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
In order to maximize the advantages of high energy density in Li metal batteries,it is necessary to match cathode materials with high specific capacities.Ni-rich layered oxides have been shown to reversibly embed more...In order to maximize the advantages of high energy density in Li metal batteries,it is necessary to match cathode materials with high specific capacities.Ni-rich layered oxides have been shown to reversibly embed more Li+during charge and discharge processes due to the increased Ni content in their crystal structure,thereby providing higher energy density.However,a significant challenge associated with Ni-rich layered oxide cathodes is the crossover effect,which arises from the dissolution of Ni^(2+)from the cathode,leading to a rapid decline in battery capacity.Through the delocalization-induced effect of solvent molecules,Ni^(2+)is transformed into a fluorinated transition metal inorganic phase layer,thereby forming a corrosion-resistant Li metal interface.This prevents solvent molecules from being reduced and degraded by Li metal anode.The surface of the Li metal anode exhibits a smooth and flat deposition morphology after long-term cycling.Furthermore,the introduction of Ni^(2+)can enhance the concentration gradient of transition metal ions near the cathode,thereby suppressing the dissolution process of transition metal ions.Even the NCM955 cathode with a mass load of 22 mg cm^(−2)also has great capacity retention after cycling.The Ni^(2+)induced by high electronegative functional groups of solvent under the electron delocalization effect,preventing the Ni ions dissolution of cathode and constructing a corrosion-resistant Li metal interface layer.This work provides new insights into suppressing crossover effects in Li metal batteries with high nickel cathodes.展开更多
Transition metal-nitrogen-carbon materials(M-N-Cs),particularly Fe-N-Cs,have been found to be electroactive for accelerating oxygen reduction reaction(ORR)kinetics.Although substantial efforts have been devoted to des...Transition metal-nitrogen-carbon materials(M-N-Cs),particularly Fe-N-Cs,have been found to be electroactive for accelerating oxygen reduction reaction(ORR)kinetics.Although substantial efforts have been devoted to design Fe-N-Cs with increased active species content,surface area,and electronic conductivity,their performance is still far from satisfactory.Hitherto,there is limited research about regulation on the electronic spin states of Fe centers for Fe-N-Cs electrocatalysts to improve their catalytic performance.Here,we introduce Ti_(3)C_(2) MXene with sulfur terminals to regulate the electronic configuration of FeN_(4) species and dramatically enhance catalytic activity toward ORR.The MXene with sulfur terminals induce the spin-state transition of FeN_(4) species and Fe 3d electron delocalization with d band center upshift,enabling the Fe(II)ions to bind oxygen in the end-on adsorption mode favorable to initiate the reduction of oxygen and boosting oxygen-containing groups adsorption on FeN_(4) species and ORR kinetics.The resulting FeN_(4)-Ti_(3)C_(2)Sx exhibits comparable catalytic performance to those of commercial Pt-C.The developed wearable ZABs using FeN_(4)-Ti_(3)C_(2)Sx also exhibit fast kinetics and excellent stability.This study confirms that regulation of the electronic structure of active species via coupling with their support can be a major contributor to enhance their catalytic activity.展开更多
Rechargeable Mg-ion batteries(MIBs)have attracted much more attentions by virtue of the high capacity from the two electrons chemistry.However,the reversible Mg^(2+)diffusion in cathode materials is restricted by the ...Rechargeable Mg-ion batteries(MIBs)have attracted much more attentions by virtue of the high capacity from the two electrons chemistry.However,the reversible Mg^(2+)diffusion in cathode materials is restricted by the strong interactions between the high-polarized bivalent Mg^(2+)ions and anionic lattice.Herein,we design and propose a hetero-structural VO_(2)(R)-VS_(4)cathode,in which the re-delocalized d-electrons can effectively shield the polarity of Mg^(2+)ions.Theoretically,the electrons should spontaneously transfer from VS_(4)to VO_(2)(R)through the interfaces of hetero-structure due to the lower work function value of VS_(4).Furthermore,the internal electrons transfer lead to the electronic injection into VO_(2)(R)from VS_(4)and the partially broken V-V dimers,indicating the presence of lone pair electrons and charge re-delocalization.Benefiting from the shield effect of re-delocalized electrons,and the weakened attraction between cations and O/S anions enables more S^(2-)-S_(2)^(2-)redox groups to participate the electrochemical reactions and compensate the double charge of Mg^(2+)ions.Accordingly,VO_(2)(R)-VS_(4)hetero-structure exhibits a high specific capacity of 554 mA h g^(-1)at 50 mA g^(-1).It is believed that the charge re-delocalization of cathode extremely boost the Mg^(2+)ions migration for the high-capacity of MIBs.展开更多
Intraparticle charge delocalization occurs when metal nanoparticles are functionalized with organic capping ligands through conjugated rnetal-ligand interfacial bonds. In this study, metal nanoparticles of 5d metals ...Intraparticle charge delocalization occurs when metal nanoparticles are functionalized with organic capping ligands through conjugated rnetal-ligand interfacial bonds. In this study, metal nanoparticles of 5d metals （Ir, Pt, and Au） and 4d metals （Ru, Rh, and Pd） were prepared and capped with ethynylphenylacetylene and the impacts of the number of metal d electrons on the nanoparticle optoelectronic properties were examined. Both FTIR and photoluminescence measurements indicate that intraparticle charge delocalization was en- hanced with the increase of the number of d electrons in the same period with palladium being an exception.展开更多
The misfit layer compound(SnS)_(1.2)(TiS_(2))_(2)is a promising low-cost thermoelectric material because of its low thermal conductivity derived from the superlattice-like structure.However,the strong covalent bonds w...The misfit layer compound(SnS)_(1.2)(TiS_(2))_(2)is a promising low-cost thermoelectric material because of its low thermal conductivity derived from the superlattice-like structure.However,the strong covalent bonds within each constituent layer highly localize the electrons thereby it is highly challenging to optimize the power factor by doping or alloying.Here,we show that Bi doping at the Sn site markedly breaks the covalent bonds networks and highly delocalizes the electrons.This results in a high charge carrier concentration and enhanced power factor throughout the whole temperature range.It is highly remarkable that Bi doping also significantly reduces the thermal conductivity by suppressing the heat conduction carried by phonons,indicating that it independently modulates phonon and charge transport properties.These effects collectively give rise to a maximum ZT of 0.3 at 720 K.In addition,we apply the single Kane band model and the Debye–Callaway model to clarify the electron and phonon transport mechanisms in the misfit layer compound(SnS)_(1.2)(TiS_(2))_(2).展开更多
