The former plant population survey has shown that three genetically-related species, Caraganamicrophylla Lam., C. davazamcii Sancz. and C. korshinskii Kom., form a geographical replacement series inNei Mongol Plateau....The former plant population survey has shown that three genetically-related species, Caraganamicrophylla Lam., C. davazamcii Sancz. and C. korshinskii Kom., form a geographical replacement series inNei Mongol Plateau. The present study on population distribution, taxonomy, morphology, development andgenetic structure demonstrated that the geographical distribution of these three species was successiveand in gradual change, thus forming a geographical cline which extended from the east to the west of NeiMongol Plateau. With an analysis of climate change over time, it was considered that the formation of thisgeographical cline was a result of plant adaptation to its natural environment.展开更多
Gradient microstructures strengthened by serrated Grain Boundaries(GBs)were achieved through a combination of Gradient Strain Deformation(GSD)and Serration Heat Treatment(SHT),with particular focus on microstructural ...Gradient microstructures strengthened by serrated Grain Boundaries(GBs)were achieved through a combination of Gradient Strain Deformation(GSD)and Serration Heat Treatment(SHT),with particular focus on microstructural evolution,underlying mechanisms,and the critical influencing factors.Dynamic recrystallization governed the microstructural evolution in the fine-grained and transition regions during GSD,where multiple nucleation mechanisms were active.Plastic deformation facilitated the dissolution ofγ'phase in fine-grained regions,ultimately resulting in its morphological transformation.During the subsequent SHT,serrated GBs formed within the gradient microstructures produced by prior GSD without disrupting the grain size gradient,thereby enhancing creep resistance.Two distinct mechanisms associated withγ'gbparticles governed the formation of the serrations at GBs.Owing to the stronger dragging effect of grain boundary junctions in fine-grained regions,the amplitude and wavelength of serrations in these regions were smaller than those in coarse-grained regions.Moreover,the formation of serrations exhibited a strong dependence on the inherent properties of the GBs.The random high-angle grain boundaries(HAGBs)with misorientation angles in the range of 30-59°tended to become serrated more easily during SHT due to their high mobility and the accelerated precipitation ofγ'gbparticles at them.Low-ΣHAGBs and low-angle GBs were not prone to form serrations.In particular,serration formation was completely inhibited atΣ3 twin boundaries due to their extremely low mobility and the absence ofγ'gbparticles.展开更多
Liverworts are an important component of terrestrial ecosystems worldwide.They have adapted to and diversified in a wide variety of environments.Investigating variation in net diversification rate is a major goal of b...Liverworts are an important component of terrestrial ecosystems worldwide.They have adapted to and diversified in a wide variety of environments.Investigating variation in net diversification rate is a major goal of biogeographers and ecologists but such investigation is lacking for liverworts at a global scale.Here,we explore global geographic patterns of mean diversification rate(MDR)within genera of liverworts,which are one of the earliest lineages of the extant land plants,and its relationship with latitude,climatic conditions,and regional species richness.We collated species lists of liverworts for each of 390 geographic units(primarily countries,provinces or states)across the world.We related MDR to geographic and current and historical climatic variables,assessed the relative importance of different sets of climatic variables on MDR,and explored the effect of MDR on species richness after accounting for major climatic factors.We analyzed the data with correlation and regression analyses,and structural equation modeling approach.We find that MDR peaks at tropical latitudes and in humid and hot environments,and that at a global scale current climate,temperature-related variables,and climatic seasonality explained more variation in MDR than Quaternary climate change,precipitation-related variables,and climatic extremes,respectively.In addition,we find a positive relationship between MDR and liverwort species richness,with the latter being directly influenced more strongly by climate than by MDR.Most importantly,we find that tropical regions of high liverwort diversity also have high current diversification rates,suggesting ongoing niche occupation.The above-described patterns are similar between the New World and Old World and between the eastern and western parts of the Old World.Our study highlights that tip diversification rates provide a complementary aspect to understand the evolution of liverwort diversity to that recovered by studying phylogenetic diversity and species richness.展开更多
The tissues spanning from tendon to bone exhibit a highly specialized extracellular matrix(ECM)architecture,characterized by hierarchical collagen alignment and a gradient mineral composition,which together enable eff...The tissues spanning from tendon to bone exhibit a highly specialized extracellular matrix(ECM)architecture,characterized by hierarchical collagen alignment and a gradient mineral composition,which together enable efficient force transfer and guide spatially organized cellular phenotypes.However,recapitulating such complex multi-scale organization and compositional gradients to achieve integrated soft-hard tissue remains challenging.Here,we report the de novo construction of biomimetic collagen-mineral matrices that mimic both the hierar-chical organization and mineral gradient distribution of the native tendon-to-bone ECM.Through synergistic electro-assembly and post-treatment,collagen molecules self-organized into aligned fibrillar matrices with multi-scale architecture,replicating tendon-side morphology while providing robust tensile mechanics.At the opposing end,intrafibrillar and interfibrillar minerals were spatially patterned to emulate the mineral gradient from tendon to bone.This structural and compositional continuum enables smooth mechanical transition across the soft-hard tissue interface and promotes region-specific regeneration of aligned tendon-like tissue,fibrocartilage and bone.In vivo studies in rabbit models confirm that these de novo constructed matrices support histological reconstruction of multiple tissues from tendon to bone at the rotator cuff,and significantly improve functional recovery.This work presents a bottom-up biomimetic strategy for engineering multiscale collagen-based scaf-folds and demonstrates the therapeutic potential of de novo constructed matrices for multiple tissue regeneration.展开更多
Magnetic hyperthermia uses magnetic nanoparticles(MNPs)to generate the heat used for damaging cancer cells under an alternating magnetic field.In fact,the MNPs tend to gather at the injection center and also occur the...Magnetic hyperthermia uses magnetic nanoparticles(MNPs)to generate the heat used for damaging cancer cells under an alternating magnetic field.In fact,the MNPs tend to gather at the injection center and also occur the clustering phenomenon at the same time when injecting into tumor tissue,which however can ultimately result in the excessive concentration of heat in the injection site.Thus,this study aims at improving the MNPs concentration distribution after the injection behavior by considering the action of a static gradient magnetic field,and finally optimizes both temperature situation and thermal damage degree for tumor tissue during magnetic hyperthermia.The MNPs distribution inside a proposed liver tumor is simulated by adopting a Monte Carlo method with adaptive step size,which consists of enough number of small size particles used to analyze the behavior of migration,diffusion,and chain-like phenomenon.The research results demonstrate that the introduction of static gradient magnetic field can disperse the MNPs and form a chainlike distribution inside tumor,and can then expand the distribution range of MNPs,thereby optimizing the thermal damage degree of tumor tissue.In addition,a PID controller with proper setting coefficients is also proven to be able to improve the therapeutic effect for hyperthermia by shortening the rising time to the critical temperature when proper coefficients are set properly during therapy.展开更多
