The severe shuttle effect and sluggish reaction kinetics in room-temperature sodium-sulfur(RT Na-S)batteries have been major bottlenecks hindering their practical application.To overcome these challenges,a straightfor...The severe shuttle effect and sluggish reaction kinetics in room-temperature sodium-sulfur(RT Na-S)batteries have been major bottlenecks hindering their practical application.To overcome these challenges,a straightforward reduction approach was employed to design three bimetallic alloy nanoparticles(FeNi,FeCo,and NiCo)supported on multistage porous carbon substrates.Experimental and theoretical calculations reveal that the charge transfer within the alloy catalyst influences the position of its d-band center and its degree of hybridization with sodium polysulfides(NaPSs).An increased charge transfer leads to a shift of the alloy’s d-band center closer to the Fermi energy level,thereby enhancing its adsorption and catalytic capabilities.Among the three alloy compositions,the FeNi alloy exhibits the highest charge transfer.Consequently,the FeNi alloy demonstrates the superior electrochemical performance,achieving a high reversible specific capacity of 848.2 mA h g^(−1),with an average capacity degradation rate of only 0.037%per cycle over 1000 cycles at 1.2 C.The S/FeNi/NC cathode exhibits a low electrolyte-to-sulfur(E/S)ratio of 6.6µL mg^(−1),while maintaining a high reversible specific capacity of 568.1 mA h g^(−1).This offers valuable insights for the application of alloy catalysts in the S/FeNi/NC cathode of RT Na-S batteries.展开更多
Fluorescent probes based on intramolecular charge transfer(ICT) have obvious advantages for accurate quantitative analysis.To obtain high-performance ratiometric probes requires distinct photophysical properties durin...Fluorescent probes based on intramolecular charge transfer(ICT) have obvious advantages for accurate quantitative analysis.To obtain high-performance ratiometric probes requires distinct photophysical properties during recognition reaction process,which is closely related to their ICT characteristics.1,8-Naphthalimide is known as a typical fluorophore with desirable ICT property when functionalized with an electron-donating moiety at the para-position of the naphthalene chromophore.Although the photophysical properties of para-substituted 1,8-naphthalimide have been well studied,its meta-substituted counterpart has not been fully evaluated since the meta-position is conventionally thought to be weakly conjugated.Herein,combined experimental and theoretical studies are performed which consistently indicate that stronger charge transfer(CT) is exhibited by the meta-amino substituted 1,8-naphthalimide(m-NH_(2)) compared to the para-amino substituted one(p-NH_(2)).The ratiometric response of fluorescence with significant changes in wavelength and intensity upon acetylation(m-NAc and p-NAc) can be attributed to the larger ICT and stronger-NH_(2) vibrations.This observation is further demonstrated by deuterium oxide experiments,viscosity experiments and quantum chemical calculations.The practical application of meta-amino-1,8-naphthalimide ICT-based probes is also confirmed.This research is expected to bring an in-depth understanding of π-conjugated systems with ICT characteristics,and facilitates the design of sensitive ICT fluorescent probes with meta-amino substitution.展开更多
The longitudinal π-extension of carbon nanohoops is one of the most effective bottom-up synthetic strategies toward carbon nanotubes(CNTs).Herein,the precise synthesis of a multi-substituted carbon nanohoop([12]CPP-8...The longitudinal π-extension of carbon nanohoops is one of the most effective bottom-up synthetic strategies toward carbon nanotubes(CNTs).Herein,the precise synthesis of a multi-substituted carbon nanohoop([12]CPP-8PBPy)based on cycloparaphenylenes(CPPs)grafted with eight pyrene-functionalized units was reported.This structurally well-defined nanohoop not only acts as a segment of armchair-type CNTs but also achieves enhanced longitudinal π-extension.The structure of[12]CPP-8PBPy was confirmed by high-resolution mass spectrometry(HRMS)and nuclear magnetic resonance(NMR).The photophysical properties were studied by UV/Vis and photoluminescence spectroscopy.The potential applications of[12]CPP-8PBPy in electron-transport devices were further investigated.展开更多
Dear Editor,Idiopathic orbital inflammation(IOI),also known as orbital inflammatory pseudotumor,is a relatively common orbital disorder[1].Its pathogenesis remains unclear,often regarded as a nonspecific immune-mediat...Dear Editor,Idiopathic orbital inflammation(IOI),also known as orbital inflammatory pseudotumor,is a relatively common orbital disorder[1].Its pathogenesis remains unclear,often regarded as a nonspecific immune-mediated response[2].IOI presents with symptoms such as pain,photophobia,proptosis,eyelid swelling,edema,conjunctival congestion,and diplopia,with possible vision loss occurring in some cases.Based on the soft tissue structures involved,IOI can be classified into subtypes such as myositis,optic neuritis,dacryoadenitis,diffuse orbital inflammation,and orbital inflammatory masses[2].展开更多
The problem of maneuvering for a servicing spacecraft(inspector)to inspect a noncooperative spacecraft(evader)in cislunar space is investigated in this paper.The evader,which may be a malfunctioning or uncontrolled sa...The problem of maneuvering for a servicing spacecraft(inspector)to inspect a noncooperative spacecraft(evader)in cislunar space is investigated in this paper.The evader,which may be a malfunctioning or uncontrolled satellite,introduces uncertainties due to its potential maneuvering capabilities.To address this challenge,the scenario is modeled as a special orbital game,incorporating the unique complexities of the cislunar environment.A variable-duration,turn-based inspection and anti-inspection game model is designed.The model defines both players'rules,constraints,and victory conditions,providing a framework for non-cooperative inspection.Strategies for both players are developed and validated based on their dynamical properties.The inspector's strategy integrates two-body Lambert transfers with shooting methods,while the evader's strategy aims to maximize the inspector's fuel consumption.Simulation results show that the evader's optimal strategy involves deliberate fluctuations in its lunar periapsis altitude,with the inspector's requiredΔV up to eight times greater than the evader's.The impact of game constraints is evaluated,and the effectiveness of deploying the inspector in low lunar orbit is compared with the inspector at the Earth-Moon Lagrange point L1.The strengths and weaknesses of both are shown.These findings provide valuable insights for future orbital servicing and orbital games.展开更多
In a superconductor embedded with a quantum magnetic impurity,the Kondo effect is involved,leading to the competition between the Kondo singlet phase and the superconductivity phase.By means of the natural orbitals re...In a superconductor embedded with a quantum magnetic impurity,the Kondo effect is involved,leading to the competition between the Kondo singlet phase and the superconductivity phase.By means of the natural orbitals renormalization group(NORG)method,we revisit the problem of a quantum magnetic impurity coupled with a conventional s-wave superconductor.Here we present a detailed study focusing on the impurity spin polarization and susceptibility,the Kondo screening cloud,as well as the number and structures of the active natural orbitals(ANOs).In the superconducting phase,the impurity spin is partially polarized,indicating that the impurity remains partially screened by the quantum fluctuations.Furthermore,the impurity spin susceptibility becomes divergent,resulting from the presence of residual local moment formed at the impurity site.Correspondingly,a non-integral(incomplete)Kondo cloud is formed,although the ground state is a spin doublet in this phase.In comparison,the Kondo cloud is complete in the Kondo singlet phase as expected.We also quantify the critical point,where the quantum phase transition from a Kondo singlet phase to a superconducting phase occurs,which is consistent with that in previous works.On the other hand,it is illustrated that only one ANO emerges in both quantum phases.The structures of the ANO,projected into both the real space and momentum space,are distinct in the Kondo singlet phase from that in the superconducting phase.More specifically,in the Kondo singlet phase,the ANO keeps fully active with half-occupied,and the superconducting gap has negligible influence on its structure.On the contrary,in the superconducting phase,the ANO tends to be inactive and its structure changes significantly as the superconducting gap increases.Additionally,our investigation demonstrates that the NORG method is reliable and convenient to solve the quantum impurity problems in superconductors as well,which will promote further theoretical studies on the Kondo problems in such systems using numerical methods.展开更多