Investigating the activation of the persulfate process through heterogeneous carbonaceous catalysts to expedite the reduction of uranyl ions(U(Ⅵ))is imperative.The primary hurdle involves understanding the transfer a...Investigating the activation of the persulfate process through heterogeneous carbonaceous catalysts to expedite the reduction of uranyl ions(U(Ⅵ))is imperative.The primary hurdle involves understanding the transfer and distribution of photogenerated carriers during the reduction process in this intricate system and deciphering the role of activated groups in promoting reduction efficiency.In this study,we strategically regulate the structure of polymeric carbon nitride to promote the N-doped state,thereby facilitating delocalization electron enrichment.The resulting active sites effectively activate peroxyl disulfate(PDS),generating radicals that expedite the selective reduction of U(VI).This strategic approach mitigates the inherent disadvantage of the short half-life of free radicals in persulfate-based advanced oxidation processes.As a consequence of our endeavors and with the simultaneous presence of PDS and hydrogen peroxide,we achieve an exceptional photoreduction efficiency of 100%within a remarkably short period of 20 min.This breakthrough presents a high-efficiency application with significant potential for addressing the pollution associated with uranylcontaining wastewater.Our findings not only contribute to the fundamental understanding of AOPs but also offer a practical solution with implications for environmental remediation.展开更多
Stretchable electronics have been recognized as intriguing next-generation electronics that possess huge market value,and stretchable electronic conductors(SECs)are essential for stretchable electronics,which not only...Stretchable electronics have been recognized as intriguing next-generation electronics that possess huge market value,and stretchable electronic conductors(SECs)are essential for stretchable electronics,which not only can serve as critical functional components but also are the indispensable electronic connections bridging various electronic components within stretchable electronic systems.Herein,we offer a comprehensive review of recent progress in SECs including the material categories,structure designs,fabrication techniques,and applications.The characteristics,performance enhancement strategies,and application requirements are emphasized.Based on the recent advances,the existing challenges and future prospects are outlined and discussed.展开更多
Permeable electronics promise improved physiological comfort,but remain constrained by limited functional integration and poor mechanical robustness.Here,we report a three-dimensional(3D)permeable electronic system th...Permeable electronics promise improved physiological comfort,but remain constrained by limited functional integration and poor mechanical robustness.Here,we report a three-dimensional(3D)permeable electronic system that overcomes these challenges by combining electrospun SEBS nanofiber mats,high-resolution liquid metal conductors patterned via thermal imprinting(50μm),and a strain isolators(SIL)that protects vertical interconnects(VIAs)from stress concentration.This architecture achieves ultrahigh air permeability(>5.09 m L cm^(-2)min^(-1)),exceptional stretchability(750%fracture strain),and reliable conductivity maintained through more than 32,500 strain cycles.Leveraging these advances,we have integrated multilayer circuits,strain sensors,and a three-axis accelerometer to achieve a fully integrated,stretchable,permeable wireless real-time gesture recognition glove.The system enables accurate sign language interpretation(98%)and seamless robotic hand control,demonstrating its potential for assistive technologies.By uniting comfort,durability,and high-density integration,this work establishes a versatile platform for nextgeneration wearable electronics and interactive human-robot interfaces.展开更多
The effects of initial spin orientation on the final electron beam polarization in laser wakefield acceleration in a pre-polarized plasma are investigated theoretically and numerically.From the results of variation of...The effects of initial spin orientation on the final electron beam polarization in laser wakefield acceleration in a pre-polarized plasma are investigated theoretically and numerically.From the results of variation of the initial spin direction,the spin dynamics of the electron beam are found to depend on the self-injection mechanism.The effects of wakefields and laser fields are studied using test particle dynamics and particle-in-cell simulations based on the Thomas-Bargmann-Michel-Telegdi equation.Compared with transverse injection,longitudinal injection is found to be preferable for obtaining a highly polarized electron beam.展开更多
The rapid advancement of machine learning based tight-binding Hamiltonian(MLTB)methods has opened new avenues for efficient and accurate electronic structure simulations,particularly in large-scale systems and long-ti...The rapid advancement of machine learning based tight-binding Hamiltonian(MLTB)methods has opened new avenues for efficient and accurate electronic structure simulations,particularly in large-scale systems and long-time scenarios.This review begins with a concise overview of traditional tight-binding(TB)models,including both(semi-)empirical and first-principles approaches,establishing the foundation for understanding MLTB developments.We then present a systematic classification of existing MLTB methodologies,grouped into two major categories:direct prediction of TB Hamiltonian elements and inference of empirical parameters.A comparative analysis with other ML-based electronic structure models is also provided,highlighting the advancement of MLTB approaches.Finally,we explore the emerging MLTB application ecosystem,highlighting how the integration of MLTB models with a diverse suite of post-processing tools from linear-scaling solvers to quantum transport frameworks and molecular dynamics interfaces is essential for tackling complex scientific problems across different domains.The continued advancement of this integrated paradigm promises to accelerate materials discovery and open new frontiers in the predictive simulation of complex quantum phenomena.展开更多