Submarine gas hydrate systems store vast carbon inventories(∼1500–12,400 Gt C)yet pose dual risks as potential geohazard multipliers and climate feedback agents under oceanic warming.Conventional seal assessment fai...Submarine gas hydrate systems store vast carbon inventories(∼1500–12,400 Gt C)yet pose dual risks as potential geohazard multipliers and climate feedback agents under oceanic warming.Conventional seal assessment fails catastrophically in unconsolidated Quaternary hydrate-bearing sediments due to core-retrieval artifacts,hydrate morphology controls on capillary trapping,and meter-scale heterogeneity unresolved by seismic methods.Here,we pioneer methane carbon isotope(δ13C1)gradients as a dynamic proxy for seal capacity in the Qiongdongnan Basin.Integrating petrographic features,natural gas geochemical characteristics,downhole logging data,and principal component analysis(PCA)from six wells,we:(1)quantified the thermogenic gas contribution of wells W6 and W8 to be 55%–73%,and that of well W1 to be 28%–32%via binary mixing models,(2)establish that methane carbon isotope gradients>0.5‰/m diagnose effective capillary barriers,correlating with zones of pore-throat disconnection,and(3)develop a PCA-integrated logging model(cumulative variance:84.02%,R2=0.78)predicting seal capacity from conventional petrophysical parameters.Furthermore,the results validate a charge-dynamic barrier-mixing accumulation model where thermogenic gas influx elevates hydrate saturation,creating self-sealing horizons that trap underlying microbial gases and subsequently charged thermogenic gases,recorded in diagnostic methane carbon isotope reversals.This approach bridges molecular-scale fractionation and reservoir-scale processes,enabling targeted identification of high-integrity seals for optimized carbon storage and safer hydrate exploitation in rapidly deposited marginal basins.展开更多
Electrocatalytic CO2 reduction(CO2 RR)toward multi-carbon compounds is a challenging but meaningful route for carbon cycling.Copper-based catalysts are the most promising candidate for C2+generation due to th...Electrocatalytic CO2 reduction(CO2 RR)toward multi-carbon compounds is a challenging but meaningful route for carbon cycling.Copper-based catalysts are the most promising candidate for C2+generation due to their unique C–C coupling activity,yet the in situ reduction from Cu+ to Cu0 under cathodic potentials causes the catalyst deactivation.Herein,we develop a transient thermal shock strategy to embed Cu+ species into CeO2 lattices,constructing a CuOx/CuCeOxcatalyst with a radial gradient Cu+ -Ov-Ce3+/Ce4+structure.Depth-profiling X-ray photoelectron spectroscopy(XPS)and density functional theory(DFT)calculations reveal that mismatched metal/oxygen diffusion kinetics drive continuous electron transfer from surface Cu+ to bulk Ce3+/Ce4+via oxygen vacancies(Ov),forming a dynamic“self-sacrificial”structure to preserve surface Cu+ states.In CO2-saturated 0.1 M KHCO3,the optimized CuOx/CuCeOx-10 achieves a high C2 Faradaic efficiency(FE)of 85.8%at-1.4 V vs.RHE.In situ attenuated total reflection surface-enhanced infrared adsorption spectroscopy(ATR-SEIRAS)identifies the key intermediates of C2 are*OCCO and*OCCOH,while DFT reveals a drastic reduction of C–C coupling barrier from 0.842 to0.274 eV.This work demonstrates kinetically tailored metal-support interactions,enabling oxidationstate control for pathway-selective catalysis.展开更多
Anammox bacteria in constructed wetlands(CWs)play pivotal role in sustainable nitrogen transformation,yet existing studies lack comprehensive analysis of environmental gradients and microbial interactions,both key fac...Anammox bacteria in constructed wetlands(CWs)play pivotal role in sustainable nitrogen transformation,yet existing studies lack comprehensive analysis of environmental gradients and microbial interactions,both key factors in anammox bacteria enrichment.This study investigated the mechanisms driving anammox bacteria enrichment in lab-scale simulated CWs treating high-nitrogen wastewater,focusing on bacterial community re-sponses across wetland layers with various strategies,including continuous up-flow influent,nitrogen loading increase,effluent recirculation,intermittent influent,and anammox bacteria inoculation.Results showed that total relative and absolute abundances of anammox bacteria ranged from 0.77%to 12.50%and from 0.13 to 6.46×107 copies/g,respectively.Dissolved oxygen and pH had significant positive correlations with the absolute abundance of anammox bacteria,while organic matter and nitrate negatively impacted their relative abundance.Permutational multivariate analysis of variance indicated that spatial heterogeneity explained more variation in anammox bacteria abundance(43.44%)compared to operational strategies(8.58%).In terms of microbial interactions,60 dominant species exhibited potential correlations with anammox bacteria,comprising 170 interactions(105 positive and 65 negative),which suggested that anammox bacteria generally foster cooperative relationships with dominant bacteria.Notably,significant interspecies interactions were observed between Candidatus Kuenenia(dominant anammox bacteria in CWs)and species within the genera Chitinivibrio-nia and Anaerolineaceae,suggesting that microbial interactions primarily manifest as indirect facilitative effects rather than direct mutualistic relationships.Given that the Normalized Stochasticity Ratio in CWs were<50%,this study inferred that environmental gradients have greater influence on anammox bacteria than microbial interactions.展开更多
This study investigates the evolution of free-radical polymerization under spatially graded conditions by constructing a position-dependent reaction probability model.Given the strong temperature dependence of thermal...This study investigates the evolution of free-radical polymerization under spatially graded conditions by constructing a position-dependent reaction probability model.Given the strong temperature dependence of thermal initiators,spatial temperature variations significantly affect both local monomer reactivity and the macroscopic evolution of polymer structures.Understanding this coupling is crucial for designing gradient-controlled synthesis strategies.The dissipative particle dynamics(DPD)method was employed to investigate free radical polymerization under gradient temperature conditions.IncreasingΔT enhances spatial heterogeneity:high-temperature regions form dense networks with lower molecular weights(Mn and Mw)due to rapid initiation and frequent termination.In contrast,low-temperature regions yield higher molecular weights and expanded chain conformations()resulting from longer radical lifetimes.These structural differences further govern pore evolution:porosity decreases rapidly and reaches lower final values in high-temperature zones,while low-temperature regions exhibit delayed evolution but higher final porosity.This study demonstrates that the precise control of polymer growth orientation,molecular weight distribution,and porous morphology can be achieved by incorporating gradient conditions,thereby establishing a new paradigm for the targeted synthesis of gradient functional materials.展开更多
Dielectric polymers commonly suffer from severe performance degradation above 150℃,hindering advanced power systems.Herein,we demonstrate a polyetherimide(PEI)nanocomposite that overcomes this by mimicking the gradie...Dielectric polymers commonly suffer from severe performance degradation above 150℃,hindering advanced power systems.Herein,we demonstrate a polyetherimide(PEI)nanocomposite that overcomes this by mimicking the gradient architecture of nacre and bamboo,incorporating a continuous vertical gradient of fluorinated boron nitride nanosheets(BNNS‐F)through sequential electrospinning.This bio‐inspired design not only reinforces mechanical and thermal stability,but also generates a spatially gradient distribution of deep charge traps.The resulting progressive trap energy barrier effectively suppresses charge transport,impedes electrical treeing propagation,and significantly reduces conduction losses at elevated temperatures.Consequently,our continuous gradient PEI/BNNS‐F cg nanocomposite achieves an exceptional breakdown strength(Eb)of 626 MV m−1and a discharged energy density(Ud)of 6.21 J cm−3with 90%efficiency at 150℃,surpassing most reported polymer‐based dielectrics.Remarkably,it retains a high Udof 3.89 J cm−3at 200℃,along with outstanding cycling stability over 10,000 cycles.This work introduces a new paradigm for controlling charge dynamics through continuous gradient structures,enabling high‐performance energy storage under extreme conditions.展开更多