A deep neural network(DNN)was developed to accurately predict the nuclear charge density distributions for nuclei with proton numbers Z≥8.By incorporating essential nuclear structure features,the model achieved a sig...A deep neural network(DNN)was developed to accurately predict the nuclear charge density distributions for nuclei with proton numbers Z≥8.By incorporating essential nuclear structure features,the model achieved a significant improvement in predictive accuracy over conventional methods.The charge density distributions were analyzed using a Fourier-Bessel(FB)series expansion,and the DNN was trained on a comprehensive dataset derived from relativistic continuum Hartree-Bogoliubov(RCHB)theory calculations.The model demonstrated exceptional performance,with root-mean-square deviations of 0.0123fm and 0.0198 fm for the charge radii on the training and validation sets,respectively,which remarkably surpassed the precision of the original RCHB calculations.In addition to advancing nuclear physics research,this high-precision model provides critical data for applications in atomic physics,nuclear astrophysics,and related fields.展开更多
In order to investigate the penetration performance of Linear-Shaped Charge(LSC),Embowed LinearShaped Charge(ELSC),and Embowed Linear Explosively Formed Projectile(ELEFP)on T-shaped stiffened plates,a series of near-f...In order to investigate the penetration performance of Linear-Shaped Charge(LSC),Embowed LinearShaped Charge(ELSC),and Embowed Linear Explosively Formed Projectile(ELEFP)on T-shaped stiffened plates,a series of near-field air-burst experiments are conducted.The damage modes and characteristics of the target plates are compared and analyzed.Each flat plate section is completely punctured,resulting in a penetration hole.The damage modes induced by the three charge types on the stiffened plate structure are consistent,characterized by shear failure in the central region of the flat plate due to penetration by the penetrator,localized plastic deformation of the flat plate,and local penetration failure resulting from partial perforation of the central stiffener.The penetration lengths caused by ELSC and ELEFP are 45.1%and 46.1% larger than that of LSC,while the half-width of the penetration hole generated by ELEFP is 54.2% and 24.7% smaller than that of ELSC and LSC,respectively.The penetration height caused by ELEFP are 17.5%and 62.1% larger than that of ELSC and LSC,respectively.The stiffener effectively segments the damage area,enhancing the local structural strength and limiting the extent of plastic deformation in the flat plate section.The comparative results show that the ELSC proves to be more effective for efficient large-scale damage,and ELEFP is more suitable for achieving efficient localized damage.展开更多
AIM:To investigate the clinical features and prognosis of patients with orbital inflammatory myofibroblastic tumor(IMT).METHODS:This retrospective study collected clinical data from 22 patients diagnosed with orbital ...AIM:To investigate the clinical features and prognosis of patients with orbital inflammatory myofibroblastic tumor(IMT).METHODS:This retrospective study collected clinical data from 22 patients diagnosed with orbital IMT based on histopathological examination.The patients were followed up to assess their prognosis.Clinical data from patients,including age,gender,course of disease,past medical history,primary symptoms,ophthalmologic examination findings,general condition,as well as imaging,laboratory,histopathological,and immunohistochemical results from digital records were collected.Orbital magnetic resonance imaging(MRI)and(or)computed tomography(CT)scans were performed to assess bone destruction of the mass,invasion of surrounding tissues,and any inflammatory changes in periorbital areas.RESULTS:The mean age of patients with orbital IMT was 28.24±3.30y,with a male-to-female ratio of 1.2:1.Main clinical manifestations were proptosis,blurred vision,palpable mass,and pain.Bone destruction and surrounding tissue invasion occurred in 72.73%and 54.55%of cases,respectively.Inflammatory changes in the periorbital site were observed in 77.27%of the patients.Hematoxylin and eosin staining showed proliferation of fibroblasts and myofibroblasts,accompanied by infiltration of lymphocytes and plasma cells.Immunohistochemical staining revealed that smooth muscle actin(SMA)and vimentin were positive in 100%of cases,while anaplastic lymphoma kinase(ALK)showed positivity in 47.37%.The recurrence rate of orbital IMT was 27.27%,and sarcomatous degeneration could occur.There were no significant correlations between recurrence and factors such as age,gender,laterality,duration of the disease,periorbital tissue invasion,bone destruction,periorbital inflammation,tumor size,fever,leukocytosis,or treatment(P>0.05).However,lymphadenopathy and a Ki-67 index of 10%or higher may be risk factors for recurrence(P=0.046;P=0.023).CONCLUSION:Orbital IMT is a locally invasive disease that may recur or lead to sarcomatoid degeneration,primarily affecting young and middle-aged patients.The presence of lymphadenopathy and a Ki-67 index of 10%or higher may signify a poor prognosis.展开更多
AIM:To define the prevalence and anatomical patterns of paranasal sinus abnormalities(PSA)in thyroid-associated ophthalmopathy(TAO)and to test the hypothesis that TAO is partially driven by contiguous orbital inflamma...AIM:To define the prevalence and anatomical patterns of paranasal sinus abnormalities(PSA)in thyroid-associated ophthalmopathy(TAO)and to test the hypothesis that TAO is partially driven by contiguous orbital inflammation rather than systemic autoimmunity or generalized orbital pressure.METHODS:Data included ophthalmic assessments and a panel of thyroid function and autoimmune biomarkers.Blinded radiological analysis of orbital computed tomography(CT)scans was performed to quantify sinus abnormalities and extraocular muscles(EOMs)involvement.Patients were categorized into two groups based on CT findings,those with no radiological evidence of sinus abnormalities(non-PSA control group)and those with identifiable PSA.Furthermore,ethmoid sinus mucosal biopsies from a subset of TAO patients and noninflammatory controls were subjected to histopathological analysis.RESULTS:Totally 121 TAO patients(mean age 42.4±12.8y,range 10-78y),male:female=42:79,were included.PSA was identified in 44.6%(n=54)of patients,with a distribution anatomically restricted to the maxillary(50.0%isolated)and ethmoid sinuses(18.5%isolated;29.6%combined).Compared to the non-PSA group(n=67),patients with PSA were significantly older(45.1±11.8 vs 40.3±13.2y;P=0.040)and were more likely to be male(55.6%vs 17.9%;P<0.001).They also had significantly higher proptosis(22.1±3.2 vs 20.7±2.9 mm;P<0.001).Medial/inferior rectus involvement was most frequent(88.4%vs 89.3%).Histopathological analysis of sinus mucosa from PSA patients provided direct evidence of pathology,revealing a dense,chronic lymphoplasmacytic infiltrate and submucosal edema,validating the radiological findings as a true inflammatory process.No significant correlation was found with systemic autoimmune markers,including thyroid-stimulating hormone(TSH)receptor antibodies(TRAb,median 4.86 vs 2.71 IU/L,P=0.104).CONCLUSION:TAO is associated with a high prevalence of PSA in a pattern consistent with the orbital anatomy.The correlation with ipsilateral muscle thickening combined with the lack of association with proptosis laterality or systemic biomarkers lend strong support to a model of contiguous inflammation over systemic autoimmunity,a hypothesis that warrants further validation through longitudinal and mechanistic studies.展开更多
To advance the theoretical understanding,technological development,and field application of electric charge induction for monitoring rock deformation and failure,this study investigates the induced electric charge gen...To advance the theoretical understanding,technological development,and field application of electric charge induction for monitoring rock deformation and failure,this study investigates the induced electric charge generated during the deformation and failure of igneous rocks.The charge originates mainly from a combination of electrical polarization and triboelectric effects.Through laboratory experiments,we analyzed the time-frequency evolution of induced electric charge signals and identified relevant monitoring parameters.An online downhole electric charge induction monitoring system was developed and validated in the field.Experimental results show that the dominant frequency range of induced electric charge signals generated during igneous rock deformation and failure lies between 0 and 23 Hz,and a low-pass finite impulse response(FIR)filter effectively suppresses noise.Optimal sensor distances for monitoring cubic and cylindrical specimens were determined to be 17 mm and 13 mm,respectively.We proposed early warning indicators,including the maximum absolute value of the induced electric charge,the arithmetic mean value,the distribution dispersion coefficient,and the cumulative sum value.In field application,time-domain curves and spatial distribution charts of these warning indicators correspond well with changes in abutment stress ahead of the mining face,offering indirect insights into local stress evolution.This research provides technical and equipment support for the application of electric charge induction technology to monitoring and early warning of coal bursts.展开更多
