Low-cost Fe-based disordered rock salt(DRX)Li_(2)FeTiO_(4)is capable of providing high capacity(295 mA h g^(-1))by redox activity of cations(Fe^(2+)/Fe^(4+)and Ti^(3+)/Ti^(4+))and anionic oxygen.However,DRX structures...Low-cost Fe-based disordered rock salt(DRX)Li_(2)FeTiO_(4)is capable of providing high capacity(295 mA h g^(-1))by redox activity of cations(Fe^(2+)/Fe^(4+)and Ti^(3+)/Ti^(4+))and anionic oxygen.However,DRX structures lack transport channels for ions and electrons,resulting in sluggish kinetics,poor electrochemical activity,and cyclability.Herein,graphene conductive carbon network permeated Li_(2)FeTiO_(4)(LFT/C/G)nanofibers are successfully prepared by a facile sol-gel assisted electrospinning method.Ultrafine Li_(2)FeTiO_(4)nanoparticles(2 nm)and one-dimensional(1D)structure provide abu ndant active sites and unobstructed diffu sion channels,accelerating ion diffusion.In addition,introducing graphene reduces the band gap and Li^(+)diffusion barrier and improves the dynamic properties of Li_(2)FeTiO_(4),thus achieving a relatively mild interfacial reaction and reversible redox reaction.As expected,the LFT/C/1.0G cathode delivers a remarkable discharge capacity(238.5 mA h g^(-1)),high energy density(508.8 Wh kg^(-1)),and excellent rate capability(51.2 mA hg^(-1)at 1.0 A g^(-1)).Besides,the LFT/C/1.0G anode also displays a high capacity(514.5 mA h g^(-1)at 500 mA g^(-1))and a remarkable rate capability(243.9 mA h g^(-1)at 8 A g^(-1)).Moreover,the full batteries based on the LFT/C/1.0G symmetric electrode demonstrate a reversible capacity of 117.0 mA h g^(-1)after 100 cycles at 50 mA g^(-1).This study presents useful insights into developing cost-effective DRX cathodes with durable and fast lithium storage.展开更多
Focused ion-beam-induced deposition （FIBID） and focused electron-beam-induced deposition （FEBID） are conve- nient and useful in nanodevice fabrication. Since the deposition is from the organometallic platinum prec...Focused ion-beam-induced deposition （FIBID） and focused electron-beam-induced deposition （FEBID） are conve- nient and useful in nanodevice fabrication. Since the deposition is from the organometallic platinum precursor, the con- ductive lines directly written by focused ion-beam （FIB） and focused electron-beam （FEB） are carbon-rich materials. We discuss an alternative approach to enhancing the platinum content and improving the conductivity of the conductive leads produced by FIBID and FEBID, namely an annealing treatment. Annealing in pure oxygen at 500 ℃ for 30 min enhances the platinum content values from ~ 18% to 30% and ~ 50% to 90% of FIBID and FEBID, respectively. Moreover, we find that thin films will be formed in the FIBID and FEBID processes. The annealing treatment is helpful to avoid the current leakage caused by these thin films. A single electron transistor is fabricated by FEBID and the current-voltage curve shows the Coulomb blockade effect.展开更多
Continuous monitoring of biosignals is essential for advancing early disease detection,personalized treatment,and health management.Flexible electronics,capable of accurately monitoring biosignals in daily life,have g...Continuous monitoring of biosignals is essential for advancing early disease detection,personalized treatment,and health management.Flexible electronics,capable of accurately monitoring biosignals in daily life,have garnered considerable attention due to their softness,conformability,and biocompatibility.However,several challenges remain,including imperfect skin-device interfaces,limited breathability,and insufficient mechanoelectrical stability.On-skin epidermal electronics,distinguished by their excellent conformability,breathability,and mechanoelectrical robustness,offer a promising solution for high-fidelity,long-term health monitoring.These devices can seamlessly integrate with the human body,leading to transformative advancements in future personalized healthcare.This review provides a systematic examination of recent advancements in on-skin epidermal electronics,with particular emphasis on critical aspects including material science,structural design,desired properties,and practical applications.We explore various materials,considering their properties and the corresponding structural designs developed to construct high-performance epidermal electronics.We then discuss different approaches for achieving the desired device properties necessary for long-term health monitoring,including adhesiveness,breathability,and mechanoelectrical stability.Additionally,we summarize the diverse applications of these devices in monitoring biophysical and physiological signals.Finally,we address the challenges facing these devices and outline future prospects,offering insights into the ongoing development of on-skin epidermal electronics for long-term health monitoring.展开更多