Gradient nanocrystalline–amorphous nanostructures are considered to be an effective approach to achieve exceptional strength–plasticity synergy,with significantly improved wear performance.Here,gradient nanostructur...Gradient nanocrystalline–amorphous nanostructures are considered to be an effective approach to achieve exceptional strength–plasticity synergy,with significantly improved wear performance.Here,gradient nanostructured Fe-based coatings were successfully fabricated by extremely high-speed-rate laser deposition and remelting.The microstructure evolution along the depth direction varies in a nanocrystalline,equiaxial dendrites,columnar dendrites gradient,respectively.Noticeably,amorphous grain boundaries and carbide nanoprecipitates could be identified within the topmost surface nanocrystalline layer owing to the extremely high cooling rate during remelting,which exhibits the highest hardness and wear resisance(microhardness of ~1136 HV,and wear rate of 4.36×10−6mm3/(m N)).The superior wear resistance is mainly attributed to the synergistic nanocrystalline–amorphous deformation and gradient refinement effects.Meanwhile,multi-scale carbides effectively impede dislocation motion and further improve strength and wear resistance at different depths.This gradient structure provides promising insights into the design of high-performance wear-resistant alloys.展开更多
Pharmaceutically active compounds have garnered increased attention as emerging contaminants due to their widespread presence and potential ecological impacts.This study conducted a field evaluation under varied rainf...Pharmaceutically active compounds have garnered increased attention as emerging contaminants due to their widespread presence and potential ecological impacts.This study conducted a field evaluation under varied rainfall conditions,assessing the effects of rainfall intensity and duration on pharmaceutical concentrations.Grab sampling was complemented by the deployment of diffusive gradients in thin films(DGT)passive samplers along two urban rivers in Beijing,China.Twenty-four target pharmaceuticals were detected,with concentrations ranging from 370 to 686 ng/L in the Beixiao River and 376 to 610 ng/L in the Qing River.Rainfall influenced pharmaceutical concentrations through either dilution or enhancement,depending on local factors.Rainfall had a minimal impact on DGT performance,while biofouling showed compound-specific effects.For about 70%of the pharmaceuticals,hydrophilic poly tetrafluoroethylene(PTFE)membranes used over 9–15 days effectively minimized biofouling influence(Mbiofouled/Mclean>0.8).The effectiveness of DGT for long-term monitoring depended on the biofilm formation time.Overall,DGT proved to be a reliable tool for accurately characterizing pharmaceutical concentrations in dynamic water systems.This study represents the first attempt to evaluate DGT performance for pharmaceuticals under fluctuating concentration scenarios in the field,providing valuable insights into the occurrence and environmental behavior of these contaminants.展开更多
The strength and damage tolerance of additively manufactured(AM)alloys are significantly influenced by their heterogeneous microstructures.However,establishing quantitative relationships between these microstructural ...The strength and damage tolerance of additively manufactured(AM)alloys are significantly influenced by their heterogeneous microstructures.However,establishing quantitative relationships between these microstructural characteristics and the resulting mechanical properties remains a challenge.Here,a microstructure-based mechanical model is established based on the heterogeneous grain distribution within the melt pool,with particular emphasis on the strain gradient effect arising from the deformation incompatibility between distinct grain regions.The strengthening mechanisms and local deformation response of AM alloys are elucidated with the finite element method(FEM).The strain gradient effect generated by the deformation incompatibility between the columnar and equiaxed grain regions enhances the local stress near the equiaxed-columnar interface,which is an important reason for the overall work hardening.Concurrently,the local stress concentration makes it easier to reach the critical stress for microcrack nucleation at the interface,leading to failure and a lack of synergy between the strength and damage tolerance.The prediction of the crack initiation location based on the simulation results is consistent with the previous experiments.By further quantitatively predicting the comprehensive effects of melt pool size on strength,strain hardening,and damage rate,small-melt-pool structures produce high strength,but microcracks originate early,whereas large-melt-pool structures have weak strengthening effects but fast damage evolution in the later stages of deformation.This study provides a pathway to predict the optimal melt pool size for achieving superior combinations of strength and damage tolerance in AM alloys.展开更多
Ultra-thick electrodes(UTEs)hold great promise for high-energy-density lithium-ion batteries(LIBs),yet the practical application is hindered by challenges in precise fabrication and reaction kinetics modification.In t...Ultra-thick electrodes(UTEs)hold great promise for high-energy-density lithium-ion batteries(LIBs),yet the practical application is hindered by challenges in precise fabrication and reaction kinetics modification.In this contribution,a solvent-free processing method is introduced to tailor UTEs through layerby-layer fabrication with positive,uniform,and negative gradient porosity from the separator side to the current collector side,denoted as P-UTEs,U-UTEs,and N-UTEs.In contrast to conventional slurry coating,the proposed solvent-free approach effectively circumvents capillary stress,thereby facilitating the fabrication of crack-free UTEs(>300μm)while simultaneously mitigating environmental toxicity concerns.The three-layer N-UTEs(>220μm)with a gradient porosity of(~34%,~31%,~27%)deliver an exceeding areal capacity over 5 m Ah/cm2 at 0.29 mA/cm2 and a high-capacity retention over 62% at 2.9 m A/cm2,indicating a favorable balance between the areal capacity and the high-rate behavior.Detailed mechanistic simulations reveal that the multi-center reaction pathways enabled by enhanced ionic accessibility in N-UTEs significantly improve reaction kinetics.This work offers new insights into the gradient porosity tailoring for high-areal-capacity and high-rate UTEs for the next generation LIBs.展开更多
Lithium-rich layered oxides are promising cathodes for high-energy lithium-ion batteries,yet their applications are hindered by voltage decay,structural instability,and heterogeneous reaction dynamics.These degradatio...Lithium-rich layered oxides are promising cathodes for high-energy lithium-ion batteries,yet their applications are hindered by voltage decay,structural instability,and heterogeneous reaction dynamics.These degradations stem from the coexistence of Li2MnO3and LiMO2domains,which exhibit distinct redox kinetics and trigger phase mismatch during cycling.To address this challenge,we propose a tailored concentration gradient design that regulates the spatial distribution of transition metals.Nickel is intentionally enriched near the surface while manganese dominates the interior,creating a coordinated balance between interfacial stability and bulk capacity retention.Regulating Ni content deliberately induces a moderate Li/Ni cation-mixed phase,and the tailored gradient builds a surface composite structure that stabilizes the layered framework and suppresses interfacial degradation.This architecture homogenizes redox activation,alleviates surface-bulk reaction mismatch,and retards the formation of spinel or rock-salt phases.Structural characterizations with in situ and ex situ methods confirm coherent variations in composition and valence states.Electrochemical analyses demonstrate suppressed voltage hysteresis,smaller polarization,and enhanced cycling stability.Simulations further verify homogeneous ion transport with stabilized phase evolution,collectively validating that surface-phase regulation enabled by tailored concentration gradients effectively mitigates reaction heterogeneity in Li-rich layered cathodes.The findings highlight surface-phase regulation enabled by tailored concentration gradients as a scalable strategy that mitigates reaction heterogeneity in lithium-rich layered cathodes and extends applicability to other cathode systems for large-scale energy storage.展开更多
