Development of robust electrocatalyst for oxygen reduction reaction(ORR)in a seawater electrolyte is the key to realize seawater electrolyte-based zinc-air batteries(SZABs).Herein,constructing a local electric field c...Development of robust electrocatalyst for oxygen reduction reaction(ORR)in a seawater electrolyte is the key to realize seawater electrolyte-based zinc-air batteries(SZABs).Herein,constructing a local electric field coupled with chloride ions(Cl-)fixation strategy in dual single-atom catalysts(DSACs)was proposed,and the resultant catalyst delivered considerable ORR performance in a seawater electrolyte,with a high half-wave potential(E_(1/2))of 0.868 V and a good maximum power density(Pmax)of 182 mW·cm^(−2)in the assembled SZABs,much higher than those of the Pt/C catalyst(E_(1/2):0.846 V;Pmax:150 mW·cm^(−2)).The in-situ characterization and theoretical calculations revealed that the Fe sites have a higher Cl^(−)adsorption affinity than the Co sites,and preferentially adsorbs Cl^(−)in a seawater electrolyte during the ORR process,and thus constructs a low-concentration Cl^(−)local microenvironment through the common-ion exclusion effect,which prevents Cl^(−)adsorption and corrosion in the Co active centers,achieving impressive catalytic stability.In addition,the directional charge movement between Fe and Co atomic pairs establishes a local electric field,optimizing the adsorption energy of Co sites for oxygen-containing intermediates,and further improving the ORR activity.展开更多
Batteries play a critical role in electric vehicles and distributed energy generation.With the growing demand for energy storage solutions,new battery materials and systems are continually being developed.In this proc...Batteries play a critical role in electric vehicles and distributed energy generation.With the growing demand for energy storage solutions,new battery materials and systems are continually being developed.In this process,molecular dynamics(MD)simulations can reveal the microscopic mechanisms of battery processes,thereby boosting the design of batteries.Compared to other MD simulation techniques,the machine learning force field(MLFF)holds the advantages of first-principles accuracy along with large spatial and temporal scale,offering opportunities to uncover new mechanisms in battery systems.This review presents a detailed overview of the fundamental principles and model types of MLFFs,as well as their applications in simulating the structure,transport properties,and chemical reaction properties of bulk battery materials and interfaces.Notably,we emphasize the long-range interaction corrections and constant-potential methods in the model design of MLFFs.Finally,we discuss the challenges and prospects of applying MLFF models in the research of batteries.展开更多
Understanding dynamic storage mechanisms and tuning electrode interfaces is vital for designing highperformance potassium-ion battery(KIB)anodes.Despite their high capacities,transition metal telluride(TMTe)anodes oft...Understanding dynamic storage mechanisms and tuning electrode interfaces is vital for designing highperformance potassium-ion battery(KIB)anodes.Despite their high capacities,transition metal telluride(TMTe)anodes often suffer from sluggish K+diffusion and severe volume expansion during cycling,highlighting the need for structurally optimized and interface-engineered architectures.While such strategies have been proven to be effective in lithium-and sodium-ion batteries,their use in TMTe-based KIB anodes remains largely unexplored.In this study,we firstly introduce a heterointerface-engineered three-dimensional microsphere composed of ZnTe nanoparticles and uniformly encapsulated by MXene(denoted MX/ZnTe@NC).Importantly,a built-in electric field(BIEF)is induced at the MXeneZnTe interface due to their work function.This interfacial field modulates the local electronic structure and significantly accelerates K^(+)adsorption and diffusion kinetics,especially under high current densities.First-principles simulations and spectroscopic analyses confirm that the BIEF significantly increases the K~+adsorption strength and lowers the energy barriers for ion transport.Electrochemical analyses reveal that the MX/ZnTe@NC anode delivers a high reversible capacity of 283 mAh g^(-1)after 1000 cycles at 0.5 A g^(-1),with nearly 100%Coulombic efficiency.Even at 10 A g^(-1),the anode retains a capacity of 83 mAh g^(-1),indicating excellent rate performance.Additionally,in-situ and ex-situ characterizations reveal a highly reversible ZnTe conversion mechanism involving dynamic intermediate phases.This study provides mechanistic insight into the structural and chemical evolution during cycling and highlights the synergistic role of interfacial field engineering and three-dimensional heterostructure design in advancing MXene-based KIB anodes.展开更多