Wide-temperature applications of sodium-ion batteries(SIBs)are severely limited by the sluggish ion insertion/diffusion kinetics of conversion-type anodes.Quantum-sized transition metal dichalcogenides possess unique ...Wide-temperature applications of sodium-ion batteries(SIBs)are severely limited by the sluggish ion insertion/diffusion kinetics of conversion-type anodes.Quantum-sized transition metal dichalcogenides possess unique advantages of charge delocalization and enrich uncoordinated electrons and short-range transfer kinetics,which are crucial to achieve rapid low-temperature charge transfer and high-temperature interface stability.Herein,a quantum-scale FeS_(2) loaded on three-dimensional Ti_(3)C_(2) MXene skeletons(FeS_(2) QD/MXene)fabricated as SIBs anode,demonstrating impressive performance under wide-temperature conditions(−35 to 65).The theoretical calculations combined with experimental characterization interprets that the unsaturated coordination edges of FeS_(2) QD can induce delocalized electronic regions,which reduces electrostatic potential and significantly facilitates efficient Na+diffusion across a broad temperature range.Moreover,the Ti_(3)C_(2) skeleton reinforces structural integrity via Fe-O-Ti bonding,while enabling excellent dispersion of FeS_(2) QD.As expected,FeS_(2) QD/MXene anode harvests capacities of 255.2 and 424.9 mAh g^(−1) at 0.1 A g^(−1) under−35 and 65,and the energy density of FeS_(2) QD/MXene//NVP full cell can reach to 162.4 Wh kg^(−1) at−35,highlighting its practical potential for wide-temperatures conditions.This work extends the uncoordinated regions induced by quantum-size effects for exceptional Na^(+)ion storage and diffusion performance at wide-temperatures environment.展开更多
Artificial intelligence(AI)is increasingly recognized as a transformative force in the field of solid organ transplantation.From enhancing donor-recipient matching to predicting clinical risks and tailoring immunosupp...Artificial intelligence(AI)is increasingly recognized as a transformative force in the field of solid organ transplantation.From enhancing donor-recipient matching to predicting clinical risks and tailoring immunosuppressive therapy,AI has the potential to improve both operational efficiency and patient outcomes.Despite these advancements,the perspectives of transplant professionals-those at the forefront of critical decision-making-remain insufficiently explored.To address this gap,this study utilizes a multi-round electronic Delphi approach to gather and analyses insights from global experts involved in organ transplantation.Participants are invited to complete structured surveys capturing demographic data,professional roles,institutional practices,and prior exposure to AI technologies.The survey also explores perceptions of AI’s potential benefits.Quantitative responses are analyzed using descriptive statistics,while open-ended qualitative responses undergo thematic analysis.Preliminary findings indicate a generally positive outlook on AI’s role in enhancing transplantation processes,particularly in areas such as donor matching and post-operative care.These mixed views reflect both optimism and caution among professionals tasked with integrating new technologies into high-stakes clinical workflows.By capturing a wide range of expert opinions,the findings will inform future policy development,regulatory considerations,and institutional readiness frameworks for the integration of AI into organ transplantation.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
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