The pre-existingα-Fe crystals have important effects on the precipitation and growth of nanocrystals and finally determine the comprehensive soft magnetic properties(SMPs)of the nanocrystalline alloys(NAs).In this wo...The pre-existingα-Fe crystals have important effects on the precipitation and growth of nanocrystals and finally determine the comprehensive soft magnetic properties(SMPs)of the nanocrystalline alloys(NAs).In this work,a high content of Cu elements has been added to Nanomet-type alloys to enhance the gradient heterogeneity in order to well control the nanocrystalline process of amorphous alloys.Crystallization kinetics reveal that α-Fe crystals in the free-side layer exhibit higher nucleation and growth activation energies,leading to a slower crystallization rate than in the wheel-side layer.This inhomogeneous crystallization behavior reduces the uneven distribution of α-Fe crystals in the as-spun high Cu content ribbons.Consequently,the Fe82.5Si3.5B9P2C1Cu1.7 alloy achieves superior SMPs through nanocrystallization,including high Bs(~1.82 T),low Hc(10,000@1 kHz)across wide TA and tA ranges.Compared to low-temperature long-time and lowtemperature short-time heat treatments,high-temperature short-time heat treatment results in better SMPs.This is because it intensifies the competition between the fast nucleation/growth of newα-Fe crystals and the slower growth of pre-existing crystals.These findings deepen the understanding of crystallization processes in gradient inhomogeneous materials and guide the optimization of annealing processes for improved performance in Fe-based NAs.展开更多
The effects of plate surface mechanical rolling treatment(P-SMRT)on the microstructure and tribological behavior of Inconel 625 alloy were investigated.The results reveal that P-SMRT induced the formation of a gradien...The effects of plate surface mechanical rolling treatment(P-SMRT)on the microstructure and tribological behavior of Inconel 625 alloy were investigated.The results reveal that P-SMRT induced the formation of a gradient nanostructure(GNS)strengthening layer with a thickness of 700μm on the surface of Inconel 625 alloy.The GNS formation was driven by the interaction between deformation twins and dislocations,leading to the development of shear bands that transformed into ultrafine grains and nanograins.The hardness of the samples with GNS was 192.7%higher than that of the untreated samples.In addition,the tribological properties of the P-SMRT and untreated samples were investigated through dry sliding friction and wear tests.These findings indicate that the P-SMRT induced GNS accommodated greater strain,reduced strain localization,and inhibited surface material exfoliation and transfer,thereby significantly enhancing the wear resistance of Inconel 625 alloy.展开更多
Dear Editor,Mountain systems have long been refuges for many species,often viewed as"islands"that promote speciation due to geographic isolation(Rahbek et al.,2019).Their high environmental heterogeneity fos...Dear Editor,Mountain systems have long been refuges for many species,often viewed as"islands"that promote speciation due to geographic isolation(Rahbek et al.,2019).Their high environmental heterogeneity fosters centers of endemism,and they harbor over 85%of global species diversity(Zhao et al.,2022).Consequently,mountains are key systems for exploring biodiversity patterns along elevational gradients,where species richness often follows four recognized models:monotonic decrease,unimodal pattern(forward and backward peak patterns),and low plateau followed by a decrease along the elevational gradient(McCain et al.,2010).展开更多
The development of intelligent electromagnetic skins demands scalable films integrating gigahertz(GHz)-terahertz(THz)wave absorption,electromagnetic interference(EMI)shielding,and programmable actuation.Here,we report...The development of intelligent electromagnetic skins demands scalable films integrating gigahertz(GHz)-terahertz(THz)wave absorption,electromagnetic interference(EMI)shielding,and programmable actuation.Here,we report a bioinspired bamboo-like layered-gradient system fabricated via scalable vacuum filtration,in which two types of films are constructed with distinct functionalities:a low-poly(3,4-ethylenedioxythiophene)(PEDOT)content film for microwave absorption and a high PEDOT content film for conductive network-enabled EMI shielding.The films precisely assemble Al-Fe3O4nanosheets,aramid nanofibers,and PEDOT into an asymmetric architecture.A monotonic through-thickness gradient in composition creates a tailored impedance profile and strong anisotropy while minimizing conductive filler content.This design achieves effective microwave absorption at low PEDOT loading(minimum reflection loss:−56.6 dB at 2.2 mm in the X-band).With increased PEDOT content,a percolative network is constructed,enabling Joule heating(233℃at 20 V)and efficient EMI shielding(42.0 dB in the GHz band and 57.8 dB in the THz band).Beyond electromagnetic performance,the gradient architecture enables programmable,ethanol-triggered anisotropic actuation via differential swelling.The films also exhibit excellent thermal stability,mechanical robustness,and flexibility,ensuring reliability in harsh environments.Collectively,this gradient architecture provides a scalable platform for intelligent electromagnetic skins integrate magnetic-dielectric coupling,conductive network tuning,and stimuli-responsive actuation.展开更多
For Li metal battery,Li metal anodes severely suffer from dendritic growth due to heterogeneous electrodeposition,which inhibits their development and application.While extensive studies for Li dendrite suppression em...For Li metal battery,Li metal anodes severely suffer from dendritic growth due to heterogeneous electrodeposition,which inhibits their development and application.While extensive studies for Li dendrite suppression empirically utilize 3D hosts to homogenize the micro-scaled electric field within the host,the inherent correlation between host structure and electric field distribution and underlying principles remains elusive,and the corresponding design of hosts to enhance the electric effects remains challenging.Here,the host microstructure-electric field correlations are established via COMSOL simulations and demonstrate the enhanced redistribution of the electric field through structural redesign of hosts.Based on a structure model,an enhanced gradient electric field host(EGHx)with a supercontinuous gradient pore architecture is fabricated with the assistance of the porogen dissolution method,which achieves a self-leveling-like Li deposition through spatially programmed charge redistribution.Through further structural optimization,the EGH2(with 2 wt%porogen)exhibits an~98%Coulombic efficiency(CE)over 350 cycles(1 mA cm-2,1 mAh cm-2).Further multidimensional testing with argon protection reveals the role of the host in modulating solid-electrolyte interphase(SEI)composition.Accordingly,the EGH2 enables stable dendrite-free Li plating/stripping behaviors for 2100 h.The assembled full cell and pouch cell also display stable cycling performance with an LFP cathode.展开更多
摘要The former plant population survey has shown that three genetically-related species, Caraganamicrophylla Lam., C. davazamcii Sancz. and C. korshinskii Kom., form a geographical replacement series inNei Mongol Plateau. The present study on population distribution, taxonomy, morphology, development andgenetic structure demonstrated that the geographical distribution of these three species was successiveand in gradual change, thus forming a geographical cline which extended from the east to the west of NeiMongol Plateau. With an analysis of climate change over time, it was considered that the formation of thisgeographical cline was a result of plant adaptation to its natural environment.