Traditional digitizers for signal readout of PET detectors are based on commercial analog-to-digital converters(ADC).However,the cost and power consumption of an entire electronic readout system based on digitizers fo...Traditional digitizers for signal readout of PET detectors are based on commercial analog-to-digital converters(ADC).However,the cost and power consumption of an entire electronic readout system based on digitizers for a PET scanner are high.To address this problem,a soft-core ADC based on a field-programmable gate array(FPGA)was proposed.An FPGA-based ADC(FPGA-ADC)combines low loss and high performance.To achieve good performance,the FPGA-ADC requires three calibrations:time-to-digital converter(TDC)length calibration,TDC alignment calibration,and TDC-to-ADC calibration.A prototype front-end electronics based on FPGA-ADC was built to evaluate the performance of time-of-flight positron emission tomography(TOF PET)detectors.Each PET detector consists of a LYSO crystal single-ended coupled to a silicon photomultiplier(SiPM).The experimental results show that the full-width at half-maximum(FWHM)energy resolution for 511 keV gamma photons after saturation correction of the SiPM was 12.3%.The FWHM coincidence timing resolution(CTR)of the TOF PET detector with the readout of the front-end electronic prototype is 385.2 ps.FPGA-ADCbased front-end electronics are very promising for multichannel,low-cost,highly integrated,and power-efficient readout electronic systems for radiation detector applications.展开更多
A rapidly growing field is piezoresistive sensor for accurate respiration rate monitoring to suppress the worldwide respiratory illness.However,a large neglected issue is the sensing durability and accuracy without in...A rapidly growing field is piezoresistive sensor for accurate respiration rate monitoring to suppress the worldwide respiratory illness.However,a large neglected issue is the sensing durability and accuracy without interference since the expiratory pressure always coupled with external humidity and temperature variations,as well as mechanical motion artifacts.Herein,a robust and biodegradable piezoresistive sensor is reported that consists of heterogeneous MXene/cellulose-gelation sensing layer and Ag-based interdigital electrode,featuring customizable cylindrical interface arrangement and compact hierarchical laminated architecture for collectively regulating the piezoresistive response and mechanical robustness,thereby realizing the long-term breath-induced pressure detection.Notably,molecular dynamics simulations reveal the frequent angle inversion and reorientation of MXene/cellulose in vacuum filtration,driven by shear forces and interfacial interactions,which facilitate the establishment of hydrogen bonds and optimize the architecture design in sensing layer.The resultant sensor delivers unprecedented collection features of superior stability for off-axis deformation(0-120°,~2.8×10^(-3) A)and sensing accuracy without crosstalk(humidity 50%-100%and temperature 30-80).Besides,the sensor-embedded mask together with machine learning models is achieved to train and classify the respiration status for volunteers with different ages(average prediction accuracy~90%).It is envisioned that the customizable architecture design and sensor paradigm will shed light on the advanced stability of sustainable electronics and pave the way for the commercial application in respiratory monitory.展开更多
Electron beam injectors are pivotal components of large-scale scientific instruments,such as synchrotron radiation sources,free-electron lasers,and electron-positron colliders.The quality of the electron beam produced...Electron beam injectors are pivotal components of large-scale scientific instruments,such as synchrotron radiation sources,free-electron lasers,and electron-positron colliders.The quality of the electron beam produced by the injector critically influences the performance of the entire accelerator-based scientific research apparatus.The injectors of such facilities usually use photocathode and thermionic-cathode electron guns.Although the photocathode injector can produce electron beams of excellent quality,its associated laser system is massive and intricate.The thermionic-cathode electron gun,especially the gridded electron gun injector,has a simple structure capable of generating numerous electron beams.However,its emittance is typically high.In this study,methods to reduce beam emittance are explored through a comprehensive analysis of various grid structures and preliminary design results,examining the evolution of beam phase space at different grid positions.An optimization method for reducing the emittance of a gridded thermionic-cathode electron gun is proposed through theoretical derivation,electromagnetic-field simulation,and beam-dynamics simulation.A 50%reduction in emittance was achieved for a 50 keV,1.7 A electron gun,laying the foundation for the subsequent design of a high-current,low-emittance injector.展开更多
Achieving high-energy density remains a key objective for advanced energy storage systems.However,challenges,such as poor cathode conductivity,anode dendrite formation,polysulfide shuttling,and electrolyte degradation...Achieving high-energy density remains a key objective for advanced energy storage systems.However,challenges,such as poor cathode conductivity,anode dendrite formation,polysulfide shuttling,and electrolyte degradation,continue to limit performance and stability.Molecular and ionic dipole interactions have emerged as an effective strategy to address these issues by regulating ionic transport,modulating solvation structures,optimizing interfacial chemistry,and enhancing charge transfer kinetics.These interactions also stabilize electrode interfaces,suppress side reactions,and mitigate anode corrosion,collectively improving the durability of high-energy batteries.A deeper understanding of these mechanisms is essential to guide the design of next-generation battery materials.Herein,this review summarizes the development,classification,and advantages of dipole interactions in high-energy batteries.The roles of dipoles,including facilitating ion transport,controlling solvation dynamics,stabilizing the electric double layer,optimizing solid electrolyte interphase and cathode–electrolyte interface layers,and inhibiting parasitic reactions—are comprehensively discussed.Finally,perspectives on future research directions are proposed to advance dipole-enabled strategies for high-performance energy storage.This review aims to provide insights into the rational design of dipole-interactive systems and promote the progress of electrochemical energy storage technologies.展开更多
