Magnesium(Mg)is a promising alternative to lithium(Li)as an anode material in solid-state batteries due to its abundance and high theoretical volumetric capacity.However,the sluggish Mg-ion conduction in the lattice o...Magnesium(Mg)is a promising alternative to lithium(Li)as an anode material in solid-state batteries due to its abundance and high theoretical volumetric capacity.However,the sluggish Mg-ion conduction in the lattice of solidstate electrolytes(SSEs)is one of the key challenges that hamper the development of Mg-ion solid-state batteries.Though various Mg-ion SSEs have been reported in recent years,key insights are hard to be derived from a single literature report.Besides,the structure-performance relationships of Mg-ion SSEs need to be further unraveled to provide a more precise design guideline for SSEs.In this viewpoint article,we analyze the structural characteristics of the Mg-based SSEs with high ionic conductivity reported in the last four decades based upon data mining-we provide big-data-derived insights into the challenges and opportunities in developing next-generation Mg-ion SSEs.展开更多
Hard carbons(HCs)are recognized as potential anode materials for sodium-ion batteries(SIBs)because of their low cost,environmental friendliness,and the abundance of their precursors.The presence of graphitic domains,n...Hard carbons(HCs)are recognized as potential anode materials for sodium-ion batteries(SIBs)because of their low cost,environmental friendliness,and the abundance of their precursors.The presence of graphitic domains,numerous pores,and disordered carbon layers in HCs plays a significant role in determining their sodium storage ability,but these structural features depend on the precursor used.The influence of functional groups,including heteroatoms and oxygen-containing groups,and the microstructure of the precursor on the physical and electrochemical properties of the HC produced are evaluated,and the effects of carbonization conditions(carbonization temperature,heating rate and atmosphere)are also discussed.展开更多
The electrochemical behavior of Al(Ⅲ)in urea-1-butyl-3-methylimidazolium chloride-aluminum chloride(urea-BMIC-AlCl_(3))ionic liquids,and the effect of potential and temperature on the characterization of cathode prod...The electrochemical behavior of Al(Ⅲ)in urea-1-butyl-3-methylimidazolium chloride-aluminum chloride(urea-BMIC-AlCl_(3))ionic liquids,and the effect of potential and temperature on the characterization of cathode products,current efficiency and energy consumption of aluminum electrorefining have been investigated.Cyclic voltammetry showed that the electrochemical reduction of Al(Ⅲ)was a one-step three-electron-transfer irreversible reaction,and the electrochemical reaction was controlled by diffusion.The diffusion coefficient of Al(Ⅲ)in urea-BMIC-AlCl_(3)ionic liquids at 313 K was 1.94×10^(−7)cm^(2)/s.The 7075 aluminum alloy was used as an anode for electrorefining,and the cathode products were analyzed by XRD,SEM and EDS.The results from XRD analysis indicated that the main phase of the cathode products was aluminum.The results from SEM and EDS characterization revealed that the cathode product obtained by electrorefining−1.2 V(vs.Al)was dense and uniform,and the mass fraction of aluminum decreased from 99.61%to 99.10%as the experimental temperature increased from 313 K to 333 K.In this work,the optimum experimental conditions were−1.2 V(vs.Al)and 313 K.At this time,the cathode current efficiency was 97.80%,while the energy consumption was 3.72 kW·h/kg.展开更多
Electrocatalytic reduction reactions,powered by clean energy sources such as solar energy and wind,offer a sustainable method for converting inexpensive feedstocks(e.g.,CO_(2),N_(2)/NO_(x),organics,and O_(2))into high...Electrocatalytic reduction reactions,powered by clean energy sources such as solar energy and wind,offer a sustainable method for converting inexpensive feedstocks(e.g.,CO_(2),N_(2)/NO_(x),organics,and O_(2))into high-value-added chemicals or fuels.The design and modification of electrocatalysts have been widely implemented to improve their performance in these reactions.However,bottle-necks are encountered,making it challenging to further improve performance through catalyst development alone.Recently,cations in the electrolyte have emerged as critical factors for tuning both the activity and product selectivity of reduction reactions.This review summarizes recent advances in understanding the role of cation effects in electrocatalytic reduction reactions.First,we introduce the mechanisms underlying cation effects.We then provide a comprehensive overview of their application in electroreduction reactions.Characterization techniques and theoretical calcula-tion methods for studying cation effects are also discussed.Finally,we address remaining challeng-es and future perspectives in this field.We hope that this review offers fundamental insights and design guidance for utilizing cation effects,thereby advancing their development.展开更多
To achieve efficient flotation separation of brucite and calcite,flotation separation experiments were conducted on two minerals using dodecylamine(DDA)as the collector and potassium dihydrogen phosphate(PDP)as the re...To achieve efficient flotation separation of brucite and calcite,flotation separation experiments were conducted on two minerals using dodecylamine(DDA)as the collector and potassium dihydrogen phosphate(PDP)as the regulator.The action mechanism of DDA and PDP was explored through contact angle measurement,zeta potential detection,solution chemistry calculation,FTIR analysis,and XPS detection.The flotation results showed that when DDA dosage was 35 mg/L and PDP dosage was 40 mg/L,the maximum floating difference between brucite and calcite was 79.81%,and the selectivity separation index was 6.46.The detection analysis showed that the main dissolved component HPO_(4)^(2−)of PDP is selectively strongly adsorbed on the Ca site on the surface of calcite,promoting the adsorption of the main dissolved component RNH_(3)^(+)of DDA on calcite surface,while brucite is basically not affected by PDP.Therefore,PDP is an effective regulator for the reverse flotation separation of brucite and calcite in DDA system.展开更多