The design and fabrication of ordered epitaxial MOF-on-MOF heterostructures as highly efficient electrocatalysts for water splitting is crucial but still challenging.In this study,a simple coordination-driven self-ass...The design and fabrication of ordered epitaxial MOF-on-MOF heterostructures as highly efficient electrocatalysts for water splitting is crucial but still challenging.In this study,a simple coordination-driven self-assembly method is used to fabricate controllable MOF-on-MOF multiscale heterostructures,where triangular host MOF(ZIF-67)nanosheets undergo in situ epitaxial growth to form uniform orthogonal vip MOF(CoFe PBA)nanosheets.Phosphorus(P)is further introduced in situ to fabricate CoP and Fe_(2)P heterostructured nanosheets(CoFe-P-NS),which exhibit excellent bifunctional electrocatalytic performance due to the enhancement of intrinsic electrocatalytic activity by p-d orbital hybridization.Specifically,the CoFe-P-NS requires low overpotential of 259 and 307 mV to reach 500 mA cm−2 for HER and OER,respectively.Remarkably,the assembled electrolysis cell maintained a large current density of 300 mA cm−2 for over 360 h with negligible voltage increase during alkaline seawater electrolysis.Experiments and theoretical calculations show that the synergistic catalytic activity of bimetallic phosphides arises from p-d orbital hybridization,where the CoP-P sites enhance HER by optimizing H*adsorption in the Volmer-Heyrovsky steps,while the Fe_(2)P-Fe sites accelerate OER by lowering the energy barrier of the rate-determining step from O*to OOH*.This study provides valuable insights into the design of a controllable MOF-on-MOF-based electrocatalyst toward alkaline seawater splitting.展开更多
To address the key scientific challenge of monitoring the dynamic fracturing of surrounding rock in deep roadways,this study systematically investigates the quantitative relationship between stress and charge signals ...To address the key scientific challenge of monitoring the dynamic fracturing of surrounding rock in deep roadways,this study systematically investigates the quantitative relationship between stress and charge signals during coal mass loading.By integrating innovative analytical approaches,introducing quantitative evaluation indices,and developing a charge–stress inversion model,and incorporating underground monitoring practices,significant progress has been achieved in elucidating the correlation between stress variations and charge signals throughout the entire coal mass fracturing process.First,in the field of stress–charge correlation analysis,empirical mode decomposition(EMD)was combined with wavelet coherence analysis for the first time,enabling the removal of slow-varying stress trends while retaining high-frequency fluctuations.This approach allowed for the quantitative characterization of the evolution of coherence between stress variations and charge fluctuations across multiple time scales.Second,coherence skewness and the proportion of high-coherence intervals were innovatively introduced to examine the influence of time scale selection on correlation results.On this basis,a criterion for determining the near-optimal observation scale of charge signals was proposed,providing a quantitative reference for time scale selection in similar signal analyses.Finally,by correlating charge signals with coal damage factors and stress states,a charge-based damage evolution equation was established to achieve effective stress inversion.Combined with in situ monitoring of stress and charge in roadway surrounding rock,this approach revealed the correlation characteristics of stress and charge intensity responses during the dynamic fracturing process.The results indicate,first,that charge signals are not significantly correlated with the absolute stress level of coal but are directly associated with stress variations following coal damage and failure,with the amplitude of charge fluctuations increasing alongside stress fluctuations.Second,coherence between stress and charge signals varies markedly across time scales,with excessively small or large scales leading to distortion,and the scale corresponding to the peak proportion of intervals with coherence>0.8 was identified as the near-optimal observation scale.Third,charge signals can effectively characterize coal damage factors,and the established damage evolution equation can effectively invert stress variation trends.Fourth,in underground roadways,zones of dynamic fracturing in surrounding rock are commonly located in areas where stress concentration overlaps with regions of high charge intensity,further confirming the strong consistency between charge and stress variations.These findings improve the theoretical framework of charge signal responses in loaded coal and provide a scientific basis for precise“stress-charge”monitoring of dynamic disasters,offering practical potential for engineering applications.展开更多
Lithium-sulfur(Li-S)batteries hold great promise for high-energy–density energy storage applications but are plagued by the severe shuttle effect and sluggish conversion kinetics of lithium polysulfides(Li PSs).We he...Lithium-sulfur(Li-S)batteries hold great promise for high-energy–density energy storage applications but are plagued by the severe shuttle effect and sluggish conversion kinetics of lithium polysulfides(Li PSs).We herein report a d-p-f orbital coupling strategy to tackle these critical challenges by incorporating Eu 4f orbitals to activate both metallic(Ni)and non-metallic(Se)sites of Ni Se.The imported Eu atoms could induce essential Ni 3d and Se 4p orbital reconstruction through gradient d-p-f coupling,thereby optimizing the band center alignment between Ni Se and Li PSs.Such electronic reconstruction strengthens both d-p hybridization between Ni and Li PSs and s-p hybridization between Se and Li PSs,which can not only enhance the chemisorption affinity toward Li PSs but also accelerate interfacial charge transfer kinetics,leading to suppressed shuttle effect and boosted Li PSs conversion kinetics.Therefore,the Li-S batteries assembled with Eu incorporated Ni Se deliver exceptional electrochemical performance with a high specific capacity of 896.2 m Ah g^(-1)at 4 C and a retained areal capacity of 5.66 m Ah cm^(-2)under a high sulfur loading of 5.94 mg cm^(-2)after 100 cycles.This work underscores the critical role of rare-earth 4f orbital coupling for modulating the active sites to construct high-efficiency electrocatalysts for Li-S batteries and beyond.展开更多
The penetration of shaped charge jets into targets at high velocities is significantly influenced by the compressibility effect,while at low velocities,the strength effect becomes predominant.In the latter regime,mate...The penetration of shaped charge jets into targets at high velocities is significantly influenced by the compressibility effect,while at low velocities,the strength effect becomes predominant.In the latter regime,material strength dictates the resistance to plastic deformation and flow,a contrast to the shockwave-dominated interactions where compressibility is key.This paper presents a self-consistent compressible penetration theory that considers both the axial penetration and radial crater growth of shaped charge jets into targets.An integrated approach where the axial and radial dynamics are coupled has been proposed,influencing each other through shared physical principles rather than being treated as separate,empirically linked phenomena.The presented theory is rooted in the compressible Bernoulli equation and the linear Rankine-Hugoniot relation.These foundational equations are employed to accurately model the high-pressure shock state and subsequent material flow at the jet-target interface,providing a robust physical basis for the penetration model.Notably,it considers the target material's compressibility,which elevates the pressure at the jet-target interface beyond that observed with incompressible materials.This pressure increase is directly proportional to the target's degree of compressibility.As such,this model of compressible penetration reorients the analytical approach:rather than merely estimating penetration resistance,it determines this value from the target material's specific compressibility and yield strength.This shift from empirical correlations to a physics-based derivation of penetration resistance enhances the model's predictive power,particularly for novel target materials or engagement conditions outside established experimental datasets.This investigation establishes a quantitative link between the material's yield strength and its penetration resistance.The accuracy of this penetration resistance value is paramount,as it significantly influences the predicted crater diameter;indeed,the crater diameter's sensitivity to this resistance underscores the necessity for its precise determination.Ultimately,by integrating the yield strength of the target material,this framework enables the prediction of both the penetration depth and the resultant crater diameter from a shaped charge jet.The theory's validation involved two experimental sets:the first focused on shaped charge jet penetration into 45#steel at varied stand-offs,while the second utilized targets of high-to ultrahigh-strength steel-fiber reactive powder concrete(RPC)with differing strength characteristics.These experimental campaigns were specifically chosen to test the theory against both ductile metallic alloys,where plastic flow is significant,and advanced quasi-brittle cementitious composites,presenting a broad spectrum of material responses and penetration challenges.Resulting hole profiles derived from theoretical calculations demonstrated a strong correspondence with empirical measurements for both material types.展开更多
