As an important form of reactors for gas/liquid/solid catalytic reaction,trickle bed reactors (TBRs) are widely applied in petroleum industry,biochemical,fine chemical and pharmaceutical industries because of their fl...As an important form of reactors for gas/liquid/solid catalytic reaction,trickle bed reactors (TBRs) are widely applied in petroleum industry,biochemical,fine chemical and pharmaceutical industries because of their flexibility,simplicity of operation and high throughput.However,TBRs also show inefficient production and hot pots caused by non-uniform fluid distribution and incomplete wetting of the catalyst,which limit their further application in chemical industry.Also,process intensification in TBRs is necessary as the decrease in quality of processed crude oil,caused by increased exploitation depths,and more restrictive environmental regulations and emission standards for industry,caused by increased environment protection consciousness.In recent years,lots of strategies for process intensification in TBRs have been proposed to improve reaction performance to meet the current and future demands of chemical industry from the environmental and economic perspective.This article summarizes the recent progress in techniques for intensifying gas/liquid/solid reaction in TBRs and application of intensified TBRs in petroleum industry.展开更多
Hybrid liquid/solid electrolytes(HLSEs) consisting of conventional organic liquid electrolyte(LE), polyacrylonitrile(PAN), and ceramic lithium ion conductor Li(1.5)Al(0.5)Ge(1.5)(PO4)3(LAGP) are propos...Hybrid liquid/solid electrolytes(HLSEs) consisting of conventional organic liquid electrolyte(LE), polyacrylonitrile(PAN), and ceramic lithium ion conductor Li(1.5)Al(0.5)Ge(1.5)(PO4)3(LAGP) are proposed and investigated. The HLSE has a high ionic conductivity of over 2.25 × 10^(-3) S/cm at 25?C, and an extended electrochemical window of up to 4.8 V versus Li/Li+. The Li|HLSE|Li symmetric cells and Li|HLSE|Li FePO4 cells exhibit small interfacial area specific resistances(ASRs) comparable to that of LE while much smaller than that of ceramic LAGP electrolyte, and excellent performance at room temperature. Bis(trifluoromethane sulfonimide) salt in HLSE significantly affects the properties and electrochemical behaviors. Side reactions can be effectively suppressed by lowering the concentration of Li salt. It is a feasible strategy for pursuing the high energy density batteries with higher safety.展开更多
The detailed understanding of various underlying processes at liquid/solid interfaces requires the development of interface-sensitive and high-resolution experimental techniques with atomic precision.In this perspecti...The detailed understanding of various underlying processes at liquid/solid interfaces requires the development of interface-sensitive and high-resolution experimental techniques with atomic precision.In this perspective,we review the recent advances in studying the liquid/solid interfaces at atomic level by electrochemical scanning tunneling microscope(EC-STM),non-contact atomic force microscopy(NC-AFM),and surface-sensitive vibrational spectroscopies.Different from the ultrahigh vacuum and cryogenic experiments,these techniques are all operated in situ under ambient condition,making the measurements close to the native state of the liquid/solid interface.In the end,we present some perspectives on emerging techniques,which can defeat the limitation of existing imaging and spectroscopic methods in the characterization of liquid/solid interfaces.展开更多
The liquid-film solution-diffusion bonding of ZCuBe2.5 alloys was conducted using Cu-based alloy powders. The tensile strength of the joint is up to 318 MPa. With the increase of temperature gradient, the bonding time...The liquid-film solution-diffusion bonding of ZCuBe2.5 alloys was conducted using Cu-based alloy powders. The tensile strength of the joint is up to 318 MPa. With the increase of temperature gradient, the bonding time decreases and the interface migration velocity increases remarkably. The appropriate temperature gradient is 5-40 K/cm. Under fixed bonding time, the thickness of diffusion layer increases with the increase of temperature gradient, and this tendency becomes more remarkable with the prolonging of bonding time.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
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
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
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
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
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