基金co-supported by the National Natural Science Foundation of China(Nos.52305421 and 52175363)the General Research Fund of Hong Kong,China(No.15223520)the projects from the Hong Kong Polytechnic University,China(Nos.4-W418,1-ZE1W,4-WZ4W and 1-CD4H)。
摘要Gradient microstructures strengthened by serrated Grain Boundaries(GBs)were achieved through a combination of Gradient Strain Deformation(GSD)and Serration Heat Treatment(SHT),with particular focus on microstructural evolution,underlying mechanisms,and the critical influencing factors.Dynamic recrystallization governed the microstructural evolution in the fine-grained and transition regions during GSD,where multiple nucleation mechanisms were active.Plastic deformation facilitated the dissolution ofγ'phase in fine-grained regions,ultimately resulting in its morphological transformation.During the subsequent SHT,serrated GBs formed within the gradient microstructures produced by prior GSD without disrupting the grain size gradient,thereby enhancing creep resistance.Two distinct mechanisms associated withγ'gbparticles governed the formation of the serrations at GBs.Owing to the stronger dragging effect of grain boundary junctions in fine-grained regions,the amplitude and wavelength of serrations in these regions were smaller than those in coarse-grained regions.Moreover,the formation of serrations exhibited a strong dependence on the inherent properties of the GBs.The random high-angle grain boundaries(HAGBs)with misorientation angles in the range of 30-59°tended to become serrated more easily during SHT due to their high mobility and the accelerated precipitation ofγ'gbparticles at them.Low-ΣHAGBs and low-angle GBs were not prone to form serrations.In particular,serration formation was completely inhibited atΣ3 twin boundaries due to their extremely low mobility and the absence ofγ'gbparticles.
摘要Liverworts are an important component of terrestrial ecosystems worldwide.They have adapted to and diversified in a wide variety of environments.Investigating variation in net diversification rate is a major goal of biogeographers and ecologists but such investigation is lacking for liverworts at a global scale.Here,we explore global geographic patterns of mean diversification rate(MDR)within genera of liverworts,which are one of the earliest lineages of the extant land plants,and its relationship with latitude,climatic conditions,and regional species richness.We collated species lists of liverworts for each of 390 geographic units(primarily countries,provinces or states)across the world.We related MDR to geographic and current and historical climatic variables,assessed the relative importance of different sets of climatic variables on MDR,and explored the effect of MDR on species richness after accounting for major climatic factors.We analyzed the data with correlation and regression analyses,and structural equation modeling approach.We find that MDR peaks at tropical latitudes and in humid and hot environments,and that at a global scale current climate,temperature-related variables,and climatic seasonality explained more variation in MDR than Quaternary climate change,precipitation-related variables,and climatic extremes,respectively.In addition,we find a positive relationship between MDR and liverwort species richness,with the latter being directly influenced more strongly by climate than by MDR.Most importantly,we find that tropical regions of high liverwort diversity also have high current diversification rates,suggesting ongoing niche occupation.The above-described patterns are similar between the New World and Old World and between the eastern and western parts of the Old World.Our study highlights that tip diversification rates provide a complementary aspect to understand the evolution of liverwort diversity to that recovered by studying phylogenetic diversity and species richness.
基金supported by the the National Natural Science Foundation of China(T2288102,32425031,32301113,82172511)the Science and Technology Inno-vation Project of Shanghai Science and Technology Committee(24CL2900800,25CL2900700)+1 种基金the Zhejiang Natural Science Founda-tion(Z25E030005)the Shanghai Sailing Program(23YF1409700).
摘要The tissues spanning from tendon to bone exhibit a highly specialized extracellular matrix(ECM)architecture,characterized by hierarchical collagen alignment and a gradient mineral composition,which together enable efficient force transfer and guide spatially organized cellular phenotypes.However,recapitulating such complex multi-scale organization and compositional gradients to achieve integrated soft-hard tissue remains challenging.Here,we report the de novo construction of biomimetic collagen-mineral matrices that mimic both the hierar-chical organization and mineral gradient distribution of the native tendon-to-bone ECM.Through synergistic electro-assembly and post-treatment,collagen molecules self-organized into aligned fibrillar matrices with multi-scale architecture,replicating tendon-side morphology while providing robust tensile mechanics.At the opposing end,intrafibrillar and interfibrillar minerals were spatially patterned to emulate the mineral gradient from tendon to bone.This structural and compositional continuum enables smooth mechanical transition across the soft-hard tissue interface and promotes region-specific regeneration of aligned tendon-like tissue,fibrocartilage and bone.In vivo studies in rabbit models confirm that these de novo constructed matrices support histological reconstruction of multiple tissues from tendon to bone at the rotator cuff,and significantly improve functional recovery.This work presents a bottom-up biomimetic strategy for engineering multiscale collagen-based scaf-folds and demonstrates the therapeutic potential of de novo constructed matrices for multiple tissue regeneration.
基金Project supported in part by the National Natural Science Foundation of China(Grant Nos.62471144 and 62071124)in part by the Conselho Nacional de Desenvolvimento Científico e Tecnológico(BR)(CNPq)(Grant No.315546/2021-2)。
摘要Magnetic hyperthermia uses magnetic nanoparticles(MNPs)to generate the heat used for damaging cancer cells under an alternating magnetic field.In fact,the MNPs tend to gather at the injection center and also occur the clustering phenomenon at the same time when injecting into tumor tissue,which however can ultimately result in the excessive concentration of heat in the injection site.Thus,this study aims at improving the MNPs concentration distribution after the injection behavior by considering the action of a static gradient magnetic field,and finally optimizes both temperature situation and thermal damage degree for tumor tissue during magnetic hyperthermia.The MNPs distribution inside a proposed liver tumor is simulated by adopting a Monte Carlo method with adaptive step size,which consists of enough number of small size particles used to analyze the behavior of migration,diffusion,and chain-like phenomenon.The research results demonstrate that the introduction of static gradient magnetic field can disperse the MNPs and form a chainlike distribution inside tumor,and can then expand the distribution range of MNPs,thereby optimizing the thermal damage degree of tumor tissue.In addition,a PID controller with proper setting coefficients is also proven to be able to improve the therapeutic effect for hyperthermia by shortening the rising time to the critical temperature when proper coefficients are set properly during therapy.
基金supported by the Postdoctoral Fellowship Program of CPSF(Grant No.GZC20242002),Chinathe Science Foundation of China University of Petroleum,Beijing(Grant No.2462024XKBH005),China+1 种基金the National Science and Technology Major Project of the Ministry of Science and Technology of China(2025ZD1402707)the 2021 AAPG Foundation Grants-in-Aid Program(Roger W.Stoneburner Memorial Grant),United States.
摘要Submarine gas hydrate systems store vast carbon inventories(∼1500–12,400 Gt C)yet pose dual risks as potential geohazard multipliers and climate feedback agents under oceanic warming.Conventional seal assessment fails catastrophically in unconsolidated Quaternary hydrate-bearing sediments due to core-retrieval artifacts,hydrate morphology controls on capillary trapping,and meter-scale heterogeneity unresolved by seismic methods.Here,we pioneer methane carbon isotope(δ13C1)gradients as a dynamic proxy for seal capacity in the Qiongdongnan Basin.Integrating petrographic features,natural gas geochemical characteristics,downhole logging data,and principal component analysis(PCA)from six wells,we:(1)quantified the thermogenic gas contribution of wells W6 and W8 to be 55%–73%,and that of well W1 to be 28%–32%via binary mixing models,(2)establish that methane carbon isotope gradients>0.5‰/m diagnose effective capillary barriers,correlating with zones of pore-throat disconnection,and(3)develop a PCA-integrated logging model(cumulative variance:84.02%,R2=0.78)predicting seal capacity from conventional petrophysical parameters.Furthermore,the results validate a charge-dynamic barrier-mixing accumulation model where thermogenic gas influx elevates hydrate saturation,creating self-sealing horizons that trap underlying microbial gases and subsequently charged thermogenic gases,recorded in diagnostic methane carbon isotope reversals.This approach bridges molecular-scale fractionation and reservoir-scale processes,enabling targeted identification of high-integrity seals for optimized carbon storage and safer hydrate exploitation in rapidly deposited marginal basins.
