In this study,the twinning-detwinning behavior and slip behavior of rolled AZ31 magnesium-alloy plates during a three-step intermittent dynamic compression process along the rolling direction(RD)and normal direction(N...In this study,the twinning-detwinning behavior and slip behavior of rolled AZ31 magnesium-alloy plates during a three-step intermittent dynamic compression process along the rolling direction(RD)and normal direction(ND),are investigated via quasi-in situ electron backscatter diffraction,and the causes of the twinning and detwinning behavior are explained according to Schmid law,local strain coordination,and slip trajectories.It is found that the twins are first nucleated and grow at a compressive strain of 3%along the RD.In addition to the Schmid factor(SF),the strain coordination factor(m’)also influences the selection of the twin variants during the twinning process,resulting in the nucleation of twins with a low SF.During the second and third steps of the application of continuous compressive strains with magnitudes and directions of 3%RD+3%ND and 3%RD+3%ND+2.5%ND,detwinning occurs to different extents.The observation of the detwinning behavior reveals that the order in which multiple twins within the same grain undergo complete detwinning is related to Schmid law and the strain concentration,with a low SF and a high strain concentration promoting complete detwinning.The interaction between slip dislocations and twin boundaries in the deformed grains as well as the pinning of dislocations at the tips of the {1012} tensile twins with a special structure result in incomplete detwinning.Understanding the microstructural evolution and twinning behavior of magnesium alloys under different deformation geometries is important for the development of high-strength and high-toughness magnesium alloys.展开更多
Bioelectronic interventions,specifically trigeminal nerve st imulat ion(TNS),have attracted considerable attention in conditions where cortical spreading depolarizations(CSDs)accompanied by compromised cerebral perfus...Bioelectronic interventions,specifically trigeminal nerve st imulat ion(TNS),have attracted considerable attention in conditions where cortical spreading depolarizations(CSDs)accompanied by compromised cerebral perfusion may exacerbate neurological damage.While pharmacological interventions have demonstrated initial potential in addressing CSDs,a standardized treatment approach has not yet been established.The objective of this perspective is to explore emerging bioelectronic methodologies for addressing CSDs,particularly emphasizing TNS,and to underscore TNS’s capacity to enhance neurovascular coupling and cerebral perfusion.展开更多
The development of electronic products and increased electronic waste have triggered a series of ecological problems on Earth.Meanwhile,amidst energy crises and the pursuit of carbon neutrality,the recycling of discar...The development of electronic products and increased electronic waste have triggered a series of ecological problems on Earth.Meanwhile,amidst energy crises and the pursuit of carbon neutrality,the recycling of discarded biomass has attracted the attention of many researchers.In recent years,the transformation of discarded biomass into value-added electronic products has emerged as a promising endeavor in the field of green and flexible electronics.In this review,the attempts and advancements in biomass conversion into flexible electronic materials and devices are systematically summarized.We focus on reviewing the research progress in biomass conversion into substrates,electrodes,and materials tailored for optical and thermal management.Furthermore,we explore component combinations suitable for applications in environmental monitoring and health management.Finally,we discuss the challenges in techniques and cost-effectiveness currently faced by biomass conversion into flexible electronic devices and propose improvement strategies.Drawing insights from both fundamental research and industrial applications,we offer prospects for future developments in this burgeoning field.展开更多
Structural regulation of Pd-based electrocatalytic hydrodechlorination(EHDC)catalyst for constructing high-efficient cathode materials with low noble metal content and high atom utilization is crucial but still challe...Structural regulation of Pd-based electrocatalytic hydrodechlorination(EHDC)catalyst for constructing high-efficient cathode materials with low noble metal content and high atom utilization is crucial but still challenging.Herein,a support electron inductive effect of Pd-Mn/Ni foam catalyst was proposed via in-situ Mn doping to optimize the electronic structure of the Ni foam(NF),which can inductive regulation of Pd for improving the EHDC performance.The mass activity and current efficiency of Pd-Mn/NF catalyst are 2.91 and 1.34 times superior to that of Pd/NF with 2,4-dichlorophenol as model compound,respectively.The Mn-doped interlayer optimized the electronic structure of Pd by bringing the d-state closer to the Fermi level than Pd on the NF surface,which optimizied the binding of EHDC intermediates.Additionally,the Mn-doped interlayer acted as a promoter for generating H∗and accelerating the EHDC reaction.This work presents a simple and effective regulation strategy for constructing high-efficient cathode catalyst for the EHDC of chlorinated organic compounds.展开更多
Up-and-coming high-temperature materials,refractory high entropy alloys,are suffering from lower oxidation resistance,restricting their applications in the aerospace field.In this study,two novel treatments of Al-depo...Up-and-coming high-temperature materials,refractory high entropy alloys,are suffering from lower oxidation resistance,restricting their applications in the aerospace field.In this study,two novel treatments of Al-deposited and remelted were developed to refine the microstructure and enhance the oxidation resistance of refractory high entropy alloy using electron beam freeform fabrication(EBF3).Finer and short-range ordering structures were observed in the remelted sample,whereas the Al-deposited sample showcased the formation of silicide and intermetallic phases.High-temperature cyclic and isothermal oxidation tests at 1000℃ were carried out.The total weight gain after 60 h of cyclic oxidation decreased by 17.49%and 30.46%for the remelted and deposited samples,respectively,compared to the as-cast state.Oxidation kinetics reveal an evident lower mass gain and oxidation rate in the treated samples.A multilayer oxide consisting of TiO_(2)+Al_(2)O_(3)+SiO_(2)+AlNbO_(4) was studied for its excellent oxidation resistance.The oxidation behavior of rutile,corundum and other oxides was analyzed using first principles calculations and chemical defect analysis.Overall,this research,which introduces novel treatments,offers promising insights for enhancing the inherent oxidation resistance of refractory high entropy alloys.展开更多
