In this paper,we present a circuit model of single-quantum-well InGaN/GaN light-emitting diodes based on the standard rate equations.Two rate equations describe carrier transport processes occurring in sep-arate confi...In this paper,we present a circuit model of single-quantum-well InGaN/GaN light-emitting diodes based on the standard rate equations.Two rate equations describe carrier transport processes occurring in sep-arate confinement heterostructure and quantum well respectively,and the third equation describes the varied photons in quantum well.By using the presented model,impacts of quantum well thickness on the static and dynamic performances are investigated.Simulated results show that LED with 4 nm well exhibits better lightcurrent(L-I)performance,but LED with 3 nm well presents wider 3 dB modulation bandwidth.It reveals that high carrier density in quantum well is detrimental to the static performance,but beneficial to the dynamic performance.展开更多
Surface polaritons,as surface electromagnetic waves propagating along the surface of a medium,have played a crucial role in enhancing photonic spin Hall effect(PSHE)and developing highly sensitive refractive index(RI)...Surface polaritons,as surface electromagnetic waves propagating along the surface of a medium,have played a crucial role in enhancing photonic spin Hall effect(PSHE)and developing highly sensitive refractive index(RI)sensors.Among them,the traditional surface plasmon polariton(SPP)based on noble metals limits its application beyond the near-infrared(IR)regime due to the large negative permittivity and optical losses.In this contribution,we theoretically proposed a highly sensitive PSHE sensor with the structure of Ge prism-SiC-Si:InAs-sensing medium,by taking advantage of the hybrid surface plasmon phonon polariton(SPPhP)in mid-IR regime.Here,heavily Si-doped InAs(Si:InAs)and SiC excite the SPP and surface phonon polariton(SPhP),and the hybrid SPPhP is realized in this system.More importantly,the designed PSHE sensor based on this SPPhP mechanism achieves the multi-stage RI measurements from 1.00025-1.00225 to 1.70025-1.70225,and the maximal intensity sensitivity and angle sensitivity can be up to 9.4×10^(4)μm/RIU and245°/RIU,respectively.These findings provide a new pathway for the enhancement of PSHE in mid-IR regime,and offer new opportunities to develop highly sensitive RI sensors in multi-scenario applications,such as harmful gas monitoring and biosensing.展开更多
A high-speed single-mode vertical-cavity surface-emitting laser(VCSEL)is one of the most important light sources for optical interconnects in data centers.Single-mode VCSEL can improve the transmission distance.In thi...A high-speed single-mode vertical-cavity surface-emitting laser(VCSEL)is one of the most important light sources for optical interconnects in data centers.Single-mode VCSEL can improve the transmission distance.In this letter,we demonstrate a single-mode 850 nm VCSEL with a bit rate of 60 Gb/s under NRZ modulation and 104 Gb/s under PAM4 modulation across a 100 m length of OM5 fiber,without the need for equalization or a filter.In addition,by using optical injection locking,the 3 dB bandwidth is enhanced to 68.5 GHz.展开更多
The increase in human population has led to imminent pressures to develop new edible proteins with decreased environmental footprints.The most promising approach involves the production of single cell protein(SCP)from...The increase in human population has led to imminent pressures to develop new edible proteins with decreased environmental footprints.The most promising approach involves the production of single cell protein(SCP)from yeasts,which have been utilized in a wide variety of foods for thousands of years.In this study,102 yeast strains isolated from traditional fermented pork(Nanx Wudl)were investigated for their potential as SCP producer for the first time.Based on preliminary screening,Saccharomyces cerevisiae Y70 and Candida parapsilosis H5Y13,both showing high protein content and excellent growth capability,were selected for further analysis via 4D-DIA proteomics technology.Proteomic analysis indicated that the oxidative metabolism pathways,including TCA cycle,oxidative phosphorylation and pentose phosphate pathway,may have a significant impact on global protein synthesis and production.This study provides useful information for selecting SCP-producing yeast from Chinese fermented meat products and contribute to a deeper understanding of the underlying metabolic mechanisms behind global protein synthesis in yeast.Furthermore,these findings also provide potential molecular targets for genetic engineering modifications in yeast,aimed at constructing highly efficient cell factories for protein production.展开更多
High-performance lead-free piezoelectric single crystals are urgently needed for next-generation actuators and transducers.In this study,we reveal that a compositionally driven tetragonal-pseudocubic(T-PC)phase bounda...High-performance lead-free piezoelectric single crystals are urgently needed for next-generation actuators and transducers.In this study,we reveal that a compositionally driven tetragonal-pseudocubic(T-PC)phase boundary,in conjunction with an octahedral order-disorder tilting transition,significantly enhances the piezoelectric response in Nb^(5+)-substitution(Bi_(0.48)Na_(0.425)K_(0.055)Ba_(0.04))(Ti_(0.98)Nb_(0.02))O_(3)(BNKBT-2Nb)single crystals.The crystal achieves an outstanding piezoelectric coefficient of d33=662 pC/N at room temperature.In situ X-ray diffraction confirms an electric field-induced transition from the PC to T phase.Atomic-resolution HADDF-STEM analysis reveals an increase in the c/a ratio(c/a>1.01)on the local scale and ordered octahe-dral tilting of the a^(0)a^(0)c+type driven by the poling field.The single crystals exhibit excellent piezoelectric per-formance over a broad temperature range,achieving a peak d_(33) of 920 pC/N at approximately 92℃.Furthermore,the polar states exhibit a pronounced frequency dependence near the depolarization temperature.These findings provide critical insight into the structure-property relationship and offer a promising pathway for designing advanced lead-free piezoelectric crystals for functional electromechanical applications.展开更多
Exploring the influence of the coordination environment of single-atom catalysts(SACs)on the electrochemical CO_(2)reduction reaction is vital for assessing the reaction mechanism and structure-performance relationshi...Exploring the influence of the coordination environment of single-atom catalysts(SACs)on the electrochemical CO_(2)reduction reaction is vital for assessing the reaction mechanism and structure-performance relationship.However,it is challenging to engineer the coordination configuration of isolated active metal atoms precisely.Herein,we strategically manipulate the coordination number of the Co-N_(x) configuration by simply changing the order of adding the metal precursor toward improved CO_(2)electrolysis performance.Compared with the symmetric Co-N_(4)coordination,the asymmetric Co-N_(3)coordination leads to reinforced Co-N interaction and downshifted 3d orbital energy toward the Fermi level of the active Co sites,promoting the activation of CO_(2)molecules and the formation of critical intermediate^(*)COOH.The as-designed Co-N_(3)SAC displays excellent Faradaic efficiency(FE)of 98.4%for CO_(2)-to-CO conversion at a low potential of-0.80 V,together with decent FE over a wide potential range(-0.50 V to-1.10 V)and high durability.This study presents an ideal platform to manipulate the coordination number of atomically dispersed metal catalysts and provides a fundamental understanding of coordination configurationperformance correlation for CO_(2)electroreduction.展开更多