Two soy protein 11S fractions with different surface sulfhydryl contents were prepared.Utilizing analytical ultracentrifugation,the effects of storage time and hydrogen peroxide at different concentrations(0.5-100 mmo...Two soy protein 11S fractions with different surface sulfhydryl contents were prepared.Utilizing analytical ultracentrifugation,the effects of storage time and hydrogen peroxide at different concentrations(0.5-100 mmol/L)on the two 11S fractions were investigated.Results show that after removing 2-mercaptoethanol(2-ME)by size exclusion chromatography,the 11S fraction with high surface sulfhydryl content(2.0 mol sulfhydryl/mol 11S)progressively formed 15S and 21S in dilute solutions during storage at 4℃ for 82 days.While,the 11s fraction with low surface sulfhydryl content(0.2 mol sulfhydryl/mol 11S)was stable under the same condition.Moreover,after treating the 11s with high surface sulfhydryl content with 1 mmol/L H_(2)O_(2),the weight percentage of 15S reached the maximum value of 20%.The 15S induced by air and H_(2)O_(2)could be totally converted to 11S with the addition of 10 mmol/L 2-ME,which could be attributed to that the disulfide bond linking two 11S molecules is on the surface of the 15S and easily accessible to the reducing agent 2-ME.This study helps us to deeply understand the formation mechanism of 15S and the stability of 11S.展开更多
Lithium-ion batteries(LIBs)are used in electric vehicles and portable smart devices,but lithium resources are dwindling and there is an increasing demand which has to be catered for.Sodium ion batteries(SIBs),which ar...Lithium-ion batteries(LIBs)are used in electric vehicles and portable smart devices,but lithium resources are dwindling and there is an increasing demand which has to be catered for.Sodium ion batteries(SIBs),which are less costly,are a promising replacement for LIBs because of the abundant natural reserves of sodium.The anode of a SIB is a necessary component of the battery but is less understood than the cathode.This review outlines the development of various types of anodes,including carbonbased,metallic and organic,which operate using different reaction mechanisms such as intercalation,alloying and conversion,and considers their challenges and prospects.Strategies for modifying their structures by doping and coating,and also modifying the solid electrolyte interface are discussed.In addition,this review also discusses the challenges encountered by the anode of SIBs and the solutions.展开更多
The unique photocatalytic mechanism of S-scheme heterojunction can be used to study new and efficient photocatalysts.By carefully selecting semiconductors for S-scheme heterojunction photocatalysts,it is possible to r...The unique photocatalytic mechanism of S-scheme heterojunction can be used to study new and efficient photocatalysts.By carefully selecting semiconductors for S-scheme heterojunction photocatalysts,it is possible to reduce the rate of photogenerated carrier recombination and increase the conversion efficiency of light into energy.Chalcogenides are a group of compounds that include sulfides and selenides(e.g.,CdS,ZnS,Bi_(2)S_(3),MoS_(2),ZnSe,CdSe,and CuSe).Chalcogenides have attracted considerable attention as heterojunction photocatalysts owing to their narrow bandgap,wide light absorption range,and excellent photoreduction properties.This paper presents a thorough analysis of S-scheme heterojunction photocatalysts based on chalcogenides.Following an introduction to the fundamental characteristics and benefits of S-scheme heterojunction photocatalysts,various chalcogenide-based S-scheme heterojunction photocatalyst synthesis techniques are summarized.These photocatalysts are used in numerous significant photocatalytic reactions,in-cluding the reduction of carbon dioxide,synthesis of hydrogen peroxide,conversion of organic matter,generation of hydrogen from water,nitrogen fixation,degradation of organic pollutants,and sterilization.In addition,cutting-edge characterization techniques,including in situ characterization techniques,are discussed to validate the steady and transient states of photocatalysts with an S-scheme heterojunction.Finally,the design and challenges of chalcogenide-based S-scheme heterojunction photocatalysts are explored and recommended in light of state-of-the-art research.展开更多
Silicon anodes are promising for use in lithium-ion batteries.However,their practical application is severely limited by their large volume expansion leading to irreversible material fracture and electrical disconnect...Silicon anodes are promising for use in lithium-ion batteries.However,their practical application is severely limited by their large volume expansion leading to irreversible material fracture and electrical disconnects.This study proposes a new top-down strategy for preparing microsize porous silicon and introduces polyacrylonitrile(PAN)for a nitrogen-doped carbon coating,which is designed to maintain the internal pore volume and lower the expansion of the anode during lithiation and delithiation.We then explore the effect of temperature on the evolution of the structure of PAN and the electrochemical behavior of the composite electrode.After treatment at 400℃,the PAN coating retains a high nitrogen content of 11.35 at%,confirming the presence of C—N and C—O bonds that improve the ionic-electronic transport properties.This treatment not only results in a more intact carbon layer structure,but also introduces carbon defects,and produces a material that has remarkable stable cycling even at high rates.When cycled at 4 A g^(-1),the anode had a specific capacity of 857.6 mAh g^(-1) even after 200 cycles,demonstrating great potential for high-capacity energy storage applications.展开更多
The bimetallic nanostructures that mix a plasmonic metal with a transition metal in the form of the core-shell nanoparticles are promising to promote catalytic performance.But it is still unclear how the heat(hot elec...The bimetallic nanostructures that mix a plasmonic metal with a transition metal in the form of the core-shell nanoparticles are promising to promote catalytic performance.But it is still unclear how the heat(hot electrons and phonons)transfers on the interface between two metals.We have designed and synthesized Au@Cu bimetallic nanoparticles with Au as core and Cu as shell.By using transient absorption spectroscopy,we find that there are two plasmon induced heat funneling processes from Au core to Cu shell.One is the electron temperature equilibrium(electron heat transfer)with equilibration time of~560 fs.The other is the lattice temperature equilibrium(lattice heat transfer)with equilibration time of~13 ps.This plasmon induced heat funneling may be universal in similar bimetallic nanostructures,so our finding could contribute to further understanding the catalytic mechanism of bimetallic plasmonic photothermal catalysis.展开更多