Catalytic oxidation of organic pollutants is a well-known and effective technique for pollutant abatement.Unfortunately,this method is significantly hindered in practical applications by the lowefficiency and difficul...Catalytic oxidation of organic pollutants is a well-known and effective technique for pollutant abatement.Unfortunately,this method is significantly hindered in practical applications by the lowefficiency and difficult recovery of the catalysts in a powdery form.Herein,a three-dimensional(3D)framework of Fe-incorporated Ni_(3)S_(2)nanosheets in-situ grown on Ni foam(Fe-Ni_(3)S_(2)@NF)was fabricated by a facile two-step hydrothermal process and applied to trigger peroxymonosulfate(PMS)oxidation of organic compounds inwater.A homogeneous growth environment enabled the uniform and scalable growth of Fe-Ni_(3)S_(2)nanosheets on the Ni foam.Fe-Ni_(3)S_(2)@NF possessed outstanding activity and durability in activating PMS,as it effectively facilitated electron transfer from organic pollutants to PMS.Fe-Ni_(3)S_(2)@NF initially supplied electrons to PMS,causing the catalyst to undergo oxidation,and subsequently accepted electrons from organic compounds,returning to its initial state.The introduction of Fe into the Ni_(3)S_(2)lattice enhanced electrical conductivity,promoting mediated electron transfer between PMS and organic compounds.The 3D conductive Ni foam provided an ideal platform for the nucleation and growth of Fe-Ni_(3)S_(2),accelerating pollutant abatement due to its porous structure and high conductivity.Furthermore,its monolithic nature simplified the catalyst recycling process.A continuous flow packed-bed reactor by encapsulating Fe-Ni_(3)S_(2)@NF catalyst achieved complete pollutant abatement with continuous operation for 240 h,highlighting its immense potential for practical environmental remediation.This study presents a facile synthesis method for creating a novel type of monolithic catalyst with high activity and durability for decontamination through Fenton-like processes.展开更多
Point defect engineering endows catalysts with novel physical and chemical properties,elevating their electrocatalytic efficiency.The introduction of defects emerges as a promising strategy,effectively modifying the e...Point defect engineering endows catalysts with novel physical and chemical properties,elevating their electrocatalytic efficiency.The introduction of defects emerges as a promising strategy,effectively modifying the electronic structure of active sites.This optimization influences the adsorption energy of intermediates,thereby mitigating reaction energy barriers,altering paths,enhancing selectivity,and ultimately improving the catalytic efficiency of electrocatalysts.To elucidate the impact of defects on the electrocatalytic process,we comprehensively outline the roles of various point defects,their synthetic methodologies,and characterization techniques.Importantly,we consolidate insights into the relationship between point defects and catalytic activity for hydrogen/oxygen evolution and CO_(2)/O_(2)/N_(2) reduction reactions by integrating mechanisms from diverse reactions.This underscores the pivotal role of point defects in enhancing catalytic performance.At last,the principal challenges and prospects associated with point defects in current electrocatalysts are proposed,emphasizing their role in advancing the efficiency of electrochemical energy storage and conversion materials.展开更多
The triple bond in N_(2)has an extremely high bond energy and is thus difficult to break.N_(2)is commonly converted into NH3 artificially via the Haber-Bosch process,and NH_(3)can be utilized to produce other nitrogen...The triple bond in N_(2)has an extremely high bond energy and is thus difficult to break.N_(2)is commonly converted into NH3 artificially via the Haber-Bosch process,and NH_(3)can be utilized to produce other nitrogen-containing chemicals.Here,we developed an electron catalyzed method to directly fix N_(2)into azos,by pushing and pulling the electron into and from the aromatic halide with the cyclic voltammetry method.The round-trip journey of electron can successfully weaken the triple bond in N_(2)through the electron pushing-induced aryl radical via a“brick trowel”transition state,and then produce the diazonium ions by pulling the electron out from the diazo radical intermediate.Different azos can be synthesized with this developed electron catalyzed approach.This approach provides a novel concept and practical route for the fixation of N_(2)at atmospheric pressure into chemical products valuable for industrial and commercial applications.展开更多
Self-trapping excitons(STEs) emission in metal halides has been a matter of interest, correlating with the strength of electron-phonon coupling in the lattice, which are usually caused by ions with ns~2 electronic str...Self-trapping excitons(STEs) emission in metal halides has been a matter of interest, correlating with the strength of electron-phonon coupling in the lattice, which are usually caused by ions with ns~2 electronic structure. In this work, Sb^(3+)/Te^(4+)ions doped Zn-based halide single crystals(SCs) with two STEs emissions have been synthesized and the possibility of its anti-counterfeiting application was explored.Further, the relationship between the strength of electron-phonon coupling and photoluminescence quantum yields(PLQYs) for STEs in a series of metal halides has been studied. And the semi-empirical range of the Huang-Rhys factors(S) for metal halides with excellent photoluminescence(PL) property has been summarized. This work provides ideas for further research into the relationship between luminescence performance and electron-phonon coupling of metal halides, and also provides a reference for designing the metal halides with high PLQYs.展开更多
Layered double hydroxide(LDH)based heterogonous peroxymonosulfate(PMS)activation degradation of pollutants has attracted extensive attention.The challenge is to selectively regulate the traditional free radical domina...Layered double hydroxide(LDH)based heterogonous peroxymonosulfate(PMS)activation degradation of pollutants has attracted extensive attention.The challenge is to selectively regulate the traditional free radical dominant degradation pathway into a nonradical degradation pathway.Herein,an interface ar-chitecture of Ti_(3) C_(2) T_(x)-MXene(MXene)loading on the Fe-Al LDH scaffold was developed,which showed excellent stability and robust resistance against harsh conditions.Significantly,the rate constant for tetra-cycline hydrochloride(TC)degradation in the MXene-LDH/PMS process was 0.421 min^(-1),which was ten times faster than the rate constant for pure Fe-Al LDH(0.042 min^(-1)).Specifically,more reactive Fe with the closer d-band center to the Fermi level results in higher electron transfer efficiency.The occupa-tions of Fe-3d orbitals in Mxene/Fe-Al LDH are pushed above the Fermi level to generate,which results in higher PMS adsorption and inhibition of the release of oxygen-containing active species intermedi-ates,leading to the enhanced^(1)O_(2) generation.Additionally,the built-in electric field in the heterojunc-tion was driven by the charge redistribution between MXene and Fe-Al LDH,resulting in a mediated-electron transfer mechanism,differentiating it from the Fe-Al LDH/PMS system.It was fascinating that MXene/Fe-Al LDH achieved satisfactory treatment efficiency in continuous column reactor and real landfill leachate.展开更多
