A new model of particle yield stress including cohesive strength is proposed,which considers the friction and cohesive strength between particles.A calculation method for the fluidization process of liquid–solid two-...A new model of particle yield stress including cohesive strength is proposed,which considers the friction and cohesive strength between particles.A calculation method for the fluidization process of liquid–solid two-phase flow in compact packing state is given,and the simulation and experimental studies of fluidization process are carried out by taking the sand–water two-phase flow in the jet dredging system as an example,and the calculation method is verified.展开更多
In the past few decades, various surface analysis techniques find wide applications in studies of interfacial phenomena ranging from fundamental surface science,catalysis, environmental science and energy materials.Wi...In the past few decades, various surface analysis techniques find wide applications in studies of interfacial phenomena ranging from fundamental surface science,catalysis, environmental science and energy materials.With the help of bright synchrotron sources, many of these techniques have been further advanced into novel in-situ/operando tools at synchrotron user facilities, providing molecular level understanding of chemical/electrochemical processes in-situ at gas–solid and liquid–solid interfaces.Designing a proper endstation for a dedicated beamline is one of the challenges in utilizing these techniques efficiently for a variety of user's requests. Many factors,including pressure differential, geometry and energy of the photon source, sample and analyzer, need to be optimized for the system of interest. In this paper, we discuss the design and performance of a new endstation at beamline02 B at the Shanghai Synchrotron Radiation Facility for ambient pressure X-ray photoelectron spectroscopy studies.This system, equipped with the newly developed hightransmission HiPP-3 analyzer, is demonstrated to be capable of efficiently collecting photoelectrons up to 1500 eV from ultrahigh vacuum to ambient pressure of 20 mbar.The spectromicroscopy mode of HiPP-3 analyzer also enables detection of photoelectron spatial distribution with resolution of 2.8 ± 0.3 lm in one dimension. In addition,the designing strategies of systems that allow investigations in phenomena at gas–solid interface and liquid–solid interface will be highlighted through our discussion.展开更多
A cold-model vertical multi-tube circulating fluidized bed evaporator was designed and built to conduct a visualization study on the pressure drop of a liquid–solid two-phase flow and the corresponding particle distr...A cold-model vertical multi-tube circulating fluidized bed evaporator was designed and built to conduct a visualization study on the pressure drop of a liquid–solid two-phase flow and the corresponding particle distribution.Water and polyformaldehyde particle(POM)were used as the liquid and solid phases,respectively.The effects of operating parameters such as the amount of added particles,circulating flow rate,and particle size were systematically investigated.The results showed that the addition of the particles increased the pressure drop in the vertical tube bundle.The maximum pressure drop ratios were 18.65%,21.15%,18.00%,and 21.15%within the experimental range of the amount of added particles for POM1,POM2,POM3,and POM4,respectively.The pressure drop ratio basically decreased with the increase in the circulating flow rate but fluctuated with the increase in the amount of added particles and particle size.The difference in pressure drop ratio decreased with the increase in the circulating flow rate.As the amount of added particles increased,the difference in pressure drop ratio fluctuated at low circulating flow rate but basically decreased at high circulating flow rate.The pressure drop in the vertical tube bundle accounted for about 70%of the overall pressure drop in the up-flow heating chamber and was the main component of the overall pressure within the experimental range.Three-dimensional phase diagrams were established to display the variation ranges of the pressure drop and pressure drop ratio in the vertical tube bundle corresponding to the operating parameters.The research results can provide some reference for the application of the fluidized bed heat transfer technology in the industry.展开更多
As for the coal seam with high stress,high gas and low permeability,a single technology cannot prevent the complex dynamic disasters.Because of this,the study proposes a new method of pressure-relief and permeability-...As for the coal seam with high stress,high gas and low permeability,a single technology cannot prevent the complex dynamic disasters.Because of this,the study proposes a new method of pressure-relief and permeability-increase technology of the high liquid–solid coupling blast.Through coal seam injection and charging structure change,the paper fully works out the dual functions of the water and explosion.Using the theoretical calculation,numerical simulation and physical experiments,we obtained that the initial blasting stress,displacement and overpressure of the liquid–solid coupling blast are much better than that of ordinary blasting.The technology has been used in the relative coal mine,and the application results show that the technique has effectively prevented the coal and gas outburst,which has a wide range of application.展开更多
The structural transformation from a liquid into a crystalline solid is an important subject in condensed matter physics and materials science. In the present study, first-principles molecular dynamics calculations ar...The structural transformation from a liquid into a crystalline solid is an important subject in condensed matter physics and materials science. In the present study, first-principles molecular dynamics calculations are performed to investigate the structure and properties of aluminum during the solidification which is induced by cooling and compression. In the cooling process and compression process, it is found that the icosahedral short-range order is initially enhanced and then begin to decay, the face-centered cubic short-range order eventually becomes dominant before it transforms into a crystalline solid.展开更多