Pediatric cancers are particularly significant due to their uncommon occurrence in children,driven by a variety of underlying factors.Because of their distinct molecular and genetic makeup,which makes early detection ...Pediatric cancers are particularly significant due to their uncommon occurrence in children,driven by a variety of underlying factors.Because of their distinct molecular and genetic makeup,which makes early detection challenging,they are linked to problems.Diagnostic methods like imaging and tissue biopsy are only effective when the tumor has reached a size that can be identified.The liquid biopsy technique,the least intrusive and most convenient diagnostic method,is the subject of this review.It focuses on the significance of single cell analysis in examining uncommon cancer types.The many biomarkers found in bodily fluids and the cancer types they are linked to in children have been assessed,as has the potential route towards early detection and cancer recurrence forecasting.Combining the single cell liquid biopsy with the newest technologies,such as computational and multi-omics approaches,which have improved the efficiency of processing massive and unique genetic data,appears promising.This article discusses on a number of case reports for uncommon pediatric malignancies,such as Neuroblastoma,Medulloblastoma,Wilms Tumor,Rhabdomyosarcoma,Ewing Sarcoma,and Retinoblastoma,as well as their liquid biopsy profiles.Furthermore,the findings raise ethical questions regarding the therapeutic application of the technology as well as possible difficulties related to clinical translation.The likelihood that this single cell liquid biopsy will be clinically validated and eventually used as a routine diagnostic tool for uncommon pediatric cancers will rise with the realistic approach to sensitivity monitoring,specificity upgrading,and optimization.展开更多
Sliver defects are a group of low-to-medium angle misoriented grains in Ni-based single crystal superalloys that have received more attention in recent years.Occurrence of these defects can negatively affect the mecha...Sliver defects are a group of low-to-medium angle misoriented grains in Ni-based single crystal superalloys that have received more attention in recent years.Occurrence of these defects can negatively affect the mechanical properties of single crystal components.Therefore,studying the mechanisms of sliver formation and its effects on the final properties of alloys is of great importance.In this article,recent studies on the sliver defects were reviewed.Accordingly,the mechanisms of sliver formation as well as factors contributing to sliver initiation were studied.Additionally,effects of slivers on the mechanical properties of single crystal superalloys were discussed.Dendrite deformation and dendrite fracture are the main mechanisms for the sliver formation.This is a consequence of local stress concentration on dendrites during solidification.Therefore,locations such as inclusions,pores,geometrically complex areas,mould walls,freckle channels,etc.can be considered as the potential factors that promote the sliver initiation.Sliver formation significantly degrades the creep life of single-crystal superalloys.Studies have shown that when crystallographic misorientation exceeds approximately15°,creep life can be reduced by up to 47%.Despite the absence of a standardized criterion for predicting or preventing sliver initiation and propagation,their occurrence can be minimized through optimization of solidification parameters,careful grain selection,proper casting geometry design,and rigorous control of material purity and equipment conditions.展开更多
Fenton-like technology based on peroxymonosulfate activation has shown great potential in refractory organics degradation.In this work,single Fe atom catalysts were synthesized through facile ball milling and exhibite...Fenton-like technology based on peroxymonosulfate activation has shown great potential in refractory organics degradation.In this work,single Fe atom catalysts were synthesized through facile ball milling and exhibited very high performance in peroxymonosulfate activation.The Fe single-atom filled an N vacancy on the triazine ring edge of C_(3)N_(4),as confirmed through X-ray absorption fine structure,density functional calculation and elec-tron paramagnetic resonance.The SAFe_(0.4)–C_(3)N_(4)/PMS system could completely remove phenol(20 mg/L)within 10 min and its first-order kinetic constant was 12.3 times that of the Fe_(3)O_(4)/PMS system.Under different ini-tial pH levels and in various anionic environments,SAFe_(0.4)–C_(3)N_(4) still demonstrated excellent catalytic activity,achieving a removal rate of over 90%for phenol within 12 min.In addition,SAFe_(0.4)–C_(3)N_(4) exhibited outstanding selectivity in reaction systems with different pollutants,showing excellent degradation effects on electron-rich pollutants only.Hydroxyl radicals(•OH),singlet oxygen(1O_(2))and high-valent iron oxide(Fe(Ⅳ)=O)were de-tected in the SAFe_(0.4)–C_(3)N_(4)/PMS system through free radical capture experiments.Further experiments on the quenching of active species and a methyl phenyl sulfoxide probe confirmed that 1O_(2) and Fe(Ⅳ)=O played dom-inant roles.Additionally,the change in the current response after adding PMS and phenol in succession proved that a direct electron transfer path between organic matter and the catalyst surface was unlikely to exist in the SAFe_(0.4)–C_(3)N_(4)/PMS/Phenol degradation system.This study provides a new demonstration of the catalytic mech-anism of single-atom catalysts.展开更多
Nickel-based single-crystal superalloy DD98M is widely used in high-temperature components such as aero-engines and gas turbines.Since it has only one crystal grain,the theory of slip deformation along the grain bound...Nickel-based single-crystal superalloy DD98M is widely used in high-temperature components such as aero-engines and gas turbines.Since it has only one crystal grain,the theory of slip deformation along the grain boundary of polycrystalline material is not suitable for the machining of a single crystal part.Therefore,micro-drilling of nickel-based single crystal superalloy still faces problems such as unclear cutting formation me-chanism and unclear surface/subsurface damage mechanism.In this paper,the formation mechanism and morphological characteristics of chips and burrs were studied by a single-factor experiment,and the plastic deformation rule and damage mechanism were investigated,combined with the changes of subsurface structure and grain type.Finally,the influence of the law and reason of tool wear condition on the hole wall and the drilled subsurface is analyzed.The experimental results indicate that drill chips mainly exhibit three morphologies.Their free surfaces feature a serrated appearance,while the contact surfaces are smooth.The entrance burrs are mainly flanging burrs.With the increase of spindle speed,the burr height decreases from 49.38 to 9.39μm.As the feed speed increases,the burr height increases from 6.50 to 63.87μm.The drilled subsurface can be divided into a white layer region,a plastic deformation region,and the matrix according to the microstructural change.As the depth from the machined surface increases,the degree of plastic deformation of the material decreases,the grain size gradually reduces,and the dislocation density decreases.Stacking fault and twinning mostly occur in the high-plastic deformation region,and recrystallization occurs on the machined surface.As the drilling length increases,the degree of tool wear increases,and the adhesion and ablation area on the hole wall surface increase.Moreover,the thickness of the white layer increases from 0 to 8.75μm,and the thickness of the plastic deformation layer increases from 1.28 to 11.31μm.The study has significant theoretical and practical implications for the efficient and low-damage machining of micro-holes in the nickel-based single crystal superalloy.展开更多