In rock drilling and blasting,the misfire of electronic detonators will not only affect the rock fragmentation result but also bring serious potential safety hazards to engineering construction.An accurate and compreh...In rock drilling and blasting,the misfire of electronic detonators will not only affect the rock fragmentation result but also bring serious potential safety hazards to engineering construction.An accurate and comprehensive understanding of the failure mechanisms of electronic detonators subjected to impact loading is of great significance to the reliability design and field safety use of electronic detonators.The spatial distribution characteristics and failure modes of misfired electronic detonators under different application scenarios are statistically analysed.The results show that under high impact loads,electronic detonators will experience failure phenomena such as rupture of the fuse head,fracture of the bridge wire,falling off of the solder joint,chip module damage and insufficient initiation energy after deformation.The lack of impact resistance is the primary cause of misfire of electronic detonators.Combined with the underwater impact resistance test and the impact load test in the adjacent blasthole on site,the formulas of the impact failure probability of the electronic detonator under different stress‒strength distribution curves are deduced.The test and evaluation method of the impact resistance of electronic detonators based on stress‒strength interference theory is proposed.Furthermore,the impact failure model of electronic detonators considering the strength degradation effect under repeated random loads is established.On this basis,the failure mechanism of electronic detonators under different application environments,such as open-pit blasting and underground blasting,is revealed,which provides scientific theory and methods for the reliability analysis,design and type selection of electronic detonators in rock drilling and blasting.展开更多
High-resolution transmission electron microscopy(HRTEM)promises rapid atomic-scale dynamic structure imaging.Yet,the precision limitations of aberration parameters and the challenge of eliminating aberrations in Cs-co...High-resolution transmission electron microscopy(HRTEM)promises rapid atomic-scale dynamic structure imaging.Yet,the precision limitations of aberration parameters and the challenge of eliminating aberrations in Cs-corrected transmission electron microscopy constrain resolution.A machine learning algorithm is developed to determine the aberration parameters with higher precision from small,lattice-periodic crystal images.The proposed algorithm is then validated with simulated HRTEM images of graphene and applied to the experimental images of a molybdenum disulfide(MoS_(2))monolayer with 25 variables(14 aberrations)resolved in wide ranges.Using these measured parameters,the phases of the exit-wave functions are reconstructed for each image in a focal series of MoS_(2)monolayers.The images were acquired due to the unexpected movement of the specimen holder.Four-dimensional data extraction reveals time-varying atomic structures and ripple.In particular,the atomic evolution of the sulfur-vacancy point and line defects,as well as the edge structure near the amorphous,is visualized as the resolution has been improved from about 1.75?to 0.9 A.This method can help salvage important transmission electron microscope images and is beneficial for the images obtained from electron microscopes with average stability.展开更多
Regulation the electronic density of solid-state electrolyte by donor–acceptor(D–A)system can achieve highly-selective Li^(+)transportation and conduction in solid-state Li metal batteries.This study reports a high-...Regulation the electronic density of solid-state electrolyte by donor–acceptor(D–A)system can achieve highly-selective Li^(+)transportation and conduction in solid-state Li metal batteries.This study reports a high-performance solid-state electrolyte thorough D–A-linked covalent organic frameworks(COFs)based on intramolecular charge transfer interactions.Unlike other reported COFbased solid-state electrolyte,the developed concept with D–A-linked COFs not only achieves electronic modulation to promote highly-selective Li^(+)migration and inhibit Li dendrite,but also offers a crucial opportunity to understand the role of electronic density in solid-state Li metal batteries.The introduced strong electronegativity F-based ligand in COF electrolyte results in highlyselective Li^(+)(transference number 0.83),high ionic conductivity(6.7×10^(-4)S cm^(−1)),excellent cyclic ability(1000 h)in Li metal symmetric cell and high-capacity retention in Li/LiFePO_(4)cell(90.8%for 300 cycles at 5C)than substituted C-and N-based ligands.This is ascribed to outstanding D–A interaction between donor porphyrin and acceptor F atoms,which effectively expedites electron transferring from porphyrin to F-based ligand and enhances Li^(+)kinetics.Consequently,we anticipate that this work creates insight into the strategy for accelerating Li^(+)conduction in high-performance solid-state Li metal batteries through D–A system.展开更多
X-ray free-electron lasers(XFELs)can generate bright X-ray pulses with short durations and narrow bandwidths,leading to extensive applica-tions in many disciplines such as biology,materials science,and ultrafast scien...X-ray free-electron lasers(XFELs)can generate bright X-ray pulses with short durations and narrow bandwidths,leading to extensive applica-tions in many disciplines such as biology,materials science,and ultrafast science.Recently,there has been a growing demand for X-ray pulses with high photon energy,especially from developments in“diffraction-before-destruction”applications and in dynamic mesoscale materials science.Here,we propose utilizing the electron beams at XFELs to drive a meter-scale two-bunch plasma wakefield accelerator and double the energy of the accelerated beam in a compact and inexpensive way.Particle-in-cell simulations are performed to study the beam quality degradation under different beam loading scenarios and nonideal issues,and the results show that more than half of the accelerated beam can meet the requirements of XFELs.After its transport to the undulator,the accelerated beam can improve the photon energy to 22 keV by a factor of around four while maintaining the peak power,thus offering a promising pathway toward high-photon-energy XFELs.展开更多
A facile method for decarboxylative amination driven by the photoactivity of electron donor-acceptor(EDA)com-plexes assembled from iodide salts and redox-active esters has been proposed.A broad array of acyclic and cy...A facile method for decarboxylative amination driven by the photoactivity of electron donor-acceptor(EDA)com-plexes assembled from iodide salts and redox-active esters has been proposed.A broad array of acyclic and cyclic protected amines were readily synthesized without requiring exogenous transition-metal or photoredox catalysts.Moreover,this ap-proach facilitates late-stage functionalization of complex molecules and is amenable to continuous-flow process on gram scale.展开更多