The widespread adoption of lithium-ion batteries has been driven by the proliferation of portable electronic devices and electric vehicles,which have increasingly stringent energy density requirements.Lithium metal ba...The widespread adoption of lithium-ion batteries has been driven by the proliferation of portable electronic devices and electric vehicles,which have increasingly stringent energy density requirements.Lithium metal batteries(LMBs),with their ultralow reduction potential and high theoretical capacity,are widely regarded as the most promising technical pathway for achieving high energy density batteries.In this review,we provide a comprehensive overview of fundamental issues related to high reactivity and migrated interfaces in LMBs.Furthermore,we propose improved strategies involving interface engineering,3D current collector design,electrolyte optimization,separator modification,application of alloyed anodes,and external field regulation to address these challenges.The utilization of solid-state electrolytes can significantly enhance the safety of LMBs and represents the only viable approach for advancing them.This review also encompasses the variation in fundamental issues and design strategies for the transition from liquid to solid electrolytes.Particularly noteworthy is that the introduction of SSEs will exacerbate differences in electrochemical and mechanical properties at the interface,leading to increased interface inhomogeneity—a critical factor contributing to failure in all-solidstate lithium metal batteries.Based on recent research works,this perspective highlights the current status of research on developing high-performance LMBs.展开更多
The performance sensitivity of the solid‐state lithium cells to the synergistic interactions of the charge‐transport and mechanical properties of the electrolyte is well acknowledged in the literature,but the quanti...The performance sensitivity of the solid‐state lithium cells to the synergistic interactions of the charge‐transport and mechanical properties of the electrolyte is well acknowledged in the literature,but the quantitative insights therein are very limited.Here,the charge‐transport and mechanical properties of a polymerized ionic‐liquid‐based solid electrolyte are reported.The transference number and diffusion coefficient of lithium in the concentrated solid electrolyte are measured as a function of concentration and stack pressure.The elastoplastic behavior of the electrolyte is quantified under compression,within a home‐made setup,to substantiate the impact of stack pressure on the stability of the Li/electrolyte interface in the symmetric lithium cells.The results spotlight the interaction between the concentration and thickness of the solid electrolyte and the stack pressure in determining the polarization and stability of the solid‐state lithium batteries during extended cycling.展开更多
Solid polymer electrolytes(SPEs)have emerged as one of the most promising candidates for building solid-state lithium batteries due to their excellent flexibility,scalability,and interfacial compatibility with electro...Solid polymer electrolytes(SPEs)have emerged as one of the most promising candidates for building solid-state lithium batteries due to their excellent flexibility,scalability,and interfacial compatibility with electrodes.However,the low ionic conductivity and poor cyclic stability of SPEs do not meet the requirements for practical applications of lithium batteries.Here,a novel polymer dispersed ionic liquid-based solid polymer electrolyte(PDIL-SPE)is fabricated using the in situ polymerization-induced phase separation(PIPS)method.The as-prepared PDIL-SPE possesses both outstanding ionic conductivity(0.74 mS cm^(-1) at 25℃)and a wide electrochemical window(up to 4.86 V),and the formed unique three-dimensional(3D)co-continuous structure of polymer matrix and ionic liquid in PDIL-SPE can promote the transport of lithium ions.Also,the 3D co-continuous structure of PDIL-SPE effectively accommodates the severe volume expansion for prolonged lithium plating and stripping processes over 1000 h at 0.5 mA cm^(-2) under 25℃.Moreover,the LiFePO_(4)//Li coin cell can work stably over 150 cycles at a 1 C rate under room temperature with a capacity retention of 90.6%from 111.1 to 100.7 mAh g^(-1).The PDIL-SPE composite is a promising material system for enabling the ultrastable operation of solid-state lithium-metal batteries.展开更多
Li(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO) solid garnet-type electrolyte has been widely reported due to its outstanding safety and electrochemical stability.However,the inherent rigidity and brittleness of LLZTO lead...Li(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO) solid garnet-type electrolyte has been widely reported due to its outstanding safety and electrochemical stability.However,the inherent rigidity and brittleness of LLZTO lead to poor contact with anode/cathode and the operation failure of full cells.Herein,the dual-interlayers are constructed as the fast interfacial ion-migration channel by using Ti_(3)C_(2)T_(x)(MXene,Txis-O,-OH,-F) with trace ionic liquid(IL),which promote the intimate contact between LLZTO and anode/cathode and suppress Li-dendrites growth.Notably,IL can wet the cathode to promote intimate interface contact and be decomposed into some inorganic compounds(such as Li3N,LiF,and Li2Sx),resulting in reduced interfacial resistance and fast Li-ion transportation.Consequently,in the prepared Li-symmetric cell,the interfacial resistance on the anode side plunges to 33.1 Ω cm^(-2),and stably maintains over 1000 h without short circuit at 0.05 mA cm^(-2).The full cell of Li|LiFePO4delivers a high initial capacity of 158.52 mA h g^(-1)and outstanding retention of 90.18% after 100 cycles at 60℃ and 0.2 C.Our work provides an efficient strategy to design dual-interlayers between LLZTO and anode/cathode for the interfacial modification to enhance the performance of solid garnet batteries.展开更多
Thermal rectification refers to the phenomenon by which the magnitude of the heat flux in one direction is much larger than that in the opposite direction.In this study,we propose to implement the thermal rectificatio...Thermal rectification refers to the phenomenon by which the magnitude of the heat flux in one direction is much larger than that in the opposite direction.In this study,we propose to implement the thermal rectification phenomenon in an asymmetric solid–liquid–solid sandwiched system with a nano-structured interface.By using the non-equilibrium molecular dynamics simulations,the thermal transport through the solid–liquid–solid system is examined,and the thermal rectification phenomenon can be observed.It is revealed that the thermal rectification effect can be attributed to the significant difference in the interfacial thermal resistance between Cassie and Wenzel states when reversing the temperature bias.In addition,effects of the liquid density,solid–liquid bonding strength and nanostructure size on the thermal rectification are examined.The findings may provide a new way for designs of certain thermal devices.展开更多