Turbine blades,due to their intricate geometry,are exposed to multiaxial stresses during operation.Consequently,it is imperative to examine the anisotropy of their stress-rupture behavior across various testing scenar...Turbine blades,due to their intricate geometry,are exposed to multiaxial stresses during operation.Consequently,it is imperative to examine the anisotropy of their stress-rupture behavior across various testing scenarios,particularly under high-temperature conditions.Stress-rupture behavior of a Ni-based single crystal superalloy was investigated under a load varying from 100 MPa to 137 MPa at 1,100℃ for both[001]-and[111]-orientated specimens.Results demonstrate that the rupture behavior of[111]-orientated specimens exhibits obviously higher sensitive to applied stress compared to[001]-orientated specimens.This difference is primarily attributed to the orientation dependentγ'coarsening behavior and distinct dislocation interactions atγ/γ'interfaces.In[001]-oriented specimens,plate-likeγ/γ'rafts rapidly form alongside well-developed interfacial dislocation networks,where theγ/γ'misfit stress dominates the microstructural evolution.In contrast,the[111]-orientated specimens exhibit retained,coarsenedγ'precipitates embedded within theγmatrix,accompanied by poorly developed interfacial dislocation networks.展开更多
The single electron capture processes in Si^(3,4+)+He collisions have been investigated theoretically employing the two-center atomic orbital close-coupling method in the energy range 0.01-100 keV/u.Total and state-se...The single electron capture processes in Si^(3,4+)+He collisions have been investigated theoretically employing the two-center atomic orbital close-coupling method in the energy range 0.01-100 keV/u.Total and state-selective electron capture cross sections for the dominant and subdominant reaction channels are calculated and compared with the available experimental and theoretical data.For the total charge transfer cross sections,the present results show better agreements with the available experimental data than the other theoretical ones in the overlapping energy region for both collision systems.For the state-selective cross sections,the present results for 3s and 3p states are in general agreement with the previous MOCC results in the low energy region for both collision systems.Furthermore,the cross sections for electron captured to the 3d,4l and 5l(l=0,1,...,n-1)states of Si^(2+)and Si^(3+)ions are first provided in a broad energy region in our work.These results are useful for the investigations in astrophysics.The datasets presented in this paper,including the total and state-selective electron capture cross sections of Si^(3,4+)+He collisions in 0.01-100 ke V/u,are openly available at https://doi.org/10.57760/sciencedb.j00113.00257.展开更多
High-performance fiber fabrics and composites experienced transverse compression deformation at ultrahigh strain rates near the impact point when subjected to high-velocity impacts,which significantly affected their b...High-performance fiber fabrics and composites experienced transverse compression deformation at ultrahigh strain rates near the impact point when subjected to high-velocity impacts,which significantly affected their ballistic limits.In this paper,a fiber-scale experimental method for characterizing ultrahigh strain-rate transverse compression behavior was proposed.To begin with,in order to measure the extremely low stress and strain in small specimens,the conventional Hopkinson bar was reduced to the hundred-micron scale,thereby achieving wave impedance matching with single fibers.In addition,tangential and normal laser Doppler velocimetry(LDV)methods were employed to realize non-contact,high-precision,and high-speed axial velocity measurements of micron-scale incident and transmission bars,respectively.Meanwhile,a microscopic observation system was used to facilitate the installation of miniature fiber samples.The experimental setup and procedures were introduced,and the system accuracy was verified through sample-free loading tests based on one-dimensional stress wave propagation theory.Dynamic compression experiments on Graphene-UHMWPE fibers were carried out,followed by post-compression microstructural characterization via scanning electron microscopy(SEM).Results demonstrated that successful mechanical characterization was achieved at strain rates exceeding 105,an order of magnitude higher than the previously reported maximum rates.Furthermore,during the loading process,the fibers underwent uniform compression deformation while exhibiting pronounced strain-rate effects.This method offers a novel approach for dynamic mechanical characterization of microscale single fibers,enabling the development of comprehensive strain-ratedependent material models to guide the design of advanced composites and high-performance fibers.展开更多
The rate capability and cycling stability of sodium metal batteries taking FeS_(2) or sulfur as cathode are limited due to their low reaction kinetics and severe shuttle effect.Herein,we rationally design a novel sing...The rate capability and cycling stability of sodium metal batteries taking FeS_(2) or sulfur as cathode are limited due to their low reaction kinetics and severe shuttle effect.Herein,we rationally design a novel single-atom-dispersed S_(2)-FeNC/FeS_(2) nanocluster heterojunction embedded in carbon spheres(SFNC/FeS_(2)) for the electrode material of sodium metal batteries.Interestingly,during the discharging process,the Na^(+) is inserted into FeS_(2) to generate Na_(2)S,as well as the unique electrochemical reaction between S_(2)-FeNC and Na^(+) to form Na_(2)S.Meanwhile,the FeNC can adsorb Na_(2)S and catalyze the conversion from Na_(2)S and Fe to FeS_(2) or from Na_(2)S and FeNC to S_(2)-FeNC for suppressing the shuttle effect and promoting the distinct hybrid reversible electrochemical behavior,which improves performance tremendously.Notably,the SFNC/FeS_(2) electrode delivers a specific capacity of 338.7 mAh g^(-1) after superlong 2000 cycles at a current density of 5.0 A g^(-1) and achieves a high energy density of 430.1 Wh Kg^(-1) at a current density of 0.05 A g^(-1).This work presents a novel approach to studying sodium metal batteries with hybrid behavior for excellent high energy density and cycling stability.展开更多
Mitochondria are the central organelles that allow eukaryotic cells to efficiently convert nutrients into energy for cellular functions such as anabolic reactions,movement,and regulation.A reduction in the number of m...Mitochondria are the central organelles that allow eukaryotic cells to efficiently convert nutrients into energy for cellular functions such as anabolic reactions,movement,and regulation.A reduction in the number of mitochondria or the occurrence of dysfunctional mitochondria leads to serious diseases such as the Leigh syndrome.However,such changes have also been connected to Alzheimer’s disease(AD)and many more diseases of different organ systems and occur during the aging process.Mitochondria are,therefore.展开更多
Bismuth vanadate(BiVO_(4))is regarded as a promising photoanode for photoelectrochemical(PEC)water splitting.Despite its advantage in band gap and visible-light response,the BiVO_(4)exhibits an unsatisfactory achievin...Bismuth vanadate(BiVO_(4))is regarded as a promising photoanode for photoelectrochemical(PEC)water splitting.Despite its advantage in band gap and visible-light response,the BiVO_(4)exhibits an unsatisfactory achieving water splitting due to severe charge recombination.Herein,we elucidate an innovative approach involving the incorporation of single Ru atom with a CoFe-LDH cocatalyst(Ru_(0.51)-CoFe-LDH)and integrating it onto the BiVO_(4)semiconductor substrate.The resulting Ru_(0.51)-CoFe-LDH/BiVO_(4)photoanode film demonstrates commendable charge injection efficiency(76%)and charge collection efficiency(100%).Interestingly,the yield of hydrogen and oxygen increases linearly at a stoichiometric ratio of about 2:1,reaching 158.6 and 67.4μmol after140 min of irradiation,respectively.According to experimental characterization and density functional theory calculation,this remarkable performance results from single Ru atoms triggering the electron rearrangement of Ru_(0.51)-CoFe-LDH to engineer active sites and optimize interfacial energetics.Additionally,the negative shift of Ru_(0.51)-CoFe-LDH band edge gives rise to more conspicuous band bending of the n-n junction formed with BiVO_(4),expediting the separation and transfer of photogenerated electron-hole pairs at the interface.This work furnishes a new preparation perspective for PEC water splitting systems to construct single atoms in the semiconductor substrate.展开更多