The separation of aromatics from aliphatics is essential for achieving maximum exploitation of oil resources in the petrochemical industry.In this study,a series of metal chloride-based ionic liquids were prepared and...The separation of aromatics from aliphatics is essential for achieving maximum exploitation of oil resources in the petrochemical industry.In this study,a series of metal chloride-based ionic liquids were prepared and their performances in the separation of 1,2,3,4-tetrahydronaphthalene(tetralin)/dodecane and tetralin/decalin systems were studied.Among these ionic liquids,1-ethyl-3-methylimidazolium tetrachloroferrate([EMIM][FeCl_(4)])with the highest selectivity was used as the extractant.Density functional theory calculations showed that[EMIM][FeCl_(4)]interacted more strongly with tetralin than with dodecane and decalin.Energy decomposition analysis of[EMIM][FeCl_(4)]-tetralin indicated that electrostatics and dispersion played essential roles,and induction cannot be neglected.The van der Waals forces was a main effect in[EMIM][FeCl_(4)]-tetralin by independent gradient model analysis.The tetralin distribution coefficient and selectivity were 0.8 and 110,respectively,with 10%(mol)tetralin in the initial tetralin/dodecane system,and 0.67 and 19.5,respectively,with 10%(mol)tetralin in the initial tetralin/decalin system.The selectivity increased with decreasing alkyl chain length of the extractant.The influence of the extraction temperature,extractant dosage,and initial concentrations of the system components on the separation performance were studied.Recycling experiments showed that the regenerated[EMIM][FeCl_(4)]could be used repeatedly.展开更多
Achieving flexible electronics with comfort and durability comparable to traditional textiles is one of the ultimate pursuits of smart wearables.Ink printing is desirable for e-textile development using a simple and i...Achieving flexible electronics with comfort and durability comparable to traditional textiles is one of the ultimate pursuits of smart wearables.Ink printing is desirable for e-textile development using a simple and inexpensive process.However,fabricating high-performance atop textiles with good dispersity,stability,biocompatibility,and wearability for high-resolution,large-scale manufacturing,and practical applications has remained challenging.Here,waterbased multi-walled carbon nanotubes(MWCNTs)-decorated liquid metal(LM)inks are proposed with carbonaceous gallium–indium micro-nanostructure.With the assistance of biopolymers,the sodium alginate-encapsulated LM droplets contain high carboxyl groups which non-covalently crosslink with silk sericin-mediated MWCNTs.E-textile can be prepared subsequently via printing technique and natural waterproof triboelectric coating,enabling good flexibility,hydrophilicity,breathability,wearability,biocompatibility,conductivity,stability,and excellent versatility,without any artificial chemicals.The obtained e-textile can be used in various applications with designable patterns and circuits.Multi-sensing applications of recognizing complex human motions,breathing,phonation,and pressure distribution are demonstrated with repeatable and reliable signals.Self-powered and energy-harvesting capabilities are also presented by driving electronic devices and lighting LEDs.As proof of concept,this work provides new opportunities in a scalable and sustainable way to develop novel wearable electronics and smart clothing for future commercial applications.展开更多
Small-scale electromagnetic soft actuators are characterized by a fast response and simplecontrol,holding prospects in the field of soft and miniaturized robotics.The use of liquid metal(LM)to replace a rigid conducto...Small-scale electromagnetic soft actuators are characterized by a fast response and simplecontrol,holding prospects in the field of soft and miniaturized robotics.The use of liquid metal(LM)to replace a rigid conductor inside soft actuators can reduce the rigidity and enhance the actuation performance and robustness.Despite research efforts,challenges persist in the flexible fabrication of LM soft actuators and in the improvement of actuation performance.To address these challenges,we developed a fast and robust electromagnetic soft microplate actuator based on a laser-induced selective adhesion transfer method.Equipped with unprecedentedly thin LM circuit and customized low Young’s modulus silicone rubber(1.03 kPa),our actuator exhibits an excellent deformation angle(265.25?)and actuation bending angular velocity(284.66 rad·s^(-1)).Furthermore,multiple actuators have been combined to build an artificial gripper with a wide range of functionalities.Our actuator presents new possibilities for designing small-scaleartificial machines and supports advancements in ultrafast soft and miniaturized robotics.展开更多