A 3D nitrogen⁃doped graphene/multi⁃walled carbon nanotube(CS⁃GO⁃NCNT)crosslinked network mate⁃rial was successfully synthesized utilizing chitosan and melamine as carbon and nitrogen sources,concomitant with the incor...A 3D nitrogen⁃doped graphene/multi⁃walled carbon nanotube(CS⁃GO⁃NCNT)crosslinked network mate⁃rial was successfully synthesized utilizing chitosan and melamine as carbon and nitrogen sources,concomitant with the incorporation of multi⁃wall carbon nanotubes and employing freeze drying technology.The material amalgamates the merits of 1D/2D hybrid carbon materials,wherein 1D carbon nanotubes confer robustness and expedited elec⁃tron transport pathways,while 2D graphene sheets facilitate rapid ion migration.Furthermore,the introduction of nitrogen heteroatoms serves to furnish additional active sites for lithium storage.When served as an anode material for lithium⁃ion batteries,the CS⁃GO⁃NCNT electrode delivered a reversible capacity surpassing 500 mAh·g^(-1),mark⁃edly outperforming commercial graphite anodes.Even after 300 cycles at a high current density of 1 A·g^(-1),it remained a reversible capacity of up to 268 mAh·g^(-1).展开更多
The low-cost Fe-Cu,Fe-Ni,and Cu-based high-entropy alloys exhibit a widespread utilization prospect.However,these potential applications have been limited by their low strength.In this study,a novel Fe_(31)Cu_(31)Ni_(...The low-cost Fe-Cu,Fe-Ni,and Cu-based high-entropy alloys exhibit a widespread utilization prospect.However,these potential applications have been limited by their low strength.In this study,a novel Fe_(31)Cu_(31)Ni_(28)Al_(4)Ti_(3)Co_(3) immiscible high-entropy alloy(HEA)was developed.After vacuum arc melting and copper mold suction casting,this HEA exhibits a unique phase separation microstructure,which consists of striped Cu-rich regions and Fe-rich region.Further magnification of the striped Cu-rich region reveals that it is composed of a Cu-rich dot-like phase and a Fe-rich region.The aging alloy is further strengthened by a L1_(2)-Ni_(3)(AlTi)nanoprecipitates,achieving excellent yield strength(1185 MPa)and uniform ductility(~8.8%).The differential distribution of the L1_(2) nanoprecipitate in the striped Cu-rich region and the external Fe-rich region increased the strength difference between these two regions,which increased the strain gradient and thus improved hetero-deformation induced(HDI)hardening.This work provides a new route to improve the HDI hardening of Fe-Cu alloys.展开更多
Dissociative adsorption of HCl on Au(111)has become one of unsolved puzzles in surface chemistry.Despite tremendous efforts in the past years,varioustheoretical models still greatly overestimate the zero-coverage init...Dissociative adsorption of HCl on Au(111)has become one of unsolved puzzles in surface chemistry.Despite tremendous efforts in the past years,varioustheoretical models still greatly overestimate the zero-coverage initial sticking probabilities(So).To find the origin of the large experiment-theory discrepancy,we have revisited the dissociative adsorption of HCl on Au(111)with a newly designed molecular beam-surface apparatus.The zero-coverage So derived from Cl-coverage measurements with varying HCl doses agree well with previous ones.However,we notice a sharp change of the coverage/dose slope with the HCl dosage at the low coverage regime,which may result in some uncertainties to the fitted So value.This seems consistent with a coverage-dependence of the dissociation barrier predicted by density functional theory at low Cl-coverages.Our results reveal the potential inconsistency of utilizing simulations with finite coverage to compare against experimental data with zero coverage in this system,and provide guidance for improving both experiment and theory in this regard.展开更多
A transition-metal-free strategy for the synthesis of tetrasubstituted furans is reported.Promoted by boron trifluo-ride diethyl etherate,the reaction of alkynyl sulfoxides with ynamides/ynol ethers proceeded via a ca...A transition-metal-free strategy for the synthesis of tetrasubstituted furans is reported.Promoted by boron trifluo-ride diethyl etherate,the reaction of alkynyl sulfoxides with ynamides/ynol ethers proceeded via a cascade process including cross-coupling of the two reactants,[3,3]-sulfonium rearrangement,and 5-exo-dig heterocyclization,leading to tetrasubstituted furan products.The resultant α-alkylthio groups can be used for further functionalization,such as to introduce other alkyl/aryl groups.展开更多
The efficient extraction of sodium(Na^(+))and lithium(Li^(+))from seawater and salt lakes is increasingly demanding due to their great application value in chemical industries.However,coexisting cations such as divale...The efficient extraction of sodium(Na^(+))and lithium(Li^(+))from seawater and salt lakes is increasingly demanding due to their great application value in chemical industries.However,coexisting cations such as divalent calcium(Ca^(2+))and magnesium(Mg^(2+))ions are at the subnanometer scale in diameter,similar to target monovalent ions,making ion separation a great challenge.Here,we propose a simple and fast secondary growth method for the preparation of MIL-53(Al)-NH_(2)membranes on the surface of anodic aluminum oxide.Such membranes contain angstrom-scale(~7Å)channels for the entrance of small monovalent ions and water molecules,endowing the selectivities for monovalent cations over divalent cations and water over salt molecules.The resulting high-connectivity MIL-53(Al)-NH_(2)membranes exhibit excellent ion separation performance(a selectivity of 121.42 for Na^(+)/Ca^(2+)and 93.81 for Li^(+)/Mg^(2+))and desalination performance(a water/salt selectivity of up to 5196).This work highlights metal–organic framework membranes as potential candidates for realizing ion separation and desalination in liquid treatment.展开更多
Industrial activities such as smelting emissions,mineral combustion and industrial wastewater discharge might lead to copper pollution in the environment.This kind of copper pollution has harmful effects on aquatic o ...Industrial activities such as smelting emissions,mineral combustion and industrial wastewater discharge might lead to copper pollution in the environment.This kind of copper pollution has harmful effects on aquatic o rganisms,plants and animals through direct or indirect exposure.However,the current understanding of the toxicity of copper is rather limited.Copper overload can perturb intracellular homeostasis and induce oxidative stress and e ven cell death.Recently,cuproptosis has been identified as a copper-dependent form of cell death induced by o xidative stress in mitochondria.We uncover here that zinc transporter 1(ZNT1)is an important regulator involved in cuproptosis.Firstly,we established the copper overload-induced cell death model with the overexpression of copper importer SLC31A1 in HeLa cells.Using this model,we conducted unbiased genome-wide CRISPR-Cas9 screens in cells treated with copper.Our results revealed a significant enrichment of ZNT1 gene in both library A