Unlike mammals,zebrafish possess a remarkable ability to regenerate their spinal cord after injury,making them an ideal vertebrate model for studying regeneration.While previous research has identified key cell types ...Unlike mammals,zebrafish possess a remarkable ability to regenerate their spinal cord after injury,making them an ideal vertebrate model for studying regeneration.While previous research has identified key cell types involved in this process,the underlying molecular and cellular mechanisms remain largely unexplored.In this study,we used single-cell RNA sequencing to profile distinct cell populations at different stages of spinal cord injury in zebrafish.Our analysis revealed that multiple subpopulations of neurons showed persistent activation of genes associated with axonal regeneration post injury,while molecular signals promoting growth cone collapse were inhibited.Radial glial cells exhibited significant proliferation and differentiation potential post injury,indicating their intrinsic roles in promoting neurogenesis and axonal regeneration,respectively.Additionally,we found that inflammatory factors rapidly decreased in the early stages following spinal cord injury,creating a microenvironment permissive for tissue repair and regeneration.Furthermore,oligodendrocytes lost maturity markers while exhibiting increased proliferation following injury.These findings demonstrated that the rapid and orderly regulation of inflammation,as well as the efficient proliferation and redifferentiation of new neurons and glial cells,enabled zebrafish to reconstruct the spinal cord.This research provides new insights into the cellular transitions and molecular programs that drive spinal cord regeneration,offering promising avenues for future research and therapeutic strategies.展开更多
The breaking of the symmetric electronic distribution of single-atom catalysts is effective in improving the intrinsic activity.However,traditional modification strategies can only disrupt the electronic distribution ...The breaking of the symmetric electronic distribution of single-atom catalysts is effective in improving the intrinsic activity.However,traditional modification strategies can only disrupt the electronic distribution in one dimension,resulting in limited regulation of electronic structure.Herein,we report a multidimensional coordination strategy to significantly break the symmetrical electron distribution of the metal single site to achieve highly efficient electrochemical CO_(2) reduction reaction(CO_(2) RR).Ni singleatom sites decorated with planar P and axial Cl atoms are successfully constructed on carbon support(Ni-NPCl-C).Ni-NPCl-C affords CO Faraday efficiency over 90%in a wide potential window range from-0.5 to-1.2 V and an ultrahigh turnover frequency of 1.17×10^(5)h^(-1),much superior to its counterparts with single-dimensional coordination.Ni-NPCl-C can be further applied as a bifunctional catalyst to construct a rechargeable Zn-CO_(2) battery.Spectroscopic characterizations and theoretical calculations demonstrate that the dual adjustments with axial Cl and planar P can synergistically disrupt the electron distribution in two dimensions to increase electrons around Ni sites with the upshift of the d-band center,thereby facilitating the formation of*COOH intermediates and improving the CO_(2) RR performance.展开更多
Temperature-dependent resistivity,upper critical field H_(c2)and its anisotropy in overdoped superconducting Ba_(1-x)K_x Fe_2As_2(x=0.6-1)single crystals have been measured in steady magnetic fields up to 44 T and low...Temperature-dependent resistivity,upper critical field H_(c2)and its anisotropy in overdoped superconducting Ba_(1-x)K_x Fe_2As_2(x=0.6-1)single crystals have been measured in steady magnetic fields up to 44 T and low temperatures down to 0.4 K.Analysis using both the quadratic term and power-law fitting demonstrates that the in-plane resistivityρ_(ab)(T)progressively approaches the Fermi-liquid T~2behavior with increasing K doping and reaches a saturation plateau at x≈0.8.The temperature dependence of both H_(c2)^(ab)and H^(c)_(c2)follows the Werthamer-Helfand-Hohenberg model,incorporating orbital and spin paramagnetic effects.For x≤0.8,the orbital effect dominates for H ab,while the Pauli paramagnetic effect prevails for H c.For x>0.8,the Pauli paramagnetic effect becomes dominant in both crystallographic directions.The anisotropy of H_(c2)(0)exhibits a discontinuity in its dependence on K doping concentration with a significant enhancement at x=0.8 and a maximum at x=0.9.These experimental results indicate that the electron correlation effect is enhanced in the heavily overdoped Ba_(1-x)K_(x)Fe_(2)As_(2)system where the underlying symmetries are broken due to the Fermi surface reconstruction before x=0.9.展开更多
Defect engineering serves as a cornerstone in the design of high-effciency single-atom catalysts(SACs)for advanced electrocatalytic systems.This study demonstrates oxygen vacancy-induced near-zero-valent Pt SACs ancho...Defect engineering serves as a cornerstone in the design of high-effciency single-atom catalysts(SACs)for advanced electrocatalytic systems.This study demonstrates oxygen vacancy-induced near-zero-valent Pt SACs anchored on TiO2 for efficient hydrogen evolution reaction(HER).Synchrotron spectroscopy and density functional theory calculation reveal that oxygen vacancies create unconventional Pt-Ti coordination while strengthening electronic metal-support interactions.This facilitates substantial electron transfer from TiO2 to Pt,generating a near-zero-valent Pt state with elevated electron density.The modified electronic structure lowers the Pt d-band center,reducing hydrogen intermediate(*H)adsorption energy and optimizing HER kinetics.Moreover,ab initio molecular dynamics and in situ Raman spectra show that the negative charge accumulated at the Pt site promotes K^(+)enrichment at the interface,which enhances H-OH bond polarization and accelerates water dissociation kinetics.The resulting D-TiO_(2)/Pt SACs exhibit superior HER activity across acidic,neutral,and alkaline conditions,achieving low overpotentials of 40,57,and 60 mV at 10 mA cm^(-2),respectively.Additionally,its mass activities at the overpotential of 100 mV are 10.3,33.9,and 20.9 times higher that of Pt/C,respectively.This study shows the key role of defectmediated electronic engineering in tailoring SACs'valence states and catalytic functions,advancing sustainable hydrogen production through rational catalyst design.展开更多
文摘In this paper,we present a circuit model of single-quantum-well InGaN/GaN light-emitting diodes based on the standard rate equations.Two rate equations describe carrier transport processes occurring in sep-arate confinement heterostructure and quantum well respectively,and the third equation describes the varied photons in quantum well.By using the presented model,impacts of quantum well thickness on the static and dynamic performances are investigated.Simulated results show that LED with 4 nm well exhibits better lightcurrent(L-I)performance,but LED with 3 nm well presents wider 3 dB modulation bandwidth.It reveals that high carrier density in quantum well is detrimental to the static performance,but beneficial to the dynamic performance.