Based on the idea of treating the anti de Sitter(AdS)radius as a fixed parameter,we study the thermodynamics and topology of d-dimensional charged AdS black holes in the restricted phase space utilizing Visser's h...Based on the idea of treating the anti de Sitter(AdS)radius as a fixed parameter,we study the thermodynamics and topology of d-dimensional charged AdS black holes in the restricted phase space utilizing Visser's holographic approach.For the charged black hole with a cloud of strings and quintessence in the higher-dimensional spacetimes with d=(4,5,6),we demonstrate that the topological number remains invariant within the same canonical ensemble;however,a distinct topological number emerges in the grand canonical ensemble for the same black hole system.Notably,these results are independent of the dimension d and other related parameters.The formalism known as restricted phase space thermodynamics is checked in detail and some interesting thermodynamic behavior is revealed in the example case of d-dimensional charged AdS black holes with a cloud of strings and quintessence.This research lays the foundation for establishing a universal framework of restricted phase space thermodynamics and investigating its fundamental thermodynamic properties.展开更多
Oxygen evolution reaction(OER)is widely recognized as a bottleneck of water electrolysis.To determine the underlying reaction mechanisms,particularly the relative contribution of the adsorbate evolution mechanism(AEM)...Oxygen evolution reaction(OER)is widely recognized as a bottleneck of water electrolysis.To determine the underlying reaction mechanisms,particularly the relative contribution of the adsorbate evolution mechanism(AEM)and lattice-oxygen participation mechanism(LOM),we conduct a comprehensive investigation combining Density Functional Theory(DFT)calculations and experimental validation.Our theoretical analysis of doped RuO_(2)catalysts reveals that heteroatom doping(Ni,Cu,and Zn)induces significant local charge transfer,leading to the increased charge state of Ru and the downshifted d-band center.This,in turn,enables the mechanism switching from the conventional AEM to the more efficient LOM,and finally improves OER activity.We also establish a simple yet powerful descriptor,Ne of Ru(representing charge density of Ru sites),which enables accurate prediction of both catalytic activity and stability.Guided by these theoretical predictions,we successfully synthesize a Ni-doped RuO_(2)catalyst,which exhibits excellent OER activity and stability in acidic media,achieving an overpotential of just 156 mV and maintaining stability for 4000 h at 10 mA cm^(−2),significantly surpassing the performance of the commercial RuO_(2).These findings not only provide fundamental insights into the mechanism-switching behavior in OER catalysis but also offer a practical strategy for designing high-performance,stable electrocatalysts for acidic water electrolysis.展开更多
Hard carbon is a vital anode material for sodium-ion batteries;however,the nonuniform growth of solid electrolyte interphase(SEI)film substantially diminishes its initial coulombic efficiency(ICE)and cycle life.The ch...Hard carbon is a vital anode material for sodium-ion batteries;however,the nonuniform growth of solid electrolyte interphase(SEI)film substantially diminishes its initial coulombic efficiency(ICE)and cycle life.The chemical and morphological properties of surface highly influence the electrode/electrolyte interfacial reactions.In this study,we have tuned orbital hybridization states forming an interface enriched with sp^(2) hybridized carbon(sp^(2)-C),which decreases the binding energy to solvent molecules and inhibits excessive solvent decomposition during SEI formation.Benefiting from successfully constructed inorganic-rich SEI,the ICE increased to 91%and sodium storage capacity reached 346 mAh/g.Besides,the capacity retention rate was 90.7%after 700 cycles at 1 A/g higher than pristine electrode(83.8%).展开更多
Deep mining of natural resources,like coal,is increasingly utilizing directional blasting technology with slit charge for rock blasting at greater depths.This study,based on numerical simulation methods,analyzes the d...Deep mining of natural resources,like coal,is increasingly utilizing directional blasting technology with slit charge for rock blasting at greater depths.This study,based on numerical simulation methods,analyzes the dynamic behavior of slit charge blasting in three aspects:slit tube dynamic response,hoop stress evolution,and crack propagation.According to research findings,the failure mode of the slit tube mainly manifests as a tensile fracture of the inner wall and a shear fracture at the end connection,where the end connection of the slit tube is the weak point of the overall structure.The dynamic response of the slit tube mainly exhibits radial response in the vertical direction of the slit and hoop response in the slit direction.The hoop tensile stress plays a crucial role in determining the spread of cracks caused by explosions.As the in situ stress increases,the peak hoop tensile stress reduces,and the peak hoop compressive stress increases.This hinders the propagation of cracks.In addition,the directional impact is most pronounced in the middle of the borehole,with the longest primary directional crack observed.Conversely,the directional impact is least favorable near the bottom of the borehole.When the in situ stress reaches 60MPa,the purpose of directional fracture has not been achieved,suggesting combining presplit blasting for in situ stress relief to improve rock breaking efficiency.展开更多
Membra ne electrode assemblies(MEAs)are pivotal to advancing proton exchange membra ne water electrolysis(PEMWE),yet conventional designs suffer from limited triple-phase boundaries(TPBs),inefficient mass/charge trans...Membra ne electrode assemblies(MEAs)are pivotal to advancing proton exchange membra ne water electrolysis(PEMWE),yet conventional designs suffer from limited triple-phase boundaries(TPBs),inefficient mass/charge transport,and insufficient durability.This study introduces a three-dimensional ordered pattern-array(3D OPA)architecture fabricated via a scalable laser-machined mask and hot-pressing strategy.The 3D OPA MEA achieves a current density of 3.73 A cm^(-2) at 2 V,demonstrating a 50%performance improvement over the conventional MEA(2.48 A cm^(-2)),alongside a degradation rate of 26.6μV h^(-1) in a highly dynamic accelerated stress test(AST).Additionally,numerical simulations corroborate that the OPA architecture optimizes localized oxygen diffusion and liquid water replenishment,enhancing reaction kinetics.The 3D OPA architecture enhances TPBs and establishes optimized gas-liquid tra nsport pathways,significantly improving catalyst utilization while minimizing mass transfer overpotential and bubble-induced losses.Furthermore,its interlocking design reinforces mechanical interactions,reducing ohmic resistance a nd ensuring sustained mecha nical integrity and electrochemical durability.This work provides a simple,cost-effective,and scalable approach for patterned MEAs,addressing critical barriers to PEMWE commercialization through rational TPB engineering and transport pathway optimization.展开更多
基金supported by Shaanxi Fundamental Science Research Project for Chemistry and Biology(23JHQ011)Natural Science Foundation of Shaanxi(2024JC-YBMS-115)Natural Science Basic Research Plan in Shaanxi Province of China(2025JC-YBMS-141)。
文摘The severe shuttle effect and sluggish reaction kinetics in room-temperature sodium-sulfur(RT Na-S)batteries have been major bottlenecks hindering their practical application.To overcome these challenges,a straightforward reduction approach was employed to design three bimetallic alloy nanoparticles(FeNi,FeCo,and NiCo)supported on multistage porous carbon substrates.Experimental and theoretical calculations reveal that the charge transfer within the alloy catalyst influences the position of its d-band center and its degree of hybridization with sodium polysulfides(NaPSs).An increased charge transfer leads to a shift of the alloy’s d-band center closer to the Fermi energy level,thereby enhancing its adsorption and catalytic capabilities.Among the three alloy compositions,the FeNi alloy exhibits the highest charge transfer.Consequently,the FeNi alloy demonstrates the superior electrochemical performance,achieving a high reversible specific capacity of 848.2 mA h g^(−1),with an average capacity degradation rate of only 0.037%per cycle over 1000 cycles at 1.2 C.The S/FeNi/NC cathode exhibits a low electrolyte-to-sulfur(E/S)ratio of 6.6µL mg^(−1),while maintaining a high reversible specific capacity of 568.1 mA h g^(−1).This offers valuable insights for the application of alloy catalysts in the S/FeNi/NC cathode of RT Na-S batteries.
