property of calcium coke also increased with increased carbonation time.The calcium coke can increase the contact area of calcium and carbon in the calcium carbide production process.Furthermore, the pore structure of the calcium coke can enhance the diffusion of gas inside the furnace, thus improving the efficiency of the oxy-thermal technology.
基金supported by the National Natural Science Foundation of China,grant number:U1732267.
文摘The quantitative understanding of how atomic-level catalyst structural changes affect the reactivity of the electrochemical CO_(2)reduction reaction is challenging.Due to the complexity of catalytic systems,conventional in situ X-ray spectroscopy plays a limited role in tracing the underlying dynamic structural changes in catalysts active sites.Herein,operando high-energy resolution fluorescence-detected X-ray absorption spectroscopy was used to precisely identify the dynamic structural transformation of well-defined active sites of a representative model copper(Ⅱ)phthalocyanine catalyst which is of guiding significance in studying single-atom catalysis system.Comprehensive X-ray spectroscopy analyses,including surface sensitive△μspectra which isolates the surface changes by subtracting the disturb of bulk base and X-ray absorption near-edge structure spectroscopy simulation,were used to discover that Cu species aggregated with increasing applied potential,which is responsible for the observed evolution of C_(2)H_(4).The approach developed in this work,characterizing the active-site geometry and dynamic structural change,is a novel and powerful technique to elucidate complex catalytic mechanisms and is expected to con tribute to the rational design of highly effective catalysts.
基金by National Key Research and Development Program of China(No.2019YFA0705600)National Natural Science Foundation of China(No.21706261)+1 种基金Science Fund for Creative Research Groups of the National Natural Science Foundation of China(No.21921005)Beijing Natural Science Foundation(No.L172045).
文摘Lithium slurry flow cell(LSFC)is a novel energy storage device that combines the concept of both lithium ion batteries(LIBs)and flow batteries(FBs).Although it is hoped to inherit the advantages of both LIBs and FBs,such as high energy density,ease of fabrication,environmental friendly,independent energy and power density,to name but a few.While unfortunately,it still has many challenges to overcome before it becoming the future star in energy storage area.Here in this paper,we briefly recall its history and try to illustrate the main issues that hindering its research as well as application.As a typical interdisciplinary product,LSFC is definitely a promising candidate for large scale energy storage application,while obviously it still has a long way to go.
基金Financial support from National Natural Science Foundation of China (22078336, U1662133, 21773158, 22008238)Innovation Academy for Green Manufacture, CAS (IAGM2020C13) is gratefully acknowledged
文摘The Ru-catalyzed carbonylation of alkenes with CO_(2)as a C1 surrogate and imidazole chlorides as the promotor is investigated by a combination of computational and experimental study.The conversion rate of CO_(2)to CO is positively correlated with the efficiency of both hydroesterification and hydroformylation,which is found facilitated in the presence of chloride additives with a decreasing order of BmimCl~B3MimCl>BmmimCl~LiCl.Taking the hydroesterification with MeOH as a representative example,BmimCl bearing C-H functionality at the C^(2)site of the cation assists the reduction of CO_(2)to CO as a hydrogen donor medium,with the anion and cation acting in a synergistic fashion.Subsequent insertion of CO_(2)into the formed Ru-H bond with the assistance of chloride anion produces the Ru-COOH species,which ultimately accelerates the activation of CO_(2).
基金financially supported by the National Natural Science Foundation of China(U1707601)project of Youth Innovation Promotion Association,Chinese Academy of Sciences(2021430)+1 种基金project of Innovation Academy for Green Manufacture,Chinese Academy of Sciences(IAGM2020C26)project of Bureau of International Cooperation,Chinese Academy of Sciences(122363KYSB20190033)。
文摘Efficient and low-cost recycling of spent lithium iron phosphate(LiFePO_(4),LFP)batteries has become an inevitable trend.In this study,an integrated closed-loop recycling strategy including isomorphic substitution leaching and solvent extraction process for spent LFP was proposed.An inexpensive FeCl_(3)was used as leaching agent to directly substitute Fe^(2+)from LFP.99%of Li can be rapidly leached in just 30 min,accompanied by 98%of FePO_(4)precipitated in lixivium.The tri-n-butyl phosphate(TBP)-sulfonated kerosene(SK)system was applied to extract Li from lixivium through a twelve-stage countercurrent process containing synchronous extraction and stepwise stripping of Li^(+)and Fe^(3+).80.81%of Li can be selectively enriched in stripping liquor containing 3.059 mol·L^(-1)of Li^(+)under optimal conditions.And the Fe stripping liquor was recovered for LFP re-leaching,of which,Fe^(2+)was oxidized to Fe^(3+)by appropriate H_(2)O_(2).Raffinate and lixivium were concentrated and entered into extraction process to accomplished closeloop recycling process.Overall,the results suggest that more than 99%of Li was recovered.FeCl_(3)holding in solution was directly regenerated without any pollutant emission.The sustainable mothed would be an alternative candidate for total element recycling of spent LFP batteries with industrial potential.