Improving the long-term cycling stability and energy density of all-solid-state lithium(Li)-metal batteries(ASSLMBs)at room temperature is a severe challenge because of the notorious solid–solid interfacial contact l...Improving the long-term cycling stability and energy density of all-solid-state lithium(Li)-metal batteries(ASSLMBs)at room temperature is a severe challenge because of the notorious solid–solid interfacial contact loss and sluggish ion transport.Solid electrolytes are generally studied as two-dimensional(2D)structures with planar interfaces,showing limited interfacial contact and further resulting in unstable Li/electrolyte and cathode/electrolyte interfaces.Herein,three-dimensional(3D)architecturally designed composite solid electrolytes are developed with independently controlled structural factors using 3D printing processing and post-curing treatment.Multiple-type electrolyte films with vertical-aligned micro-pillar(p-3DSE)and spiral(s-3DSE)structures are rationally designed and developed,which can be employed for both Li metal anode and cathode in terms of accelerating the Li+transport within electrodes and reinforcing the interfacial adhesion.The printed p-3DSE delivers robust long-term cycle life of up to 2600 cycles and a high critical current density of 1.92 mA cm^(−2).The optimized electrolyte structure could lead to ASSLMBs with a superior full-cell areal capacity of 2.75 mAh cm^(−2)(LFP)and 3.92 mAh cm^(−2)(NCM811).This unique design provides enhancements for both anode and cathode electrodes,thereby alleviating interfacial degradation induced by dendrite growth and contact loss.The approach in this study opens a new design strategy for advanced composite solid polymer electrolytes in ASSLMBs operating under high rates/capacities and room temperature.展开更多
The multiphase flow characteristic is one of the most concerning problems during solid fluidization exploitation of marine natural gas hydrate reservoirs.In this research,a new transient gas-liquid-solid multiphase fl...The multiphase flow characteristic is one of the most concerning problems during solid fluidization exploitation of marine natural gas hydrate reservoirs.In this research,a new transient gas-liquid-solid multiphase flow model with hydrate phase transition was developed.Meanwhile,this model considered the coupling relationship among convective heat transfer,hydrate dynamic decomposition,and multi-phase flow.The model can simulate the change of flow pattern from solid-liquid to gas-liquid-solid flow,and describe the distribution character of volume fraction of phase,wellbore temperature and pressure,and hydrate decomposition rate during transportation.The simulation results indicate that the hydrate decomposition region in the wellbore gradually expands,but the hydrate decomposition rate gradually decreases during the solid fluidization exploitation of hydrate.When mining time lasts for 4 h,and the bottom hole pressure decreases by about 0.4 MPa.Increasing NaCl concentration in seawater helps expand hydrate decomposition regions and improves the wellbore hydrate decomposition rate.When the Nacl mass fraction in seawater reaches 15%,it will raise the hydrate decomposition regions to the whole wellbore.In addition,the higher the wellhead backpressure,the lower the decomposition area and decomposition rate of hydrate in the wellbore.When wellhead backpressure reaches 2 MPa,the volume fraction of gas near the wellhead will reduce to about 12%.This work is expected to provide a theoretical basis for the development of marine hydrate reservoirs.展开更多
Developing efficient and stable cathodes for low-temperature solid oxide fuel cells(LT-SOFCs) is of great importance for the practical commercialization.Herein,we propose a series of Sm-modified Bi_(0.7-x)Sm_xSr_(0.3)...Developing efficient and stable cathodes for low-temperature solid oxide fuel cells(LT-SOFCs) is of great importance for the practical commercialization.Herein,we propose a series of Sm-modified Bi_(0.7-x)Sm_xSr_(0.3)FeO_(3-δ) perovskites as highly-active catalysts for LT-SOFCs.Sm doping can significantly enhance the electrocata lytic activity and chemical stability of cathode.At 600℃,Bi_(0.675)Sm_(0.025)Sr_(0.3)FeO_(3-δ)(BSSF25) cathode has been found to be the optimum composition with a polarization resistance of 0.098 Ω cm^2,which is only around 22.8% of Bi_(0.7)Sr_(0.3)FeO_(3-δ)(BSF).A full cell utilizing BSSF25 displays an exceptional output density of 790 mW cm^(-2),which can operate continuously over100 h without obvious degradation.The remarkable electrochemical performance observed can be attributed to the improved O_(2) transport kinetics,superior surface oxygen adsorption capacity,as well as O_(2)p band centers in close proximity to the Fermi level.Moreover,larger average bonding energy(ABE) and the presence of highly acidic Bi,Sm,and Fe ions restrict the adsorption of CO_(2) on the cathode surface,resulting in excellent CO_(2) resistivity.This work provides valuable guidance for systematic design of efficient and durable catalysts for LT-SOFCs.展开更多
Since the advent of the solid-state batteries,employing solid polymer electrolytes(SPEs)to replace routine flammable liquid electrolytes is regarded to be one of the most promising solutions in pursing highenergy-dens...Since the advent of the solid-state batteries,employing solid polymer electrolytes(SPEs)to replace routine flammable liquid electrolytes is regarded to be one of the most promising solutions in pursing highenergy-density battery systems.SPEs with superior thermal stability,good processability,and high mechanical modulus obtain increasing attentions.However,SPE-based batteries are not impenetrable due to their decomposition and combustibility under extreme conditions.Researchers believe incorporating appropriate flame-retardant additives/solvents/fragments into SPEs can intrinsically reduce their flammability to solve the battery safety issues.In this review,the recent research progress of incombustible SPEs,with special emphasis on flame-retardant structural design,is summarized.Specifically,a brief introduction of flame-retardant mechanism,evaluation index for safety of SPEs,and a detailed overview of the latest advances on diverse-types SPEs in various battery systems are highlighted.The deep insight into thermal ru naway process,the free-standing incombustible GPEs,and the ratio nal design of pouch cell structures may be the main directions to motivate revolutionary next-generation for safety batteries.展开更多
The ionic liquid(IL) 1-butyl-3-methylimidazolium tetrafluoroborate treated with radiofrequency plasma is proposed for functionalization and immobilization on polyethersulfone supports to form supported ionic liquid me...The ionic liquid(IL) 1-butyl-3-methylimidazolium tetrafluoroborate treated with radiofrequency plasma is proposed for functionalization and immobilization on polyethersulfone supports to form supported ionic liquid membranes for CO_(2) separation.The effects of treatment time and transmembrane pressure difference on CO_(2) permeance were evaluated.The best gas permeation performance was obtained with a treatment time of 10 min and the transmembrane pressure difference was 0.25 MPa.Characterization of the materials by Fourier transform infrared spectroscopy,x-ray photoelectron spectroscopy and nuclear magnetic resonance spectroscopy demonstrates that the IL is grafted with carboxyl groups and deprotonated through plasma treatment.A preliminary mechanism for the plasma treatment and facilitated transport of CO_(2)has been proposed on this basis.展开更多