In this study,the dosimetric characteristics(thickness applicability,preheating time,temperature and humidity dependence,in-batch uniformity,readout reproducibility,dose linearity,self-decay,and electron energy respon...In this study,the dosimetric characteristics(thickness applicability,preheating time,temperature and humidity dependence,in-batch uniformity,readout reproducibility,dose linearity,self-decay,and electron energy response)of engineered polycarbonate films irradiated with an electron beam(0–600 kGy)were investigated using photoluminescence spectroscopy.The results show a linear relationship between photoluminescence intensity and radiation dose when the thickness of the polycarbonate film is 0.3 mm.A higher fluorescence intensity can be obtained by preheating at 60℃ for 180 min before photoluminescence spectrum analysis.As the temperature during spectral testing and the ambient humidity(during and after irradiation)increased,the photoluminescence intensity of the polycarbonate films decreased.The photoluminescence intensity deviation of the polycarbonate films produced within the same batch at 100 kGy is 2.73%.After ten times of repeated excitations and readouts,the coefficients of variation in photoluminescence intensity are less than 8.6%,and the linear correlation coefficient between photoluminescence intensity and irradiation dose is 0.965 in the dose capture range of 20–600 kGy.Within 60 days of irradiation,the photoluminescence intensity of the polycarbonate film decreased to 60%of the initial value.The response of the 0.3 mm polycarbonate films to electron beams with energies exceeding 3.5 MeV does not differ significantly.This comprehensive analysis indicates the potential of polycarbonate films as a high-radiation dose detection material.展开更多
We report a theoretical investigation into superconductivity within the MAXH_(6) quaternary hydride system using first-principles calculations,where M and A denote alkali and alkaline earth elements,respectively,and X...We report a theoretical investigation into superconductivity within the MAXH_(6) quaternary hydride system using first-principles calculations,where M and A denote alkali and alkaline earth elements,respectively,and X represents transition metal elements.Systematic analysis of electronic band structures,phonon dispersions,and electron-phonon coupling reveals that substitution of MA binary metal combinations and X metal atoms can create favorable conditions for superconductivity.Mapping of superconducting critical temperatures,combined with dynamical stability analysis through phonon calculations,identifies ten superconducting candidates at ambient pressure.Among these,LiNaAgH_(6) exhibits nearly-free-electron behavior reminiscent of monovalent electron superconductors.It demonstrates exceptional superconducting properties with electron–phonon coupling λ=2.707,which yields a superconducting transition temperature T_(c) of 206.4 K using the Allen–Dynes formula.Its structural analogs MgNaPdH_(6),LiMgPdH_(6),LiMgAgH_(6),LiMgAuH_(6) all exhibit superconducting transition temperatures above 110 K.These findings advance our fundamental understanding of superconductivity in quaternary hydrides and provide guidance for rational design of new high-temperature superconducting materials.展开更多
Robotic electronic skin(e-skin)is inspired by human skin and endows robots with tactile perception,temperature detection,and environmental interaction capabilities.However,its development is hampered by prolonged desi...Robotic electronic skin(e-skin)is inspired by human skin and endows robots with tactile perception,temperature detection,and environmental interaction capabilities.However,its development is hampered by prolonged design cycles,limited signal enhancement,and weak cognitive abilities.Given that the convergence of artificial intelligence(AI)with e-skin is fundamentally transforming this landscape,the present review highlights the pivotal contributions of AI across the entire development spectrum of robotic e-skin,including design optimization,signal processing,and cognitive enhancement.AI-driven design paradigms dramatically shorten development time and enable the discovery of optimal sensor materials and structures.In signal processing,AI algorithms notably improve the ability to decouple complex sensory data,enabling robust,multimodal,super-resolution sensing.AI endows e-skin with advanced cognitive capabilities,allowing it to interpret intricate tactile information and intelligently respond to external environments.By underscoring the potential of AI throughout the entire development pipeline,this review aims to drive the creation of e-skin with minimal hardware and maximal cognition and thus achieve revolutionary breakthroughs in cutting-edge fields such as human-robot interactions,precise robot control,and soft robotics for environmental exploration.展开更多
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.
基金the support from Yunnan Fundamental Research Projects(202301BE070001-029,202401CF070129,202501CF070181)National Natural Science Foundation of China(22209012,22479067)Kunming University of Science and Technology Analysis and Testing Fund Support Project(2023T20220172)。
文摘In order to maximize the advantages of high energy density in Li metal batteries,it is necessary to match cathode materials with high specific capacities.Ni-rich layered oxides have been shown to reversibly embed more Li+during charge and discharge processes due to the increased Ni content in their crystal structure,thereby providing higher energy density.However,a significant challenge associated with Ni-rich layered oxide cathodes is the crossover effect,which arises from the dissolution of Ni^(2+)from the cathode,leading to a rapid decline in battery capacity.Through the delocalization-induced effect of solvent molecules,Ni^(2+)is transformed into a fluorinated transition metal inorganic phase layer,thereby forming a corrosion-resistant Li metal interface.This prevents solvent molecules from being reduced and degraded by Li metal anode.The surface of the Li metal anode exhibits a smooth and flat deposition morphology after long-term cycling.Furthermore,the introduction of Ni^(2+)can enhance the concentration gradient of transition metal ions near the cathode,thereby suppressing the dissolution process of transition metal ions.Even the NCM955 cathode with a mass load of 22 mg cm^(−2)also has great capacity retention after cycling.The Ni^(2+)induced by high electronegative functional groups of solvent under the electron delocalization effect,preventing the Ni ions dissolution of cathode and constructing a corrosion-resistant Li metal interface layer.This work provides new insights into suppressing crossover effects in Li metal batteries with high nickel cathodes.