基金the National Natural Science Foundation of China(Nos.51974287 and 21736010)Innovation Academy for Green Manufacture,Chinese Academy of Sciences(No.IAGM-2019-A11).
文摘Magnetization roasting is one of the most effective way of utilizing low-grade refractory iron ore.However,the reduction roasting of siderite(FeCO3)generates weakly magnetic wüstite,thus reducing iron recovery via weak magnetic separation.We systematically studied and proposed the fluidized preoxidation-low-temperature reduction magnetization roasting process for siderite.We found that the maghemite generated during the air oxidation roasting of siderite would be further reduced into wüstite at 500 and 550℃due to the unstable intermediate product magnetite(Fe_(3)O_(4)).Stable magnetite can be obtained through maghemite reduction only at low temperature.The optimal fluidized magnetization roasting parameters included preoxidation at 610℃for 2.5 min,followed by reduction at 450℃for 5 min.For roasted ore,weak magnetic separation yielded an iron ore concentrate grade of 62.0wt%and an iron recovery rate of 88.36%.Compared with that of conventional direct reduction magnetization roasting,the iron recovery rate of weak magnetic separation had greatly improved by 34.33%.The proposed fluidized preoxidation-low-temperature reduction magnetization roasting process can realize the efficient magnetization roasting utilization of low-grade refractory siderite-containing iron ore without wüstite generation and is unlimited by the proportion of siderite and hematite in iron ore.
基金supported by the National Natural Science Foundation of China(52230002 and 52170118)the Key Research and Development Program of Hebei Province(22373701D)the"Clean Combustion and Low-carbon Utilization of Coal,"Strategic Priority Research Program of the Chinese Academy of Sciences(XDA 29000000)。
文摘As the largest steel-producing country,China’s steel industry has experienced rapid development in terms of production level and quality.Owing to the high consumption of coal in the iron and steel industry,air pollutants and carbon dioxide(CO_(2))show similar emission properties in flue gas.In view of the collaborative reduction of pollution and carbon emissions,the emission standards for pollutants and carbon were first analyzed,suggesting that carbon emission standards for the iron and steel industry should be accelerated.A collaborative technology system for the reduction of pollution and carbon emissions from the iron and steel industry in China is demonstrated,consisting of(1)optimization of present ultra-low emission technology,(2)low-carbon innovation for present production processes,(3)steel production process reengineering,and(4)carbon capture,utilization,and storage(CCUS).Finally,the technical prospect for collaborative reduction of pollution and carbon emissions from the iron and steel industry in China is suggested to support high-quality green development in this industry.
基金support of the Startup Foundation of China(3160011181808)the National Natural Scientific Foundation of China(21878292,81673400)K.C.Wong Education Foundation(GJTD-2018-04).
文摘Chitin is a widely used important industrial polymer mainly from shrimp shells, but its commercial preparation is under the great challenge of serious pollution due to the requirement of HCl and Na OH.Herein, we demonstrated that high purity chitin can be obtained from waste shrimp shells(WSSs) by cascade separation with transition metal salt aqueous solution and ionic liquid(IL). Firstly, calcium carbonate of WSSs was effectively removed in the metal salt aqueous solution driven by the ion exchange interaction. Subsequently, 1-butyl-3-methylimidazolium chloride([Bmim]Cl) had bifunctional abilities to remove residual protein and introduced metal salts simultaneously by hydrogen bonding and coordination interactions. The key experimental factors affecting the separation process were systematically studied, including the type of metal salts, temperature, and [Bmim]Cl loading. After sequential treatment with a 20%(mass) Ni SO4aqueous solution at 130 ℃ and [Bmim]Cl at 150 ℃, the purity of a-chitin can be up to 96.5%(mass) that meets commercial requirements. The use of metal salts with higher coordination ability makes the preparation of chitin no longer depend on the commonly acid-base reaction, which is conducive to the preservation of chitin structure.