基金financially supported by the National Natural Science Foundation of China(22378428,22138013)the National Key Research and Development Program of China(2023YFB4104500,2023YFB4104503)+1 种基金the Key Research and Development Program of Shandong Province(2024ZLGX08)the Science and Technology Innovation Project of the Shandong Energy Group Co.,Ltd.(SNKJ2023A03)。
摘要Electrocatalytic CO2 reduction(CO2 RR)toward multi-carbon compounds is a challenging but meaningful route for carbon cycling.Copper-based catalysts are the most promising candidate for C2+generation due to their unique C–C coupling activity,yet the in situ reduction from Cu+ to Cu0 under cathodic potentials causes the catalyst deactivation.Herein,we develop a transient thermal shock strategy to embed Cu+ species into CeO2 lattices,constructing a CuOx/CuCeOxcatalyst with a radial gradient Cu+ -Ov-Ce3+/Ce4+structure.Depth-profiling X-ray photoelectron spectroscopy(XPS)and density functional theory(DFT)calculations reveal that mismatched metal/oxygen diffusion kinetics drive continuous electron transfer from surface Cu+ to bulk Ce3+/Ce4+via oxygen vacancies(Ov),forming a dynamic“self-sacrificial”structure to preserve surface Cu+ states.In CO2-saturated 0.1 M KHCO3,the optimized CuOx/CuCeOx-10 achieves a high C2 Faradaic efficiency(FE)of 85.8%at-1.4 V vs.RHE.In situ attenuated total reflection surface-enhanced infrared adsorption spectroscopy(ATR-SEIRAS)identifies the key intermediates of C2 are*OCCO and*OCCOH,while DFT reveals a drastic reduction of C–C coupling barrier from 0.842 to0.274 eV.This work demonstrates kinetically tailored metal-support interactions,enabling oxidationstate control for pathway-selective catalysis.
基金supported by Natural Science Foundation of Xiamen,China(No.3502Z20227232)the STS Project of Fujian-CAS(No.2023T3018)Bureau of International Cooperation,Chinese Academy of Sciences(No.322GJHZ2022035MI).
摘要Anammox bacteria in constructed wetlands(CWs)play pivotal role in sustainable nitrogen transformation,yet existing studies lack comprehensive analysis of environmental gradients and microbial interactions,both key factors in anammox bacteria enrichment.This study investigated the mechanisms driving anammox bacteria enrichment in lab-scale simulated CWs treating high-nitrogen wastewater,focusing on bacterial community re-sponses across wetland layers with various strategies,including continuous up-flow influent,nitrogen loading increase,effluent recirculation,intermittent influent,and anammox bacteria inoculation.Results showed that total relative and absolute abundances of anammox bacteria ranged from 0.77%to 12.50%and from 0.13 to 6.46×107 copies/g,respectively.Dissolved oxygen and pH had significant positive correlations with the absolute abundance of anammox bacteria,while organic matter and nitrate negatively impacted their relative abundance.Permutational multivariate analysis of variance indicated that spatial heterogeneity explained more variation in anammox bacteria abundance(43.44%)compared to operational strategies(8.58%).In terms of microbial interactions,60 dominant species exhibited potential correlations with anammox bacteria,comprising 170 interactions(105 positive and 65 negative),which suggested that anammox bacteria generally foster cooperative relationships with dominant bacteria.Notably,significant interspecies interactions were observed between Candidatus Kuenenia(dominant anammox bacteria in CWs)and species within the genera Chitinivibrio-nia and Anaerolineaceae,suggesting that microbial interactions primarily manifest as indirect facilitative effects rather than direct mutualistic relationships.Given that the Normalized Stochasticity Ratio in CWs were<50%,this study inferred that environmental gradients have greater influence on anammox bacteria than microbial interactions.
基金financially supported by the National Natural Science Foundation of China(No.22463006)Qinzhou District Science and Technology Major Special Project in Tianshui City(No.2024-NCKJG-4929)。
摘要This study investigates the evolution of free-radical polymerization under spatially graded conditions by constructing a position-dependent reaction probability model.Given the strong temperature dependence of thermal initiators,spatial temperature variations significantly affect both local monomer reactivity and the macroscopic evolution of polymer structures.Understanding this coupling is crucial for designing gradient-controlled synthesis strategies.The dissipative particle dynamics(DPD)method was employed to investigate free radical polymerization under gradient temperature conditions.IncreasingΔT enhances spatial heterogeneity:high-temperature regions form dense networks with lower molecular weights(Mn and Mw)due to rapid initiation and frequent termination.In contrast,low-temperature regions yield higher molecular weights and expanded chain conformations()resulting from longer radical lifetimes.These structural differences further govern pore evolution:porosity decreases rapidly and reaches lower final values in high-temperature zones,while low-temperature regions exhibit delayed evolution but higher final porosity.This study demonstrates that the precise control of polymer growth orientation,molecular weight distribution,and porous morphology can be achieved by incorporating gradient conditions,thereby establishing a new paradigm for the targeted synthesis of gradient functional materials.
基金financially supported by the National Natural Science Foundation of China(Grants 52503094 and 52462036)the Key Research and Development Program of Ningxia(Grant 2023BSB03035)the Seventh Group Youth Science and Technology Talents Project of Ningxia.
摘要Dielectric polymers commonly suffer from severe performance degradation above 150℃,hindering advanced power systems.Herein,we demonstrate a polyetherimide(PEI)nanocomposite that overcomes this by mimicking the gradient architecture of nacre and bamboo,incorporating a continuous vertical gradient of fluorinated boron nitride nanosheets(BNNS‐F)through sequential electrospinning.This bio‐inspired design not only reinforces mechanical and thermal stability,but also generates a spatially gradient distribution of deep charge traps.The resulting progressive trap energy barrier effectively suppresses charge transport,impedes electrical treeing propagation,and significantly reduces conduction losses at elevated temperatures.Consequently,our continuous gradient PEI/BNNS‐F cg nanocomposite achieves an exceptional breakdown strength(Eb)of 626 MV m−1and a discharged energy density(Ud)of 6.21 J cm−3with 90%efficiency at 150℃,surpassing most reported polymer‐based dielectrics.Remarkably,it retains a high Udof 3.89 J cm−3at 200℃,along with outstanding cycling stability over 10,000 cycles.This work introduces a new paradigm for controlling charge dynamics through continuous gradient structures,enabling high‐performance energy storage under extreme conditions.
基金financially supported by the Key Program of National Natural Science Foundation of China(No.52331004)the National Natural Science Foundation of China-Shandong Joint Fund for Marine Science Research Centers(No.U2106216)+4 种基金the National Natural Science Foundation of China(No.52101188)the Key Program of Natural Science Foundation of Shandong Province of China(Nos.ZR2022ZD12 and ZR2024ZD14)the Key Research and Development Program of Shandong Province(Nos.2023ZLGX05 and 2023CXGC010406)the Taishan Scholars of Climbing Plan(No.tspd20230603)the Fundamental Research Funds for the Central Universities(No.202561098).