The traditional von Neumann architecture faces inherent limitations due to the separation of memory and computa-tion,leading to high energy consumption,significant latency,and reduced operational efficiency.Neuromorph...The traditional von Neumann architecture faces inherent limitations due to the separation of memory and computa-tion,leading to high energy consumption,significant latency,and reduced operational efficiency.Neuromorphic computing,inspired by the architecture of the human brain,offers a promising alternative by integrating memory and computational func-tions,enabling parallel,high-speed,and energy-efficient information processing.Among various neuromorphic technologies,ion-modulated optoelectronic devices have garnered attention due to their excellent ionic tunability and the availability of multi-dimensional control strategies.This review provides a comprehensive overview of recent progress in ion-modulation optoelec-tronic neuromorphic devices.It elucidates the key mechanisms underlying ionic modulation of light fields,including ion migra-tion dynamics and capture and release of charge through ions.Furthermore,the synthesis of active materials and the proper-ties of these devices are analyzed in detail.The review also highlights the application of ion-modulation optoelectronic devices in artificial vision systems,neuromorphic computing,and other bionic fields.Finally,the existing challenges and future direc-tions for the development of optoelectronic neuromorphic devices are discussed,providing critical insights for advancing this promising field.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
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
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
Despite their attractive features of high energy density,low cost,and safety,polysulfide/iodide flow batteries(SIFBs)are hampered by the sluggish kinetics of the iodide redox couple,which restricts overall performance...Despite their attractive features of high energy density,low cost,and safety,polysulfide/iodide flow batteries(SIFBs)are hampered by the sluggish kinetics of the iodide redox couple,which restricts overall performance.Multicomponent sulfides are demonstrated as promising catalysts for accelerating I^(-)/I_(3)^(-) redox reactions.Concurrently,the enhanced configurational entropy arising from multinary compositions drives synergistic effects among constituent elements,establishing a viable pathway to optimize catalytic performance.Building on these foundations,this work introduces a targeted orbital hybridization-optimized electron density strategy to enhance the catalytic activity.Implementing this concept,we developed an in-situ solvothermal synthesis process for an entropy-enhanced AgCuZnSnS_(4) loaded graphite felt(ACZTS/GF)electrode.The engineered electrode demonstrates exceptional electrocatalytic performance with improved bulk conductivity and interfacial charge transfer kinetics within a SIFB.The cell achieves a high energy efficiency of 88.5%at 20 mA·cm^(−2) with 10%state-of-charge.Furthermore,the battery delivers a maximum power density of 119.8 mW·cm^(−2) and exhibits excellent long-term cycling stability.These significant results stem from orbital hybridization-driven electronic state optimization and entropy effect-induced synergistic catalysis.展开更多
We report a study on the electronic structure and chemical bonding of the PB and AsB diatomic molecules using high-resolution photoelectron imaging of cryogenically-cooled PB^(−)and AsB^(−)anions.The electron affiniti...We report a study on the electronic structure and chemical bonding of the PB and AsB diatomic molecules using high-resolution photoelectron imaging of cryogenically-cooled PB^(−)and AsB^(−)anions.The electron affinities of PB and AsB are measured to be 2.751(1)and 2.600(1)eV,respectively.The ground states of the PB^(−)and AsB−anions are determined to be ^(2)Σ^(+) with a σ^(1)π^(4) valence electron configuration.The ground states of neutral PB and AsB are found to be ^(3)Π_(2) with a σ^(1)π^(3) electron configuration.The spin-orbit excited states(^(3)Π_(1) and ^(3)Π_(0)),as well as two low-lying singlet excited states(^(1)Σ^(+)and ^(1)Π),are observed.Unusual spectroscopic characteristics are observed in the ^(3)Π_(2) ground state of AsB,probably due to state mixing with a higher-lying ^(1)Δ_(2) state.The current work provides extensive electronic and spectroscopic information for the PB and AsB molecules.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