The deformation characteristics and thermal response of anchor rods are crucial for ensuring the stability and safety of surrounding rock support structures.However,existing research has predominantly concentrated on ...The deformation characteristics and thermal response of anchor rods are crucial for ensuring the stability and safety of surrounding rock support structures.However,existing research has predominantly concentrated on the mechanical performance of anchor rods,with limited attention to the coupled evolution of strain and temperature fields during tensile deformation.This knowledge gap hinders a comprehensive understanding of the synergistic mechanical-thermal response mechanisms in anchor rods under loading conditions.To address this limitation,the present study systematically investigated the evolution of strain and temperature fields,along with their correlation,during the test of micro-negative Poisson's ratio(NPR)and ordinary Poisson's ratio(PR)anchor rods.Digital image correlation(DIC)and infrared thermography(IRT)techniques were employed for this exploration.The uniaxial tensile tests were conducted at two different rates,and the ordinary PR anchor rod(Q235 anchor rod)was established as a control group for comparative analysis.The findings reveal that the micro-NPR anchor rod exhibit strain localization at multiple locations during the tensile process,whereas Q235 anchors show local strain concentration in only one region.The standard deviation evolution curves for both the strain and temperature field exhibit two distinct phases in the two anchor rods.The evolution patterns between these two types of curves are basically consistent.The two standard deviation curves for the micro-NPR anchor rod display a wavy increase in the second phase,while for the Q235 anchor rod,they increase steadily until the specimen is damaged.The correlation analysis reveals that the standard deviations of strain and temperature differences for both types of anchor rods are significantly correlated.These findings demonstrate the synergistic evolution mechanism of deformation and thermal response,providing a potential foundation for utilizing thermal monitoring to assess the stability of rock support structures.展开更多
In a rapid cycling synchrotron(RCS),the magnetic field is synchronized with the beam energy,creating a highly dynamic magnetic environment.A ceramic chamber with a shielding layer(RF shield),composed of a series of co...In a rapid cycling synchrotron(RCS),the magnetic field is synchronized with the beam energy,creating a highly dynamic magnetic environment.A ceramic chamber with a shielding layer(RF shield),composed of a series of copper strips connected to a capacitor at either end,is typically employed as a vacuum chamber to mitigate eddy current effects and beam coupling impedance.Consequently,the ceramic chamber exhibits a thin-walled multilayered complex structure.Previous theoretical studies have suggested that the impedance of such a structure has a negligible impact on the beam.However,recent impedance measurements of the ceramic chamber in the China Spallation Neutron Source(CSNS)RCS revealed a resonance in the low-frequency range,which was confirmed by further theoretical analysis as a source of beam instability in the RCS.Currently,the magnitude of this impedance cannot be accurately assessed using theoretical calculations.In this study,we used the CST Microwave Studio to confirm the impedance of the ceramic chamber.Further simulations covering six different types of ceramic chambers were conducted to develop an impedance model in the RCS.Additionally,this study investigates the resonant characteristics of the ceramic chamber impedance,finding that the resonant frequency is closely related to the capacitance of the capacitors.This finding provides clear directions for further impedance optimization and is crucial for achieving a beam power of 500 kW for the CSNS Phase-Ⅱ project(CSNS-Ⅱ).However,careful attention must be paid to the voltage across the capacitors.展开更多