and library B plasmids.Knocking out of ZNT1 in HeLa cells notably prevented cuproptosis.Subsequent knockout of metal transcription factor 1(MTF1)in ZNT1-deficient cells nearly abolished their ability to resist copper-induced cell death.However,overexpression of metallothionein 1X(MT1X)in the double-knockout cells could p artially restored the resistance to cuproptosis by loss of MTF1.Mechanistically,knockout of ZNT1 could promote MT1X expression by activating MTF1.As a consequence,the interaction between MT1X and copper was e nhanced,reducing the flow of copper into mitochondria and eliminating mitochondria damage.Taken together,this study reveals the important role of ZNT1 in cuproptosis and shows MTF1-MT1X axis mediated resistance to c uproptosis.Moreover,our study will help to understand the regulatory mechanism of cellular and systemic copper homeostasis under copper overload,and present insights into novel treatments for damages caused by both genetic copper overload diseases and environmental copper contamination.展开更多
As by-products of petroleum refining,heavy oils are characterized by a high carbon content,low cost and great variability,making them competitive precursors for the anodes of potassium ion batteries(PIBs).However,the ...As by-products of petroleum refining,heavy oils are characterized by a high carbon content,low cost and great variability,making them competitive precursors for the anodes of potassium ion batteries(PIBs).However,the relationship between heavy oil composition and potassium storage performance remains unclear.Using heavy oils containing distinct chemical groups as the carbon source,namely fluid catalytic cracking slurry(FCCS),petroleum asphalt(PA)and deoiled asphalt(DOA),three carbon nanosheets(CNS)were prepared through a molten salt method,and used as the anodes for PIBs.The composition of the heavy oil determines the lamellar thicknesses,sp3-C/sp2-C ratio and defect concentration,thereby affecting the potassium storage performance.The high content of aromatic hydrocarbons and moderate amount of heavy component moieties in FCCS produce carbon nanosheets(CNS-FCCS)that have a smaller layer thickness,larger interlayer spacing(0.372 nm),and increased number of folds than in CNS derived from the other three precursors.These features give it faster charge/ion transfer,more potassium storage sites and better reaction kinetics.CNS-FCCS has a remarkable K^(+)storage capacity(248.7 mAh g^(-1) after 100 cycles at 0.1 A g^(-1)),long cycle lifespan(190.8 mAh g^(-1) after 800 cycles at 1.0 A g^(-1))and excellent rate capability,ranking it among the best materials for this application.This work sheds light on the influence of heavy oil composition on carbon structure and electrochemical performance,and provides guidance for the design and development of advanced heavy oil-derived carbon electrodes for PIBs.展开更多
The separation of halogens and recovery of heavy metals from secondary copper smelting(SCS)dust using a sulfating roasting−water leaching process were investigated.The thermodynamic analysis results confirm the feasib...The separation of halogens and recovery of heavy metals from secondary copper smelting(SCS)dust using a sulfating roasting−water leaching process were investigated.The thermodynamic analysis results confirm the feasibility of the phase transformation to metal sulfates and to gaseous HF and HCl.Under the sulfating roasting conditions of the roasting temperature of 250℃ and the sulfuric acid excess coefficient of 1.8,over 74 wt.%of F and 98 wt.%of Cl were volatilized into flue gas.Approximately 98.6 wt.%of Zn and 96.5 wt.%of Cu in the roasting product were dissolved into the leaching solution after the water leaching process,while the leaching efficiencies of Pb and Sn were only 0.12%and 0.22%,respectively.The mechanism studies indicate the pivotal effect of roasting temperature on the sulphation reactions from various metal species to metal sulfates and the salting out reactions from various metal halides to gaseous hydrogen halides.展开更多
In the development of rechargeable lithium ion batteries(LIBs),silicon anodes have attracted much attention because of their extremely high theoretical capacity,relatively low Li-insertion voltage and the availability...In the development of rechargeable lithium ion batteries(LIBs),silicon anodes have attracted much attention because of their extremely high theoretical capacity,relatively low Li-insertion voltage and the availability of silicon resources.However,their large volume expansion and fragile solid electrolyte interface(SEI)film hinder their commercial application.To solve these problems,Si has been combined with various carbon materials to increase their structural stability and improve their interface properties.The use of different carbon materials,such as amorphous carbon and graphite,as three-dimensional(3D)protective anode coatings that help buffer mechanical strain and isolate the electrolyte is detailed,and novel methods for applying the coatings are outlined.However,carbon materials used as a protective layer still have some disadvantages,necessitating their modification.Recent developments have focused on modifying the protective carbon shells,and substitutes for the carbon have been suggested.展开更多
Exploitation of sustainable energy sources requires the use of unique conversion and storage systems,such as solar panels,batteries,fuel cells,and electronic equipment.Thermal load management of these energy conversio...Exploitation of sustainable energy sources requires the use of unique conversion and storage systems,such as solar panels,batteries,fuel cells,and electronic equipment.Thermal load management of these energy conversion and storage systems is one of their challenges and concerns.In this article,the thermal management of these systems using thermoelectric modules is reviewed.The results show that by choosing the right option to remove heat from the hot side of the thermoelectric modules,it will be a suitable local cooling,and the thermoelectric modules increase the power and lifespan of the system by reducing the spot temperature.Thermoelectric modules were effective in reducing panel temperature.They increase the time to reach a temperature above 50℃ in batteries by 3 to 4 times.Also,in their integration with fuel cells,they increase the power density of the fuel cell.展开更多
基金supported by the Ensemble Grant for Early Career Researchers 2022-2023 and the 2023 Ensemble Continuation Grant of Tohoku University,the Hirose Foundation,and the AIMR Fusion Research Grantsupported by JSPS KAKENHI Nos.JP23K13599,JP23K13703,JP22H01803,JP18H05513,and JP23K13542.F.Y.and Q.W.acknowledge the China Scholarship Council(CSC)to support their studies in Japan.