基金financially supported by National Key Research and Development Programs (Nos.2022YFD1700403 and 2023YFD1700303)National Natural Science Foundation of China (Nos.12274128 and 12250003)+2 种基金Shanghai Rising-Star Program (No.21QA1402600)the support of NYU-ECNU Center for Computational Chemistry at NYU Shanghaithe University of Bath and the Open Research Fund of the School of Chemistry and Chemical Engineering,Henan Normal University (No.2020ZD01) for support。
文摘Fluorescent probes based on intramolecular charge transfer(ICT) have obvious advantages for accurate quantitative analysis.To obtain high-performance ratiometric probes requires distinct photophysical properties during recognition reaction process,which is closely related to their ICT characteristics.1,8-Naphthalimide is known as a typical fluorophore with desirable ICT property when functionalized with an electron-donating moiety at the para-position of the naphthalene chromophore.Although the photophysical properties of para-substituted 1,8-naphthalimide have been well studied,its meta-substituted counterpart has not been fully evaluated since the meta-position is conventionally thought to be weakly conjugated.Herein,combined experimental and theoretical studies are performed which consistently indicate that stronger charge transfer(CT) is exhibited by the meta-amino substituted 1,8-naphthalimide(m-NH_(2)) compared to the para-amino substituted one(p-NH_(2)).The ratiometric response of fluorescence with significant changes in wavelength and intensity upon acetylation(m-NAc and p-NAc) can be attributed to the larger ICT and stronger-NH_(2) vibrations.This observation is further demonstrated by deuterium oxide experiments,viscosity experiments and quantum chemical calculations.The practical application of meta-amino-1,8-naphthalimide ICT-based probes is also confirmed.This research is expected to bring an in-depth understanding of π-conjugated systems with ICT characteristics,and facilitates the design of sensitive ICT fluorescent probes with meta-amino substitution.
文摘The longitudinal π-extension of carbon nanohoops is one of the most effective bottom-up synthetic strategies toward carbon nanotubes(CNTs).Herein,the precise synthesis of a multi-substituted carbon nanohoop([12]CPP-8PBPy)based on cycloparaphenylenes(CPPs)grafted with eight pyrene-functionalized units was reported.This structurally well-defined nanohoop not only acts as a segment of armchair-type CNTs but also achieves enhanced longitudinal π-extension.The structure of[12]CPP-8PBPy was confirmed by high-resolution mass spectrometry(HRMS)and nuclear magnetic resonance(NMR).The photophysical properties were studied by UV/Vis and photoluminescence spectroscopy.The potential applications of[12]CPP-8PBPy in electron-transport devices were further investigated.
基金Supported by the National Natural Science Foundation of China(No.82388101,No.81930024)the Science and Technology Commission of Shanghai(No.22YS1400400,No.20DZ2270800).
文摘Dear Editor,Idiopathic orbital inflammation(IOI),also known as orbital inflammatory pseudotumor,is a relatively common orbital disorder[1].Its pathogenesis remains unclear,often regarded as a nonspecific immune-mediated response[2].IOI presents with symptoms such as pain,photophobia,proptosis,eyelid swelling,edema,conjunctival congestion,and diplopia,with possible vision loss occurring in some cases.Based on the soft tissue structures involved,IOI can be classified into subtypes such as myositis,optic neuritis,dacryoadenitis,diffuse orbital inflammation,and orbital inflammatory masses[2].
基金supported by the National Key R&D Pro-gram of China:Gravitational Wave Detection Project(Nos.2021YFC2026,2021YFC2202601,2021YFC2202603)the National Natural Science Foundation of China(Nos.12172288 and 12472046)。
文摘The problem of maneuvering for a servicing spacecraft(inspector)to inspect a noncooperative spacecraft(evader)in cislunar space is investigated in this paper.The evader,which may be a malfunctioning or uncontrolled satellite,introduces uncertainties due to its potential maneuvering capabilities.To address this challenge,the scenario is modeled as a special orbital game,incorporating the unique complexities of the cislunar environment.A variable-duration,turn-based inspection and anti-inspection game model is designed.The model defines both players'rules,constraints,and victory conditions,providing a framework for non-cooperative inspection.Strategies for both players are developed and validated based on their dynamical properties.The inspector's strategy integrates two-body Lambert transfers with shooting methods,while the evader's strategy aims to maximize the inspector's fuel consumption.Simulation results show that the evader's optimal strategy involves deliberate fluctuations in its lunar periapsis altitude,with the inspector's requiredΔV up to eight times greater than the evader's.The impact of game constraints is evaluated,and the effectiveness of deploying the inspector in low lunar orbit is compared with the inspector at the Earth-Moon Lagrange point L1.The strengths and weaknesses of both are shown.These findings provide valuable insights for future orbital servicing and orbital games.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.12104247 and 11934020)。
文摘In a superconductor embedded with a quantum magnetic impurity,the Kondo effect is involved,leading to the competition between the Kondo singlet phase and the superconductivity phase.By means of the natural orbitals renormalization group(NORG)method,we revisit the problem of a quantum magnetic impurity coupled with a conventional s-wave superconductor.Here we present a detailed study focusing on the impurity spin polarization and susceptibility,the Kondo screening cloud,as well as the number and structures of the active natural orbitals(ANOs).In the superconducting phase,the impurity spin is partially polarized,indicating that the impurity remains partially screened by the quantum fluctuations.Furthermore,the impurity spin susceptibility becomes divergent,resulting from the presence of residual local moment formed at the impurity site.Correspondingly,a non-integral(incomplete)Kondo cloud is formed,although the ground state is a spin doublet in this phase.In comparison,the Kondo cloud is complete in the Kondo singlet phase as expected.We also quantify the critical point,where the quantum phase transition from a Kondo singlet phase to a superconducting phase occurs,which is consistent with that in previous works.On the other hand,it is illustrated that only one ANO emerges in both quantum phases.The structures of the ANO,projected into both the real space and momentum space,are distinct in the Kondo singlet phase from that in the superconducting phase.More specifically,in the Kondo singlet phase,the ANO keeps fully active with half-occupied,and the superconducting gap has negligible influence on its structure.On the contrary,in the superconducting phase,the ANO tends to be inactive and its structure changes significantly as the superconducting gap increases.Additionally,our investigation demonstrates that the NORG method is reliable and convenient to solve the quantum impurity problems in superconductors as well,which will promote further theoretical studies on the Kondo problems in such systems using numerical methods.