Peroxymonosulfate(PMS)-based advanced oxidation processes(AOPs)are an effective way to remove emerging contaminants(ECs)from water.The catalytic process involving PMS is hindered by the suboptimal electron trans-fer e...Peroxymonosulfate(PMS)-based advanced oxidation processes(AOPs)are an effective way to remove emerging contaminants(ECs)from water.The catalytic process involving PMS is hindered by the suboptimal electron trans-fer efficiency of current catalysts,the further application of AOPs technology is limited.Here,it is proposed that the interfacial electric field can be controlled by bor(B)-doped FeNC catalysts,which shows significant advantages in the efficient generation,release and participation of reactive oxygen species(ROS)in the reaction.The super exchange interaction between Fe sites and N and B sites is realized through the directional transfer of electrons in the interfacial electric field,which ensures the high efficiency and stability of the PMS catalytic process.B doping increases the d orbitals distribution at Fermi level,which facilitates enhanced electron transition activity,thereby promoting the effective generation of (1)^O_(2).At the same time,orbital hybridization causes the center of the d band to move to a lower energy level,which not only contributes to the desorption process of (1)^O_(2),but also accelerates its release.In addition,B-doping also improved the adsorption capacity of organic pollutants and shortened the migration distance of ROS,thereby significantly improving the degradation efficiency of ECs.The B-doping strategy outlined offers a novel approach to the development of FeNC catalysts,it lays a theoretical foundation and offers technical insights for the integration of PMS/AOPs technology in the ECs management.展开更多
Violet phosphorus,a recently explored layered elemental semiconductor,has attracted much attention due to its unique photoelectric,mechanical properties,and high hole mobility.Herein,violet arsenic phosphorus has for ...Violet phosphorus,a recently explored layered elemental semiconductor,has attracted much attention due to its unique photoelectric,mechanical properties,and high hole mobility.Herein,violet arsenic phosphorus has for the first time been synthesized by a molten lead method.The crystal structure of violet arsenic phosphorus(P^(83.4)As_(0.6),CSD-2408761)was determined by single crystal X-ray diffraction to have similar structure as that of violet phosphorus,where P12 is occupied by arsenic/phosphorus(As/P)atoms as mixed occupancy sites As1/P12.The arsenic substitution has been demonstrated to tune the band structure of violet phosphorus,switching p-type of violet phosphorus to high-performance n-type violet arsenic phosphorus.The effective electron mass along the<010>direction is significantly reduced from 1.792 to 0.515 m_(0)by arsenic substitution,resulting in an extremely high electron mobility of 2622.503 cm^(2)V^(-1)s^(-1).The field effect transistor built with P_(83.4)As_(0.6)nanosheets was measured to have a high electron mobility(137.06 cm^(2)V^(-1)s^(-1),61.2 nm),even under ambient conditions for 5 h,much higher than the hole mobility of violet phosphorene nanosheets(4.07 cm^(2)V^(-1)s^(-1),73.3 nm).This work provides a new idea for designing phosphorus-based materials for field effect transistors,giving significant potential in complementary metal-oxide-semiconductor applications.展开更多
Tilted metasurface nanostructures,with excellent physical properties and enormous application potential,pose an urgent need for manufacturing methods.Here,electric-field-driven generative-nanoimprinting technique is p...Tilted metasurface nanostructures,with excellent physical properties and enormous application potential,pose an urgent need for manufacturing methods.Here,electric-field-driven generative-nanoimprinting technique is proposed.The electric field applied between the template and the substrate drives the contact,tilting,filling,and holding processes.By accurately controlling the introduced included angle between the flexible template and the substrate,tilted nanostructures with a controllable angle are imprinted onto the substrate,although they are vertical on the template.By flexibly adjusting the electric field intensity and the included angle,large-area uniform-tilted,gradient-tilted,and high-angle-tilted nanostructures are fabricated.In contrast to traditional replication,the morphology of the nanoimprinting structure is extended to customized control.This work provides a cost-effective,efficient,and versatile technology for the fabrication of various large-area tilted metasurface structures.As an illustration,a tilted nanograting with a high coupling efficiency is fabricated and integrated into augmented reality displays,demonstrating superior imaging quality.展开更多
基金supported by the National Natural Science Foundation of China(52164028,52274297)the Start-up Research Foundation of Hainan University(KYQD(ZR)20008,KYQD(ZR)21125,KYQD(ZR)23169))+1 种基金Collaborative Innovation Center of Marine Science and Technology of Hainan University(XTCX2022HYC14)Innovative Research Project for Postgraduate Students in Hainan Province(Qhyb2024-95).