The synthesis of methacrylic acid from biomass-derived itaconic acid is a green route,for it can get rid of the dependence on fossil resource.In order to solve the problems on this route such as use of a preciousmetal...The synthesis of methacrylic acid from biomass-derived itaconic acid is a green route,for it can get rid of the dependence on fossil resource.In order to solve the problems on this route such as use of a preciousmetal catalyst and a corrosive homogeneous alkali,we prepared a series of hydroxyapatite catalysts by an ionic liquid-assisted hydrothermal method and evaluated their catalytic performance.The results showed that the ionic liquid[Bmim]BF_(4) can affect the crystal growth of hydroxyapatite,provide fluoride ion for fluorination of hydroxyapatite,and adjust the surface acidity and basicity,morphology,textural properties,crystallinity,and composition of hydroxyapatite.The[Bmim]BF4 dosage and hydrothermal temperature can affect the fluoride ion concentration in the hydrothermal system,thus changing the degree of fluoridation of hydroxyapatite.High fluoride-ion concentration can lead to the formation of CaF_(2) and thus significantly decrease the catalytic performance of hydroxyapatite.The hydrothermal time mainly affects the growth of hydroxyapatite crystals on the c axis,leading to different catalytic performance.The suitable conditions for the preparation of this fluoridized hydroxyapatite are as follows:a mass ratio of[Bmim]BF4 to calcium salt=0.2:1,a hydrothermal time of 12 h,and a hydrothermal temperature of 130℃.A maximal methacrylic acid yield of 54.7%was obtained using the fluoridized hydroxyapatite under relatively mild reaction conditions(250℃ and 2 MPa of N_(2))in the absence of a precious-metal catalyst and a corrosive homogeneous alkali.展开更多
As global economic growth increases,the demand for energy sources boosts.While fossil fuels have traditionally satisfied this demand,their environmental influence and limited reserves require alternatives.Fossil fuel co...As global economic growth increases,the demand for energy sources boosts.While fossil fuels have traditionally satisfied this demand,their environmental influence and limited reserves require alternatives.Fossil fuel combustion contributes substantially to greenhouse gas emissions,with a pressing need to halve these emissions by 2030 and target net-zero by 2050.Renewable energy sources,contributing currently to 29%of global electricity,are viewed as promising substitutes.With wind energy's potential,Zheng's team developed a novel method to harness even low wind speeds using well-aligned nanofibers and an innovative“drop wind generator”.This system,combining moisture-saturated ionic liquid 3-Methyl-1-octylimidazolium chloride with specific nanofiber arrays,exploits wind-inducedflows for energy conversion.This study highlights the vast untapped potential of low-speed wind as a sustainable energy source potentially for electronics.展开更多
基金the support of National Natural Science Foundation of China(21878019)Beijing Natural Science Foundation(2182063)。
文摘As an important form of reactors for gas/liquid/solid catalytic reaction,trickle bed reactors (TBRs) are widely applied in petroleum industry,biochemical,fine chemical and pharmaceutical industries because of their flexibility,simplicity of operation and high throughput.However,TBRs also show inefficient production and hot pots caused by non-uniform fluid distribution and incomplete wetting of the catalyst,which limit their further application in chemical industry.Also,process intensification in TBRs is necessary as the decrease in quality of processed crude oil,caused by increased exploitation depths,and more restrictive environmental regulations and emission standards for industry,caused by increased environment protection consciousness.In recent years,lots of strategies for process intensification in TBRs have been proposed to improve reaction performance to meet the current and future demands of chemical industry from the environmental and economic perspective.This article summarizes the recent progress in techniques for intensifying gas/liquid/solid reaction in TBRs and application of intensified TBRs in petroleum industry.
基金supported by the National Key Basic Research Program of China(Grant No.2014CB932400)the National Natural Science Foundation of China(Grant No.51772167)+1 种基金the China Postdoctoral Science Foundation(Grant No.2016M591169)the Shenzhen Municipal Basic Research Project,China(Grant No.JCYJ20170412171311288)
文摘Hybrid liquid/solid electrolytes(HLSEs) consisting of conventional organic liquid electrolyte(LE), polyacrylonitrile(PAN), and ceramic lithium ion conductor Li(1.5)Al(0.5)Ge(1.5)(PO4)3(LAGP) are proposed and investigated. The HLSE has a high ionic conductivity of over 2.25 × 10^(-3) S/cm at 25?C, and an extended electrochemical window of up to 4.8 V versus Li/Li+. The Li|HLSE|Li symmetric cells and Li|HLSE|Li FePO4 cells exhibit small interfacial area specific resistances(ASRs) comparable to that of LE while much smaller than that of ceramic LAGP electrolyte, and excellent performance at room temperature. Bis(trifluoromethane sulfonimide) salt in HLSE significantly affects the properties and electrochemical behaviors. Side reactions can be effectively suppressed by lowering the concentration of Li salt. It is a feasible strategy for pursuing the high energy density batteries with higher safety.