摘要Gradient nanocrystalline–amorphous nanostructures are considered to be an effective approach to achieve exceptional strength–plasticity synergy,with significantly improved wear performance.Here,gradient nanostructured Fe-based coatings were successfully fabricated by extremely high-speed-rate laser deposition and remelting.The microstructure evolution along the depth direction varies in a nanocrystalline,equiaxial dendrites,columnar dendrites gradient,respectively.Noticeably,amorphous grain boundaries and carbide nanoprecipitates could be identified within the topmost surface nanocrystalline layer owing to the extremely high cooling rate during remelting,which exhibits the highest hardness and wear resisance(microhardness of ~1136 HV,and wear rate of 4.36×10−6mm3/(m N)).The superior wear resistance is mainly attributed to the synergistic nanocrystalline–amorphous deformation and gradient refinement effects.Meanwhile,multi-scale carbides effectively impede dislocation motion and further improve strength and wear resistance at different depths.This gradient structure provides promising insights into the design of high-performance wear-resistant alloys.
基金supported by the National Natural Science Foundation of China(Nos.42477046,42277406 and 21777188).
摘要Pharmaceutically active compounds have garnered increased attention as emerging contaminants due to their widespread presence and potential ecological impacts.This study conducted a field evaluation under varied rainfall conditions,assessing the effects of rainfall intensity and duration on pharmaceutical concentrations.Grab sampling was complemented by the deployment of diffusive gradients in thin films(DGT)passive samplers along two urban rivers in Beijing,China.Twenty-four target pharmaceuticals were detected,with concentrations ranging from 370 to 686 ng/L in the Beixiao River and 376 to 610 ng/L in the Qing River.Rainfall influenced pharmaceutical concentrations through either dilution or enhancement,depending on local factors.Rainfall had a minimal impact on DGT performance,while biofouling showed compound-specific effects.For about 70%of the pharmaceuticals,hydrophilic poly tetrafluoroethylene(PTFE)membranes used over 9–15 days effectively minimized biofouling influence(Mbiofouled/Mclean>0.8).The effectiveness of DGT for long-term monitoring depended on the biofilm formation time.Overall,DGT proved to be a reliable tool for accurately characterizing pharmaceutical concentrations in dynamic water systems.This study represents the first attempt to evaluate DGT performance for pharmaceuticals under fluctuating concentration scenarios in the field,providing valuable insights into the occurrence and environmental behavior of these contaminants.
基金Project supported by the National Natural Science Foundation of China(Nos.12372069 and 12502072)the Natural Science Foundation of Hunan Province of China(No.2025JJ60048)+1 种基金the Changsha Municipal Natural Science Foundation of China(No.kq2502186)the Postdoctoral Fellowship Program of CPSF(No.GZB20250464)。
摘要The strength and damage tolerance of additively manufactured(AM)alloys are significantly influenced by their heterogeneous microstructures.However,establishing quantitative relationships between these microstructural characteristics and the resulting mechanical properties remains a challenge.Here,a microstructure-based mechanical model is established based on the heterogeneous grain distribution within the melt pool,with particular emphasis on the strain gradient effect arising from the deformation incompatibility between distinct grain regions.The strengthening mechanisms and local deformation response of AM alloys are elucidated with the finite element method(FEM).The strain gradient effect generated by the deformation incompatibility between the columnar and equiaxed grain regions enhances the local stress near the equiaxed-columnar interface,which is an important reason for the overall work hardening.Concurrently,the local stress concentration makes it easier to reach the critical stress for microcrack nucleation at the interface,leading to failure and a lack of synergy between the strength and damage tolerance.The prediction of the crack initiation location based on the simulation results is consistent with the previous experiments.By further quantitatively predicting the comprehensive effects of melt pool size on strength,strain hardening,and damage rate,small-melt-pool structures produce high strength,but microcracks originate early,whereas large-melt-pool structures have weak strengthening effects but fast damage evolution in the later stages of deformation.This study provides a pathway to predict the optimal melt pool size for achieving superior combinations of strength and damage tolerance in AM alloys.
基金sponsored by the financial support from the National Natural Science Foundation of China(No.52307249)National Science Foundation of Shanghai Province(No.23ZR1465900)+2 种基金Chenguang Program of Shanghai Education Development Foundation and Shanghai Municipal Education Commission(No.23CGA25)Fundamental Research Funds for the Central Universities at Tongji UniversityStudents Innovation Training Program of Tongji University(No.202410247028)。
摘要Ultra-thick electrodes(UTEs)hold great promise for high-energy-density lithium-ion batteries(LIBs),yet the practical application is hindered by challenges in precise fabrication and reaction kinetics modification.In this contribution,a solvent-free processing method is introduced to tailor UTEs through layerby-layer fabrication with positive,uniform,and negative gradient porosity from the separator side to the current collector side,denoted as P-UTEs,U-UTEs,and N-UTEs.In contrast to conventional slurry coating,the proposed solvent-free approach effectively circumvents capillary stress,thereby facilitating the fabrication of crack-free UTEs(>300μm)while simultaneously mitigating environmental toxicity concerns.The three-layer N-UTEs(>220μm)with a gradient porosity of(~34%,~31%,~27%)deliver an exceeding areal capacity over 5 m Ah/cm2 at 0.29 mA/cm2 and a high-capacity retention over 62% at 2.9 m A/cm2,indicating a favorable balance between the areal capacity and the high-rate behavior.Detailed mechanistic simulations reveal that the multi-center reaction pathways enabled by enhanced ionic accessibility in N-UTEs significantly improve reaction kinetics.This work offers new insights into the gradient porosity tailoring for high-areal-capacity and high-rate UTEs for the next generation LIBs.
基金supported by the National Natural Science Foundation of China(21875022,22179008)the Yibin‘Jie Bang Gua Shuai’(2022JB004)+2 种基金the support from the High-Level Talent Introduction Project of Yibin(2024YG03)the support from the Postdoctoral Fellowship Program of CPSF(GZB20230931)the Special Support of Chongqing Postdoctoral Research Project(2023CQBSHTB2041).
摘要Lithium-rich layered oxides are promising cathodes for high-energy lithium-ion batteries,yet their applications are hindered by voltage decay,structural instability,and heterogeneous reaction dynamics.These degradations stem from the coexistence of Li2MnO3and LiMO2domains,which exhibit distinct redox kinetics and trigger phase mismatch during cycling.To address this challenge,we propose a tailored concentration gradient design that regulates the spatial distribution of transition metals.Nickel is intentionally enriched near the surface while manganese dominates the interior,creating a coordinated balance between interfacial stability and bulk capacity retention.Regulating Ni content deliberately induces a moderate Li/Ni cation-mixed phase,and the tailored gradient builds a surface composite structure that stabilizes the layered framework and suppresses interfacial degradation.This architecture homogenizes redox activation,alleviates surface-bulk reaction mismatch,and retards the formation of spinel or rock-salt phases.Structural characterizations with in situ and ex situ methods confirm coherent variations in composition and valence states.Electrochemical analyses demonstrate suppressed voltage hysteresis,smaller polarization,and enhanced cycling stability.Simulations further verify homogeneous ion transport with stabilized phase evolution,collectively validating that surface-phase regulation enabled by tailored concentration gradients effectively mitigates reaction heterogeneity in Li-rich layered cathodes.The findings highlight surface-phase regulation enabled by tailored concentration gradients as a scalable strategy that mitigates reaction heterogeneity in lithium-rich layered cathodes and extends applicability to other cathode systems for large-scale energy storage.