文摘Development of robust electrocatalyst for oxygen reduction reaction(ORR)in a seawater electrolyte is the key to realize seawater electrolyte-based zinc-air batteries(SZABs).Herein,constructing a local electric field coupled with chloride ions(Cl-)fixation strategy in dual single-atom catalysts(DSACs)was proposed,and the resultant catalyst delivered considerable ORR performance in a seawater electrolyte,with a high half-wave potential(E_(1/2))of 0.868 V and a good maximum power density(Pmax)of 182 mW·cm^(−2)in the assembled SZABs,much higher than those of the Pt/C catalyst(E_(1/2):0.846 V;Pmax:150 mW·cm^(−2)).The in-situ characterization and theoretical calculations revealed that the Fe sites have a higher Cl^(−)adsorption affinity than the Co sites,and preferentially adsorbs Cl^(−)in a seawater electrolyte during the ORR process,and thus constructs a low-concentration Cl^(−)local microenvironment through the common-ion exclusion effect,which prevents Cl^(−)adsorption and corrosion in the Co active centers,achieving impressive catalytic stability.In addition,the directional charge movement between Fe and Co atomic pairs establishes a local electric field,optimizing the adsorption energy of Co sites for oxygen-containing intermediates,and further improving the ORR activity.
基金funding support from the National Natural Science Foundation of China(92472109,T2325012)the Program for HUST Academic Frontier Youth Team+1 种基金support from the Fundamental Research Funds for the Central Universities(HUST,5003120083)supported by the Postdoctoral Fellowship Program of CPSF(GZC20240532)。
文摘Batteries play a critical role in electric vehicles and distributed energy generation.With the growing demand for energy storage solutions,new battery materials and systems are continually being developed.In this process,molecular dynamics(MD)simulations can reveal the microscopic mechanisms of battery processes,thereby boosting the design of batteries.Compared to other MD simulation techniques,the machine learning force field(MLFF)holds the advantages of first-principles accuracy along with large spatial and temporal scale,offering opportunities to uncover new mechanisms in battery systems.This review presents a detailed overview of the fundamental principles and model types of MLFFs,as well as their applications in simulating the structure,transport properties,and chemical reaction properties of bulk battery materials and interfaces.Notably,we emphasize the long-range interaction corrections and constant-potential methods in the model design of MLFFs.Finally,we discuss the challenges and prospects of applying MLFF models in the research of batteries.
基金supported by the Materials/Parts Technology Development Program(No.RS-2024-00456324)funded by the Ministry of Trade,Industry and Energy(MOTIE,Korea)the 2025 Research Fund of Hongik Universitysupported by the MSIT,Korea,under the ITRC support program(IITP-RS-2024-00436248)supervised by the IITP。
文摘Understanding dynamic storage mechanisms and tuning electrode interfaces is vital for designing highperformance potassium-ion battery(KIB)anodes.Despite their high capacities,transition metal telluride(TMTe)anodes often suffer from sluggish K+diffusion and severe volume expansion during cycling,highlighting the need for structurally optimized and interface-engineered architectures.While such strategies have been proven to be effective in lithium-and sodium-ion batteries,their use in TMTe-based KIB anodes remains largely unexplored.In this study,we firstly introduce a heterointerface-engineered three-dimensional microsphere composed of ZnTe nanoparticles and uniformly encapsulated by MXene(denoted MX/ZnTe@NC).Importantly,a built-in electric field(BIEF)is induced at the MXeneZnTe interface due to their work function.This interfacial field modulates the local electronic structure and significantly accelerates K^(+)adsorption and diffusion kinetics,especially under high current densities.First-principles simulations and spectroscopic analyses confirm that the BIEF significantly increases the K~+adsorption strength and lowers the energy barriers for ion transport.Electrochemical analyses reveal that the MX/ZnTe@NC anode delivers a high reversible capacity of 283 mAh g^(-1)after 1000 cycles at 0.5 A g^(-1),with nearly 100%Coulombic efficiency.Even at 10 A g^(-1),the anode retains a capacity of 83 mAh g^(-1),indicating excellent rate performance.Additionally,in-situ and ex-situ characterizations reveal a highly reversible ZnTe conversion mechanism involving dynamic intermediate phases.This study provides mechanistic insight into the structural and chemical evolution during cycling and highlights the synergistic role of interfacial field engineering and three-dimensional heterostructure design in advancing MXene-based KIB anodes.