基金supported by the National Natural Science Foundation of China (No.52170119)the Youth Innovation Promotion Association of the Chinese Academy of Sciences (No.2021044)。
文摘Carbon dioxide(CO_(2))emissions from the cement industry account for 26%of the total industrial emissions,and the need to develop low-carbon techniques within the cement industry is extremely urgent.Low-carbon projects and technologies for the cement industry in different regions and countries have been thoroughly reviewed in this manuscript,and the low-carbon development concept for each county has been analyzed.For developing countries such as China and India,energy saving and efficiency enhancement are currently the key points,while for developed countries and regions such as Europe,more efforts have been focused on carbon capture,utilization,and storage(CCUS).Global CCUS projects have been previously conducted,and the majority of CCUS projects are currently performed in Europe where major projects such as the CEMCAP,CLEANKER,and IEILAC projects represent the latest research progress in cement production technologies and low-carbon technologies for the global cement industry.The development of low-carbon cement technologies has changed from focusing on the end point to instead focusing on the source and process through the exploration of hydrogen and solar energies,and more disruptive and original technologies are expected to be developed,particularly in the cement industry in China.
基金supported by the National Key Research and Development Program of China(grant No.2020YFC1908805)the National Natural Science Foundation of China(grant Nos.22293024 and 22078330)the Youth Innovation Promotion Association,Chinese Academy of Sciences(grant No.2019050).
文摘By modeling a group of neighboring real particles as a single coarse-grained particle(CGP),discrete particle method(DPM)is now capable of simulating industrial-scale particle-fluid systems.However,a systematic approach to determine the CGP properties and develop their interaction models is still lacking,which casts uncertainty on the predictivity of the method.In this study,collisions between predefined particle groups are analyzed to construct kernel functions for modeling the CGPs and then the model parameters are determined by equating the statistical properties of the CGPs and the real particles in the physical process studied.This approach is implemented for homogeneous cooling of granular gas,then demonstrated effective in simulating experimental fluidized beds.
基金funding by the National Natural Science Foundation of China(No.51978643)Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDA21021102)+2 种基金14th Five-year Informatization Plan of Chinese Academy of Sciences,Construction of Scientific Data Center System(WX145XQ07-12)Youth Innovation Promotion Association,CAS(Y201814)the National Youth Talent Support Program of China
文摘The sustainability of the coking industry is supported by reasonable production profit and environmental quality requirements.The traditional measures substantially increased the related costs for enterprises to reach standards.This paper aims to develop a comprehensive cost combined environmental impact assessment method that is necessary for the analysis of wastewater treatment systems.Typical three coking wastewater treatment processes in China were evaluated.Results showed that eutrophication dominantly contributed to the overall environmental effect.Improving effluent quality could significantly reduce the total environmental impact.In terms of an economic perspective,the price of raw materials was the main factor that affected the operating cost of comprehensive treatment.Based on subsystem analysis,the pretreatment stage accounted for the majority of environmental and cost burdens,respectively reaching 64%-78%and 64%-86%.Optimizing the pretreatment process by enhancing the efficiency of high concentration raw material recovery and substituting toxic raw materials for extractant could reduce the environmental impact and economic cost by 43.8%and 57%,respectively,which was an effective way to improve the potential performance of coking wastewater treatment plants(WWTPs).
基金This work was supported by Basic Frontier Scientific Research of the Chinese Academy of Sciences(ZDBS-LY-JSC041)the National Natural Science Foundation of China(22178348)+1 种基金the open research fund of the State Key Laboratory of Mesoscience and Engineering(MESO-23-D06)the Youth Innovation Promotion Association CAS(292021000085).We also thank Wenchang Wang at Shimadzu(China)for help with the XPS analysis.