1.Introduction Cities are responsible for approximately 70%of all anthropogenic greenhouse gas(GHG)emissions and about 60%of all anthropogenic methane(CH4)emissions[1,2].Solid waste disposal sites(including landfills ...1.Introduction Cities are responsible for approximately 70%of all anthropogenic greenhouse gas(GHG)emissions and about 60%of all anthropogenic methane(CH4)emissions[1,2].Solid waste disposal sites(including landfills and dumpsites),which are prevalent in global cities,emit CH4 generated from the anaerobic biodegradation of municipal solid waste(MSW).Notably,the proportions of CH4 emissions from disposal sites surpass 50%of the total CH4 emissions in some megalopolises[3].CH4 has a high global warming potential(GWP),being 28 times stronger than carbon dioxide(CO_(2))over a 100-year period and 80 times stronger over a 20-year period[4].Understanding and mitigating CH4 emissions from solid waste disposal sites is particularly pertinent and pressing,considering that the latest Synthesis Report from the Intergovernmental Panel on Climate Change(IPCC)emphasizes that the current pace of mitigation and adaptation policies and measures falls short of restraining global temperature rise to under 1.5℃ within the 21st century[4].More than 150 countries signed the Global Methane Pledge at the United Nations Climate Change Conference in Glasgow(COP26),which aims to reduce global annual CH4 emissions by 30%by 2030,compared with emissions in 2020[5].展开更多
CO_(2) electrochemical reduction(CO_(2)ER)is an important research area for carbon neutralization.However,available catalysts for CO_(2) reduction are still characterized by limited stability and activity.Recently,met...CO_(2) electrochemical reduction(CO_(2)ER)is an important research area for carbon neutralization.However,available catalysts for CO_(2) reduction are still characterized by limited stability and activity.Recently,metallic bismuth(Bi)has emerged as a promising catalyst for CO_(2) ER.Herein,we report the solid cathode electroreduction of commercial micronized Bi2O3as a straightforward approach for the preparation of nanostructured Bi.At-1.1 V versus reversible hydrogen electrode in a KHCO3aqueous electrolyte,the resulting nanostructure Bi delivers a formate current density of~40 mA·cm^(-2) with a current efficiency of~86%,and the formate selectivity reaches97.6% at-0.78 V.Using nanosized Bi2O3as the precursor can further reduce the primary particle sizes of the resulting Bi,leading to a significantly increased formate selectivity at relatively low overpotentials.The high catalytic activity of nanostructured Bi is attributable to the ultrafine and interconnected Bi nanoparticles in the nanoporous structure,which exposes abundant active sites for CO_(2) electrocatalytic reduction.展开更多
An efficient mass transfer process is a critical factor for regulating catalytic activity in a photocatalytic desulfurization system.Herein,a phosphotungstic acid(HPW)active center is successfully composited with a qu...An efficient mass transfer process is a critical factor for regulating catalytic activity in a photocatalytic desulfurization system.Herein,a phosphotungstic acid(HPW)active center is successfully composited with a quaternary ammonium phosphotungstate-based hexadecyltrimethylammonium chloride ionic liquid(CTAC-HPW)by the ion exchange method for the photocatalytic oxidative desulfurization of dibenzothiophene sulfide.The keggin structure of HPW and highly mass transfer performance of organic cations synergistically enhanced the photocatalytic activity towards the effective convertion of dibenzothiophene(DBT)with the excitation of visible light.The deep desulfurization(<10 mg·kg^(-1))is attained within 30 min,and well stability is demonstrated within 25 cycles.Moreover,the CTAC-HPW photocatalyst projects well selectivity to interference from coexisting compounds such as olefins and aromatic hydrocarbons and universality of dibenzothiophenes,for example,4-methyldibenzothiophene(4-MDBT)and 4,6-dimethyldibenzothiophene(4,6-DMDBT).Ultimately,a possible photocatalytic desulfurization mechanism is proposed according to the Gaschromatography-mass spectrometry(GC-MS),proving that the final product is the corresponding sulfone.The trapping experiment and electron spin resonance(ESR)analysis confirmed that h^(+)and,COOH played critical roles in the oxidation process.The work offers a practicable strategy for efficiently converting DBT to DBTO_(2) with added value.展开更多
A method of analysis for the simultaneous determination of methylisothiazolinone (MI), methylchloroisothiazolinone (CMI), benzisothiazolinone (BIT) and Bronopol (BNP) in washing-up liquid was established. The method c...A method of analysis for the simultaneous determination of methylisothiazolinone (MI), methylchloroisothiazolinone (CMI), benzisothiazolinone (BIT) and Bronopol (BNP) in washing-up liquid was established. The method consisted of a gradient HPLC analysis at three different wavelengths. The four compounds could be analyzed with good precision and accuracy.展开更多
Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid electrolytes.Cross-linked pol...Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid electrolytes.Cross-linked polymers have the potential to further improve the mechanical property without trading off Li-ion conductivity.In this study,focusing on a recently developed cross-linked SPE,i.e.,the one based on poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network(PVCN),we used solid-state nuclear magnetic resonance(NMR)techniques to investigate the fundamental interaction between the chain segments and Li ions,as well as the lithium-ion motion.By utilizing homonuclear/heteronuclear correlation,CP(cross-polarization)kinetics,and spin-lattice relaxation experiments,etc.,we revealed the structural characteristics and their relations to lithium-ion mobilities.It is found that the network formation prevents poly(ethylene oxide)chains from crystallization,which could create sufficient space for segmental tumbling and Li-ion co nductio n.As such,the mechanical property is greatly improved with even higher Li-ion mobilities compared to the poly(vinylene carbonate)or poly(ethylene oxide)based SPE analogues.展开更多
基金Project supported by the National Natural Science Foundation of China(Grant No.11772046)the Young Scientists Fund of the National Natural Science Foundation of China(Grant No.51705342)
文摘A new model of particle yield stress including cohesive strength is proposed,which considers the friction and cohesive strength between particles.A calculation method for the fluidization process of liquid–solid two-phase flow in compact packing state is given,and the simulation and experimental studies of fluidization process are carried out by taking the sand–water two-phase flow in the jet dredging system as an example,and the calculation method is verified.