文摘Magnesium(Mg)is a promising alternative to lithium(Li)as an anode material in solid-state batteries due to its abundance and high theoretical volumetric capacity.However,the sluggish Mg-ion conduction in the lattice of solidstate electrolytes(SSEs)is one of the key challenges that hamper the development of Mg-ion solid-state batteries.Though various Mg-ion SSEs have been reported in recent years,key insights are hard to be derived from a single literature report.Besides,the structure-performance relationships of Mg-ion SSEs need to be further unraveled to provide a more precise design guideline for SSEs.In this viewpoint article,we analyze the structural characteristics of the Mg-based SSEs with high ionic conductivity reported in the last four decades based upon data mining-we provide big-data-derived insights into the challenges and opportunities in developing next-generation Mg-ion SSEs.
文摘Hard carbons(HCs)are recognized as potential anode materials for sodium-ion batteries(SIBs)because of their low cost,environmental friendliness,and the abundance of their precursors.The presence of graphitic domains,numerous pores,and disordered carbon layers in HCs plays a significant role in determining their sodium storage ability,but these structural features depend on the precursor used.The influence of functional groups,including heteroatoms and oxygen-containing groups,and the microstructure of the precursor on the physical and electrochemical properties of the HC produced are evaluated,and the effects of carbonization conditions(carbonization temperature,heating rate and atmosphere)are also discussed.
基金Project(52004062)supported by the National Natural Science Foundation of ChinaProject(2020-MS-084)supported by the Natural Science Foundation of Liaoning Province,ChinaProject(N2125014)supported by the Fundamental Research Funds for the Central Universities,China。
文摘The electrochemical behavior of Al(Ⅲ)in urea-1-butyl-3-methylimidazolium chloride-aluminum chloride(urea-BMIC-AlCl_(3))ionic liquids,and the effect of potential and temperature on the characterization of cathode products,current efficiency and energy consumption of aluminum electrorefining have been investigated.Cyclic voltammetry showed that the electrochemical reduction of Al(Ⅲ)was a one-step three-electron-transfer irreversible reaction,and the electrochemical reaction was controlled by diffusion.The diffusion coefficient of Al(Ⅲ)in urea-BMIC-AlCl_(3)ionic liquids at 313 K was 1.94×10^(−7)cm^(2)/s.The 7075 aluminum alloy was used as an anode for electrorefining,and the cathode products were analyzed by XRD,SEM and EDS.The results from XRD analysis indicated that the main phase of the cathode products was aluminum.The results from SEM and EDS characterization revealed that the cathode product obtained by electrorefining−1.2 V(vs.Al)was dense and uniform,and the mass fraction of aluminum decreased from 99.61%to 99.10%as the experimental temperature increased from 313 K to 333 K.In this work,the optimum experimental conditions were−1.2 V(vs.Al)and 313 K.At this time,the cathode current efficiency was 97.80%,while the energy consumption was 3.72 kW·h/kg.
文摘Electrocatalytic reduction reactions,powered by clean energy sources such as solar energy and wind,offer a sustainable method for converting inexpensive feedstocks(e.g.,CO_(2),N_(2)/NO_(x),organics,and O_(2))into high-value-added chemicals or fuels.The design and modification of electrocatalysts have been widely implemented to improve their performance in these reactions.However,bottle-necks are encountered,making it challenging to further improve performance through catalyst development alone.Recently,cations in the electrolyte have emerged as critical factors for tuning both the activity and product selectivity of reduction reactions.This review summarizes recent advances in understanding the role of cation effects in electrocatalytic reduction reactions.First,we introduce the mechanisms underlying cation effects.We then provide a comprehensive overview of their application in electroreduction reactions.Characterization techniques and theoretical calcula-tion methods for studying cation effects are also discussed.Finally,we address remaining challeng-es and future perspectives in this field.We hope that this review offers fundamental insights and design guidance for utilizing cation effects,thereby advancing their development.
基金the General Program of the National Natural Science Foundation of China(Nos.51974064,52174239)the National Key R&D Program of China(No.2021YFC2902400)the Outstanding Postdoctoral Program of Jiangsu Province,China(No.2022ZB521).
文摘To achieve efficient flotation separation of brucite and calcite,flotation separation experiments were conducted on two minerals using dodecylamine(DDA)as the collector and potassium dihydrogen phosphate(PDP)as the regulator.The action mechanism of DDA and PDP was explored through contact angle measurement,zeta potential detection,solution chemistry calculation,FTIR analysis,and XPS detection.The flotation results showed that when DDA dosage was 35 mg/L and PDP dosage was 40 mg/L,the maximum floating difference between brucite and calcite was 79.81%,and the selectivity separation index was 6.46.The detection analysis showed that the main dissolved component HPO_(4)^(2−)of PDP is selectively strongly adsorbed on the Ca site on the surface of calcite,promoting the adsorption of the main dissolved component RNH_(3)^(+)of DDA on calcite surface,while brucite is basically not affected by PDP.Therefore,PDP is an effective regulator for the reverse flotation separation of brucite and calcite in DDA system.