基金supported by a Grant of the Innovation and Technology Commission of Hong Kong(Project number:ITS/461/18)City University of Hong Kong(Project number:9678179).
文摘Transition metal-nitrogen-carbon materials(M-N-Cs),particularly Fe-N-Cs,have been found to be electroactive for accelerating oxygen reduction reaction(ORR)kinetics.Although substantial efforts have been devoted to design Fe-N-Cs with increased active species content,surface area,and electronic conductivity,their performance is still far from satisfactory.Hitherto,there is limited research about regulation on the electronic spin states of Fe centers for Fe-N-Cs electrocatalysts to improve their catalytic performance.Here,we introduce Ti_(3)C_(2) MXene with sulfur terminals to regulate the electronic configuration of FeN_(4) species and dramatically enhance catalytic activity toward ORR.The MXene with sulfur terminals induce the spin-state transition of FeN_(4) species and Fe 3d electron delocalization with d band center upshift,enabling the Fe(II)ions to bind oxygen in the end-on adsorption mode favorable to initiate the reduction of oxygen and boosting oxygen-containing groups adsorption on FeN_(4) species and ORR kinetics.The resulting FeN_(4)-Ti_(3)C_(2)Sx exhibits comparable catalytic performance to those of commercial Pt-C.The developed wearable ZABs using FeN_(4)-Ti_(3)C_(2)Sx also exhibit fast kinetics and excellent stability.This study confirms that regulation of the electronic structure of active species via coupling with their support can be a major contributor to enhance their catalytic activity.
基金the financial support of this work by the National Natural Science Foundation of China(No.52034011)the Key R&D Program of Shanxi(No.2019ZDLGY04-05)+2 种基金the National Natural Science Foundation of Shaanxi(No.2019JLZ-01)the Fundamental Research Funds for the Central Universities(No.G2020KY05129)the Research Fund of the State Key Laboratory of Solidification Processing(NPU),China(No.2020-BJ-03)。
文摘Rechargeable Mg-ion batteries(MIBs)have attracted much more attentions by virtue of the high capacity from the two electrons chemistry.However,the reversible Mg^(2+)diffusion in cathode materials is restricted by the strong interactions between the high-polarized bivalent Mg^(2+)ions and anionic lattice.Herein,we design and propose a hetero-structural VO_(2)(R)-VS_(4)cathode,in which the re-delocalized d-electrons can effectively shield the polarity of Mg^(2+)ions.Theoretically,the electrons should spontaneously transfer from VS_(4)to VO_(2)(R)through the interfaces of hetero-structure due to the lower work function value of VS_(4).Furthermore,the internal electrons transfer lead to the electronic injection into VO_(2)(R)from VS_(4)and the partially broken V-V dimers,indicating the presence of lone pair electrons and charge re-delocalization.Benefiting from the shield effect of re-delocalized electrons,and the weakened attraction between cations and O/S anions enables more S^(2-)-S_(2)^(2-)redox groups to participate the electrochemical reactions and compensate the double charge of Mg^(2+)ions.Accordingly,VO_(2)(R)-VS_(4)hetero-structure exhibits a high specific capacity of 554 mA h g^(-1)at 50 mA g^(-1).It is believed that the charge re-delocalization of cathode extremely boost the Mg^(2+)ions migration for the high-capacity of MIBs.
基金supported,in part,by the National Science Foundation(DMR-1409396 and CHE-1710408)carried out at the National Center for Electron Microscopy and Molecular Foundry of Lawrence Berkeley National Laboratory,which is supported by the US Department of Energy
文摘Intraparticle charge delocalization occurs when metal nanoparticles are functionalized with organic capping ligands through conjugated rnetal-ligand interfacial bonds. In this study, metal nanoparticles of 5d metals （Ir, Pt, and Au） and 4d metals （Ru, Rh, and Pd） were prepared and capped with ethynylphenylacetylene and the impacts of the number of metal d electrons on the nanoparticle optoelectronic properties were examined. Both FTIR and photoluminescence measurements indicate that intraparticle charge delocalization was en- hanced with the increase of the number of d electrons in the same period with palladium being an exception.
基金financially supported by the National Key Research and Development Program of China(Grant No.2018YFA0702100)the Joint Funds of the National Natural Science Foundation of China+1 种基金the Chinese Academy of Sciences’Large-Scale Scientific Facility(Grant No.U1932106)the Sichuan University Innovation Research Program of China(Grant No.2020SCUNL112)。
文摘The misfit layer compound(SnS)_(1.2)(TiS_(2))_(2)is a promising low-cost thermoelectric material because of its low thermal conductivity derived from the superlattice-like structure.However,the strong covalent bonds within each constituent layer highly localize the electrons thereby it is highly challenging to optimize the power factor by doping or alloying.Here,we show that Bi doping at the Sn site markedly breaks the covalent bonds networks and highly delocalizes the electrons.This results in a high charge carrier concentration and enhanced power factor throughout the whole temperature range.It is highly remarkable that Bi doping also significantly reduces the thermal conductivity by suppressing the heat conduction carried by phonons,indicating that it independently modulates phonon and charge transport properties.These effects collectively give rise to a maximum ZT of 0.3 at 720 K.In addition,we apply the single Kane band model and the Debye–Callaway model to clarify the electron and phonon transport mechanisms in the misfit layer compound(SnS)_(1.2)(TiS_(2))_(2).