Influences of swift heavy ion(SHI)irradiation induced defects on electronic properties of the bulk SnSe_(2)based FETs are explored.Latent tracks and amounts of Se vacancies in the irradiated SnSe_(2)were confirmed.Red...Influences of swift heavy ion(SHI)irradiation induced defects on electronic properties of the bulk SnSe_(2)based FETs are explored.Latent tracks and amounts of Se vacancies in the irradiated SnSe_(2)were confirmed.Red shift of the A1g peak indicates that the resonance frequency of the phonons is reduced due to the defect generation in SnSe_(2).The source–drain current Ids increased at ion fluence of 1×10^(10)ions·cm^(-2),which was attributeded to the irradiation caused Se vacancies,which hence increases the concentration of conduction electrons.The carrier mobility was about 16.9 cm^(2)·V^(-1)·s^(-1)for the devices irradiated at ion fluence of 1×10^(9)ions·cm^(-2),which benefited from heavy ion irradiation enhanced interlayer coupling.The mechanism of device performance optimization after irradiation is discussed in detail.This work provides evidence that,given the electronic properties of two-dimensional material-based device,vacancies and interlayer coupling effects caused by SHI irradiation should not be ignored.展开更多
03-type layered oxide serves as dominant components in sodium ion batteries;however,the unstable electronic structure between transition metal and oxygen inevitably induces framework instability and severe kinetic hin...03-type layered oxide serves as dominant components in sodium ion batteries;however,the unstable electronic structure between transition metal and oxygen inevitably induces framework instability and severe kinetic hindrance.In this study,a two-in-one approach to synergistically modulate the local electro nic and interfacial structure of NaNi_(1/3)Fe_(1/3)Mn_(1/3)O_(2)by Ce modification is proposed.We present an indepth study to reveal the strong-covalent Ce-O bonds,which make local charge around oxygen more negative,enhance O 2p-Mn 3d hybridization,and preserve the octahedral structural integrity.This modification tailors local electronic structure between the octahedral metal center and oxygen,thus enhancing reversibility of 03-P3-03 phase transition and expanding Na+octahedral-tetrahedral-octahedral transport channel.Additionally,the nanoscale perovskite layer induced by Ce element is in favor of minimizing interfacial side reaction as well as enhancing Na^(+)diffusivity.As a result,the designed 03-NaNi_(0.305)Fe_(0.33)Mn_(0.33)Ce_(0.025)O_(2)material delivers an exceptionally low volume variation,an ultrahigh rate capacity of 76.9 mA h g^(-1)at 10 C,and remarkable cycling life over 250 cycles with capacity retention of 80% at 5 C.展开更多
Lithium plating/stripping occurs at the a node/electrolyte interface which involves the flow of electrons from the current collector and the migration of lithium ions from the solid-electrolyte interphase(SEI).The dua...Lithium plating/stripping occurs at the a node/electrolyte interface which involves the flow of electrons from the current collector and the migration of lithium ions from the solid-electrolyte interphase(SEI).The dual continuous rapid transport of interfacial electron/ion is required for homogeneous Li deposition.Herein,we propose a strategy to improve the Li metal anode performance by rationally regulating the interfacial electron density and Li ion transport through the SEI film.This key technique involves decreasing the interfacial oxygen density of biomass-derived carbon host by regulating the arrangement of the celluloses precursor fibrils.The higher specific surface area and lower interfacial oxygen density decrease the local current density and ensure the formation of thin and even SEI film,which stabilized Li^(+)transfer through the Li/electrolyte interface.Moreover,the improved graphitization and the interconnected conducting network enhance the surface electronegativity of carbon and enable uninterruptible electron conduction.The result is continuous and rapid coupled interfacial electron/ion transport at the anode/electrolyte reaction interface,which facilitates uniform Li deposition and improves Li anode performance.The Li/C anode shows a high initial Coulombic efficiency of 98%and a long-term lifespan of over 150cycles at a practical low N/P(negative-to-positive)ratio of 1.44 in full cells.展开更多
基金supported by the National Natural Science Foundation of China(22278347)the Excellent Doctoral Student Research Innovation Project of Xinjiang University of China(XJU2022BS048)the Postgraduate Innovation Project of Xinjiang Uygur Autonomous Region of China(XJ2023G027).