文摘The detailed understanding of various underlying processes at liquid/solid interfaces requires the development of interface-sensitive and high-resolution experimental techniques with atomic precision.In this perspective,we review the recent advances in studying the liquid/solid interfaces at atomic level by electrochemical scanning tunneling microscope(EC-STM),non-contact atomic force microscopy(NC-AFM),and surface-sensitive vibrational spectroscopies.Different from the ultrahigh vacuum and cryogenic experiments,these techniques are all operated in situ under ambient condition,making the measurements close to the native state of the liquid/solid interface.In the end,we present some perspectives on emerging techniques,which can defeat the limitation of existing imaging and spectroscopic methods in the characterization of liquid/solid interfaces.
文摘The liquid-film solution-diffusion bonding of ZCuBe2.5 alloys was conducted using Cu-based alloy powders. The tensile strength of the joint is up to 318 MPa. With the increase of temperature gradient, the bonding time decreases and the interface migration velocity increases remarkably. The appropriate temperature gradient is 5-40 K/cm. Under fixed bonding time, the thickness of diffusion layer increases with the increase of temperature gradient, and this tendency becomes more remarkable with the prolonging of bonding time.
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 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 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.
基金supported by the National Natural Science Foundation of China(22125802,22078010).
文摘The separation of aromatics from aliphatics is essential for achieving maximum exploitation of oil resources in the petrochemical industry.In this study,a series of metal chloride-based ionic liquids were prepared and their performances in the separation of 1,2,3,4-tetrahydronaphthalene(tetralin)/dodecane and tetralin/decalin systems were studied.Among these ionic liquids,1-ethyl-3-methylimidazolium tetrachloroferrate([EMIM][FeCl_(4)])with the highest selectivity was used as the extractant.Density functional theory calculations showed that[EMIM][FeCl_(4)]interacted more strongly with tetralin than with dodecane and decalin.Energy decomposition analysis of[EMIM][FeCl_(4)]-tetralin indicated that electrostatics and dispersion played essential roles,and induction cannot be neglected.The van der Waals forces was a main effect in[EMIM][FeCl_(4)]-tetralin by independent gradient model analysis.The tetralin distribution coefficient and selectivity were 0.8 and 110,respectively,with 10%(mol)tetralin in the initial tetralin/dodecane system,and 0.67 and 19.5,respectively,with 10%(mol)tetralin in the initial tetralin/decalin system.The selectivity increased with decreasing alkyl chain length of the extractant.The influence of the extraction temperature,extractant dosage,and initial concentrations of the system components on the separation performance were studied.Recycling experiments showed that the regenerated[EMIM][FeCl_(4)]could be used repeatedly.
基金funded by The Hong Kong Polytechnic University(Project No.1-WZ1Y,1-YXAK,1-W21C).
文摘Achieving flexible electronics with comfort and durability comparable to traditional textiles is one of the ultimate pursuits of smart wearables.Ink printing is desirable for e-textile development using a simple and inexpensive process.However,fabricating high-performance atop textiles with good dispersity,stability,biocompatibility,and wearability for high-resolution,large-scale manufacturing,and practical applications has remained challenging.Here,waterbased multi-walled carbon nanotubes(MWCNTs)-decorated liquid metal(LM)inks are proposed with carbonaceous gallium–indium micro-nanostructure.With the assistance of biopolymers,the sodium alginate-encapsulated LM droplets contain high carboxyl groups which non-covalently crosslink with silk sericin-mediated MWCNTs.E-textile can be prepared subsequently via printing technique and natural waterproof triboelectric coating,enabling good flexibility,hydrophilicity,breathability,wearability,biocompatibility,conductivity,stability,and excellent versatility,without any artificial chemicals.The obtained e-textile can be used in various applications with designable patterns and circuits.Multi-sensing applications of recognizing complex human motions,breathing,phonation,and pressure distribution are demonstrated with repeatable and reliable signals.Self-powered and energy-harvesting capabilities are also presented by driving electronic devices and lighting LEDs.As proof of concept,this work provides new opportunities in a scalable and sustainable way to develop novel wearable electronics and smart clothing for future commercial applications.