The Standard Model of particle physics assumes that fundamental fermions are point particles with zero radius, no spatial dimensions, and infinite matter density. This alternative model treats the nine charged fundame...The Standard Model of particle physics assumes that fundamental fermions are point particles with zero radius, no spatial dimensions, and infinite matter density. This alternative model treats the nine charged fundamental fermions (three leptons and nine quarks) as spheres with non-zero holographic radius. Holographic analysis (based on quantum mechanics, general relativity, thermodynamics, and Shannon information theory) specifies electron mass by five fundamental constants: Planck’s constant ℏ, gravitational constant G, fine structure constant α, cosmological constant Λ, and vacuum energy fraction ΩΛ. Protons and neutrons are composite systems of up and down quarks. Describing forces between quark constituents confined within nucleons as inverse square attractive forces, this alternative model identifies composition factors Cpand Cnto relate proton and neutron masses to electron mass and thus to fundamental constants. An appendix summarizes holographic analyses characterizing astronomical masses at the opposite end of the mass scale for objects in the universe.展开更多
By simplifying catalyst-product separation and reducing phosphorus waste,heterogeneous hydroformylation offers a more sustainable alternative to homogeneous processes.However,heterogeneous hydroformylation catalysts d...By simplifying catalyst-product separation and reducing phosphorus waste,heterogeneous hydroformylation offers a more sustainable alternative to homogeneous processes.However,heterogeneous hydroformylation catalysts developed thus far still suffer from the issues of much lower activity and metal leaching,which severely hinder their practical application.Here,we demonstrate that incorporating phosphorus(P)atoms into graphitic carbon nitride(PCN)supports facilitates charge transfer from Rh to the PCN support,thus largely enhancing electronic metal-support interactions(EMSIs).In the styrene hydroformylation reaction,the activity of Rh_(1)/PCN single-atom catalysts(SACs)with varying P contents exhibited a volcano-shaped relationship with P doping,where the Rh_(1)/PCN SAC with optimal P doping showed exceptional activity,approximately 5.8-and 3.3-fold greater than that of the Rh_(1)/g-C_(3)N_(4)SAC without P doping and the industrial homogeneous catalyst HRh(CO)(PPh_(3))_(3),respectively.In addition,the optimal Rh_(1)/PCN SAC catalyst also demonstrated largely enhanced multicycle stability without any visible metal aggregation owing to the increased EMSIs,which sharply differed from the severe metal aggregation of large nanoparticles on the Rh_(1)/g-C_(3)N_(4)SAC.Mechan-istic studies revealed that the enhanced catalytic performance could be attributed to electron-deficient Rh species,which reduced CO adsorption while simultaneously promoting alkene adsorption through increased EMSIs.These findings suggest that tuning EMSIs is an effective way to achieve SACs with high activity and durability.展开更多
We present a theoretical scheme to realize two-dimensional(2D)asymmetric diffraction grating in a five-level inverted Y-type asymmetric double semiconductor quantum wells(SQWs)structure with resonant tunneling.The SQW...We present a theoretical scheme to realize two-dimensional(2D)asymmetric diffraction grating in a five-level inverted Y-type asymmetric double semiconductor quantum wells(SQWs)structure with resonant tunneling.The SQW structure interacts with a weak probe laser field,a spatially independent 2D standing-wave(SW)field,and a Laguerre–Gaussian(LG)vortex field,respectively.The results indicate that the diffraction patterns are highly sensitive to amplitude modulation and phase modulation.Because of the existence of vortex light,it is possible to realize asymmetric high-order diffraction in the SQW structure,and then a 2D asymmetric grating is established.By adjusting the detunings of the probe field,vortex field,and SW field,as well as the interaction length,diffraction intensity,and direction of the 2D asymmetric electromagnetically induced grating(EIG)can be controlled effectively.In addition,the number of orbital angular momenta(OAM)and beam waist parameter can be used to modulate the diffraction intensity and energy transfer of the probe light in different regions.High-order diffraction intensity is enhanced and high-efficiency 2D asymmetric diffraction grating with different diffraction patterns is obtained in the scheme.Such 2D asymmetric diffraction grating may be beneficial to the research of optical communication and innovative semiconductor quantum devices.展开更多
Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Her...Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Herein,with crystal and atomic structures of the self-assembled PDI revealed from the X-ray diffraction pattern,the electronic structure is theoretically illustrated by the first-principles density functional theory calculations,suggesting the suitable band structure and the direct electronic transition for efficient photocatalytic oxygen evolution over PDI.It is confirmed that the carbonyl O atoms on the conjugation structure serve as the active sites for oxygen evolution reaction by the crystal orbital Hamiltonian group analysis.The calculations of reaction free energy changes indicate that the oxygen evolution reaction should follow the reaction pathway of H_(2)O→^(*)OH→^(*)O→^(*)OOH→^(*)O_(2)with an overpotential of 0.81 V.Through an in-depth theoretical computational analysis in the atomic and electronic structures,the origin of photocatalytic oxygen evolution activity for PDI is well illustrated,which would help the rational design and modification of polymeric photocatalysts for efficient oxygen evolution.展开更多
基金supported by the General Project of Liaoning Provincial Department of Education(NO:JYTMS20231199)Project of Liaoning Education Department(No:LKMZ20220462 and No:LJKMZ20220467)+1 种基金Basic scientific research project of Liaoning Provincial Department of Education(key research project)(No:JYTZD2023108)Liaoning Nature Fund Guidance Plan(No:42022-BS.179)。
文摘In this study,the twinning-detwinning behavior and slip behavior of rolled AZ31 magnesium-alloy plates during a three-step intermittent dynamic compression process along the rolling direction(RD)and normal direction(ND),are investigated via quasi-in situ electron backscatter diffraction,and the causes of the twinning and detwinning behavior are explained according to Schmid law,local strain coordination,and slip trajectories.It is found that the twins are first nucleated and grow at a compressive strain of 3%along the RD.In addition to the Schmid factor(SF),the strain coordination factor(m’)also influences the selection of the twin variants during the twinning process,resulting in the nucleation of twins with a low SF.During the second and third steps of the application of continuous compressive strains with magnitudes and directions of 3%RD+3%ND and 3%RD+3%ND+2.5%ND,detwinning occurs to different extents.The observation of the detwinning behavior reveals that the order in which multiple twins within the same grain undergo complete detwinning is related to Schmid law and the strain concentration,with a low SF and a high strain concentration promoting complete detwinning.The interaction between slip dislocations and twin boundaries in the deformed grains as well as the pinning of dislocations at the tips of the {1012} tensile twins with a special structure result in incomplete detwinning.Understanding the microstructural evolution and twinning behavior of magnesium alloys under different deformation geometries is important for the development of high-strength and high-toughness magnesium alloys.