基金supported by the National Natural Science Foundation of China(No.22173092 and No.21674107).
文摘Two soy protein 11S fractions with different surface sulfhydryl contents were prepared.Utilizing analytical ultracentrifugation,the effects of storage time and hydrogen peroxide at different concentrations(0.5-100 mmol/L)on the two 11S fractions were investigated.Results show that after removing 2-mercaptoethanol(2-ME)by size exclusion chromatography,the 11S fraction with high surface sulfhydryl content(2.0 mol sulfhydryl/mol 11S)progressively formed 15S and 21S in dilute solutions during storage at 4℃ for 82 days.While,the 11s fraction with low surface sulfhydryl content(0.2 mol sulfhydryl/mol 11S)was stable under the same condition.Moreover,after treating the 11s with high surface sulfhydryl content with 1 mmol/L H_(2)O_(2),the weight percentage of 15S reached the maximum value of 20%.The 15S induced by air and H_(2)O_(2)could be totally converted to 11S with the addition of 10 mmol/L 2-ME,which could be attributed to that the disulfide bond linking two 11S molecules is on the surface of the 15S and easily accessible to the reducing agent 2-ME.This study helps us to deeply understand the formation mechanism of 15S and the stability of 11S.
文摘Lithium-ion batteries(LIBs)are used in electric vehicles and portable smart devices,but lithium resources are dwindling and there is an increasing demand which has to be catered for.Sodium ion batteries(SIBs),which are less costly,are a promising replacement for LIBs because of the abundant natural reserves of sodium.The anode of a SIB is a necessary component of the battery but is less understood than the cathode.This review outlines the development of various types of anodes,including carbonbased,metallic and organic,which operate using different reaction mechanisms such as intercalation,alloying and conversion,and considers their challenges and prospects.Strategies for modifying their structures by doping and coating,and also modifying the solid electrolyte interface are discussed.In addition,this review also discusses the challenges encountered by the anode of SIBs and the solutions.
文摘The unique photocatalytic mechanism of S-scheme heterojunction can be used to study new and efficient photocatalysts.By carefully selecting semiconductors for S-scheme heterojunction photocatalysts,it is possible to reduce the rate of photogenerated carrier recombination and increase the conversion efficiency of light into energy.Chalcogenides are a group of compounds that include sulfides and selenides(e.g.,CdS,ZnS,Bi_(2)S_(3),MoS_(2),ZnSe,CdSe,and CuSe).Chalcogenides have attracted considerable attention as heterojunction photocatalysts owing to their narrow bandgap,wide light absorption range,and excellent photoreduction properties.This paper presents a thorough analysis of S-scheme heterojunction photocatalysts based on chalcogenides.Following an introduction to the fundamental characteristics and benefits of S-scheme heterojunction photocatalysts,various chalcogenide-based S-scheme heterojunction photocatalyst synthesis techniques are summarized.These photocatalysts are used in numerous significant photocatalytic reactions,in-cluding the reduction of carbon dioxide,synthesis of hydrogen peroxide,conversion of organic matter,generation of hydrogen from water,nitrogen fixation,degradation of organic pollutants,and sterilization.In addition,cutting-edge characterization techniques,including in situ characterization techniques,are discussed to validate the steady and transient states of photocatalysts with an S-scheme heterojunction.Finally,the design and challenges of chalcogenide-based S-scheme heterojunction photocatalysts are explored and recommended in light of state-of-the-art research.
文摘Silicon anodes are promising for use in lithium-ion batteries.However,their practical application is severely limited by their large volume expansion leading to irreversible material fracture and electrical disconnects.This study proposes a new top-down strategy for preparing microsize porous silicon and introduces polyacrylonitrile(PAN)for a nitrogen-doped carbon coating,which is designed to maintain the internal pore volume and lower the expansion of the anode during lithiation and delithiation.We then explore the effect of temperature on the evolution of the structure of PAN and the electrochemical behavior of the composite electrode.After treatment at 400℃,the PAN coating retains a high nitrogen content of 11.35 at%,confirming the presence of C—N and C—O bonds that improve the ionic-electronic transport properties.This treatment not only results in a more intact carbon layer structure,but also introduces carbon defects,and produces a material that has remarkable stable cycling even at high rates.When cycled at 4 A g^(-1),the anode had a specific capacity of 857.6 mAh g^(-1) even after 200 cycles,demonstrating great potential for high-capacity energy storage applications.
基金supported by the National Naural Science Foudation of China(No.21873013 and No.22273006).
文摘The bimetallic nanostructures that mix a plasmonic metal with a transition metal in the form of the core-shell nanoparticles are promising to promote catalytic performance.But it is still unclear how the heat(hot electrons and phonons)transfers on the interface between two metals.We have designed and synthesized Au@Cu bimetallic nanoparticles with Au as core and Cu as shell.By using transient absorption spectroscopy,we find that there are two plasmon induced heat funneling processes from Au core to Cu shell.One is the electron temperature equilibrium(electron heat transfer)with equilibration time of~560 fs.The other is the lattice temperature equilibrium(lattice heat transfer)with equilibration time of~13 ps.This plasmon induced heat funneling may be universal in similar bimetallic nanostructures,so our finding could contribute to further understanding the catalytic mechanism of bimetallic plasmonic photothermal catalysis.