文摘Low-cost Fe-based disordered rock salt(DRX)Li_(2)FeTiO_(4)is capable of providing high capacity(295 mA h g^(-1))by redox activity of cations(Fe^(2+)/Fe^(4+)and Ti^(3+)/Ti^(4+))and anionic oxygen.However,DRX structures lack transport channels for ions and electrons,resulting in sluggish kinetics,poor electrochemical activity,and cyclability.Herein,graphene conductive carbon network permeated Li_(2)FeTiO_(4)(LFT/C/G)nanofibers are successfully prepared by a facile sol-gel assisted electrospinning method.Ultrafine Li_(2)FeTiO_(4)nanoparticles(2 nm)and one-dimensional(1D)structure provide abu ndant active sites and unobstructed diffu sion channels,accelerating ion diffusion.In addition,introducing graphene reduces the band gap and Li^(+)diffusion barrier and improves the dynamic properties of Li_(2)FeTiO_(4),thus achieving a relatively mild interfacial reaction and reversible redox reaction.As expected,the LFT/C/1.0G cathode delivers a remarkable discharge capacity(238.5 mA h g^(-1)),high energy density(508.8 Wh kg^(-1)),and excellent rate capability(51.2 mA hg^(-1)at 1.0 A g^(-1)).Besides,the LFT/C/1.0G anode also displays a high capacity(514.5 mA h g^(-1)at 500 mA g^(-1))and a remarkable rate capability(243.9 mA h g^(-1)at 8 A g^(-1)).Moreover,the full batteries based on the LFT/C/1.0G symmetric electrode demonstrate a reversible capacity of 117.0 mA h g^(-1)after 100 cycles at 50 mA g^(-1).This study presents useful insights into developing cost-effective DRX cathodes with durable and fast lithium storage.
基金Project supported by the Research Project of National University of Defense Technology,China(Grant No.JC13-02-14)the National Natural Science Foundation of China(Grant No.11104349)
文摘Focused ion-beam-induced deposition （FIBID） and focused electron-beam-induced deposition （FEBID） are conve- nient and useful in nanodevice fabrication. Since the deposition is from the organometallic platinum precursor, the con- ductive lines directly written by focused ion-beam （FIB） and focused electron-beam （FEB） are carbon-rich materials. We discuss an alternative approach to enhancing the platinum content and improving the conductivity of the conductive leads produced by FIBID and FEBID, namely an annealing treatment. Annealing in pure oxygen at 500 ℃ for 30 min enhances the platinum content values from ~ 18% to 30% and ~ 50% to 90% of FIBID and FEBID, respectively. Moreover, we find that thin films will be formed in the FIBID and FEBID processes. The annealing treatment is helpful to avoid the current leakage caused by these thin films. A single electron transistor is fabricated by FEBID and the current-voltage curve shows the Coulomb blockade effect.
基金supported by National Natural Science Foundation of China(Grant Nos.52025055,52375576,52350349)Key Research and Development Program of Shaanxi(Program No.2022GXLH-01-12)+2 种基金Joint Fund of Ministry of Education for Equipment Pre-research(No.8091B03012304)Aeronautical Science Foundation of China(No.2022004607001)the Fundamental Research Funds for the Central Universities(No.xtr072024031).