基金supported by State Key Laboratory for Geomechanics and Deep Underground Engineering,China University of Mining&Technology,Beijing(Grant No.SKLGDUEK2120)。
文摘The deformation characteristics and thermal response of anchor rods are crucial for ensuring the stability and safety of surrounding rock support structures.However,existing research has predominantly concentrated on the mechanical performance of anchor rods,with limited attention to the coupled evolution of strain and temperature fields during tensile deformation.This knowledge gap hinders a comprehensive understanding of the synergistic mechanical-thermal response mechanisms in anchor rods under loading conditions.To address this limitation,the present study systematically investigated the evolution of strain and temperature fields,along with their correlation,during the test of micro-negative Poisson's ratio(NPR)and ordinary Poisson's ratio(PR)anchor rods.Digital image correlation(DIC)and infrared thermography(IRT)techniques were employed for this exploration.The uniaxial tensile tests were conducted at two different rates,and the ordinary PR anchor rod(Q235 anchor rod)was established as a control group for comparative analysis.The findings reveal that the micro-NPR anchor rod exhibit strain localization at multiple locations during the tensile process,whereas Q235 anchors show local strain concentration in only one region.The standard deviation evolution curves for both the strain and temperature field exhibit two distinct phases in the two anchor rods.The evolution patterns between these two types of curves are basically consistent.The two standard deviation curves for the micro-NPR anchor rod display a wavy increase in the second phase,while for the Q235 anchor rod,they increase steadily until the specimen is damaged.The correlation analysis reveals that the standard deviations of strain and temperature differences for both types of anchor rods are significantly correlated.These findings demonstrate the synergistic evolution mechanism of deformation and thermal response,providing a potential foundation for utilizing thermal monitoring to assess the stability of rock support structures.
基金supported by the Guangdong Basic and Applied Basic Research Foundation,China(No.2021B1515140007).
文摘In a rapid cycling synchrotron(RCS),the magnetic field is synchronized with the beam energy,creating a highly dynamic magnetic environment.A ceramic chamber with a shielding layer(RF shield),composed of a series of copper strips connected to a capacitor at either end,is typically employed as a vacuum chamber to mitigate eddy current effects and beam coupling impedance.Consequently,the ceramic chamber exhibits a thin-walled multilayered complex structure.Previous theoretical studies have suggested that the impedance of such a structure has a negligible impact on the beam.However,recent impedance measurements of the ceramic chamber in the China Spallation Neutron Source(CSNS)RCS revealed a resonance in the low-frequency range,which was confirmed by further theoretical analysis as a source of beam instability in the RCS.Currently,the magnitude of this impedance cannot be accurately assessed using theoretical calculations.In this study,we used the CST Microwave Studio to confirm the impedance of the ceramic chamber.Further simulations covering six different types of ceramic chambers were conducted to develop an impedance model in the RCS.Additionally,this study investigates the resonant characteristics of the ceramic chamber impedance,finding that the resonant frequency is closely related to the capacitance of the capacitors.This finding provides clear directions for further impedance optimization and is crucial for achieving a beam power of 500 kW for the CSNS Phase-Ⅱ project(CSNS-Ⅱ).However,careful attention must be paid to the voltage across the capacitors.
基金supported by the National Natural Science Foundation of China(No.22278156)the Guangdong Special Support Program Project(No.2021JC060580)+1 种基金the Young Elite Scientists Sponsorship Program by CAST-Doctoral Student Special Plan,the China Scholarship Council Program(No.202406150148)the Natural Science Foundation of Guangdong Province(No.2023A1515011186).