基金National Natural Science Foundation of China,Grant/Award Numbers:22162009,32360236。
文摘Investigating the activation of the persulfate process through heterogeneous carbonaceous catalysts to expedite the reduction of uranyl ions(U(Ⅵ))is imperative.The primary hurdle involves understanding the transfer and distribution of photogenerated carriers during the reduction process in this intricate system and deciphering the role of activated groups in promoting reduction efficiency.In this study,we strategically regulate the structure of polymeric carbon nitride to promote the N-doped state,thereby facilitating delocalization electron enrichment.The resulting active sites effectively activate peroxyl disulfate(PDS),generating radicals that expedite the selective reduction of U(VI).This strategic approach mitigates the inherent disadvantage of the short half-life of free radicals in persulfate-based advanced oxidation processes.As a consequence of our endeavors and with the simultaneous presence of PDS and hydrogen peroxide,we achieve an exceptional photoreduction efficiency of 100%within a remarkably short period of 20 min.This breakthrough presents a high-efficiency application with significant potential for addressing the pollution associated with uranylcontaining wastewater.Our findings not only contribute to the fundamental understanding of AOPs but also offer a practical solution with implications for environmental remediation.
基金supported by the National Natural Science Foundation of China(52172170)Guangdong Natural Science Foundation for Distinguished Young Scholars(2023B1515020114)+2 种基金Fundamental Research Funds for the Central Universities(24lgqb003)Guangdong University Innovation and Enhancement Program(2024KTSCX003)Science and Technology Projects of Guangzhou(2025A04J4230).
文摘Stretchable electronics have been recognized as intriguing next-generation electronics that possess huge market value,and stretchable electronic conductors(SECs)are essential for stretchable electronics,which not only can serve as critical functional components but also are the indispensable electronic connections bridging various electronic components within stretchable electronic systems.Herein,we offer a comprehensive review of recent progress in SECs including the material categories,structure designs,fabrication techniques,and applications.The characteristics,performance enhancement strategies,and application requirements are emphasized.Based on the recent advances,the existing challenges and future prospects are outlined and discussed.
基金supported in part by the National Key R&D Program of China under Grant 2024YFB4405300 and 2022YFA1204300the Natural Science Foundation of Hunan Province under Grant 2023JJ20016+2 种基金the National Natural Science Foundation of China under Grants of 52221001 and 62090035the Key Research and Development Plan of Hunan Province under grants of 2022GK3002 and 2023GK2012the Key Program of Science and Technology Department of Hunan Province under grant of 2020XK2001。
文摘Permeable electronics promise improved physiological comfort,but remain constrained by limited functional integration and poor mechanical robustness.Here,we report a three-dimensional(3D)permeable electronic system that overcomes these challenges by combining electrospun SEBS nanofiber mats,high-resolution liquid metal conductors patterned via thermal imprinting(50μm),and a strain isolators(SIL)that protects vertical interconnects(VIAs)from stress concentration.This architecture achieves ultrahigh air permeability(>5.09 m L cm^(-2)min^(-1)),exceptional stretchability(750%fracture strain),and reliable conductivity maintained through more than 32,500 strain cycles.Leveraging these advances,we have integrated multilayer circuits,strain sensors,and a three-axis accelerometer to achieve a fully integrated,stretchable,permeable wireless real-time gesture recognition glove.The system enables accurate sign language interpretation(98%)and seamless robotic hand control,demonstrating its potential for assistive technologies.By uniting comfort,durability,and high-density integration,this work establishes a versatile platform for nextgeneration wearable electronics and interactive human-robot interfaces.
基金supported by the National Natural Science Foundation of China(Grant Nos.11804348,11775056,11975154,12225505,and 12405281)the Science Challenge(Project No.TZ2018005)+2 种基金supported by the Shanghai Pujiang Program(Grant No.23PJ1414600)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant No.XDB0890203)supported by the Accelerator Technology Helmholtz Infrastructure consortium ATHENA.
文摘The effects of initial spin orientation on the final electron beam polarization in laser wakefield acceleration in a pre-polarized plasma are investigated theoretically and numerically.From the results of variation of the initial spin direction,the spin dynamics of the electron beam are found to depend on the self-injection mechanism.The effects of wakefields and laser fields are studied using test particle dynamics and particle-in-cell simulations based on the Thomas-Bargmann-Michel-Telegdi equation.Compared with transverse injection,longitudinal injection is found to be preferable for obtaining a highly polarized electron beam.
基金supported by the Advanced Materials-National Science and Technology Major Project(Grant No.2025ZD0618401)the National Natural Science Foundation of China(Grant No.12504285)+1 种基金the Natural Science Foundation of Jiangsu Province(Grant No.BK20250472)NFSG grant from BITS-Pilani,Dubai campus。
文摘The rapid advancement of machine learning based tight-binding Hamiltonian(MLTB)methods has opened new avenues for efficient and accurate electronic structure simulations,particularly in large-scale systems and long-time scenarios.This review begins with a concise overview of traditional tight-binding(TB)models,including both(semi-)empirical and first-principles approaches,establishing the foundation for understanding MLTB developments.We then present a systematic classification of existing MLTB methodologies,grouped into two major categories:direct prediction of TB Hamiltonian elements and inference of empirical parameters.A comparative analysis with other ML-based electronic structure models is also provided,highlighting the advancement of MLTB approaches.Finally,we explore the emerging MLTB application ecosystem,highlighting how the integration of MLTB models with a diverse suite of post-processing tools from linear-scaling solvers to quantum transport frameworks and molecular dynamics interfaces is essential for tackling complex scientific problems across different domains.The continued advancement of this integrated paradigm promises to accelerate materials discovery and open new frontiers in the predictive simulation of complex quantum phenomena.