基金supported by the National Natural Science Foundation of China(Nos.52122511,61927814,and U20A20290)Anhui Provincial Natural Science Foundation(2308085QF218)+5 种基金China National Postdoctoral Program for Innovative Talents(BX20230351)China Postdoctoral Science Foundation(2023M733382)National Key R&D Program of China(2021YFF0502700)Major Scientific and Technological Projects in Anhui Province(202203a05020014)Fundamental Research Funds for the Central Universities(WK5290000003 and WK2090000058)Youth Innovation Promotion Association CAS(Y2021118)。
文摘Small-scale electromagnetic soft actuators are characterized by a fast response and simplecontrol,holding prospects in the field of soft and miniaturized robotics.The use of liquid metal(LM)to replace a rigid conductor inside soft actuators can reduce the rigidity and enhance the actuation performance and robustness.Despite research efforts,challenges persist in the flexible fabrication of LM soft actuators and in the improvement of actuation performance.To address these challenges,we developed a fast and robust electromagnetic soft microplate actuator based on a laser-induced selective adhesion transfer method.Equipped with unprecedentedly thin LM circuit and customized low Young’s modulus silicone rubber(1.03 kPa),our actuator exhibits an excellent deformation angle(265.25?)and actuation bending angular velocity(284.66 rad·s^(-1)).Furthermore,multiple actuators have been combined to build an artificial gripper with a wide range of functionalities.Our actuator presents new possibilities for designing small-scaleartificial machines and supports advancements in ultrafast soft and miniaturized robotics.
基金supported by National Natural Science Foundation of China(21978066)Basic Research Program of Hebei Province for Natural Science Foundation and Key Basic Research Project(18964308D)the Key Program of Natural Science Foundation of Hebei Province(B2020202048).
文摘The synthesis of methacrylic acid from biomass-derived itaconic acid is a green route,for it can get rid of the dependence on fossil resource.In order to solve the problems on this route such as use of a preciousmetal catalyst and a corrosive homogeneous alkali,we prepared a series of hydroxyapatite catalysts by an ionic liquid-assisted hydrothermal method and evaluated their catalytic performance.The results showed that the ionic liquid[Bmim]BF_(4) can affect the crystal growth of hydroxyapatite,provide fluoride ion for fluorination of hydroxyapatite,and adjust the surface acidity and basicity,morphology,textural properties,crystallinity,and composition of hydroxyapatite.The[Bmim]BF4 dosage and hydrothermal temperature can affect the fluoride ion concentration in the hydrothermal system,thus changing the degree of fluoridation of hydroxyapatite.High fluoride-ion concentration can lead to the formation of CaF_(2) and thus significantly decrease the catalytic performance of hydroxyapatite.The hydrothermal time mainly affects the growth of hydroxyapatite crystals on the c axis,leading to different catalytic performance.The suitable conditions for the preparation of this fluoridized hydroxyapatite are as follows:a mass ratio of[Bmim]BF4 to calcium salt=0.2:1,a hydrothermal time of 12 h,and a hydrothermal temperature of 130℃.A maximal methacrylic acid yield of 54.7%was obtained using the fluoridized hydroxyapatite under relatively mild reaction conditions(250℃ and 2 MPa of N_(2))in the absence of a precious-metal catalyst and a corrosive homogeneous alkali.
基金funding of the National Natural Science Foundation of China(no.21776235,no.21376197)the studentship by the Hong Kong Polytechnic University。
文摘As global economic growth increases,the demand for energy sources boosts.While fossil fuels have traditionally satisfied this demand,their environmental influence and limited reserves require alternatives.Fossil fuel combustion contributes substantially to greenhouse gas emissions,with a pressing need to halve these emissions by 2030 and target net-zero by 2050.Renewable energy sources,contributing currently to 29%of global electricity,are viewed as promising substitutes.With wind energy's potential,Zheng's team developed a novel method to harness even low wind speeds using well-aligned nanofibers and an innovative“drop wind generator”.This system,combining moisture-saturated ionic liquid 3-Methyl-1-octylimidazolium chloride with specific nanofiber arrays,exploits wind-inducedflows for energy conversion.This study highlights the vast untapped potential of low-speed wind as a sustainable energy source potentially for electronics.