基金Project supported by the National Natural Science Foundation of China(Grant No.12175107)the Qing Lan Project of Jiangsu Province+2 种基金the Hua Li Talents Program of Nanjing University of PostsTelecommunications,Natural Science Foundation of Nanjing Vocational University of Industry Technology(Grant No.YK22-02-08)the Fund from the Research Center of Industrial Perception and Intelligent Manufacturing Equipment Engineering of Jiangsu Province,China(Grant No.ZK21-05-09)。
文摘Surface polaritons,as surface electromagnetic waves propagating along the surface of a medium,have played a crucial role in enhancing photonic spin Hall effect(PSHE)and developing highly sensitive refractive index(RI)sensors.Among them,the traditional surface plasmon polariton(SPP)based on noble metals limits its application beyond the near-infrared(IR)regime due to the large negative permittivity and optical losses.In this contribution,we theoretically proposed a highly sensitive PSHE sensor with the structure of Ge prism-SiC-Si:InAs-sensing medium,by taking advantage of the hybrid surface plasmon phonon polariton(SPPhP)in mid-IR regime.Here,heavily Si-doped InAs(Si:InAs)and SiC excite the SPP and surface phonon polariton(SPhP),and the hybrid SPPhP is realized in this system.More importantly,the designed PSHE sensor based on this SPPhP mechanism achieves the multi-stage RI measurements from 1.00025-1.00225 to 1.70025-1.70225,and the maximal intensity sensitivity and angle sensitivity can be up to 9.4×10^(4)μm/RIU and245°/RIU,respectively.These findings provide a new pathway for the enhancement of PSHE in mid-IR regime,and offer new opportunities to develop highly sensitive RI sensors in multi-scenario applications,such as harmful gas monitoring and biosensing.
基金supported by the National Key R&D Program of China(2021YFB2801000).
文摘A high-speed single-mode vertical-cavity surface-emitting laser(VCSEL)is one of the most important light sources for optical interconnects in data centers.Single-mode VCSEL can improve the transmission distance.In this letter,we demonstrate a single-mode 850 nm VCSEL with a bit rate of 60 Gb/s under NRZ modulation and 104 Gb/s under PAM4 modulation across a 100 m length of OM5 fiber,without the need for equalization or a filter.In addition,by using optical injection locking,the 3 dB bandwidth is enhanced to 68.5 GHz.
基金financial support of the National Natural Science Foundation of China(32102016)the Taishan Industrial Experts Program,Beijing Postdoctoral Research Foundation(2323ZZ122).
文摘The increase in human population has led to imminent pressures to develop new edible proteins with decreased environmental footprints.The most promising approach involves the production of single cell protein(SCP)from yeasts,which have been utilized in a wide variety of foods for thousands of years.In this study,102 yeast strains isolated from traditional fermented pork(Nanx Wudl)were investigated for their potential as SCP producer for the first time.Based on preliminary screening,Saccharomyces cerevisiae Y70 and Candida parapsilosis H5Y13,both showing high protein content and excellent growth capability,were selected for further analysis via 4D-DIA proteomics technology.Proteomic analysis indicated that the oxidative metabolism pathways,including TCA cycle,oxidative phosphorylation and pentose phosphate pathway,may have a significant impact on global protein synthesis and production.This study provides useful information for selecting SCP-producing yeast from Chinese fermented meat products and contribute to a deeper understanding of the underlying metabolic mechanisms behind global protein synthesis in yeast.Furthermore,these findings also provide potential molecular targets for genetic engineering modifications in yeast,aimed at constructing highly efficient cell factories for protein production.
基金supported by the National Natural Science Foundation of China(Grant No.11704301)the Natural Science Basic Research Plan in Shaanxi Province of China(Program No.2022JM212)supported by the Ministry of Science and Higher Education of the Russian Federation(FSEG-2023-0016).
文摘High-performance lead-free piezoelectric single crystals are urgently needed for next-generation actuators and transducers.In this study,we reveal that a compositionally driven tetragonal-pseudocubic(T-PC)phase boundary,in conjunction with an octahedral order-disorder tilting transition,significantly enhances the piezoelectric response in Nb^(5+)-substitution(Bi_(0.48)Na_(0.425)K_(0.055)Ba_(0.04))(Ti_(0.98)Nb_(0.02))O_(3)(BNKBT-2Nb)single crystals.The crystal achieves an outstanding piezoelectric coefficient of d33=662 pC/N at room temperature.In situ X-ray diffraction confirms an electric field-induced transition from the PC to T phase.Atomic-resolution HADDF-STEM analysis reveals an increase in the c/a ratio(c/a>1.01)on the local scale and ordered octahe-dral tilting of the a^(0)a^(0)c+type driven by the poling field.The single crystals exhibit excellent piezoelectric per-formance over a broad temperature range,achieving a peak d_(33) of 920 pC/N at approximately 92℃.Furthermore,the polar states exhibit a pronounced frequency dependence near the depolarization temperature.These findings provide critical insight into the structure-property relationship and offer a promising pathway for designing advanced lead-free piezoelectric crystals for functional electromechanical applications.
基金financially supported by the Program for the Development of Science and Technology of Jilin Province(No.20240101004JJ)the National Natural Science Foundation of China(No.22409165)+4 种基金the National Foreign Experts Program of the Ministry of Human Resources and Social Security(No.Y20240003)the Shaanxi Province Talent Programfinancially supported by the Strategic Priority Research Program of the Chinese Academy of Sciences(Nos.XDB0600000,XDB0600100,XDB0600200,XDB0600300,XDB0600400)Liaoning Binhai Laboratory(No.LILBLB-2023-04)Dalian Revitalization Talents Program(No.2022RG01)。
文摘Exploring the influence of the coordination environment of single-atom catalysts(SACs)on the electrochemical CO_(2)reduction reaction is vital for assessing the reaction mechanism and structure-performance relationship.However,it is challenging to engineer the coordination configuration of isolated active metal atoms precisely.Herein,we strategically manipulate the coordination number of the Co-N_(x) configuration by simply changing the order of adding the metal precursor toward improved CO_(2)electrolysis performance.Compared with the symmetric Co-N_(4)coordination,the asymmetric Co-N_(3)coordination leads to reinforced Co-N interaction and downshifted 3d orbital energy toward the Fermi level of the active Co sites,promoting the activation of CO_(2)molecules and the formation of critical intermediate^(*)COOH.The as-designed Co-N_(3)SAC displays excellent Faradaic efficiency(FE)of 98.4%for CO_(2)-to-CO conversion at a low potential of-0.80 V,together with decent FE over a wide potential range(-0.50 V to-1.10 V)and high durability.This study presents an ideal platform to manipulate the coordination number of atomically dispersed metal catalysts and provides a fundamental understanding of coordination configurationperformance correlation for CO_(2)electroreduction.