文摘Continuous monitoring of biosignals is essential for advancing early disease detection,personalized treatment,and health management.Flexible electronics,capable of accurately monitoring biosignals in daily life,have garnered considerable attention due to their softness,conformability,and biocompatibility.However,several challenges remain,including imperfect skin-device interfaces,limited breathability,and insufficient mechanoelectrical stability.On-skin epidermal electronics,distinguished by their excellent conformability,breathability,and mechanoelectrical robustness,offer a promising solution for high-fidelity,long-term health monitoring.These devices can seamlessly integrate with the human body,leading to transformative advancements in future personalized healthcare.This review provides a systematic examination of recent advancements in on-skin epidermal electronics,with particular emphasis on critical aspects including material science,structural design,desired properties,and practical applications.We explore various materials,considering their properties and the corresponding structural designs developed to construct high-performance epidermal electronics.We then discuss different approaches for achieving the desired device properties necessary for long-term health monitoring,including adhesiveness,breathability,and mechanoelectrical stability.Additionally,we summarize the diverse applications of these devices in monitoring biophysical and physiological signals.Finally,we address the challenges facing these devices and outline future prospects,offering insights into the ongoing development of on-skin epidermal electronics for long-term health monitoring.
基金supported by the National Nature Science Foundation of China(Nos.52202335 and 52171227)Natural Science Foundation of Jiangsu Province(No.BK20221137)National Key R&D Program of China(2024YFE0108500).
文摘Wide-temperature applications of sodium-ion batteries(SIBs)are severely limited by the sluggish ion insertion/diffusion kinetics of conversion-type anodes.Quantum-sized transition metal dichalcogenides possess unique advantages of charge delocalization and enrich uncoordinated electrons and short-range transfer kinetics,which are crucial to achieve rapid low-temperature charge transfer and high-temperature interface stability.Herein,a quantum-scale FeS_(2) loaded on three-dimensional Ti_(3)C_(2) MXene skeletons(FeS_(2) QD/MXene)fabricated as SIBs anode,demonstrating impressive performance under wide-temperature conditions(−35 to 65).The theoretical calculations combined with experimental characterization interprets that the unsaturated coordination edges of FeS_(2) QD can induce delocalized electronic regions,which reduces electrostatic potential and significantly facilitates efficient Na+diffusion across a broad temperature range.Moreover,the Ti_(3)C_(2) skeleton reinforces structural integrity via Fe-O-Ti bonding,while enabling excellent dispersion of FeS_(2) QD.As expected,FeS_(2) QD/MXene anode harvests capacities of 255.2 and 424.9 mAh g^(−1) at 0.1 A g^(−1) under−35 and 65,and the energy density of FeS_(2) QD/MXene//NVP full cell can reach to 162.4 Wh kg^(−1) at−35,highlighting its practical potential for wide-temperatures conditions.This work extends the uncoordinated regions induced by quantum-size effects for exceptional Na^(+)ion storage and diffusion performance at wide-temperatures environment.
文摘Artificial intelligence(AI)is increasingly recognized as a transformative force in the field of solid organ transplantation.From enhancing donor-recipient matching to predicting clinical risks and tailoring immunosuppressive therapy,AI has the potential to improve both operational efficiency and patient outcomes.Despite these advancements,the perspectives of transplant professionals-those at the forefront of critical decision-making-remain insufficiently explored.To address this gap,this study utilizes a multi-round electronic Delphi approach to gather and analyses insights from global experts involved in organ transplantation.Participants are invited to complete structured surveys capturing demographic data,professional roles,institutional practices,and prior exposure to AI technologies.The survey also explores perceptions of AI’s potential benefits.Quantitative responses are analyzed using descriptive statistics,while open-ended qualitative responses undergo thematic analysis.Preliminary findings indicate a generally positive outlook on AI’s role in enhancing transplantation processes,particularly in areas such as donor matching and post-operative care.These mixed views reflect both optimism and caution among professionals tasked with integrating new technologies into high-stakes clinical workflows.By capturing a wide range of expert opinions,the findings will inform future policy development,regulatory considerations,and institutional readiness frameworks for the integration of AI into organ transplantation.
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 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 National Natural Science Foundation of China(62174164,U23A20568,and U22A2075)National Key Research and Development Project(2021YFA1202600)+2 种基金Talent Plan of Shanghai Branch,Chinese Academy of Sciences(CASSHB-QNPD-2023-022)Ningbo Technology Project(2022A-007-C)Ningbo Key Research and Development Project(2023Z021).