基金supported by the National Natural Science Foundation of China(No.11227902)part of NSFC ME~2 beamline project and Science and Technology Commission of Shanghai Municipality(No.14520722100)supported by National Natural Science Foundation of China(Nos.21802096,21832004,and11805255)
文摘In the past few decades, various surface analysis techniques find wide applications in studies of interfacial phenomena ranging from fundamental surface science,catalysis, environmental science and energy materials.With the help of bright synchrotron sources, many of these techniques have been further advanced into novel in-situ/operando tools at synchrotron user facilities, providing molecular level understanding of chemical/electrochemical processes in-situ at gas–solid and liquid–solid interfaces.Designing a proper endstation for a dedicated beamline is one of the challenges in utilizing these techniques efficiently for a variety of user's requests. Many factors,including pressure differential, geometry and energy of the photon source, sample and analyzer, need to be optimized for the system of interest. In this paper, we discuss the design and performance of a new endstation at beamline02 B at the Shanghai Synchrotron Radiation Facility for ambient pressure X-ray photoelectron spectroscopy studies.This system, equipped with the newly developed hightransmission HiPP-3 analyzer, is demonstrated to be capable of efficiently collecting photoelectrons up to 1500 eV from ultrahigh vacuum to ambient pressure of 20 mbar.The spectromicroscopy mode of HiPP-3 analyzer also enables detection of photoelectron spatial distribution with resolution of 2.8 ± 0.3 lm in one dimension. In addition,the designing strategies of systems that allow investigations in phenomena at gas–solid interface and liquid–solid interface will be highlighted through our discussion.
基金supported by the open foundation of State Key Laboratory of Chemical Engineering (SKL-ChE-18B03)the Municipal Science and Technology Commission of Tianjin (No. 2009ZCKFGX01900)
文摘A cold-model vertical multi-tube circulating fluidized bed evaporator was designed and built to conduct a visualization study on the pressure drop of a liquid–solid two-phase flow and the corresponding particle distribution.Water and polyformaldehyde particle(POM)were used as the liquid and solid phases,respectively.The effects of operating parameters such as the amount of added particles,circulating flow rate,and particle size were systematically investigated.The results showed that the addition of the particles increased the pressure drop in the vertical tube bundle.The maximum pressure drop ratios were 18.65%,21.15%,18.00%,and 21.15%within the experimental range of the amount of added particles for POM1,POM2,POM3,and POM4,respectively.The pressure drop ratio basically decreased with the increase in the circulating flow rate but fluctuated with the increase in the amount of added particles and particle size.The difference in pressure drop ratio decreased with the increase in the circulating flow rate.As the amount of added particles increased,the difference in pressure drop ratio fluctuated at low circulating flow rate but basically decreased at high circulating flow rate.The pressure drop in the vertical tube bundle accounted for about 70%of the overall pressure drop in the up-flow heating chamber and was the main component of the overall pressure within the experimental range.Three-dimensional phase diagrams were established to display the variation ranges of the pressure drop and pressure drop ratio in the vertical tube bundle corresponding to the operating parameters.The research results can provide some reference for the application of the fluidized bed heat transfer technology in the industry.
基金provided by the National Eleventh Five-Year scientific and Technological Support Plan Subject of China (No.2007BAK29B01)the National Natural Science Foundation (No.50534090)+2 种基金the National Key Basic Research Development Program of China (No.2011CB201205)State Key Laboratory of Coal Resources and Mine Safety of China University of Mining Technology of China (No.SKLCRSM08X03)the Youth Science and Technology Fund of China University of Mining and Technology (No.JGY101605)
文摘As for the coal seam with high stress,high gas and low permeability,a single technology cannot prevent the complex dynamic disasters.Because of this,the study proposes a new method of pressure-relief and permeability-increase technology of the high liquid–solid coupling blast.Through coal seam injection and charging structure change,the paper fully works out the dual functions of the water and explosion.Using the theoretical calculation,numerical simulation and physical experiments,we obtained that the initial blasting stress,displacement and overpressure of the liquid–solid coupling blast are much better than that of ordinary blasting.The technology has been used in the relative coal mine,and the application results show that the technique has effectively prevented the coal and gas outburst,which has a wide range of application.
基金Project supported by the National Natural Science Foundation of China(Grant No.51701180)the Foundation of the State Key Laboratory of Coal Conversion,China(Grant No.J22-23-103)。
文摘The structural transformation from a liquid into a crystalline solid is an important subject in condensed matter physics and materials science. In the present study, first-principles molecular dynamics calculations are performed to investigate the structure and properties of aluminum during the solidification which is induced by cooling and compression. In the cooling process and compression process, it is found that the icosahedral short-range order is initially enhanced and then begin to decay, the face-centered cubic short-range order eventually becomes dominant before it transforms into a crystalline solid.
基金This work is supported by the Technologies R&D Program of Huzhou City(No.2022JB01)the Key Research and Development Program of Zhejiang Province(No.2023C01127)the Highstar Corporation HSD20210118.
文摘The widespread adoption of lithium-ion batteries has been driven by the proliferation of portable electronic devices and electric vehicles,which have increasingly stringent energy density requirements.Lithium metal batteries(LMBs),with their ultralow reduction potential and high theoretical capacity,are widely regarded as the most promising technical pathway for achieving high energy density batteries.In this review,we provide a comprehensive overview of fundamental issues related to high reactivity and migrated interfaces in LMBs.Furthermore,we propose improved strategies involving interface engineering,3D current collector design,electrolyte optimization,separator modification,application of alloyed anodes,and external field regulation to address these challenges.The utilization of solid-state electrolytes can significantly enhance the safety of LMBs and represents the only viable approach for advancing them.This review also encompasses the variation in fundamental issues and design strategies for the transition from liquid to solid electrolytes.Particularly noteworthy is that the introduction of SSEs will exacerbate differences in electrochemical and mechanical properties at the interface,leading to increased interface inhomogeneity—a critical factor contributing to failure in all-solidstate lithium metal batteries.Based on recent research works,this perspective highlights the current status of research on developing high-performance LMBs.