文摘MXenes have aroused intensive enthusiasm because of their exotic properties and promising applications.However,to date,they are usually synthesized by etching technologies.Developing synthetic technologies provides more opportunities for innovation and may extend unexplored applications.Here,we report a bottom-up gas-phase synthesis of Cl-terminated MXene(Ti_(2)CCl_(2)).The gas-phase synthesis endows Ti_(2)CCl_(2) with unique surface chemistry,high phase purity,and excellent metallic conductivity,which can be used to accelerate polysulfide conversion kinetics and dramatically prolong the cyclability of Li-S batteries.In-depth mechanistic analysis deciphers the origin of the formation of Ti_(2)CCl_(2) and offers a paradigm for tuning MXene chemical vapor deposition.In brief,the gas-phase synthesis transforms the synthesis of MXenes and unlocks the hardly achieved potentials of MXenes.
基金supported by the National Key Research and Development Program of China under the contract number of 2017YFB0308000Program of Innovation Academy for Green Manufacture,CAS(IAGM2020C04)+1 种基金the State Key Laboratory of Heavy Oil Processing(SKLOP201903001)Key Research and Development Program of Hebei Province,China(20374001D)。
文摘Discharging untreated oily wastewater into the environment disrupts the ecological balance,which is a global problem that requires urgent solutions.Superhydrophilic and superoleophilic fibrous medium(FM)effectively separated oil–water emulsion as it was hydrophobic underwater.But its separation efficiencies(SEs)first increased to 98.9%,then dropped to 97.6%in 10 min because of oil-fouling.To tackle this problem,FM deposited with 0%–10%silica nanoparticle(NPsFMs),then coated by fluorocarbon polymer(X-[CH_(2)CH_(2)O]nCH_(2)CH_(2)O-Y-NH-COOCH_(2)C4F9)(FCNPs FMs),was used to enhance its roughness and regulate its initial wettability to improve the anti-fouling property.FCFM and FCNPs FMs were hydrophobic and oleophobic in air and oleophobic underwater.Their water contact angles,oil contact angles and oil contact angles were 115.3°–121.1°,128.8°–136.5°,and 131.6°–136.7°,respectively,meeting the requirement of 90°–140°for coalescence separation.FCNPs FM-5 had the best separation performance with a constant value of 99.8%in 10 min,while that of FCNPs FM-10 slightly decreased to 99.5%.Theoretical released droplet(TRD)diameter,calculated by the square root of the product of pore radius and fiber diameter,was used for the evaluation of coalescence performance.Analyzed by two ideal models,TRD diameter and fiber diameter showed a parabola type relationship,proving that the separation efficiency was a collaborative work of wettability,pore size and fiber diameter.Also,it explained the SEs reduction from FCNPs FM-5 to FCNPs FM-10 was revelent to the three parameters.Moreover,FCNPsFMs effectively separated emulsions stabilized by cationic surfactant CTAB(SEs:97.3%–98.4%)and anionic surfactant SDBS(SEs:91.3%–93.4%).But they had an adverse effect on nonionic surfactant Tween-80 emulsion separation(SEs:94.0%–71.76%).Emulsions made by diverse oils can be effectively separated:octane(SEs:99.4%–100%),rapeseed oil(SEs:97.3%–98.8%),and diesel(SEs:95.2%–97.0%).These findings provide new insights for designing novel materials for oil–water separation by coalescence mechanism.
基金the National Natural Science Foundation of China(Nos.51604255 and U1702251)。
文摘The low O^(2-)diffusion rate in the electro-deoxidation of titanium containing compounds by either the OS process or the FFC process leads to a low reaction speed and a low current efficiency.In this study,Ca_(3)Ti_(2)O_(7) was used as a precursor to improve the reduction speed of titanium.Because of the greater number of"diffusion channels"created in cathode as Ca^(2+) liberates from Ca_(3)Ti_(2)O_(7) precursor in the electrodeoxidation process,the O^(2-)diffusion rate was improved significantly by using Ca_(3)Ti_(2)O_(7) instead of CaTiO3 as precursor.Parallel constant voltage electrolysis(3.2 V)confirms that Ca_(3)Ti_(2)O_(7) and CaTiO3 are reduced simultaneously because of their similar crystal structures.However,the reduction area of Ca_(3)Ti_(2)O_(7) spreads much faster than that of CaTiO3,indicating a difference in the O^(2-) diffusion rate.Constant voltage cyclic voltammetry(CV)and theoretical analysis of the crystal structure were also conducted to compare the differences between Ca_(3)Ti_(2)O_(7) and CaTiO3.The results indicate that using a precursor with a greater number of soluble cations,titanium reduction speed can be greatly improved in the electro-deoxidation process.Finally,a new electrolysis method for converting and recycling excess CaO from the Ca_(3)Ti_(2)O_(7) precursor was proposed.