文摘The traditional von Neumann architecture faces inherent limitations due to the separation of memory and computa-tion,leading to high energy consumption,significant latency,and reduced operational efficiency.Neuromorphic computing,inspired by the architecture of the human brain,offers a promising alternative by integrating memory and computational func-tions,enabling parallel,high-speed,and energy-efficient information processing.Among various neuromorphic technologies,ion-modulated optoelectronic devices have garnered attention due to their excellent ionic tunability and the availability of multi-dimensional control strategies.This review provides a comprehensive overview of recent progress in ion-modulation optoelec-tronic neuromorphic devices.It elucidates the key mechanisms underlying ionic modulation of light fields,including ion migra-tion dynamics and capture and release of charge through ions.Furthermore,the synthesis of active materials and the proper-ties of these devices are analyzed in detail.The review also highlights the application of ion-modulation optoelectronic devices in artificial vision systems,neuromorphic computing,and other bionic fields.Finally,the existing challenges and future direc-tions for the development of optoelectronic neuromorphic devices are discussed,providing critical insights for advancing this promising field.
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 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 National Natural Science Foundation of China(Nos.22171180,22461142137,and 22478242)the Shanghai Municipal Science and Technology Major Project,China.
文摘Despite their attractive features of high energy density,low cost,and safety,polysulfide/iodide flow batteries(SIFBs)are hampered by the sluggish kinetics of the iodide redox couple,which restricts overall performance.Multicomponent sulfides are demonstrated as promising catalysts for accelerating I^(-)/I_(3)^(-) redox reactions.Concurrently,the enhanced configurational entropy arising from multinary compositions drives synergistic effects among constituent elements,establishing a viable pathway to optimize catalytic performance.Building on these foundations,this work introduces a targeted orbital hybridization-optimized electron density strategy to enhance the catalytic activity.Implementing this concept,we developed an in-situ solvothermal synthesis process for an entropy-enhanced AgCuZnSnS_(4) loaded graphite felt(ACZTS/GF)electrode.The engineered electrode demonstrates exceptional electrocatalytic performance with improved bulk conductivity and interfacial charge transfer kinetics within a SIFB.The cell achieves a high energy efficiency of 88.5%at 20 mA·cm^(−2) with 10%state-of-charge.Furthermore,the battery delivers a maximum power density of 119.8 mW·cm^(−2) and exhibits excellent long-term cycling stability.These significant results stem from orbital hybridization-driven electronic state optimization and entropy effect-induced synergistic catalysis.
基金supported by the National Science Foundation (Grant No.CHE-2403841)。
文摘We report a study on the electronic structure and chemical bonding of the PB and AsB diatomic molecules using high-resolution photoelectron imaging of cryogenically-cooled PB^(−)and AsB^(−)anions.The electron affinities of PB and AsB are measured to be 2.751(1)and 2.600(1)eV,respectively.The ground states of the PB^(−)and AsB−anions are determined to be ^(2)Σ^(+) with a σ^(1)π^(4) valence electron configuration.The ground states of neutral PB and AsB are found to be ^(3)Π_(2) with a σ^(1)π^(3) electron configuration.The spin-orbit excited states(^(3)Π_(1) and ^(3)Π_(0)),as well as two low-lying singlet excited states(^(1)Σ^(+)and ^(1)Π),are observed.Unusual spectroscopic characteristics are observed in the ^(3)Π_(2) ground state of AsB,probably due to state mixing with a higher-lying ^(1)Δ_(2) state.The current work provides extensive electronic and spectroscopic information for the PB and AsB molecules.
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Project supported by the National Natural Science Foundation of China(Grant Nos.12375261,12175287,12205350,and 62234013)the Youth Innovation Promotion Association of the Chinese Academy of Sciences(Grant No.2022424).