文摘Pediatric cancers are particularly significant due to their uncommon occurrence in children,driven by a variety of underlying factors.Because of their distinct molecular and genetic makeup,which makes early detection challenging,they are linked to problems.Diagnostic methods like imaging and tissue biopsy are only effective when the tumor has reached a size that can be identified.The liquid biopsy technique,the least intrusive and most convenient diagnostic method,is the subject of this review.It focuses on the significance of single cell analysis in examining uncommon cancer types.The many biomarkers found in bodily fluids and the cancer types they are linked to in children have been assessed,as has the potential route towards early detection and cancer recurrence forecasting.Combining the single cell liquid biopsy with the newest technologies,such as computational and multi-omics approaches,which have improved the efficiency of processing massive and unique genetic data,appears promising.This article discusses on a number of case reports for uncommon pediatric malignancies,such as Neuroblastoma,Medulloblastoma,Wilms Tumor,Rhabdomyosarcoma,Ewing Sarcoma,and Retinoblastoma,as well as their liquid biopsy profiles.Furthermore,the findings raise ethical questions regarding the therapeutic application of the technology as well as possible difficulties related to clinical translation.The likelihood that this single cell liquid biopsy will be clinically validated and eventually used as a routine diagnostic tool for uncommon pediatric cancers will rise with the realistic approach to sensitivity monitoring,specificity upgrading,and optimization.
文摘Sliver defects are a group of low-to-medium angle misoriented grains in Ni-based single crystal superalloys that have received more attention in recent years.Occurrence of these defects can negatively affect the mechanical properties of single crystal components.Therefore,studying the mechanisms of sliver formation and its effects on the final properties of alloys is of great importance.In this article,recent studies on the sliver defects were reviewed.Accordingly,the mechanisms of sliver formation as well as factors contributing to sliver initiation were studied.Additionally,effects of slivers on the mechanical properties of single crystal superalloys were discussed.Dendrite deformation and dendrite fracture are the main mechanisms for the sliver formation.This is a consequence of local stress concentration on dendrites during solidification.Therefore,locations such as inclusions,pores,geometrically complex areas,mould walls,freckle channels,etc.can be considered as the potential factors that promote the sliver initiation.Sliver formation significantly degrades the creep life of single-crystal superalloys.Studies have shown that when crystallographic misorientation exceeds approximately15°,creep life can be reduced by up to 47%.Despite the absence of a standardized criterion for predicting or preventing sliver initiation and propagation,their occurrence can be minimized through optimization of solidification parameters,careful grain selection,proper casting geometry design,and rigorous control of material purity and equipment conditions.
基金supported by the National Natural Science Foundation of China(Nos.22406081,22276086,22306086)the Natural Science Foundation of Jiangxi Province(No.20232BAB213029),all of which are greatly acknowledged by the authors.
文摘Fenton-like technology based on peroxymonosulfate activation has shown great potential in refractory organics degradation.In this work,single Fe atom catalysts were synthesized through facile ball milling and exhibited very high performance in peroxymonosulfate activation.The Fe single-atom filled an N vacancy on the triazine ring edge of C_(3)N_(4),as confirmed through X-ray absorption fine structure,density functional calculation and elec-tron paramagnetic resonance.The SAFe_(0.4)–C_(3)N_(4)/PMS system could completely remove phenol(20 mg/L)within 10 min and its first-order kinetic constant was 12.3 times that of the Fe_(3)O_(4)/PMS system.Under different ini-tial pH levels and in various anionic environments,SAFe_(0.4)–C_(3)N_(4) still demonstrated excellent catalytic activity,achieving a removal rate of over 90%for phenol within 12 min.In addition,SAFe_(0.4)–C_(3)N_(4) exhibited outstanding selectivity in reaction systems with different pollutants,showing excellent degradation effects on electron-rich pollutants only.Hydroxyl radicals(•OH),singlet oxygen(1O_(2))and high-valent iron oxide(Fe(Ⅳ)=O)were de-tected in the SAFe_(0.4)–C_(3)N_(4)/PMS system through free radical capture experiments.Further experiments on the quenching of active species and a methyl phenyl sulfoxide probe confirmed that 1O_(2) and Fe(Ⅳ)=O played dom-inant roles.Additionally,the change in the current response after adding PMS and phenol in succession proved that a direct electron transfer path between organic matter and the catalyst surface was unlikely to exist in the SAFe_(0.4)–C_(3)N_(4)/PMS/Phenol degradation system.This study provides a new demonstration of the catalytic mech-anism of single-atom catalysts.
基金Supported by National Natural Science Foundation of China(Grant Nos.52475433,52305453)Hebei Provincial Natural Science Foundation(Grant No.E2022501004)+1 种基金the Fundamental Research Funds for the Central Universities(Grant No.2023GFYD002)Shijiazhuang Municipal Science and Technology Plan Project(Grant No.241790747A).
文摘Nickel-based single-crystal superalloy DD98M is widely used in high-temperature components such as aero-engines and gas turbines.Since it has only one crystal grain,the theory of slip deformation along the grain boundary of polycrystalline material is not suitable for the machining of a single crystal part.Therefore,micro-drilling of nickel-based single crystal superalloy still faces problems such as unclear cutting formation me-chanism and unclear surface/subsurface damage mechanism.In this paper,the formation mechanism and morphological characteristics of chips and burrs were studied by a single-factor experiment,and the plastic deformation rule and damage mechanism were investigated,combined with the changes of subsurface structure and grain type.Finally,the influence of the law and reason of tool wear condition on the hole wall and the drilled subsurface is analyzed.The experimental results indicate that drill chips mainly exhibit three morphologies.Their free surfaces feature a serrated appearance,while the contact surfaces are smooth.The entrance burrs are mainly flanging burrs.With the increase of spindle speed,the burr height decreases from 49.38 to 9.39μm.As the feed speed increases,the burr height increases from 6.50 to 63.87μm.The drilled subsurface can be divided into a white layer region,a plastic deformation region,and the matrix according to the microstructural change.As the depth from the machined surface increases,the degree of plastic deformation of the material decreases,the grain size gradually reduces,and the dislocation density decreases.Stacking fault and twinning mostly occur in the high-plastic deformation region,and recrystallization occurs on the machined surface.As the drilling length increases,the degree of tool wear increases,and the adhesion and ablation area on the hole wall surface increase.Moreover,the thickness of the white layer increases from 0 to 8.75μm,and the thickness of the plastic deformation layer increases from 1.28 to 11.31μm.The study has significant theoretical and practical implications for the efficient and low-damage machining of micro-holes in the nickel-based single crystal superalloy.
基金financially supported by the National Science and Technology Major Project of China(No.2019-VII-0019-0161 and No.2019-VII-0004-0144)the National Natural Science Foundation of China(No.92360302)the Shandong Provincial Natural Science Foundation of China(No.ZR2021QE103)。
文摘Turbine blades,due to their intricate geometry,are exposed to multiaxial stresses during operation.Consequently,it is imperative to examine the anisotropy of their stress-rupture behavior across various testing scenarios,particularly under high-temperature conditions.Stress-rupture behavior of a Ni-based single crystal superalloy was investigated under a load varying from 100 MPa to 137 MPa at 1,100℃ for both[001]-and[111]-orientated specimens.Results demonstrate that the rupture behavior of[111]-orientated specimens exhibits obviously higher sensitive to applied stress compared to[001]-orientated specimens.This difference is primarily attributed to the orientation dependentγ'coarsening behavior and distinct dislocation interactions atγ/γ'interfaces.In[001]-oriented specimens,plate-likeγ/γ'rafts rapidly form alongside well-developed interfacial dislocation networks,where theγ/γ'misfit stress dominates the microstructural evolution.In contrast,the[111]-orientated specimens exhibit retained,coarsenedγ'precipitates embedded within theγmatrix,accompanied by poorly developed interfacial dislocation networks.