基金supported by National Institute of Neurological Disorders and Stroke of the National Institutes of Health under award number R21NS114763US Army Medical Research and Materiel Command (USAMRMC) under award#W81XWH-18-1-0773merit-based career enhancement award at the Feinstein Institutes for Medical Research (to CL)
文摘Bioelectronic interventions,specifically trigeminal nerve st imulat ion(TNS),have attracted considerable attention in conditions where cortical spreading depolarizations(CSDs)accompanied by compromised cerebral perfusion may exacerbate neurological damage.While pharmacological interventions have demonstrated initial potential in addressing CSDs,a standardized treatment approach has not yet been established.The objective of this perspective is to explore emerging bioelectronic methodologies for addressing CSDs,particularly emphasizing TNS,and to underscore TNS’s capacity to enhance neurovascular coupling and cerebral perfusion.
基金supported by the National Key R&D Program of China(2018YFA0901700)National Natural Science Foundation of China(22278241)+1 种基金a grant from the Institute Guo Qiang,Tsinghua University(2021GQG1016)Department of Chemical Engineering-iBHE Joint Cooperation Fund。
文摘The development of electronic products and increased electronic waste have triggered a series of ecological problems on Earth.Meanwhile,amidst energy crises and the pursuit of carbon neutrality,the recycling of discarded biomass has attracted the attention of many researchers.In recent years,the transformation of discarded biomass into value-added electronic products has emerged as a promising endeavor in the field of green and flexible electronics.In this review,the attempts and advancements in biomass conversion into flexible electronic materials and devices are systematically summarized.We focus on reviewing the research progress in biomass conversion into substrates,electrodes,and materials tailored for optical and thermal management.Furthermore,we explore component combinations suitable for applications in environmental monitoring and health management.Finally,we discuss the challenges in techniques and cost-effectiveness currently faced by biomass conversion into flexible electronic devices and propose improvement strategies.Drawing insights from both fundamental research and industrial applications,we offer prospects for future developments in this burgeoning field.
基金supported by the National Natural Science Foundation of China(Nos.22178388 and 22108306)Taishan Scholars Program of Shandong Province(No.tsqn201909065)Chongqing Science and Technology Bureau(No.cstc2019jscx-gksb X0032).
文摘Structural regulation of Pd-based electrocatalytic hydrodechlorination(EHDC)catalyst for constructing high-efficient cathode materials with low noble metal content and high atom utilization is crucial but still challenging.Herein,a support electron inductive effect of Pd-Mn/Ni foam catalyst was proposed via in-situ Mn doping to optimize the electronic structure of the Ni foam(NF),which can inductive regulation of Pd for improving the EHDC performance.The mass activity and current efficiency of Pd-Mn/NF catalyst are 2.91 and 1.34 times superior to that of Pd/NF with 2,4-dichlorophenol as model compound,respectively.The Mn-doped interlayer optimized the electronic structure of Pd by bringing the d-state closer to the Fermi level than Pd on the NF surface,which optimizied the binding of EHDC intermediates.Additionally,the Mn-doped interlayer acted as a promoter for generating H∗and accelerating the EHDC reaction.This work presents a simple and effective regulation strategy for constructing high-efficient cathode catalyst for the EHDC of chlorinated organic compounds.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFF0609000)National Natural Science Foundation of China(Grant Nos.52171034 and 52101037)Postdoctoral Fellowship Program of CPSFara(No.GZB20230944).
文摘Up-and-coming high-temperature materials,refractory high entropy alloys,are suffering from lower oxidation resistance,restricting their applications in the aerospace field.In this study,two novel treatments of Al-deposited and remelted were developed to refine the microstructure and enhance the oxidation resistance of refractory high entropy alloy using electron beam freeform fabrication(EBF3).Finer and short-range ordering structures were observed in the remelted sample,whereas the Al-deposited sample showcased the formation of silicide and intermetallic phases.High-temperature cyclic and isothermal oxidation tests at 1000℃ were carried out.The total weight gain after 60 h of cyclic oxidation decreased by 17.49%and 30.46%for the remelted and deposited samples,respectively,compared to the as-cast state.Oxidation kinetics reveal an evident lower mass gain and oxidation rate in the treated samples.A multilayer oxide consisting of TiO_(2)+Al_(2)O_(3)+SiO_(2)+AlNbO_(4) was studied for its excellent oxidation resistance.The oxidation behavior of rutile,corundum and other oxides was analyzed using first principles calculations and chemical defect analysis.Overall,this research,which introduces novel treatments,offers promising insights for enhancing the inherent oxidation resistance of refractory high entropy alloys.