基金H2020 LEIT Advanced Materials,Grant/Award Number:875557。
文摘The performance sensitivity of the solid‐state lithium cells to the synergistic interactions of the charge‐transport and mechanical properties of the electrolyte is well acknowledged in the literature,but the quantitative insights therein are very limited.Here,the charge‐transport and mechanical properties of a polymerized ionic‐liquid‐based solid electrolyte are reported.The transference number and diffusion coefficient of lithium in the concentrated solid electrolyte are measured as a function of concentration and stack pressure.The elastoplastic behavior of the electrolyte is quantified under compression,within a home‐made setup,to substantiate the impact of stack pressure on the stability of the Li/electrolyte interface in the symmetric lithium cells.The results spotlight the interaction between the concentration and thickness of the solid electrolyte and the stack pressure in determining the polarization and stability of the solid‐state lithium batteries during extended cycling.
基金supported by the National Key R&D Program of China (2020YFE0100200)the National Natural Science Foundation of China (Grant Nos.51921002,51927806).
文摘Solid polymer electrolytes(SPEs)have emerged as one of the most promising candidates for building solid-state lithium batteries due to their excellent flexibility,scalability,and interfacial compatibility with electrodes.However,the low ionic conductivity and poor cyclic stability of SPEs do not meet the requirements for practical applications of lithium batteries.Here,a novel polymer dispersed ionic liquid-based solid polymer electrolyte(PDIL-SPE)is fabricated using the in situ polymerization-induced phase separation(PIPS)method.The as-prepared PDIL-SPE possesses both outstanding ionic conductivity(0.74 mS cm^(-1) at 25℃)and a wide electrochemical window(up to 4.86 V),and the formed unique three-dimensional(3D)co-continuous structure of polymer matrix and ionic liquid in PDIL-SPE can promote the transport of lithium ions.Also,the 3D co-continuous structure of PDIL-SPE effectively accommodates the severe volume expansion for prolonged lithium plating and stripping processes over 1000 h at 0.5 mA cm^(-2) under 25℃.Moreover,the LiFePO_(4)//Li coin cell can work stably over 150 cycles at a 1 C rate under room temperature with a capacity retention of 90.6%from 111.1 to 100.7 mAh g^(-1).The PDIL-SPE composite is a promising material system for enabling the ultrastable operation of solid-state lithium-metal batteries.
基金financially supported by the National Natural Science Foundation of China(NSFC)(52172096)。
文摘Li(6.4)La_(3)Zr_(1.4)Ta_(0.6)O_(12)(LLZTO) solid garnet-type electrolyte has been widely reported due to its outstanding safety and electrochemical stability.However,the inherent rigidity and brittleness of LLZTO lead to poor contact with anode/cathode and the operation failure of full cells.Herein,the dual-interlayers are constructed as the fast interfacial ion-migration channel by using Ti_(3)C_(2)T_(x)(MXene,Txis-O,-OH,-F) with trace ionic liquid(IL),which promote the intimate contact between LLZTO and anode/cathode and suppress Li-dendrites growth.Notably,IL can wet the cathode to promote intimate interface contact and be decomposed into some inorganic compounds(such as Li3N,LiF,and Li2Sx),resulting in reduced interfacial resistance and fast Li-ion transportation.Consequently,in the prepared Li-symmetric cell,the interfacial resistance on the anode side plunges to 33.1 Ω cm^(-2),and stably maintains over 1000 h without short circuit at 0.05 mA cm^(-2).The full cell of Li|LiFePO4delivers a high initial capacity of 158.52 mA h g^(-1)and outstanding retention of 90.18% after 100 cycles at 60℃ and 0.2 C.Our work provides an efficient strategy to design dual-interlayers between LLZTO and anode/cathode for the interfacial modification to enhance the performance of solid garnet batteries.
基金the National Natural Science Foundation of China(Grant No.51976002)the Beijing Nova Program of Science and Technology(Grant No.Z191100001119033)。
文摘Thermal rectification refers to the phenomenon by which the magnitude of the heat flux in one direction is much larger than that in the opposite direction.In this study,we propose to implement the thermal rectification phenomenon in an asymmetric solid–liquid–solid sandwiched system with a nano-structured interface.By using the non-equilibrium molecular dynamics simulations,the thermal transport through the solid–liquid–solid system is examined,and the thermal rectification phenomenon can be observed.It is revealed that the thermal rectification effect can be attributed to the significant difference in the interfacial thermal resistance between Cassie and Wenzel states when reversing the temperature bias.In addition,effects of the liquid density,solid–liquid bonding strength and nanostructure size on the thermal rectification are examined.The findings may provide a new way for designs of certain thermal devices.
基金This work was financially supported by Stable Support Plan Program for Higher Education Institutions(20220815094504001)Shenzhen Key Laboratory of Advanced Energy Storage(ZDSYS20220401141000001)+1 种基金This work was also financially supported by the Shenzhen Science and Technology Innovation Commission(GJHZ20200731095606021,20200925155544005)the Project of Hetao Shenzhen-Hong Kong Science and Technology Innovation Cooperation Zone(HZQB-KCZYB-2020083)。
文摘Improving the long-term cycling stability and energy density of all-solid-state lithium(Li)-metal batteries(ASSLMBs)at room temperature is a severe challenge because of the notorious solid–solid interfacial contact loss and sluggish ion transport.Solid electrolytes are generally studied as two-dimensional(2D)structures with planar interfaces,showing limited interfacial contact and further resulting in unstable Li/electrolyte and cathode/electrolyte interfaces.Herein,three-dimensional(3D)architecturally designed composite solid electrolytes are developed with independently controlled structural factors using 3D printing processing and post-curing treatment.Multiple-type electrolyte films with vertical-aligned micro-pillar(p-3DSE)and spiral(s-3DSE)structures are rationally designed and developed,which can be employed for both Li metal anode and cathode in terms of accelerating the Li+transport within electrodes and reinforcing the interfacial adhesion.The printed p-3DSE delivers robust long-term cycle life of up to 2600 cycles and a high critical current density of 1.92 mA cm^(−2).The optimized electrolyte structure could lead to ASSLMBs with a superior full-cell areal capacity of 2.75 mAh cm^(−2)(LFP)and 3.92 mAh cm^(−2)(NCM811).This unique design provides enhancements for both anode and cathode electrodes,thereby alleviating interfacial degradation induced by dendrite growth and contact loss.The approach in this study opens a new design strategy for advanced composite solid polymer electrolytes in ASSLMBs operating under high rates/capacities and room temperature.