基金supported by the National Key Research and Development Program of China(Grant No.2022YFA1602504)the National Natural Science Foundation of China(Grant Nos.12274040 and U2430208)。
文摘The single electron capture processes in Si^(3,4+)+He collisions have been investigated theoretically employing the two-center atomic orbital close-coupling method in the energy range 0.01-100 keV/u.Total and state-selective electron capture cross sections for the dominant and subdominant reaction channels are calculated and compared with the available experimental and theoretical data.For the total charge transfer cross sections,the present results show better agreements with the available experimental data than the other theoretical ones in the overlapping energy region for both collision systems.For the state-selective cross sections,the present results for 3s and 3p states are in general agreement with the previous MOCC results in the low energy region for both collision systems.Furthermore,the cross sections for electron captured to the 3d,4l and 5l(l=0,1,...,n-1)states of Si^(2+)and Si^(3+)ions are first provided in a broad energy region in our work.These results are useful for the investigations in astrophysics.The datasets presented in this paper,including the total and state-selective electron capture cross sections of Si^(3,4+)+He collisions in 0.01-100 ke V/u,are openly available at https://doi.org/10.57760/sciencedb.j00113.00257.
基金financial support provided by the National Natural Science Foundation of China(Grant No.12302472)the Science and Technology Support Program of Jiangsu Province(Grant No.BK20230874)+2 种基金the Aeronautical Science Fund(ASF)(Grant No.2023Z057052005)the Research Fund of State Key Laboratory of Mechanics and Control for Aerospace Structures(Nanjing University of Aeronautics and Astronautics)(Grant No.MCAS-I-0124G02)the funding received from Jiangsu Hanvo Safety Product Co.,Ltd。
文摘High-performance fiber fabrics and composites experienced transverse compression deformation at ultrahigh strain rates near the impact point when subjected to high-velocity impacts,which significantly affected their ballistic limits.In this paper,a fiber-scale experimental method for characterizing ultrahigh strain-rate transverse compression behavior was proposed.To begin with,in order to measure the extremely low stress and strain in small specimens,the conventional Hopkinson bar was reduced to the hundred-micron scale,thereby achieving wave impedance matching with single fibers.In addition,tangential and normal laser Doppler velocimetry(LDV)methods were employed to realize non-contact,high-precision,and high-speed axial velocity measurements of micron-scale incident and transmission bars,respectively.Meanwhile,a microscopic observation system was used to facilitate the installation of miniature fiber samples.The experimental setup and procedures were introduced,and the system accuracy was verified through sample-free loading tests based on one-dimensional stress wave propagation theory.Dynamic compression experiments on Graphene-UHMWPE fibers were carried out,followed by post-compression microstructural characterization via scanning electron microscopy(SEM).Results demonstrated that successful mechanical characterization was achieved at strain rates exceeding 105,an order of magnitude higher than the previously reported maximum rates.Furthermore,during the loading process,the fibers underwent uniform compression deformation while exhibiting pronounced strain-rate effects.This method offers a novel approach for dynamic mechanical characterization of microscale single fibers,enabling the development of comprehensive strain-ratedependent material models to guide the design of advanced composites and high-performance fibers.
基金financially supported by the National Natural Science Foundation of China (No. 22579095)the Beijing-Tianjin-Hebei Basic Research Cooperation Special Project (B2024204027)+2 种基金the Youth Top-notch Talent Foundation of Hebei Provincial Universities (BJK2022023)the Natural Science Foundation of Hebei Province (B2023204006)the talent training project of Hebei province (No. B20231004)。
文摘The rate capability and cycling stability of sodium metal batteries taking FeS_(2) or sulfur as cathode are limited due to their low reaction kinetics and severe shuttle effect.Herein,we rationally design a novel single-atom-dispersed S_(2)-FeNC/FeS_(2) nanocluster heterojunction embedded in carbon spheres(SFNC/FeS_(2)) for the electrode material of sodium metal batteries.Interestingly,during the discharging process,the Na^(+) is inserted into FeS_(2) to generate Na_(2)S,as well as the unique electrochemical reaction between S_(2)-FeNC and Na^(+) to form Na_(2)S.Meanwhile,the FeNC can adsorb Na_(2)S and catalyze the conversion from Na_(2)S and Fe to FeS_(2) or from Na_(2)S and FeNC to S_(2)-FeNC for suppressing the shuttle effect and promoting the distinct hybrid reversible electrochemical behavior,which improves performance tremendously.Notably,the SFNC/FeS_(2) electrode delivers a specific capacity of 338.7 mAh g^(-1) after superlong 2000 cycles at a current density of 5.0 A g^(-1) and achieves a high energy density of 430.1 Wh Kg^(-1) at a current density of 0.05 A g^(-1).This work presents a novel approach to studying sodium metal batteries with hybrid behavior for excellent high energy density and cycling stability.
文摘Mitochondria are the central organelles that allow eukaryotic cells to efficiently convert nutrients into energy for cellular functions such as anabolic reactions,movement,and regulation.A reduction in the number of mitochondria or the occurrence of dysfunctional mitochondria leads to serious diseases such as the Leigh syndrome.However,such changes have also been connected to Alzheimer’s disease(AD)and many more diseases of different organ systems and occur during the aging process.Mitochondria are,therefore.
基金financially supported by the Hunan Provincial Natural Science Foundation for Distinguished Young Scholars(2025JJ20019)the National Key R&D Program of China(2025YFE0107600)。
文摘Bismuth vanadate(BiVO_(4))is regarded as a promising photoanode for photoelectrochemical(PEC)water splitting.Despite its advantage in band gap and visible-light response,the BiVO_(4)exhibits an unsatisfactory achieving water splitting due to severe charge recombination.Herein,we elucidate an innovative approach involving the incorporation of single Ru atom with a CoFe-LDH cocatalyst(Ru_(0.51)-CoFe-LDH)and integrating it onto the BiVO_(4)semiconductor substrate.The resulting Ru_(0.51)-CoFe-LDH/BiVO_(4)photoanode film demonstrates commendable charge injection efficiency(76%)and charge collection efficiency(100%).Interestingly,the yield of hydrogen and oxygen increases linearly at a stoichiometric ratio of about 2:1,reaching 158.6 and 67.4μmol after140 min of irradiation,respectively.According to experimental characterization and density functional theory calculation,this remarkable performance results from single Ru atoms triggering the electron rearrangement of Ru_(0.51)-CoFe-LDH to engineer active sites and optimize interfacial energetics.Additionally,the negative shift of Ru_(0.51)-CoFe-LDH band edge gives rise to more conspicuous band bending of the n-n junction formed with BiVO_(4),expediting the separation and transfer of photogenerated electron-hole pairs at the interface.This work furnishes a new preparation perspective for PEC water splitting systems to construct single atoms in the semiconductor substrate.