基金supported by the Key R&D Program of Shandong Province(No.2023SFGC0101)Shandong Excellent Young Scientists Fund Program(Overseas)(No.2023HWYQ-047)+1 种基金the Natural Science Foundation of Shandong Province(No.ZR2022QA039)the National Natural Science Foundation of China(NSFC)(No.U2106202).
文摘Traditional digitizers for signal readout of PET detectors are based on commercial analog-to-digital converters(ADC).However,the cost and power consumption of an entire electronic readout system based on digitizers for a PET scanner are high.To address this problem,a soft-core ADC based on a field-programmable gate array(FPGA)was proposed.An FPGA-based ADC(FPGA-ADC)combines low loss and high performance.To achieve good performance,the FPGA-ADC requires three calibrations:time-to-digital converter(TDC)length calibration,TDC alignment calibration,and TDC-to-ADC calibration.A prototype front-end electronics based on FPGA-ADC was built to evaluate the performance of time-of-flight positron emission tomography(TOF PET)detectors.Each PET detector consists of a LYSO crystal single-ended coupled to a silicon photomultiplier(SiPM).The experimental results show that the full-width at half-maximum(FWHM)energy resolution for 511 keV gamma photons after saturation correction of the SiPM was 12.3%.The FWHM coincidence timing resolution(CTR)of the TOF PET detector with the readout of the front-end electronic prototype is 385.2 ps.FPGA-ADCbased front-end electronics are very promising for multichannel,low-cost,highly integrated,and power-efficient readout electronic systems for radiation detector applications.
基金supported by the National Natural Science Foundation of China(22074072,22274083,52376199)the Shandong Provincial Natural Science Foundation(ZR2023LZY005)+1 种基金the Exploration Project of the State Key Laboratory of BioFibers and EcoTextiles of Qingdao University(TSKT202101)the Fundamental Research Funds for the Central Universities(2022BLRD13,2023BLRD01).
文摘A rapidly growing field is piezoresistive sensor for accurate respiration rate monitoring to suppress the worldwide respiratory illness.However,a large neglected issue is the sensing durability and accuracy without interference since the expiratory pressure always coupled with external humidity and temperature variations,as well as mechanical motion artifacts.Herein,a robust and biodegradable piezoresistive sensor is reported that consists of heterogeneous MXene/cellulose-gelation sensing layer and Ag-based interdigital electrode,featuring customizable cylindrical interface arrangement and compact hierarchical laminated architecture for collectively regulating the piezoresistive response and mechanical robustness,thereby realizing the long-term breath-induced pressure detection.Notably,molecular dynamics simulations reveal the frequent angle inversion and reorientation of MXene/cellulose in vacuum filtration,driven by shear forces and interfacial interactions,which facilitate the establishment of hydrogen bonds and optimize the architecture design in sensing layer.The resultant sensor delivers unprecedented collection features of superior stability for off-axis deformation(0-120°,~2.8×10^(-3) A)and sensing accuracy without crosstalk(humidity 50%-100%and temperature 30-80).Besides,the sensor-embedded mask together with machine learning models is achieved to train and classify the respiration status for volunteers with different ages(average prediction accuracy~90%).It is envisioned that the customizable architecture design and sensor paradigm will shed light on the advanced stability of sustainable electronics and pave the way for the commercial application in respiratory monitory.
基金supported by the Hundred-person Program of Chinese Academy of Sciences and the National Natural Science Foundation of China(No.11905074).
文摘Electron beam injectors are pivotal components of large-scale scientific instruments,such as synchrotron radiation sources,free-electron lasers,and electron-positron colliders.The quality of the electron beam produced by the injector critically influences the performance of the entire accelerator-based scientific research apparatus.The injectors of such facilities usually use photocathode and thermionic-cathode electron guns.Although the photocathode injector can produce electron beams of excellent quality,its associated laser system is massive and intricate.The thermionic-cathode electron gun,especially the gridded electron gun injector,has a simple structure capable of generating numerous electron beams.However,its emittance is typically high.In this study,methods to reduce beam emittance are explored through a comprehensive analysis of various grid structures and preliminary design results,examining the evolution of beam phase space at different grid positions.An optimization method for reducing the emittance of a gridded thermionic-cathode electron gun is proposed through theoretical derivation,electromagnetic-field simulation,and beam-dynamics simulation.A 50%reduction in emittance was achieved for a 50 keV,1.7 A electron gun,laying the foundation for the subsequent design of a high-current,low-emittance injector.
基金supported by the introduction of Talent Research Fund in Nanjing Institute of Technology(YKJ202204)the National Natural Science Foundation of China(52401282 and 52300206)the Natural Science Foundation of Jiangsu Province(BK20230701 and BK20230705).
文摘Achieving high-energy density remains a key objective for advanced energy storage systems.However,challenges,such as poor cathode conductivity,anode dendrite formation,polysulfide shuttling,and electrolyte degradation,continue to limit performance and stability.Molecular and ionic dipole interactions have emerged as an effective strategy to address these issues by regulating ionic transport,modulating solvation structures,optimizing interfacial chemistry,and enhancing charge transfer kinetics.These interactions also stabilize electrode interfaces,suppress side reactions,and mitigate anode corrosion,collectively improving the durability of high-energy batteries.A deeper understanding of these mechanisms is essential to guide the design of next-generation battery materials.Herein,this review summarizes the development,classification,and advantages of dipole interactions in high-energy batteries.The roles of dipoles,including facilitating ion transport,controlling solvation dynamics,stabilizing the electric double layer,optimizing solid electrolyte interphase and cathode–electrolyte interface layers,and inhibiting parasitic reactions—are comprehensively discussed.Finally,perspectives on future research directions are proposed to advance dipole-enabled strategies for high-performance energy storage.This review aims to provide insights into the rational design of dipole-interactive systems and promote the progress of electrochemical energy storage technologies.