基金supported by the National Natural Science Foundation of China(No.21876039)Y.Yao acknowledges the scholarship support from the China Scholarship Council(No.202106695010)Partial support from the Australian Research Council for DP230102406 is also acknowledged.
文摘Catalytic oxidation of organic pollutants is a well-known and effective technique for pollutant abatement.Unfortunately,this method is significantly hindered in practical applications by the lowefficiency and difficult recovery of the catalysts in a powdery form.Herein,a three-dimensional(3D)framework of Fe-incorporated Ni_(3)S_(2)nanosheets in-situ grown on Ni foam(Fe-Ni_(3)S_(2)@NF)was fabricated by a facile two-step hydrothermal process and applied to trigger peroxymonosulfate(PMS)oxidation of organic compounds inwater.A homogeneous growth environment enabled the uniform and scalable growth of Fe-Ni_(3)S_(2)nanosheets on the Ni foam.Fe-Ni_(3)S_(2)@NF possessed outstanding activity and durability in activating PMS,as it effectively facilitated electron transfer from organic pollutants to PMS.Fe-Ni_(3)S_(2)@NF initially supplied electrons to PMS,causing the catalyst to undergo oxidation,and subsequently accepted electrons from organic compounds,returning to its initial state.The introduction of Fe into the Ni_(3)S_(2)lattice enhanced electrical conductivity,promoting mediated electron transfer between PMS and organic compounds.The 3D conductive Ni foam provided an ideal platform for the nucleation and growth of Fe-Ni_(3)S_(2),accelerating pollutant abatement due to its porous structure and high conductivity.Furthermore,its monolithic nature simplified the catalyst recycling process.A continuous flow packed-bed reactor by encapsulating Fe-Ni_(3)S_(2)@NF catalyst achieved complete pollutant abatement with continuous operation for 240 h,highlighting its immense potential for practical environmental remediation.This study presents a facile synthesis method for creating a novel type of monolithic catalyst with high activity and durability for decontamination through Fenton-like processes.
基金supported by the National Natural Science Foundation of China(U21A20281)the Special Fund for Young Teachers from Zhengzhou University(JC23557030,JC23257011)+1 种基金the Key Research Projects of Higher Education Institutions of Henan Province(24A530009)the Project of Zhongyuan Critical Metals Laboratory(GJJSGFYQ202336).
文摘Point defect engineering endows catalysts with novel physical and chemical properties,elevating their electrocatalytic efficiency.The introduction of defects emerges as a promising strategy,effectively modifying the electronic structure of active sites.This optimization influences the adsorption energy of intermediates,thereby mitigating reaction energy barriers,altering paths,enhancing selectivity,and ultimately improving the catalytic efficiency of electrocatalysts.To elucidate the impact of defects on the electrocatalytic process,we comprehensively outline the roles of various point defects,their synthetic methodologies,and characterization techniques.Importantly,we consolidate insights into the relationship between point defects and catalytic activity for hydrogen/oxygen evolution and CO_(2)/O_(2)/N_(2) reduction reactions by integrating mechanisms from diverse reactions.This underscores the pivotal role of point defects in enhancing catalytic performance.At last,the principal challenges and prospects associated with point defects in current electrocatalysts are proposed,emphasizing their role in advancing the efficiency of electrochemical energy storage and conversion materials.
文摘The triple bond in N_(2)has an extremely high bond energy and is thus difficult to break.N_(2)is commonly converted into NH3 artificially via the Haber-Bosch process,and NH_(3)can be utilized to produce other nitrogen-containing chemicals.Here,we developed an electron catalyzed method to directly fix N_(2)into azos,by pushing and pulling the electron into and from the aromatic halide with the cyclic voltammetry method.The round-trip journey of electron can successfully weaken the triple bond in N_(2)through the electron pushing-induced aryl radical via a“brick trowel”transition state,and then produce the diazonium ions by pulling the electron out from the diazo radical intermediate.Different azos can be synthesized with this developed electron catalyzed approach.This approach provides a novel concept and practical route for the fixation of N_(2)at atmospheric pressure into chemical products valuable for industrial and commercial applications.
基金supported by the financial aid from the National Natural Science Foundation of China (No. 22271273)International Partnership Program of Chinese Academy of Sciences (No. 121522KYSB20190022)。
文摘Self-trapping excitons(STEs) emission in metal halides has been a matter of interest, correlating with the strength of electron-phonon coupling in the lattice, which are usually caused by ions with ns~2 electronic structure. In this work, Sb^(3+)/Te^(4+)ions doped Zn-based halide single crystals(SCs) with two STEs emissions have been synthesized and the possibility of its anti-counterfeiting application was explored.Further, the relationship between the strength of electron-phonon coupling and photoluminescence quantum yields(PLQYs) for STEs in a series of metal halides has been studied. And the semi-empirical range of the Huang-Rhys factors(S) for metal halides with excellent photoluminescence(PL) property has been summarized. This work provides ideas for further research into the relationship between luminescence performance and electron-phonon coupling of metal halides, and also provides a reference for designing the metal halides with high PLQYs.
基金financially supported by the Second Tibetan Plateau Scientific Expedition and Research Program(STEP)(No.2019QZKK1003)the Science and Technology Innovation Pro-gram of Hunan Province(No.2022RC1122)。
文摘Layered double hydroxide(LDH)based heterogonous peroxymonosulfate(PMS)activation degradation of pollutants has attracted extensive attention.The challenge is to selectively regulate the traditional free radical dominant degradation pathway into a nonradical degradation pathway.Herein,an interface ar-chitecture of Ti_(3) C_(2) T_(x)-MXene(MXene)loading on the Fe-Al LDH scaffold was developed,which showed excellent stability and robust resistance against harsh conditions.Significantly,the rate constant for tetra-cycline hydrochloride(TC)degradation in the MXene-LDH/PMS process was 0.421 min^(-1),which was ten times faster than the rate constant for pure Fe-Al LDH(0.042 min^(-1)).Specifically,more reactive Fe with the closer d-band center to the Fermi level results in higher electron transfer efficiency.The occupa-tions of Fe-3d orbitals in Mxene/Fe-Al LDH are pushed above the Fermi level to generate,which results in higher PMS adsorption and inhibition of the release of oxygen-containing active species intermedi-ates,leading to the enhanced^(1)O_(2) generation.Additionally,the built-in electric field in the heterojunc-tion was driven by the charge redistribution between MXene and Fe-Al LDH,resulting in a mediated-electron transfer mechanism,differentiating it from the Fe-Al LDH/PMS system.It was fascinating that MXene/Fe-Al LDH achieved satisfactory treatment efficiency in continuous column reactor and real landfill leachate.