基金supported by the Jiangsu Province Traditional Chinese Medicine Technology Development Plan Project,Nos.MS2023113(to JC),MS2022090Young and Middle-aged Academic Leaders of Jiangsu Qing-Lan Project(to GL).
文摘Unlike mammals,zebrafish possess a remarkable ability to regenerate their spinal cord after injury,making them an ideal vertebrate model for studying regeneration.While previous research has identified key cell types involved in this process,the underlying molecular and cellular mechanisms remain largely unexplored.In this study,we used single-cell RNA sequencing to profile distinct cell populations at different stages of spinal cord injury in zebrafish.Our analysis revealed that multiple subpopulations of neurons showed persistent activation of genes associated with axonal regeneration post injury,while molecular signals promoting growth cone collapse were inhibited.Radial glial cells exhibited significant proliferation and differentiation potential post injury,indicating their intrinsic roles in promoting neurogenesis and axonal regeneration,respectively.Additionally,we found that inflammatory factors rapidly decreased in the early stages following spinal cord injury,creating a microenvironment permissive for tissue repair and regeneration.Furthermore,oligodendrocytes lost maturity markers while exhibiting increased proliferation following injury.These findings demonstrated that the rapid and orderly regulation of inflammation,as well as the efficient proliferation and redifferentiation of new neurons and glial cells,enabled zebrafish to reconstruct the spinal cord.This research provides new insights into the cellular transitions and molecular programs that drive spinal cord regeneration,offering promising avenues for future research and therapeutic strategies.
基金supported by the National Natural Science Foundation of China(Nos.22422806,22378136,and 22138003)the Guangdong Pearl River Talents Program(Nos.2021QN02C847and 2021ZT09Z109)+4 种基金the Natural Science Foundation of Guangdong Province(Nos.2024A1515011196 and 2023B1515040005)the Fundamental Research Funds for the Central Universities(Nos.2024ZYGXZR011,2025ZYGXZR025)the Science and Technology Program of Guangzhou(No.2025A04J5244)the State Key Laboratory of Pulp and Paper Engineering(No.2024ZD09)the TCL Young Talent Program。
文摘The breaking of the symmetric electronic distribution of single-atom catalysts is effective in improving the intrinsic activity.However,traditional modification strategies can only disrupt the electronic distribution in one dimension,resulting in limited regulation of electronic structure.Herein,we report a multidimensional coordination strategy to significantly break the symmetrical electron distribution of the metal single site to achieve highly efficient electrochemical CO_(2) reduction reaction(CO_(2) RR).Ni singleatom sites decorated with planar P and axial Cl atoms are successfully constructed on carbon support(Ni-NPCl-C).Ni-NPCl-C affords CO Faraday efficiency over 90%in a wide potential window range from-0.5 to-1.2 V and an ultrahigh turnover frequency of 1.17×10^(5)h^(-1),much superior to its counterparts with single-dimensional coordination.Ni-NPCl-C can be further applied as a bifunctional catalyst to construct a rechargeable Zn-CO_(2) battery.Spectroscopic characterizations and theoretical calculations demonstrate that the dual adjustments with axial Cl and planar P can synergistically disrupt the electron distribution in two dimensions to increase electrons around Ni sites with the upshift of the d-band center,thereby facilitating the formation of*COOH intermediates and improving the CO_(2) RR performance.
基金supported by the National Key Research and Development Program of China(Grant Nos.2024YFA1611100,2023YFA1406100,and 2018YFA0704201)the Systematic Fundamental Research Program Leveraging Major Scientific and Technological Infrastructure,Chinese Academy of Sciences(Grant No.JZHKYPT-2021-08)+1 种基金the National Natural Science Foundation of China(Grant Nos.11704385,11874359,and 12274444)the Strategic Priority Research Program(B)of the Chinese Academy of Sciences(Grant No.XDB25000000)。
文摘Temperature-dependent resistivity,upper critical field H_(c2)and its anisotropy in overdoped superconducting Ba_(1-x)K_x Fe_2As_2(x=0.6-1)single crystals have been measured in steady magnetic fields up to 44 T and low temperatures down to 0.4 K.Analysis using both the quadratic term and power-law fitting demonstrates that the in-plane resistivityρ_(ab)(T)progressively approaches the Fermi-liquid T~2behavior with increasing K doping and reaches a saturation plateau at x≈0.8.The temperature dependence of both H_(c2)^(ab)and H^(c)_(c2)follows the Werthamer-Helfand-Hohenberg model,incorporating orbital and spin paramagnetic effects.For x≤0.8,the orbital effect dominates for H ab,while the Pauli paramagnetic effect prevails for H c.For x>0.8,the Pauli paramagnetic effect becomes dominant in both crystallographic directions.The anisotropy of H_(c2)(0)exhibits a discontinuity in its dependence on K doping concentration with a significant enhancement at x=0.8 and a maximum at x=0.9.These experimental results indicate that the electron correlation effect is enhanced in the heavily overdoped Ba_(1-x)K_(x)Fe_(2)As_(2)system where the underlying symmetries are broken due to the Fermi surface reconstruction before x=0.9.
基金financially supported by the National Oversea Postdoctoral Talent Attraction Programthe Pilot Group Program of the Research Fund for International Senior Scientists(52350710795)+2 种基金the Youth Fund of the National Natural Science Foundation of China(52402288)the Young Elite Scientists Sponsorship Program by China Association for Science and Technology(YESS20230183)the Yangfan Special Program of Shanghai Star Project(24YF2729700)。
文摘Defect engineering serves as a cornerstone in the design of high-effciency single-atom catalysts(SACs)for advanced electrocatalytic systems.This study demonstrates oxygen vacancy-induced near-zero-valent Pt SACs anchored on TiO2 for efficient hydrogen evolution reaction(HER).Synchrotron spectroscopy and density functional theory calculation reveal that oxygen vacancies create unconventional Pt-Ti coordination while strengthening electronic metal-support interactions.This facilitates substantial electron transfer from TiO2 to Pt,generating a near-zero-valent Pt state with elevated electron density.The modified electronic structure lowers the Pt d-band center,reducing hydrogen intermediate(*H)adsorption energy and optimizing HER kinetics.Moreover,ab initio molecular dynamics and in situ Raman spectra show that the negative charge accumulated at the Pt site promotes K^(+)enrichment at the interface,which enhances H-OH bond polarization and accelerates water dissociation kinetics.The resulting D-TiO_(2)/Pt SACs exhibit superior HER activity across acidic,neutral,and alkaline conditions,achieving low overpotentials of 40,57,and 60 mV at 10 mA cm^(-2),respectively.Additionally,its mass activities at the overpotential of 100 mV are 10.3,33.9,and 20.9 times higher that of Pt/C,respectively.This study shows the key role of defectmediated electronic engineering in tailoring SACs'valence states and catalytic functions,advancing sustainable hydrogen production through rational catalyst design.