基金the National Natural Science Foundation of China(No.12475119)the Key Laboratory of Nuclear Data Foundation(JCKY2025201C154)the JSPS Grant-in-Aid for Scientific Research(S)(No.20H05648)。
文摘A deep neural network(DNN)was developed to accurately predict the nuclear charge density distributions for nuclei with proton numbers Z≥8.By incorporating essential nuclear structure features,the model achieved a significant improvement in predictive accuracy over conventional methods.The charge density distributions were analyzed using a Fourier-Bessel(FB)series expansion,and the DNN was trained on a comprehensive dataset derived from relativistic continuum Hartree-Bogoliubov(RCHB)theory calculations.The model demonstrated exceptional performance,with root-mean-square deviations of 0.0123fm and 0.0198 fm for the charge radii on the training and validation sets,respectively,which remarkably surpassed the precision of the original RCHB calculations.In addition to advancing nuclear physics research,this high-precision model provides critical data for applications in atomic physics,nuclear astrophysics,and related fields.
基金supported by the National Natural Science Foundation of China(Grant Nos.52271307,52061135107,52192692,11802025)the Liao Ning Excellent Youth Fund Program(Grant No.2023JH3/10200012)+1 种基金the Liao Ning Revitalization Tal-ents Program(Grant No.XLYC1908027)the Fundamental Research Funds for the Central Universities(Grant Nos.DUT20RC(3)025,DUT20TD108,DUT20LAB308)。
文摘In order to investigate the penetration performance of Linear-Shaped Charge(LSC),Embowed LinearShaped Charge(ELSC),and Embowed Linear Explosively Formed Projectile(ELEFP)on T-shaped stiffened plates,a series of near-field air-burst experiments are conducted.The damage modes and characteristics of the target plates are compared and analyzed.Each flat plate section is completely punctured,resulting in a penetration hole.The damage modes induced by the three charge types on the stiffened plate structure are consistent,characterized by shear failure in the central region of the flat plate due to penetration by the penetrator,localized plastic deformation of the flat plate,and local penetration failure resulting from partial perforation of the central stiffener.The penetration lengths caused by ELSC and ELEFP are 45.1%and 46.1% larger than that of LSC,while the half-width of the penetration hole generated by ELEFP is 54.2% and 24.7% smaller than that of ELSC and LSC,respectively.The penetration height caused by ELEFP are 17.5%and 62.1% larger than that of ELSC and LSC,respectively.The stiffener effectively segments the damage area,enhancing the local structural strength and limiting the extent of plastic deformation in the flat plate section.The comparative results show that the ELSC proves to be more effective for efficient large-scale damage,and ELEFP is more suitable for achieving efficient localized damage.
基金Supported by the National Key R&D Program of China(No.2023YFC2410203)Beijing Hospitals Authority Clinical Medicine Development of Special Funding Support(No.ZLRK202503).
文摘AIM:To investigate the clinical features and prognosis of patients with orbital inflammatory myofibroblastic tumor(IMT).METHODS:This retrospective study collected clinical data from 22 patients diagnosed with orbital IMT based on histopathological examination.The patients were followed up to assess their prognosis.Clinical data from patients,including age,gender,course of disease,past medical history,primary symptoms,ophthalmologic examination findings,general condition,as well as imaging,laboratory,histopathological,and immunohistochemical results from digital records were collected.Orbital magnetic resonance imaging(MRI)and(or)computed tomography(CT)scans were performed to assess bone destruction of the mass,invasion of surrounding tissues,and any inflammatory changes in periorbital areas.RESULTS:The mean age of patients with orbital IMT was 28.24±3.30y,with a male-to-female ratio of 1.2:1.Main clinical manifestations were proptosis,blurred vision,palpable mass,and pain.Bone destruction and surrounding tissue invasion occurred in 72.73%and 54.55%of cases,respectively.Inflammatory changes in the periorbital site were observed in 77.27%of the patients.Hematoxylin and eosin staining showed proliferation of fibroblasts and myofibroblasts,accompanied by infiltration of lymphocytes and plasma cells.Immunohistochemical staining revealed that smooth muscle actin(SMA)and vimentin were positive in 100%of cases,while anaplastic lymphoma kinase(ALK)showed positivity in 47.37%.The recurrence rate of orbital IMT was 27.27%,and sarcomatous degeneration could occur.There were no significant correlations between recurrence and factors such as age,gender,laterality,duration of the disease,periorbital tissue invasion,bone destruction,periorbital inflammation,tumor size,fever,leukocytosis,or treatment(P>0.05).However,lymphadenopathy and a Ki-67 index of 10%or higher may be risk factors for recurrence(P=0.046;P=0.023).CONCLUSION:Orbital IMT is a locally invasive disease that may recur or lead to sarcomatoid degeneration,primarily affecting young and middle-aged patients.The presence of lymphadenopathy and a Ki-67 index of 10%or higher may signify a poor prognosis.
基金Supported by The National Natural Science Foundation of China(No.82101180)the Fund for Beijing Science&Technology Development of TCM(No.BJZYYB-2023-17)the Beijing Municipal Natural Science Foundation grant(No.7252093).
文摘AIM:To define the prevalence and anatomical patterns of paranasal sinus abnormalities(PSA)in thyroid-associated ophthalmopathy(TAO)and to test the hypothesis that TAO is partially driven by contiguous orbital inflammation rather than systemic autoimmunity or generalized orbital pressure.METHODS:Data included ophthalmic assessments and a panel of thyroid function and autoimmune biomarkers.Blinded radiological analysis of orbital computed tomography(CT)scans was performed to quantify sinus abnormalities and extraocular muscles(EOMs)involvement.Patients were categorized into two groups based on CT findings,those with no radiological evidence of sinus abnormalities(non-PSA control group)and those with identifiable PSA.Furthermore,ethmoid sinus mucosal biopsies from a subset of TAO patients and noninflammatory controls were subjected to histopathological analysis.RESULTS:Totally 121 TAO patients(mean age 42.4±12.8y,range 10-78y),male:female=42:79,were included.PSA was identified in 44.6%(n=54)of patients,with a distribution anatomically restricted to the maxillary(50.0%isolated)and ethmoid sinuses(18.5%isolated;29.6%combined).Compared to the non-PSA group(n=67),patients with PSA were significantly older(45.1±11.8 vs 40.3±13.2y;P=0.040)and were more likely to be male(55.6%vs 17.9%;P<0.001).They also had significantly higher proptosis(22.1±3.2 vs 20.7±2.9 mm;P<0.001).Medial/inferior rectus involvement was most frequent(88.4%vs 89.3%).Histopathological analysis of sinus mucosa from PSA patients provided direct evidence of pathology,revealing a dense,chronic lymphoplasmacytic infiltrate and submucosal edema,validating the radiological findings as a true inflammatory process.No significant correlation was found with systemic autoimmune markers,including thyroid-stimulating hormone(TSH)receptor antibodies(TRAb,median 4.86 vs 2.71 IU/L,P=0.104).CONCLUSION:TAO is associated with a high prevalence of PSA in a pattern consistent with the orbital anatomy.The correlation with ipsilateral muscle thickening combined with the lack of association with proptosis laterality or systemic biomarkers lend strong support to a model of contiguous inflammation over systemic autoimmunity,a hypothesis that warrants further validation through longitudinal and mechanistic studies.
基金supported by the National Key Research and Development Project of the National Natural Science Foundation of China(Grant No.2022YFC3004605)the National Natural Science Foundation of China Youth Science Fund(Grant No.52104087).