文摘Influences of swift heavy ion(SHI)irradiation induced defects on electronic properties of the bulk SnSe_(2)based FETs are explored.Latent tracks and amounts of Se vacancies in the irradiated SnSe_(2)were confirmed.Red shift of the A1g peak indicates that the resonance frequency of the phonons is reduced due to the defect generation in SnSe_(2).The source–drain current Ids increased at ion fluence of 1×10^(10)ions·cm^(-2),which was attributeded to the irradiation caused Se vacancies,which hence increases the concentration of conduction electrons.The carrier mobility was about 16.9 cm^(2)·V^(-1)·s^(-1)for the devices irradiated at ion fluence of 1×10^(9)ions·cm^(-2),which benefited from heavy ion irradiation enhanced interlayer coupling.The mechanism of device performance optimization after irradiation is discussed in detail.This work provides evidence that,given the electronic properties of two-dimensional material-based device,vacancies and interlayer coupling effects caused by SHI irradiation should not be ignored.
基金supported by the Science and technology plan project of Yulin(2023-CXY-193)the Project funded by Shaanxi Postdoctoral Science Foundation(2023BSHEDZZ274)+2 种基金the Shaanxi Province(2023-ZDLGY-24,2023-JC-QN-0588,Z20210201)the Science and technology plan project of Beilin(GX2319)the Science and technology plan project of Ankang(AK2023-GY-08)。
文摘03-type layered oxide serves as dominant components in sodium ion batteries;however,the unstable electronic structure between transition metal and oxygen inevitably induces framework instability and severe kinetic hindrance.In this study,a two-in-one approach to synergistically modulate the local electro nic and interfacial structure of NaNi_(1/3)Fe_(1/3)Mn_(1/3)O_(2)by Ce modification is proposed.We present an indepth study to reveal the strong-covalent Ce-O bonds,which make local charge around oxygen more negative,enhance O 2p-Mn 3d hybridization,and preserve the octahedral structural integrity.This modification tailors local electronic structure between the octahedral metal center and oxygen,thus enhancing reversibility of 03-P3-03 phase transition and expanding Na+octahedral-tetrahedral-octahedral transport channel.Additionally,the nanoscale perovskite layer induced by Ce element is in favor of minimizing interfacial side reaction as well as enhancing Na^(+)diffusivity.As a result,the designed 03-NaNi_(0.305)Fe_(0.33)Mn_(0.33)Ce_(0.025)O_(2)material delivers an exceptionally low volume variation,an ultrahigh rate capacity of 76.9 mA h g^(-1)at 10 C,and remarkable cycling life over 250 cycles with capacity retention of 80% at 5 C.
基金supported by the National Natural Science Foundation of China(21975091,22122902,and 52272208)the Fundamental Research Fund for the Central Universities of China(2662023LXPY001 and 2662021JC004).
文摘Lithium plating/stripping occurs at the a node/electrolyte interface which involves the flow of electrons from the current collector and the migration of lithium ions from the solid-electrolyte interphase(SEI).The dual continuous rapid transport of interfacial electron/ion is required for homogeneous Li deposition.Herein,we propose a strategy to improve the Li metal anode performance by rationally regulating the interfacial electron density and Li ion transport through the SEI film.This key technique involves decreasing the interfacial oxygen density of biomass-derived carbon host by regulating the arrangement of the celluloses precursor fibrils.The higher specific surface area and lower interfacial oxygen density decrease the local current density and ensure the formation of thin and even SEI film,which stabilized Li^(+)transfer through the Li/electrolyte interface.Moreover,the improved graphitization and the interconnected conducting network enhance the surface electronegativity of carbon and enable uninterruptible electron conduction.The result is continuous and rapid coupled interfacial electron/ion transport at the anode/electrolyte reaction interface,which facilitates uniform Li deposition and improves Li anode performance.The Li/C anode shows a high initial Coulombic efficiency of 98%and a long-term lifespan of over 150cycles at a practical low N/P(negative-to-positive)ratio of 1.44 in full cells.