基金financially supported by the Central Guidance for Local Technology Development Fund(Grant No.ZYYD2025ZY07)the National Natural Science Foundation of China(Grant No.52261033)+2 种基金Guangdong Basic and Applied Basic Research,China(Grant No.2024B1515120012)the National Key Research and Development Program of China(Grant No.2021YFB3800504)the National Natural Science Foundation of China(Grant No.52192602)。
摘要The pre-existingα-Fe crystals have important effects on the precipitation and growth of nanocrystals and finally determine the comprehensive soft magnetic properties(SMPs)of the nanocrystalline alloys(NAs).In this work,a high content of Cu elements has been added to Nanomet-type alloys to enhance the gradient heterogeneity in order to well control the nanocrystalline process of amorphous alloys.Crystallization kinetics reveal that α-Fe crystals in the free-side layer exhibit higher nucleation and growth activation energies,leading to a slower crystallization rate than in the wheel-side layer.This inhomogeneous crystallization behavior reduces the uneven distribution of α-Fe crystals in the as-spun high Cu content ribbons.Consequently,the Fe82.5Si3.5B9P2C1Cu1.7 alloy achieves superior SMPs through nanocrystallization,including high Bs(~1.82 T),low Hc(10,000@1 kHz)across wide TA and tA ranges.Compared to low-temperature long-time and lowtemperature short-time heat treatments,high-temperature short-time heat treatment results in better SMPs.This is because it intensifies the competition between the fast nucleation/growth of newα-Fe crystals and the slower growth of pre-existing crystals.These findings deepen the understanding of crystallization processes in gradient inhomogeneous materials and guide the optimization of annealing processes for improved performance in Fe-based NAs.
基金supported by the National Natural Science Foundation of China(Nos.52265049,12162023)Gansu Provincial Talent Project,China(No.2024QNTD44)+4 种基金Industrial Support Program for Colleges and Universities in Gansu Province,China(No.2022CYZC-26)Key Research and Development Plan of Gansu Province-Industrial Projects,China(No.23YFGA0054),Lanzhou University of Technology Support Plan for Distinguished Young Scholars,China(No.HLJQ2402)Natural Science Foundation of Gansu Province,China(No.23JRRA922)Gansu Basic Research Innovation Group Project,China(No.23JRRA757)the Key Talent Projects of Gansu Province,China,and Incubation Program of Excellent Doctoral Dissertation-Lanzhou University of Technology,and Research Institute for Advanced Manufacturing of The Hong Kong Polytechnic University,China(No.1-CD4P).
摘要The effects of plate surface mechanical rolling treatment(P-SMRT)on the microstructure and tribological behavior of Inconel 625 alloy were investigated.The results reveal that P-SMRT induced the formation of a gradient nanostructure(GNS)strengthening layer with a thickness of 700μm on the surface of Inconel 625 alloy.The GNS formation was driven by the interaction between deformation twins and dislocations,leading to the development of shear bands that transformed into ultrafine grains and nanograins.The hardness of the samples with GNS was 192.7%higher than that of the untreated samples.In addition,the tribological properties of the P-SMRT and untreated samples were investigated through dry sliding friction and wear tests.These findings indicate that the P-SMRT induced GNS accommodated greater strain,reduced strain localization,and inhibited surface material exfoliation and transfer,thereby significantly enhancing the wear resistance of Inconel 625 alloy.
基金supported by grants from the National Natural Science Foundation of China(Grant No.32360333)the Guizhou Provincial Science and Technology Projects(Grant Nos.ZK[2022]540 and[2023]099)+1 种基金the Survey of Amphibian and Reptile Resources in Leigongshan National Nature Reserve and Literature Publishing Services(P5226002023000019)the Guizhou Provincial Science and Technology Innovation Talent Team Construction Project 2024[Qian Ke He Talent CXTD(2025)053].
摘要Dear Editor,Mountain systems have long been refuges for many species,often viewed as"islands"that promote speciation due to geographic isolation(Rahbek et al.,2019).Their high environmental heterogeneity fosters centers of endemism,and they harbor over 85%of global species diversity(Zhao et al.,2022).Consequently,mountains are key systems for exploring biodiversity patterns along elevational gradients,where species richness often follows four recognized models:monotonic decrease,unimodal pattern(forward and backward peak patterns),and low plateau followed by a decrease along the elevational gradient(McCain et al.,2010).
基金granted by National Natural Science Foundation(NSFC,51873004).
摘要The development of intelligent electromagnetic skins demands scalable films integrating gigahertz(GHz)-terahertz(THz)wave absorption,electromagnetic interference(EMI)shielding,and programmable actuation.Here,we report a bioinspired bamboo-like layered-gradient system fabricated via scalable vacuum filtration,in which two types of films are constructed with distinct functionalities:a low-poly(3,4-ethylenedioxythiophene)(PEDOT)content film for microwave absorption and a high PEDOT content film for conductive network-enabled EMI shielding.The films precisely assemble Al-Fe3O4nanosheets,aramid nanofibers,and PEDOT into an asymmetric architecture.A monotonic through-thickness gradient in composition creates a tailored impedance profile and strong anisotropy while minimizing conductive filler content.This design achieves effective microwave absorption at low PEDOT loading(minimum reflection loss:−56.6 dB at 2.2 mm in the X-band).With increased PEDOT content,a percolative network is constructed,enabling Joule heating(233℃at 20 V)and efficient EMI shielding(42.0 dB in the GHz band and 57.8 dB in the THz band).Beyond electromagnetic performance,the gradient architecture enables programmable,ethanol-triggered anisotropic actuation via differential swelling.The films also exhibit excellent thermal stability,mechanical robustness,and flexibility,ensuring reliability in harsh environments.Collectively,this gradient architecture provides a scalable platform for intelligent electromagnetic skins integrate magnetic-dielectric coupling,conductive network tuning,and stimuli-responsive actuation.
基金LiaoNing Revitalization Talents Program(XLYC2202003)National Natural Science Foundation of China(NSFC,U24B20198)+1 种基金Fundamental Research Funds for the Central Universities(DUT23LAB612)National Key Research and Development Program of China(2022YFB4101602)。
摘要For Li metal battery,Li metal anodes severely suffer from dendritic growth due to heterogeneous electrodeposition,which inhibits their development and application.While extensive studies for Li dendrite suppression empirically utilize 3D hosts to homogenize the micro-scaled electric field within the host,the inherent correlation between host structure and electric field distribution and underlying principles remains elusive,and the corresponding design of hosts to enhance the electric effects remains challenging.Here,the host microstructure-electric field correlations are established via COMSOL simulations and demonstrate the enhanced redistribution of the electric field through structural redesign of hosts.Based on a structure model,an enhanced gradient electric field host(EGHx)with a supercontinuous gradient pore architecture is fabricated with the assistance of the porogen dissolution method,which achieves a self-leveling-like Li deposition through spatially programmed charge redistribution.Through further structural optimization,the EGH2(with 2 wt%porogen)exhibits an~98%Coulombic efficiency(CE)over 350 cycles(1 mA cm-2,1 mAh cm-2).Further multidimensional testing with argon protection reveals the role of the host in modulating solid-electrolyte interphase(SEI)composition.Accordingly,the EGH2 enables stable dendrite-free Li plating/stripping behaviors for 2100 h.The assembled full cell and pouch cell also display stable cycling performance with an LFP cathode.