文摘To advance the theoretical understanding,technological development,and field application of electric charge induction for monitoring rock deformation and failure,this study investigates the induced electric charge generated during the deformation and failure of igneous rocks.The charge originates mainly from a combination of electrical polarization and triboelectric effects.Through laboratory experiments,we analyzed the time-frequency evolution of induced electric charge signals and identified relevant monitoring parameters.An online downhole electric charge induction monitoring system was developed and validated in the field.Experimental results show that the dominant frequency range of induced electric charge signals generated during igneous rock deformation and failure lies between 0 and 23 Hz,and a low-pass finite impulse response(FIR)filter effectively suppresses noise.Optimal sensor distances for monitoring cubic and cylindrical specimens were determined to be 17 mm and 13 mm,respectively.We proposed early warning indicators,including the maximum absolute value of the induced electric charge,the arithmetic mean value,the distribution dispersion coefficient,and the cumulative sum value.In field application,time-domain curves and spatial distribution charts of these warning indicators correspond well with changes in abutment stress ahead of the mining face,offering indirect insights into local stress evolution.This research provides technical and equipment support for the application of electric charge induction technology to monitoring and early warning of coal bursts.
基金financial support of the National Natural Science Foundation of China (21875247,21072221, 21172252)the Project of Talent Cultivation for Carbon Peak and Carbon Neutrality of the University of Chinese of Academy of Science
文摘The design and fabrication of ordered epitaxial MOF-on-MOF heterostructures as highly efficient electrocatalysts for water splitting is crucial but still challenging.In this study,a simple coordination-driven self-assembly method is used to fabricate controllable MOF-on-MOF multiscale heterostructures,where triangular host MOF(ZIF-67)nanosheets undergo in situ epitaxial growth to form uniform orthogonal vip MOF(CoFe PBA)nanosheets.Phosphorus(P)is further introduced in situ to fabricate CoP and Fe_(2)P heterostructured nanosheets(CoFe-P-NS),which exhibit excellent bifunctional electrocatalytic performance due to the enhancement of intrinsic electrocatalytic activity by p-d orbital hybridization.Specifically,the CoFe-P-NS requires low overpotential of 259 and 307 mV to reach 500 mA cm−2 for HER and OER,respectively.Remarkably,the assembled electrolysis cell maintained a large current density of 300 mA cm−2 for over 360 h with negligible voltage increase during alkaline seawater electrolysis.Experiments and theoretical calculations show that the synergistic catalytic activity of bimetallic phosphides arises from p-d orbital hybridization,where the CoP-P sites enhance HER by optimizing H*adsorption in the Volmer-Heyrovsky steps,while the Fe_(2)P-Fe sites accelerate OER by lowering the energy barrier of the rate-determining step from O*to OOH*.This study provides valuable insights into the design of a controllable MOF-on-MOF-based electrocatalyst toward alkaline seawater splitting.
基金supported by the Research Fund of the National Natural Science Foundation of China(No.52374205)the Fundamental Research Project of the Educational Department of Liaoning Province(No.JYTMS20230793)the Research Fund of the State Key Laboratory of Coal Resources and Safe Mining,CUMT(No.YJY-XD-2024-A-016).
文摘To address the key scientific challenge of monitoring the dynamic fracturing of surrounding rock in deep roadways,this study systematically investigates the quantitative relationship between stress and charge signals during coal mass loading.By integrating innovative analytical approaches,introducing quantitative evaluation indices,and developing a charge–stress inversion model,and incorporating underground monitoring practices,significant progress has been achieved in elucidating the correlation between stress variations and charge signals throughout the entire coal mass fracturing process.First,in the field of stress–charge correlation analysis,empirical mode decomposition(EMD)was combined with wavelet coherence analysis for the first time,enabling the removal of slow-varying stress trends while retaining high-frequency fluctuations.This approach allowed for the quantitative characterization of the evolution of coherence between stress variations and charge fluctuations across multiple time scales.Second,coherence skewness and the proportion of high-coherence intervals were innovatively introduced to examine the influence of time scale selection on correlation results.On this basis,a criterion for determining the near-optimal observation scale of charge signals was proposed,providing a quantitative reference for time scale selection in similar signal analyses.Finally,by correlating charge signals with coal damage factors and stress states,a charge-based damage evolution equation was established to achieve effective stress inversion.Combined with in situ monitoring of stress and charge in roadway surrounding rock,this approach revealed the correlation characteristics of stress and charge intensity responses during the dynamic fracturing process.The results indicate,first,that charge signals are not significantly correlated with the absolute stress level of coal but are directly associated with stress variations following coal damage and failure,with the amplitude of charge fluctuations increasing alongside stress fluctuations.Second,coherence between stress and charge signals varies markedly across time scales,with excessively small or large scales leading to distortion,and the scale corresponding to the peak proportion of intervals with coherence>0.8 was identified as the near-optimal observation scale.Third,charge signals can effectively characterize coal damage factors,and the established damage evolution equation can effectively invert stress variation trends.Fourth,in underground roadways,zones of dynamic fracturing in surrounding rock are commonly located in areas where stress concentration overlaps with regions of high charge intensity,further confirming the strong consistency between charge and stress variations.These findings improve the theoretical framework of charge signal responses in loaded coal and provide a scientific basis for precise“stress-charge”monitoring of dynamic disasters,offering practical potential for engineering applications.
基金supported by the Natural Science Foundation of Jiangsu Province(BK20250050)the National Natural Science Foundation of China(22472111,12275189)+4 种基金the National Key Research Program of China(2022YFA1503101)the Postdoctoral Fellowship Program of CPSF(GZC20250614)Jiangsu Funding Program for Excellent Postdoctoral Talent(2025ZB299)Collaborative Innovation Center of Suzhou Nano Science&Technologythe 111 Project。
文摘Lithium-sulfur(Li-S)batteries hold great promise for high-energy–density energy storage applications but are plagued by the severe shuttle effect and sluggish conversion kinetics of lithium polysulfides(Li PSs).We herein report a d-p-f orbital coupling strategy to tackle these critical challenges by incorporating Eu 4f orbitals to activate both metallic(Ni)and non-metallic(Se)sites of Ni Se.The imported Eu atoms could induce essential Ni 3d and Se 4p orbital reconstruction through gradient d-p-f coupling,thereby optimizing the band center alignment between Ni Se and Li PSs.Such electronic reconstruction strengthens both d-p hybridization between Ni and Li PSs and s-p hybridization between Se and Li PSs,which can not only enhance the chemisorption affinity toward Li PSs but also accelerate interfacial charge transfer kinetics,leading to suppressed shuttle effect and boosted Li PSs conversion kinetics.Therefore,the Li-S batteries assembled with Eu incorporated Ni Se deliver exceptional electrochemical performance with a high specific capacity of 896.2 m Ah g^(-1)at 4 C and a retained areal capacity of 5.66 m Ah cm^(-2)under a high sulfur loading of 5.94 mg cm^(-2)after 100 cycles.This work underscores the critical role of rare-earth 4f orbital coupling for modulating the active sites to construct high-efficiency electrocatalysts for Li-S batteries and beyond.