基金supported by the Youth Program of National Natural Science Foundation of China(Grant No.52104012)the Key Program of the National Natural Science Foundation of China(Grant No.51734010)the Key Natural Science Projects of Scientific Research Plan in Colleges and Universities of Xinjiang Uygur Autonomous Region(Grant No.XJEDU20211028).
文摘The multiphase flow characteristic is one of the most concerning problems during solid fluidization exploitation of marine natural gas hydrate reservoirs.In this research,a new transient gas-liquid-solid multiphase flow model with hydrate phase transition was developed.Meanwhile,this model considered the coupling relationship among convective heat transfer,hydrate dynamic decomposition,and multi-phase flow.The model can simulate the change of flow pattern from solid-liquid to gas-liquid-solid flow,and describe the distribution character of volume fraction of phase,wellbore temperature and pressure,and hydrate decomposition rate during transportation.The simulation results indicate that the hydrate decomposition region in the wellbore gradually expands,but the hydrate decomposition rate gradually decreases during the solid fluidization exploitation of hydrate.When mining time lasts for 4 h,and the bottom hole pressure decreases by about 0.4 MPa.Increasing NaCl concentration in seawater helps expand hydrate decomposition regions and improves the wellbore hydrate decomposition rate.When the Nacl mass fraction in seawater reaches 15%,it will raise the hydrate decomposition regions to the whole wellbore.In addition,the higher the wellhead backpressure,the lower the decomposition area and decomposition rate of hydrate in the wellbore.When wellhead backpressure reaches 2 MPa,the volume fraction of gas near the wellhead will reduce to about 12%.This work is expected to provide a theoretical basis for the development of marine hydrate reservoirs.
基金supported by the National Natural Science Foundation of China(22279025,21773048)the Natural Science Foundation of Heilongjiang Province(LH2021A013)+1 种基金the Sichuan Science and Technology Program(2021YFSY0022)the Fundamental Research Funds for the Central Universities(2023FRFK06005,HIT.NSRIF202204)。
文摘Developing efficient and stable cathodes for low-temperature solid oxide fuel cells(LT-SOFCs) is of great importance for the practical commercialization.Herein,we propose a series of Sm-modified Bi_(0.7-x)Sm_xSr_(0.3)FeO_(3-δ) perovskites as highly-active catalysts for LT-SOFCs.Sm doping can significantly enhance the electrocata lytic activity and chemical stability of cathode.At 600℃,Bi_(0.675)Sm_(0.025)Sr_(0.3)FeO_(3-δ)(BSSF25) cathode has been found to be the optimum composition with a polarization resistance of 0.098 Ω cm^2,which is only around 22.8% of Bi_(0.7)Sr_(0.3)FeO_(3-δ)(BSF).A full cell utilizing BSSF25 displays an exceptional output density of 790 mW cm^(-2),which can operate continuously over100 h without obvious degradation.The remarkable electrochemical performance observed can be attributed to the improved O_(2) transport kinetics,superior surface oxygen adsorption capacity,as well as O_(2)p band centers in close proximity to the Fermi level.Moreover,larger average bonding energy(ABE) and the presence of highly acidic Bi,Sm,and Fe ions restrict the adsorption of CO_(2) on the cathode surface,resulting in excellent CO_(2) resistivity.This work provides valuable guidance for systematic design of efficient and durable catalysts for LT-SOFCs.
基金supported by the National Natural Science Youth Fund of China(52302247)the Natural Youth Science Foundation of Hunan Province(2022JJ40070)。
文摘Since the advent of the solid-state batteries,employing solid polymer electrolytes(SPEs)to replace routine flammable liquid electrolytes is regarded to be one of the most promising solutions in pursing highenergy-density battery systems.SPEs with superior thermal stability,good processability,and high mechanical modulus obtain increasing attentions.However,SPE-based batteries are not impenetrable due to their decomposition and combustibility under extreme conditions.Researchers believe incorporating appropriate flame-retardant additives/solvents/fragments into SPEs can intrinsically reduce their flammability to solve the battery safety issues.In this review,the recent research progress of incombustible SPEs,with special emphasis on flame-retardant structural design,is summarized.Specifically,a brief introduction of flame-retardant mechanism,evaluation index for safety of SPEs,and a detailed overview of the latest advances on diverse-types SPEs in various battery systems are highlighted.The deep insight into thermal ru naway process,the free-standing incombustible GPEs,and the ratio nal design of pouch cell structures may be the main directions to motivate revolutionary next-generation for safety batteries.
基金supported by the National Key R&D Program of China ‘Intergovernmental International Scientific and Technological Innovation Cooperation’ (No. 2019YFE0122100)。
文摘The ionic liquid(IL) 1-butyl-3-methylimidazolium tetrafluoroborate treated with radiofrequency plasma is proposed for functionalization and immobilization on polyethersulfone supports to form supported ionic liquid membranes for CO_(2) separation.The effects of treatment time and transmembrane pressure difference on CO_(2) permeance were evaluated.The best gas permeation performance was obtained with a treatment time of 10 min and the transmembrane pressure difference was 0.25 MPa.Characterization of the materials by Fourier transform infrared spectroscopy,x-ray photoelectron spectroscopy and nuclear magnetic resonance spectroscopy demonstrates that the IL is grafted with carboxyl groups and deprotonated through plasma treatment.A preliminary mechanism for the plasma treatment and facilitated transport of CO_(2)has been proposed on this basis.