文摘A 3D nitrogen⁃doped graphene/multi⁃walled carbon nanotube(CS⁃GO⁃NCNT)crosslinked network mate⁃rial was successfully synthesized utilizing chitosan and melamine as carbon and nitrogen sources,concomitant with the incorporation of multi⁃wall carbon nanotubes and employing freeze drying technology.The material amalgamates the merits of 1D/2D hybrid carbon materials,wherein 1D carbon nanotubes confer robustness and expedited elec⁃tron transport pathways,while 2D graphene sheets facilitate rapid ion migration.Furthermore,the introduction of nitrogen heteroatoms serves to furnish additional active sites for lithium storage.When served as an anode material for lithium⁃ion batteries,the CS⁃GO⁃NCNT electrode delivered a reversible capacity surpassing 500 mAh·g^(-1),mark⁃edly outperforming commercial graphite anodes.Even after 300 cycles at a high current density of 1 A·g^(-1),it remained a reversible capacity of up to 268 mAh·g^(-1).
基金Projects(52001083,52171111,U2141207)supported by the National Natural Science Foundation of ChinaProject(LH2020E060)supported by the Natural Science Foundation of Heilongjiang,China。
文摘The low-cost Fe-Cu,Fe-Ni,and Cu-based high-entropy alloys exhibit a widespread utilization prospect.However,these potential applications have been limited by their low strength.In this study,a novel Fe_(31)Cu_(31)Ni_(28)Al_(4)Ti_(3)Co_(3) immiscible high-entropy alloy(HEA)was developed.After vacuum arc melting and copper mold suction casting,this HEA exhibits a unique phase separation microstructure,which consists of striped Cu-rich regions and Fe-rich region.Further magnification of the striped Cu-rich region reveals that it is composed of a Cu-rich dot-like phase and a Fe-rich region.The aging alloy is further strengthened by a L1_(2)-Ni_(3)(AlTi)nanoprecipitates,achieving excellent yield strength(1185 MPa)and uniform ductility(~8.8%).The differential distribution of the L1_(2) nanoprecipitate in the striped Cu-rich region and the external Fe-rich region increased the strength difference between these two regions,which increased the strain gradient and thus improved hetero-deformation induced(HDI)hardening.This work provides a new route to improve the HDI hardening of Fe-Cu alloys.
基金supported by the National Natural Science Foundation of China(No.22173042,No.21973037,No.22073089,and No.22327801)the In-novation program for Quantum Science and Technolo-gy(No.2021ZD0303304)+2 种基金the Guangdong Science and Technology Program(No.2019ZT08L455 and No.2019JC01X091)the Shenzhen Science and Technology Program(No.ZDSYS2020421111001787)Strategic Priority Research Program of the Chinese Academy of Sciences(XDB0450101).
文摘Dissociative adsorption of HCl on Au(111)has become one of unsolved puzzles in surface chemistry.Despite tremendous efforts in the past years,varioustheoretical models still greatly overestimate the zero-coverage initial sticking probabilities(So).To find the origin of the large experiment-theory discrepancy,we have revisited the dissociative adsorption of HCl on Au(111)with a newly designed molecular beam-surface apparatus.The zero-coverage So derived from Cl-coverage measurements with varying HCl doses agree well with previous ones.However,we notice a sharp change of the coverage/dose slope with the HCl dosage at the low coverage regime,which may result in some uncertainties to the fitted So value.This seems consistent with a coverage-dependence of the dissociation barrier predicted by density functional theory at low Cl-coverages.Our results reveal the potential inconsistency of utilizing simulations with finite coverage to compare against experimental data with zero coverage in this system,and provide guidance for improving both experiment and theory in this regard.
文摘A transition-metal-free strategy for the synthesis of tetrasubstituted furans is reported.Promoted by boron trifluo-ride diethyl etherate,the reaction of alkynyl sulfoxides with ynamides/ynol ethers proceeded via a cascade process including cross-coupling of the two reactants,[3,3]-sulfonium rearrangement,and 5-exo-dig heterocyclization,leading to tetrasubstituted furan products.The resultant α-alkylthio groups can be used for further functionalization,such as to introduce other alkyl/aryl groups.
基金supported by the Fundamental Research Funds for the Central Universities(WK2060000030)USTC Research Funds of the Double First Class Initiative(YD2060002022)Major Science and Technology Innovation Projects in Shandong Province(2022CXGC020415).
文摘The efficient extraction of sodium(Na^(+))and lithium(Li^(+))from seawater and salt lakes is increasingly demanding due to their great application value in chemical industries.However,coexisting cations such as divalent calcium(Ca^(2+))and magnesium(Mg^(2+))ions are at the subnanometer scale in diameter,similar to target monovalent ions,making ion separation a great challenge.Here,we propose a simple and fast secondary growth method for the preparation of MIL-53(Al)-NH_(2)membranes on the surface of anodic aluminum oxide.Such membranes contain angstrom-scale(~7Å)channels for the entrance of small monovalent ions and water molecules,endowing the selectivities for monovalent cations over divalent cations and water over salt molecules.The resulting high-connectivity MIL-53(Al)-NH_(2)membranes exhibit excellent ion separation performance(a selectivity of 121.42 for Na^(+)/Ca^(2+)and 93.81 for Li^(+)/Mg^(2+))and desalination performance(a water/salt selectivity of up to 5196).This work highlights metal–organic framework membranes as potential candidates for realizing ion separation and desalination in liquid treatment.