基金the Fundamental Research Funds for the Central Universities of Nanjing University of Science and Technology(CN)under Grant No.30924010803。
文摘The penetration of shaped charge jets into targets at high velocities is significantly influenced by the compressibility effect,while at low velocities,the strength effect becomes predominant.In the latter regime,material strength dictates the resistance to plastic deformation and flow,a contrast to the shockwave-dominated interactions where compressibility is key.This paper presents a self-consistent compressible penetration theory that considers both the axial penetration and radial crater growth of shaped charge jets into targets.An integrated approach where the axial and radial dynamics are coupled has been proposed,influencing each other through shared physical principles rather than being treated as separate,empirically linked phenomena.The presented theory is rooted in the compressible Bernoulli equation and the linear Rankine-Hugoniot relation.These foundational equations are employed to accurately model the high-pressure shock state and subsequent material flow at the jet-target interface,providing a robust physical basis for the penetration model.Notably,it considers the target material's compressibility,which elevates the pressure at the jet-target interface beyond that observed with incompressible materials.This pressure increase is directly proportional to the target's degree of compressibility.As such,this model of compressible penetration reorients the analytical approach:rather than merely estimating penetration resistance,it determines this value from the target material's specific compressibility and yield strength.This shift from empirical correlations to a physics-based derivation of penetration resistance enhances the model's predictive power,particularly for novel target materials or engagement conditions outside established experimental datasets.This investigation establishes a quantitative link between the material's yield strength and its penetration resistance.The accuracy of this penetration resistance value is paramount,as it significantly influences the predicted crater diameter;indeed,the crater diameter's sensitivity to this resistance underscores the necessity for its precise determination.Ultimately,by integrating the yield strength of the target material,this framework enables the prediction of both the penetration depth and the resultant crater diameter from a shaped charge jet.The theory's validation involved two experimental sets:the first focused on shaped charge jet penetration into 45#steel at varied stand-offs,while the second utilized targets of high-to ultrahigh-strength steel-fiber reactive powder concrete(RPC)with differing strength characteristics.These experimental campaigns were specifically chosen to test the theory against both ductile metallic alloys,where plastic flow is significant,and advanced quasi-brittle cementitious composites,presenting a broad spectrum of material responses and penetration challenges.Resulting hole profiles derived from theoretical calculations demonstrated a strong correspondence with empirical measurements for both material types.
基金supported by the Natural Science Foundation of Shanxi Province(202303021211180)the Program of State Key Laboratory of Quantum Optics and Quantum Optics Devices(KF202403)。
文摘Based on the idea of treating the anti de Sitter(AdS)radius as a fixed parameter,we study the thermodynamics and topology of d-dimensional charged AdS black holes in the restricted phase space utilizing Visser's holographic approach.For the charged black hole with a cloud of strings and quintessence in the higher-dimensional spacetimes with d=(4,5,6),we demonstrate that the topological number remains invariant within the same canonical ensemble;however,a distinct topological number emerges in the grand canonical ensemble for the same black hole system.Notably,these results are independent of the dimension d and other related parameters.The formalism known as restricted phase space thermodynamics is checked in detail and some interesting thermodynamic behavior is revealed in the example case of d-dimensional charged AdS black holes with a cloud of strings and quintessence.This research lays the foundation for establishing a universal framework of restricted phase space thermodynamics and investigating its fundamental thermodynamic properties.
基金supported by the National Natural Science Foundation of China(22472104)Guangdong Basic and Applied Basic Research Foundation(2024A1515012075,2024A1515010028)the Postdoctoral Fellowship Program of CPS Funder(GZC20241083,2025M771117)。
文摘Oxygen evolution reaction(OER)is widely recognized as a bottleneck of water electrolysis.To determine the underlying reaction mechanisms,particularly the relative contribution of the adsorbate evolution mechanism(AEM)and lattice-oxygen participation mechanism(LOM),we conduct a comprehensive investigation combining Density Functional Theory(DFT)calculations and experimental validation.Our theoretical analysis of doped RuO_(2)catalysts reveals that heteroatom doping(Ni,Cu,and Zn)induces significant local charge transfer,leading to the increased charge state of Ru and the downshifted d-band center.This,in turn,enables the mechanism switching from the conventional AEM to the more efficient LOM,and finally improves OER activity.We also establish a simple yet powerful descriptor,Ne of Ru(representing charge density of Ru sites),which enables accurate prediction of both catalytic activity and stability.Guided by these theoretical predictions,we successfully synthesize a Ni-doped RuO_(2)catalyst,which exhibits excellent OER activity and stability in acidic media,achieving an overpotential of just 156 mV and maintaining stability for 4000 h at 10 mA cm^(−2),significantly surpassing the performance of the commercial RuO_(2).These findings not only provide fundamental insights into the mechanism-switching behavior in OER catalysis but also offer a practical strategy for designing high-performance,stable electrocatalysts for acidic water electrolysis.
基金support from the Heilongjiang Province"Double First Class"Discipline Collaborative Innovation Project(No.LJGXCG2023-061).
文摘Hard carbon is a vital anode material for sodium-ion batteries;however,the nonuniform growth of solid electrolyte interphase(SEI)film substantially diminishes its initial coulombic efficiency(ICE)and cycle life.The chemical and morphological properties of surface highly influence the electrode/electrolyte interfacial reactions.In this study,we have tuned orbital hybridization states forming an interface enriched with sp^(2) hybridized carbon(sp^(2)-C),which decreases the binding energy to solvent molecules and inhibits excessive solvent decomposition during SEI formation.Benefiting from successfully constructed inorganic-rich SEI,the ICE increased to 91%and sodium storage capacity reached 346 mAh/g.Besides,the capacity retention rate was 90.7%after 700 cycles at 1 A/g higher than pristine electrode(83.8%).
基金National Natural Science Foundation of China,Grant/Award Numbers:52204085,52227805。
文摘Deep mining of natural resources,like coal,is increasingly utilizing directional blasting technology with slit charge for rock blasting at greater depths.This study,based on numerical simulation methods,analyzes the dynamic behavior of slit charge blasting in three aspects:slit tube dynamic response,hoop stress evolution,and crack propagation.According to research findings,the failure mode of the slit tube mainly manifests as a tensile fracture of the inner wall and a shear fracture at the end connection,where the end connection of the slit tube is the weak point of the overall structure.The dynamic response of the slit tube mainly exhibits radial response in the vertical direction of the slit and hoop response in the slit direction.The hoop tensile stress plays a crucial role in determining the spread of cracks caused by explosions.As the in situ stress increases,the peak hoop tensile stress reduces,and the peak hoop compressive stress increases.This hinders the propagation of cracks.In addition,the directional impact is most pronounced in the middle of the borehole,with the longest primary directional crack observed.Conversely,the directional impact is least favorable near the bottom of the borehole.When the in situ stress reaches 60MPa,the purpose of directional fracture has not been achieved,suggesting combining presplit blasting for in situ stress relief to improve rock breaking efficiency.
基金supported by the National Natural Science Foundation of China(22579043,52461040,22202053,52274297)the Hainan Provincial Department of Science and Technology(G20250218018E)+2 种基金the first batch of“Nanhai New Star”industrial innovation talent platform project(202309006)the Hainan Province Science and Technology Special Fund(ZDYF2025GXJS004)the Start-up Research Foundation of Hainan University(KYQD(ZR)-21124)。
文摘Membra ne electrode assemblies(MEAs)are pivotal to advancing proton exchange membra ne water electrolysis(PEMWE),yet conventional designs suffer from limited triple-phase boundaries(TPBs),inefficient mass/charge transport,and insufficient durability.This study introduces a three-dimensional ordered pattern-array(3D OPA)architecture fabricated via a scalable laser-machined mask and hot-pressing strategy.The 3D OPA MEA achieves a current density of 3.73 A cm^(-2) at 2 V,demonstrating a 50%performance improvement over the conventional MEA(2.48 A cm^(-2)),alongside a degradation rate of 26.6μV h^(-1) in a highly dynamic accelerated stress test(AST).Additionally,numerical simulations corroborate that the OPA architecture optimizes localized oxygen diffusion and liquid water replenishment,enhancing reaction kinetics.The 3D OPA architecture enhances TPBs and establishes optimized gas-liquid tra nsport pathways,significantly improving catalyst utilization while minimizing mass transfer overpotential and bubble-induced losses.Furthermore,its interlocking design reinforces mechanical interactions,reducing ohmic resistance a nd ensuring sustained mecha nical integrity and electrochemical durability.This work provides a simple,cost-effective,and scalable approach for patterned MEAs,addressing critical barriers to PEMWE commercialization through rational TPB engineering and transport pathway optimization.