文摘Peroxymonosulfate(PMS)-based advanced oxidation processes(AOPs)are an effective way to remove emerging contaminants(ECs)from water.The catalytic process involving PMS is hindered by the suboptimal electron trans-fer efficiency of current catalysts,the further application of AOPs technology is limited.Here,it is proposed that the interfacial electric field can be controlled by bor(B)-doped FeNC catalysts,which shows significant advantages in the efficient generation,release and participation of reactive oxygen species(ROS)in the reaction.The super exchange interaction between Fe sites and N and B sites is realized through the directional transfer of electrons in the interfacial electric field,which ensures the high efficiency and stability of the PMS catalytic process.B doping increases the d orbitals distribution at Fermi level,which facilitates enhanced electron transition activity,thereby promoting the effective generation of (1)^O_(2).At the same time,orbital hybridization causes the center of the d band to move to a lower energy level,which not only contributes to the desorption process of (1)^O_(2),but also accelerates its release.In addition,B-doping also improved the adsorption capacity of organic pollutants and shortened the migration distance of ROS,thereby significantly improving the degradation efficiency of ECs.The B-doping strategy outlined offers a novel approach to the development of FeNC catalysts,it lays a theoretical foundation and offers technical insights for the integration of PMS/AOPs technology in the ECs management.
基金supported by the National Natural Science Foundation of China(Grant No.22175136)the State Key Laboratory of Electrical Insulation and Power Equipment(Grant No.EIPE23127)the Fundamental Research Funds for the Central Universities(xtr052024009,xtr052025002).
文摘Violet phosphorus,a recently explored layered elemental semiconductor,has attracted much attention due to its unique photoelectric,mechanical properties,and high hole mobility.Herein,violet arsenic phosphorus has for the first time been synthesized by a molten lead method.The crystal structure of violet arsenic phosphorus(P^(83.4)As_(0.6),CSD-2408761)was determined by single crystal X-ray diffraction to have similar structure as that of violet phosphorus,where P12 is occupied by arsenic/phosphorus(As/P)atoms as mixed occupancy sites As1/P12.The arsenic substitution has been demonstrated to tune the band structure of violet phosphorus,switching p-type of violet phosphorus to high-performance n-type violet arsenic phosphorus.The effective electron mass along the<010>direction is significantly reduced from 1.792 to 0.515 m_(0)by arsenic substitution,resulting in an extremely high electron mobility of 2622.503 cm^(2)V^(-1)s^(-1).The field effect transistor built with P_(83.4)As_(0.6)nanosheets was measured to have a high electron mobility(137.06 cm^(2)V^(-1)s^(-1),61.2 nm),even under ambient conditions for 5 h,much higher than the hole mobility of violet phosphorene nanosheets(4.07 cm^(2)V^(-1)s^(-1),73.3 nm).This work provides a new idea for designing phosphorus-based materials for field effect transistors,giving significant potential in complementary metal-oxide-semiconductor applications.
基金supported by National Natural Science Foundation of China(No.52025055 and 52275571)Basic Research Operation Fund of China(No.xzy012024024).
文摘Tilted metasurface nanostructures,with excellent physical properties and enormous application potential,pose an urgent need for manufacturing methods.Here,electric-field-driven generative-nanoimprinting technique is proposed.The electric field applied between the template and the substrate drives the contact,tilting,filling,and holding processes.By accurately controlling the introduced included angle between the flexible template and the substrate,tilted nanostructures with a controllable angle are imprinted onto the substrate,although they are vertical on the template.By flexibly adjusting the electric field intensity and the included angle,large-area uniform-tilted,gradient-tilted,and high-angle-tilted nanostructures are fabricated.In contrast to traditional replication,the morphology of the nanoimprinting structure is extended to customized control.This work provides a cost-effective,efficient,and versatile technology for the fabrication of various large-area tilted metasurface structures.As an illustration,a tilted nanograting with a high coupling efficiency is fabricated and integrated into augmented reality displays,demonstrating superior imaging quality.