基金supported by the National Natural Science Foundation of China(No.12305385)Key Projects of Scientific Research of the Hunan Provincial Department of Education(22A0310)the Research Startup Project of University of South China(220XQD025).
文摘In this study,the dosimetric characteristics(thickness applicability,preheating time,temperature and humidity dependence,in-batch uniformity,readout reproducibility,dose linearity,self-decay,and electron energy response)of engineered polycarbonate films irradiated with an electron beam(0–600 kGy)were investigated using photoluminescence spectroscopy.The results show a linear relationship between photoluminescence intensity and radiation dose when the thickness of the polycarbonate film is 0.3 mm.A higher fluorescence intensity can be obtained by preheating at 60℃ for 180 min before photoluminescence spectrum analysis.As the temperature during spectral testing and the ambient humidity(during and after irradiation)increased,the photoluminescence intensity of the polycarbonate films decreased.The photoluminescence intensity deviation of the polycarbonate films produced within the same batch at 100 kGy is 2.73%.After ten times of repeated excitations and readouts,the coefficients of variation in photoluminescence intensity are less than 8.6%,and the linear correlation coefficient between photoluminescence intensity and irradiation dose is 0.965 in the dose capture range of 20–600 kGy.Within 60 days of irradiation,the photoluminescence intensity of the polycarbonate film decreased to 60%of the initial value.The response of the 0.3 mm polycarbonate films to electron beams with energies exceeding 3.5 MeV does not differ significantly.This comprehensive analysis indicates the potential of polycarbonate films as a high-radiation dose detection material.
基金supported by the National Key R&D Program of China (Grant No.2022YFA1403201)the National Natural Science Foundation of China (Grant Nos.12125404,T2495231,123B2049,and 12204138)+9 种基金the Advanced MaterialsNational Science and Technology Major Project (Grant No.2024ZD0607000)the Natural Science Foundation of Jiangsu Province (Grant Nos.BK20233001 and BK20253009)the Jiangsu Funding Program for Excellent Postdoctoral Talent (Grant No.2024ZB002)the China Postdoctoral Science Foundation (Grant No.2025M773331)the Fundamental and Interdisciplinary Disciplines Breakthrough Plan of the Ministry of Education of Chinathe AI&AI for Science program of Nanjing UniversityArtificial Intelligence and Quantum physics (AIQ) program of Nanjing Universitythe Fundamental Research Funds for the Central Universitiesthe Natural Science Foundation of Nanjing University of Posts and Telecommunications(Grant Nos.NY224165,NY220038,and NY219087)the Hua Li Talents Program of Nanjing University of Posts and Telecommunications。
文摘We report a theoretical investigation into superconductivity within the MAXH_(6) quaternary hydride system using first-principles calculations,where M and A denote alkali and alkaline earth elements,respectively,and X represents transition metal elements.Systematic analysis of electronic band structures,phonon dispersions,and electron-phonon coupling reveals that substitution of MA binary metal combinations and X metal atoms can create favorable conditions for superconductivity.Mapping of superconducting critical temperatures,combined with dynamical stability analysis through phonon calculations,identifies ten superconducting candidates at ambient pressure.Among these,LiNaAgH_(6) exhibits nearly-free-electron behavior reminiscent of monovalent electron superconductors.It demonstrates exceptional superconducting properties with electron–phonon coupling λ=2.707,which yields a superconducting transition temperature T_(c) of 206.4 K using the Allen–Dynes formula.Its structural analogs MgNaPdH_(6),LiMgPdH_(6),LiMgAgH_(6),LiMgAuH_(6) all exhibit superconducting transition temperatures above 110 K.These findings advance our fundamental understanding of superconductivity in quaternary hydrides and provide guidance for rational design of new high-temperature superconducting materials.
基金supported by the National Natural Science Foundation of China(No.52375031)the Dongfang Electric Corporation-Zhejiang University Joint Innovation Research Institutethe Bellwethers Research and Development Plan of Zhejiang Province(No.2023C01045)。
文摘Robotic electronic skin(e-skin)is inspired by human skin and endows robots with tactile perception,temperature detection,and environmental interaction capabilities.However,its development is hampered by prolonged design cycles,limited signal enhancement,and weak cognitive abilities.Given that the convergence of artificial intelligence(AI)with e-skin is fundamentally transforming this landscape,the present review highlights the pivotal contributions of AI across the entire development spectrum of robotic e-skin,including design optimization,signal processing,and cognitive enhancement.AI-driven design paradigms dramatically shorten development time and enable the discovery of optimal sensor materials and structures.In signal processing,AI algorithms notably improve the ability to decouple complex sensory data,enabling robust,multimodal,super-resolution sensing.AI endows e-skin with advanced cognitive capabilities,allowing it to interpret intricate tactile information and intelligently respond to external environments.By underscoring the potential of AI throughout the entire development pipeline,this review aims to drive the creation of e-skin with minimal hardware and maximal cognition and thus achieve revolutionary breakthroughs in cutting-edge fields such as human-robot interactions,precise robot control,and soft robotics for environmental exploration.