文摘Industrial activities such as smelting emissions,mineral combustion and industrial wastewater discharge might lead to copper pollution in the environment.This kind of copper pollution has harmful effects on aquatic o rganisms,plants and animals through direct or indirect exposure.However,the current understanding of the toxicity of copper is rather limited.Copper overload can perturb intracellular homeostasis and induce oxidative stress and e ven cell death.Recently,cuproptosis has been identified as a copper-dependent form of cell death induced by o xidative stress in mitochondria.We uncover here that zinc transporter 1(ZNT1)is an important regulator involved in cuproptosis.Firstly,we established the copper overload-induced cell death model with the overexpression of copper importer SLC31A1 in HeLa cells.Using this model,we conducted unbiased genome-wide CRISPR-Cas9 screens in cells treated with copper.Our results revealed a significant enrichment of ZNT1 gene in both library A and library B plasmids.Knocking out of ZNT1 in HeLa cells notably prevented cuproptosis.Subsequent knockout of metal transcription factor 1(MTF1)in ZNT1-deficient cells nearly abolished their ability to resist copper-induced cell death.However,overexpression of metallothionein 1X(MT1X)in the double-knockout cells could p artially restored the resistance to cuproptosis by loss of MTF1.Mechanistically,knockout of ZNT1 could promote MT1X expression by activating MTF1.As a consequence,the interaction between MT1X and copper was e nhanced,reducing the flow of copper into mitochondria and eliminating mitochondria damage.Taken together,this study reveals the important role of ZNT1 in cuproptosis and shows MTF1-MT1X axis mediated resistance to c uproptosis.Moreover,our study will help to understand the regulatory mechanism of cellular and systemic copper homeostasis under copper overload,and present insights into novel treatments for damages caused by both genetic copper overload diseases and environmental copper contamination.
文摘As by-products of petroleum refining,heavy oils are characterized by a high carbon content,low cost and great variability,making them competitive precursors for the anodes of potassium ion batteries(PIBs).However,the relationship between heavy oil composition and potassium storage performance remains unclear.Using heavy oils containing distinct chemical groups as the carbon source,namely fluid catalytic cracking slurry(FCCS),petroleum asphalt(PA)and deoiled asphalt(DOA),three carbon nanosheets(CNS)were prepared through a molten salt method,and used as the anodes for PIBs.The composition of the heavy oil determines the lamellar thicknesses,sp3-C/sp2-C ratio and defect concentration,thereby affecting the potassium storage performance.The high content of aromatic hydrocarbons and moderate amount of heavy component moieties in FCCS produce carbon nanosheets(CNS-FCCS)that have a smaller layer thickness,larger interlayer spacing(0.372 nm),and increased number of folds than in CNS derived from the other three precursors.These features give it faster charge/ion transfer,more potassium storage sites and better reaction kinetics.CNS-FCCS has a remarkable K^(+)storage capacity(248.7 mAh g^(-1) after 100 cycles at 0.1 A g^(-1)),long cycle lifespan(190.8 mAh g^(-1) after 800 cycles at 1.0 A g^(-1))and excellent rate capability,ranking it among the best materials for this application.This work sheds light on the influence of heavy oil composition on carbon structure and electrochemical performance,and provides guidance for the design and development of advanced heavy oil-derived carbon electrodes for PIBs.
基金the National Key Research and Development Program of China(No.2019YFC1908400)the National Natural Science Foundation of China(Nos.52174334,52374413)+3 种基金the Jiangxi Provincial Cultivation Program for Academic and Technical Leaders of Major Subjects,China(Nos.20212BCJ23007,20212BCJL23052)the Jiangxi Provincial Natural Science Foundation,China(Nos.20224ACB214009,20224BAB214040)the Double Thousand Plan of Jiangxi Province,China(No.S2021GDQN2970)the Distinguished Professor Program of Jinggang Scholars in Institutions of Higher Learning of Jiangxi Province,China.
文摘The separation of halogens and recovery of heavy metals from secondary copper smelting(SCS)dust using a sulfating roasting−water leaching process were investigated.The thermodynamic analysis results confirm the feasibility of the phase transformation to metal sulfates and to gaseous HF and HCl.Under the sulfating roasting conditions of the roasting temperature of 250℃ and the sulfuric acid excess coefficient of 1.8,over 74 wt.%of F and 98 wt.%of Cl were volatilized into flue gas.Approximately 98.6 wt.%of Zn and 96.5 wt.%of Cu in the roasting product were dissolved into the leaching solution after the water leaching process,while the leaching efficiencies of Pb and Sn were only 0.12%and 0.22%,respectively.The mechanism studies indicate the pivotal effect of roasting temperature on the sulphation reactions from various metal species to metal sulfates and the salting out reactions from various metal halides to gaseous hydrogen halides.
文摘In the development of rechargeable lithium ion batteries(LIBs),silicon anodes have attracted much attention because of their extremely high theoretical capacity,relatively low Li-insertion voltage and the availability of silicon resources.However,their large volume expansion and fragile solid electrolyte interface(SEI)film hinder their commercial application.To solve these problems,Si has been combined with various carbon materials to increase their structural stability and improve their interface properties.The use of different carbon materials,such as amorphous carbon and graphite,as three-dimensional(3D)protective anode coatings that help buffer mechanical strain and isolate the electrolyte is detailed,and novel methods for applying the coatings are outlined.However,carbon materials used as a protective layer still have some disadvantages,necessitating their modification.Recent developments have focused on modifying the protective carbon shells,and substitutes for the carbon have been suggested.
文摘Exploitation of sustainable energy sources requires the use of unique conversion and storage systems,such as solar panels,batteries,fuel cells,and electronic equipment.Thermal load management of these energy conversion and storage systems is one of their challenges and concerns.In this article,the thermal management of these systems using thermoelectric modules is reviewed.The results show that by choosing the right option to remove heat from the hot side of the thermoelectric modules,it will be a suitable local cooling,and the thermoelectric modules increase the power and lifespan of the system by reducing the spot temperature.Thermoelectric modules were effective in reducing panel temperature.They increase the time to reach a temperature above 50℃ in batteries by 3 to 4 times.Also,in their integration with fuel cells,they increase the power density of the fuel cell.