基金Nanyang Technological University(NTU),Singapore,for providing research scholarships for this study.The authors thank the supports from Debris of the Anthropocene to Resources(DotA2)Lab at NTU.
文摘1.Introduction Cities are responsible for approximately 70%of all anthropogenic greenhouse gas(GHG)emissions and about 60%of all anthropogenic methane(CH4)emissions[1,2].Solid waste disposal sites(including landfills and dumpsites),which are prevalent in global cities,emit CH4 generated from the anaerobic biodegradation of municipal solid waste(MSW).Notably,the proportions of CH4 emissions from disposal sites surpass 50%of the total CH4 emissions in some megalopolises[3].CH4 has a high global warming potential(GWP),being 28 times stronger than carbon dioxide(CO_(2))over a 100-year period and 80 times stronger over a 20-year period[4].Understanding and mitigating CH4 emissions from solid waste disposal sites is particularly pertinent and pressing,considering that the latest Synthesis Report from the Intergovernmental Panel on Climate Change(IPCC)emphasizes that the current pace of mitigation and adaptation policies and measures falls short of restraining global temperature rise to under 1.5℃ within the 21st century[4].More than 150 countries signed the Global Methane Pledge at the United Nations Climate Change Conference in Glasgow(COP26),which aims to reduce global annual CH4 emissions by 30%by 2030,compared with emissions in 2020[5].
基金financially supported by the National Natural Science Foundation of China(Nos.22072110 and 21872107)the Key Research and Development Projects of Hubei Province,China(2022BAA083)。
文摘CO_(2) electrochemical reduction(CO_(2)ER)is an important research area for carbon neutralization.However,available catalysts for CO_(2) reduction are still characterized by limited stability and activity.Recently,metallic bismuth(Bi)has emerged as a promising catalyst for CO_(2) ER.Herein,we report the solid cathode electroreduction of commercial micronized Bi2O3as a straightforward approach for the preparation of nanostructured Bi.At-1.1 V versus reversible hydrogen electrode in a KHCO3aqueous electrolyte,the resulting nanostructure Bi delivers a formate current density of~40 mA·cm^(-2) with a current efficiency of~86%,and the formate selectivity reaches97.6% at-0.78 V.Using nanosized Bi2O3as the precursor can further reduce the primary particle sizes of the resulting Bi,leading to a significantly increased formate selectivity at relatively low overpotentials.The high catalytic activity of nanostructured Bi is attributable to the ultrafine and interconnected Bi nanoparticles in the nanoporous structure,which exposes abundant active sites for CO_(2) electrocatalytic reduction.
基金the financial supports from National Natural Science Foundation of China(22172066,22378176)supported by State Key Laboratory of Heavy Oil ProcessingSupported by Jiangsu Collaborative Innovation Center of Technology and Material of Water Treatment,Suzhou University of Science and Technology。
文摘An efficient mass transfer process is a critical factor for regulating catalytic activity in a photocatalytic desulfurization system.Herein,a phosphotungstic acid(HPW)active center is successfully composited with a quaternary ammonium phosphotungstate-based hexadecyltrimethylammonium chloride ionic liquid(CTAC-HPW)by the ion exchange method for the photocatalytic oxidative desulfurization of dibenzothiophene sulfide.The keggin structure of HPW and highly mass transfer performance of organic cations synergistically enhanced the photocatalytic activity towards the effective convertion of dibenzothiophene(DBT)with the excitation of visible light.The deep desulfurization(<10 mg·kg^(-1))is attained within 30 min,and well stability is demonstrated within 25 cycles.Moreover,the CTAC-HPW photocatalyst projects well selectivity to interference from coexisting compounds such as olefins and aromatic hydrocarbons and universality of dibenzothiophenes,for example,4-methyldibenzothiophene(4-MDBT)and 4,6-dimethyldibenzothiophene(4,6-DMDBT).Ultimately,a possible photocatalytic desulfurization mechanism is proposed according to the Gaschromatography-mass spectrometry(GC-MS),proving that the final product is the corresponding sulfone.The trapping experiment and electron spin resonance(ESR)analysis confirmed that h^(+)and,COOH played critical roles in the oxidation process.The work offers a practicable strategy for efficiently converting DBT to DBTO_(2) with added value.
文摘A method of analysis for the simultaneous determination of methylisothiazolinone (MI), methylchloroisothiazolinone (CMI), benzisothiazolinone (BIT) and Bronopol (BNP) in washing-up liquid was established. The method consisted of a gradient HPLC analysis at three different wavelengths. The four compounds could be analyzed with good precision and accuracy.
基金financially supported by the National Natural Science Foundation of China(Grant No.22325405,22321002,22279153)Liaoning Revitalization Talents Program(XLYC1807207,XLYC2203134)DICP I202104。
文摘Solid polymer electrolytes(SPEs)have become increasingly important in advanced lithium-ion batteries(LIBs)due to their improved safety and mechanical properties compared to organic liquid electrolytes.Cross-linked polymers have the potential to further improve the mechanical property without trading off Li-ion conductivity.In this study,focusing on a recently developed cross-linked SPE,i.e.,the one based on poly(vinylene carbonate)-poly(ethylene oxide)cross-linked network(PVCN),we used solid-state nuclear magnetic resonance(NMR)techniques to investigate the fundamental interaction between the chain segments and Li ions,as well as the lithium-ion motion.By utilizing homonuclear/heteronuclear correlation,CP(cross-polarization)kinetics,and spin-lattice relaxation experiments,etc.,we revealed the structural characteristics and their relations to lithium-ion mobilities.It is found that the network formation prevents poly(ethylene oxide)chains from crystallization,which could create sufficient space for segmental tumbling and Li-ion co nductio n.As such,the mechanical property is greatly improved with even higher Li-ion mobilities compared to the poly(vinylene carbonate)or poly(ethylene oxide)based SPE analogues.