基金supported by the Chongqing Youth Talent Support Program(Cstc2022ycjh-bgzxm0079)the Chinese National Natural Science Foundation(52379128,51979152)+2 种基金Science Fund for Distinguished Young Scholars of Hubei Proivnce(2023AFA048)Educational Commission of Hubei Province of China(T2020005)the Young Top-notch Talent Cultivation Program of Hubei Province.
文摘In rock drilling and blasting,the misfire of electronic detonators will not only affect the rock fragmentation result but also bring serious potential safety hazards to engineering construction.An accurate and comprehensive understanding of the failure mechanisms of electronic detonators subjected to impact loading is of great significance to the reliability design and field safety use of electronic detonators.The spatial distribution characteristics and failure modes of misfired electronic detonators under different application scenarios are statistically analysed.The results show that under high impact loads,electronic detonators will experience failure phenomena such as rupture of the fuse head,fracture of the bridge wire,falling off of the solder joint,chip module damage and insufficient initiation energy after deformation.The lack of impact resistance is the primary cause of misfire of electronic detonators.Combined with the underwater impact resistance test and the impact load test in the adjacent blasthole on site,the formulas of the impact failure probability of the electronic detonator under different stress‒strength distribution curves are deduced.The test and evaluation method of the impact resistance of electronic detonators based on stress‒strength interference theory is proposed.Furthermore,the impact failure model of electronic detonators considering the strength degradation effect under repeated random loads is established.On this basis,the failure mechanism of electronic detonators under different application environments,such as open-pit blasting and underground blasting,is revealed,which provides scientific theory and methods for the reliability analysis,design and type selection of electronic detonators in rock drilling and blasting.
基金financial support from the National Natural Science Foundation of China(Grant No.61971201)。
文摘High-resolution transmission electron microscopy(HRTEM)promises rapid atomic-scale dynamic structure imaging.Yet,the precision limitations of aberration parameters and the challenge of eliminating aberrations in Cs-corrected transmission electron microscopy constrain resolution.A machine learning algorithm is developed to determine the aberration parameters with higher precision from small,lattice-periodic crystal images.The proposed algorithm is then validated with simulated HRTEM images of graphene and applied to the experimental images of a molybdenum disulfide(MoS_(2))monolayer with 25 variables(14 aberrations)resolved in wide ranges.Using these measured parameters,the phases of the exit-wave functions are reconstructed for each image in a focal series of MoS_(2)monolayers.The images were acquired due to the unexpected movement of the specimen holder.Four-dimensional data extraction reveals time-varying atomic structures and ripple.In particular,the atomic evolution of the sulfur-vacancy point and line defects,as well as the edge structure near the amorphous,is visualized as the resolution has been improved from about 1.75?to 0.9 A.This method can help salvage important transmission electron microscope images and is beneficial for the images obtained from electron microscopes with average stability.
基金financial support provided by National Natural Science Foundation of China(52303283,52372232,52064049)the Major Science and Technology Projects of Yunnan Province(202302AB080019-3)+2 种基金National Natural Science Foundation of Yunnan Province(202301AS070040,202401AU070201)the Analysis and Measurements Center of Yunnan University for the sample testing servicethe Electron Microscope Center of Yunnan University for the support of this work.
文摘Regulation the electronic density of solid-state electrolyte by donor–acceptor(D–A)system can achieve highly-selective Li^(+)transportation and conduction in solid-state Li metal batteries.This study reports a high-performance solid-state electrolyte thorough D–A-linked covalent organic frameworks(COFs)based on intramolecular charge transfer interactions.Unlike other reported COFbased solid-state electrolyte,the developed concept with D–A-linked COFs not only achieves electronic modulation to promote highly-selective Li^(+)migration and inhibit Li dendrite,but also offers a crucial opportunity to understand the role of electronic density in solid-state Li metal batteries.The introduced strong electronegativity F-based ligand in COF electrolyte results in highlyselective Li^(+)(transference number 0.83),high ionic conductivity(6.7×10^(-4)S cm^(−1)),excellent cyclic ability(1000 h)in Li metal symmetric cell and high-capacity retention in Li/LiFePO_(4)cell(90.8%for 300 cycles at 5C)than substituted C-and N-based ligands.This is ascribed to outstanding D–A interaction between donor porphyrin and acceptor F atoms,which effectively expedites electron transferring from porphyrin to F-based ligand and enhances Li^(+)kinetics.Consequently,we anticipate that this work creates insight into the strategy for accelerating Li^(+)conduction in high-performance solid-state Li metal batteries through D–A system.
基金supported by the National Grand Instrument Project No. SQ2019YFF01014400the Natural Science Foundation of China (Grant Nos. 12375147, 12435011, 12075030)+2 种基金the Beijing Outstanding Young Scientist Project, Project for Young Scientists in Basic Research of Chinese Academy of Sciences (YSBR-115)the Beijing Normal University Scientific Research Initiation Fund for Introducing Talents No. 310432104the Fundamental Research Funds for the Central Universities, Peking University
文摘X-ray free-electron lasers(XFELs)can generate bright X-ray pulses with short durations and narrow bandwidths,leading to extensive applica-tions in many disciplines such as biology,materials science,and ultrafast science.Recently,there has been a growing demand for X-ray pulses with high photon energy,especially from developments in“diffraction-before-destruction”applications and in dynamic mesoscale materials science.Here,we propose utilizing the electron beams at XFELs to drive a meter-scale two-bunch plasma wakefield accelerator and double the energy of the accelerated beam in a compact and inexpensive way.Particle-in-cell simulations are performed to study the beam quality degradation under different beam loading scenarios and nonideal issues,and the results show that more than half of the accelerated beam can meet the requirements of XFELs.After its transport to the undulator,the accelerated beam can improve the photon energy to 22 keV by a factor of around four while maintaining the peak power,thus offering a promising pathway toward high-photon-energy XFELs.