基金supported by the National Key Research and Development Program of China(No.2017YFB0308000)the National Natural Science Foundation of China(No.21706259)+3 种基金the State Key Laboratory of Heavy Oil Processing(SKLOP201903001)Guizhou Science Technology Support Program([2019]2839)the Natural Science Youth Foundation of Shanxi Province(No.201701D221033)Program of Innovation Academy for Green Manufacture,CAS(IAGM2020C04)。
文摘A novel and high-efficiency coalescence membrane enhanced by nano-sized polyvinylidene fluoride(PVDF)nanofibers based on polyester(PET)substrate was fabricated using electrospinning method.The properties of the electrospun nanofibers such as roughness and surface morphology greatly affected the oil droplet interception efficiency and surface wettability of the membrane.A series of coalescence units were prepared with different layers of nanofibrous membrane and the separation efficiencies at different initial concentrations,flow rates,and oil types were tested.It is very interesting that the obtained nanofibrous membrane exhibited superoleophilicity in air but poor oleophilicity under water,which was beneficial to the coalescence process.The coalescence unit with four membrane layers had excellent performances under different initial concentrations and flow rates.The separation efficiency of the 4-layers unit remained above 98.2%when the initial concentration reached up to 2000 mg·L-1.Furthermore,the unit also exhibited good performance with the increasing oil density and viscosity,which is promising for large-scale oil wastewater treatment.
基金supported by the Science Fund for Major Program of National Natural Science Foundation of China(21890762)Innovation Academy for Green Manufacture,Chinese Academy of Sciences(IAGM-2020-C28).
文摘In light of the increasing demand for environmental protection and energy conservation,the recovery of highly valuable metals,such as Li,Co,and Ni,from spent lithium-ion batteries(LIBs)has attracted widespread attention.Most conventional recycling strategies,however,suffer from a lack of lithium recycling,although they display high efficiency in the recovery of Co and Ni.In this work,we report an efficient extraction process of lithium from the spent LIBs by using a functional imidazolium ionic liquid.The extraction efficiency can be reached to 92.5%after a three-stage extraction,while the extraction efficiency of Ni-Co-Mn is less than 4.0%.The new process shows a high selectivity of lithium ion.FTIR spectroscopy and ultraviolet are utilized to characterize the variations in the functional groups during extraction to reveal that the possible extraction mechanism is cation exchange.The results of this work provide an effective and sustainable strategy of lithium recycling from spent LIBs.
基金financially supported by the National Key Research and Development Program of China(2019YFC1908204)the National Natural Scientific Fund of China(No.21878292,21776289,21908232,21978291)+1 种基金Innovation Academy forGreen Manufacture,Chinese Academy of Sciences(No.IAGM2020C12,IAGM2020C21 and IAGM-2019-A06)K.C.Wong Education Foundation(No.GJTD-2018-04)。
文摘Studies on the degradation process of waste polyethylene terephthalate(PET)have become increasingly mature,but there are relatively few studies on the separation of degradation products.The products contain many components and the separation of which is difficult.Therefore,the study on phase equilibrium thermodynamics of bis-2-hydroxyethyl terephthalate(BHET)is of great theoretical significance and practical value to provide basic data for the BHET crystallization separation.In this work,the degraded products were purified and characterized.The solubility of BHET in methanol,ethanol,ethylene glycol,water and the mixture of ethylene glycol+water were determined by static method.The experimental results were correlated with different models,such as ideal solution(IS)model,λh equation,Apelblat equation and NRTL model.Based on the van’t Hoff equation,the mixing Gibbs energy,enthalpy and entropy were calculated.From this work,the basic data which can be used to guide the crystallization process of BHET were obtained,including solubility data,correlation model and thermodynamic properties.