文摘A facile method for decarboxylative amination driven by the photoactivity of electron donor-acceptor(EDA)com-plexes assembled from iodide salts and redox-active esters has been proposed.A broad array of acyclic and cyclic protected amines were readily synthesized without requiring exogenous transition-metal or photoredox catalysts.Moreover,this ap-proach facilitates late-stage functionalization of complex molecules and is amenable to continuous-flow process on gram scale.
文摘The Standard Model of particle physics assumes that fundamental fermions are point particles with zero radius, no spatial dimensions, and infinite matter density. This alternative model treats the nine charged fundamental fermions (three leptons and nine quarks) as spheres with non-zero holographic radius. Holographic analysis (based on quantum mechanics, general relativity, thermodynamics, and Shannon information theory) specifies electron mass by five fundamental constants: Planck’s constant ℏ, gravitational constant G, fine structure constant α, cosmological constant Λ, and vacuum energy fraction ΩΛ. Protons and neutrons are composite systems of up and down quarks. Describing forces between quark constituents confined within nucleons as inverse square attractive forces, this alternative model identifies composition factors Cpand Cnto relate proton and neutron masses to electron mass and thus to fundamental constants. An appendix summarizes holographic analyses characterizing astronomical masses at the opposite end of the mass scale for objects in the universe.
基金supported by the Petrochemical Research Institute Foundation(21-CB-09-01)the National Natural Science Foundation of China(22302186,22025205)+1 种基金the China Postdoctoral Science Foundation(2022M713030,2023T160618)the Fundamental Research Funds for the Central Universities(WK2060000058,WK2060000038).
文摘By simplifying catalyst-product separation and reducing phosphorus waste,heterogeneous hydroformylation offers a more sustainable alternative to homogeneous processes.However,heterogeneous hydroformylation catalysts developed thus far still suffer from the issues of much lower activity and metal leaching,which severely hinder their practical application.Here,we demonstrate that incorporating phosphorus(P)atoms into graphitic carbon nitride(PCN)supports facilitates charge transfer from Rh to the PCN support,thus largely enhancing electronic metal-support interactions(EMSIs).In the styrene hydroformylation reaction,the activity of Rh_(1)/PCN single-atom catalysts(SACs)with varying P contents exhibited a volcano-shaped relationship with P doping,where the Rh_(1)/PCN SAC with optimal P doping showed exceptional activity,approximately 5.8-and 3.3-fold greater than that of the Rh_(1)/g-C_(3)N_(4)SAC without P doping and the industrial homogeneous catalyst HRh(CO)(PPh_(3))_(3),respectively.In addition,the optimal Rh_(1)/PCN SAC catalyst also demonstrated largely enhanced multicycle stability without any visible metal aggregation owing to the increased EMSIs,which sharply differed from the severe metal aggregation of large nanoparticles on the Rh_(1)/g-C_(3)N_(4)SAC.Mechan-istic studies revealed that the enhanced catalytic performance could be attributed to electron-deficient Rh species,which reduced CO adsorption while simultaneously promoting alkene adsorption through increased EMSIs.These findings suggest that tuning EMSIs is an effective way to achieve SACs with high activity and durability.
基金supported by the National Natural Science Foundation of China(Grant No.12105210)the Knowledge Innovation Program of Wuhan-Basi Research(Grant No.2023010201010149)。
文摘We present a theoretical scheme to realize two-dimensional(2D)asymmetric diffraction grating in a five-level inverted Y-type asymmetric double semiconductor quantum wells(SQWs)structure with resonant tunneling.The SQW structure interacts with a weak probe laser field,a spatially independent 2D standing-wave(SW)field,and a Laguerre–Gaussian(LG)vortex field,respectively.The results indicate that the diffraction patterns are highly sensitive to amplitude modulation and phase modulation.Because of the existence of vortex light,it is possible to realize asymmetric high-order diffraction in the SQW structure,and then a 2D asymmetric grating is established.By adjusting the detunings of the probe field,vortex field,and SW field,as well as the interaction length,diffraction intensity,and direction of the 2D asymmetric electromagnetically induced grating(EIG)can be controlled effectively.In addition,the number of orbital angular momenta(OAM)and beam waist parameter can be used to modulate the diffraction intensity and energy transfer of the probe light in different regions.High-order diffraction intensity is enhanced and high-efficiency 2D asymmetric diffraction grating with different diffraction patterns is obtained in the scheme.Such 2D asymmetric diffraction grating may be beneficial to the research of optical communication and innovative semiconductor quantum devices.
基金supported by National Natural Science Foundation of China(No.523B2070,No.52225606).
文摘Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Herein,with crystal and atomic structures of the self-assembled PDI revealed from the X-ray diffraction pattern,the electronic structure is theoretically illustrated by the first-principles density functional theory calculations,suggesting the suitable band structure and the direct electronic transition for efficient photocatalytic oxygen evolution over PDI.It is confirmed that the carbonyl O atoms on the conjugation structure serve as the active sites for oxygen evolution reaction by the crystal orbital Hamiltonian group analysis.The calculations of reaction free energy changes indicate that the oxygen evolution reaction should follow the reaction pathway of H_(2)O→^(*)OH→^(*)O→^(*)OOH→^(*)O_(2)with an overpotential of 0.81 V.Through an in-depth theoretical computational analysis in the atomic and electronic structures,the origin of photocatalytic oxygen evolution activity for PDI is well illustrated,which would help the rational design and modification of polymeric photocatalysts for efficient oxygen evolution.
