The migration mechanisms of ore-forming fluids have long been a focus in the field of ore deposit studies.Calcite is ubiquitously present in various types of rocks in the lithosphere,and the underlying mechanisms of i...The migration mechanisms of ore-forming fluids have long been a focus in the field of ore deposit studies.Calcite is ubiquitously present in various types of rocks in the lithosphere,and the underlying mechanisms of its influence on fluid migration are of crucial importance.While previous studies have revealed that salinity changes can modulate fluid migration,the underlying mechanisms remain poorly understood.We employ molecular dynamics simulations to elucidate how salinity variations in ore-forming fluids modulate the adsorption onto calcite nanopore walls,thereby revealing the microscopic mechanisms governing ore fluid transport through calcite nano-fractures.The results show that the adsorption energy Eint of the solution on the calcite surface increased from -14,948.84±182.48 kcal/mol to -12,144.08±118.2 kcal/mol as salinity increased,which is conducive to the long-range transport of the fluid in the calcite nanopore.展开更多
The equilibrium dynamics and nonlinear rheology of unentangled polymer blends remain inadequately understood,especially regarding the influence of short-chain matrix length N_(S) on the structure and rheological behav...The equilibrium dynamics and nonlinear rheology of unentangled polymer blends remain inadequately understood,especially regarding the influence of short-chain matrix length N_(S) on the structure and rheological behavior of dispersed long chains.Using molecular dynamics simulations based on the Kremer-Grest model,we systematically explore the N_(S)-dependence of static conformations,equilibrium dynamics,and nonlinear shear responses in unentangled long-chain/short-chain polymer blends.Our results demonstrate a decoupling between the static and dynamic sensitivity to N_(S):while the static chain size,R_g,follows Flory theory with slight swelling at small N_(S) due to incomplete excluded volume screening,the diffusion coefficient,D,and the relaxation time,τ_(0),exhibit a strong,non-monotonic N_(S)-dependence,transitioning from monomeric friction dominance at small N_(S) to collective segmental rearrangement at large N_(S).Additionally,we observe partial decoupling between the viscous and normal stress responses:while the zero-shear viscosity,η,is strongly N_(S)-dependent,the first and second normal stress coefficients,Ψ_(1) and Ψ_(2),collapse onto universal curves when scaled by the dimensionless shear rate,γτ_(0),suggesting a common mechanism of orientation and stretching.Under shear,long chains compress in the vorticity direction λ_(z)~Wi^(-0.2),which reduces collision frequency and contributes to shear thinning,while the scaling of weaker orientation resistance m_(G)~Wi^(0.35)reflects hydrodynamic screening by the short-chain matrix.These findings highlight the limitations of single-chain models and emphasize the necessity of considering N_(S)-dependent matrix dynamics and flow-induced structural changes in understanding the rheology of unentangled polymer blends.展开更多
The study presents an analysis of the spatiotemporal evolution of vegetation cover in the Izarene forest,using LANDSAT satellite images collected for the years 1984,2003,and 2022.The methodological approach is based o...The study presents an analysis of the spatiotemporal evolution of vegetation cover in the Izarene forest,using LANDSAT satellite images collected for the years 1984,2003,and 2022.The methodological approach is based on the use of ArcGIS 10.8 software for processing multispectral images,as well as the calculation of the Normalized Difference Vegetation Index(NDVI),which enables the observation of variations in vegetation cover over time.The findings show that biodiversity is pretty abundant,but they also show that some places with low vegetation density are under a lot of stress.Due in large part to overuse of natural resources,uncontrolled human activity,and environmental factors,these regions seem to be more vulnerable to degradation.However,a decrease in deforestation over the past 20 years is revealed by comparing the two periods(1984–2003 and 2003–2022).The participation of governmental agencies,especially the Department of Water and Forests,through concrete projects like reforestation,forest fire prevention,and awareness-raising campaigns among local communities,is responsible for this progress.In several areas,these measures have stabilized or even improved the state of the vegetation.The analysis emphasizes how crucial sustainable,integrated,and participatory management is to protecting the Izarene forest,which is a significant resource for maintaining the region’s ecological balance.展开更多
In response to the increasing demand for hadron therapy facilities,significant efforts have been directed toward enhancing the performance of high-gradient and high-transmission injectors for light ion beams.For carbo...In response to the increasing demand for hadron therapy facilities,significant efforts have been directed toward enhancing the performance of high-gradient and high-transmission injectors for light ion beams.For carbon ion irradiations,which offer greater radiobiological efficiency in tumor treatment,recent research has focused on developing high-production sources of fully stripped C^(6+)ions and highly compact,high-frequency RFQ cavities.This study explores the design possibilities of a carbon ion acceleration section using 750 MHz Interdigital H-mode Drift Tube Linacs(IH-DTLs)as a high-efficiency solution for accelerating ions in the 5-10 MeV per nucleon energy range.A particle-tracking routine based on the TRAVEL code was developed to design the acceleration line through a tailored KONUS-type configuration.Three design solutions were proposed and compared,exploring different alternatives regarding the use of a MEBT to match the output beam phase space of the RFQ to the optics of the line,as well as varying considerations for magnetic systems to focus the beam.Additionally,the compatibility of the proposed solutions with the existing design of the carbon ion bent-linac for hadron therapy was assessed.展开更多
Like-charge pairing is a physical manifestation of the unique solvation properties of certain ion pairs in water.Water's high dielectric constant and related charge screening capability significantly influence the...Like-charge pairing is a physical manifestation of the unique solvation properties of certain ion pairs in water.Water's high dielectric constant and related charge screening capability significantly influence the interaction between like-charged ions,with the possibility to transform it-in exceptional cases when noncovalent interactions are involved-from repulsion to attraction.Guanidinium cations(Gdm^(+))represent a quintessential example of such like-charge pairing due to their specific geometry and electronic structure.In this work,we present experimental validation and quantification of Gdm^(+)-Gdm contact ion pairing in water utilizing nuclear magnetic resonance(NMR)spectroscopy complemented by molecular dynamics(MD)simulations and density functional theory(DFT)calculations.The observed Gdm^(+)-Gdm^(+)interaction is attractive albeit weak-about 0.5 kJ·mol^(-1)-which aligns with theoretical estimation from MD simulations.We contrast the behavior of Gdm^(+) with that of NH_(4)^(+) cations,which exhibit no contact ion pairing in water.DFT calculations predict that the NMR chemical shift of Gdm^(+) dimers is different than that of monomers,in agreement with NMR titration curves that display a nonlinear Langmuir-like behavior.Additionally,we conducted cryo-electron microscopy-to our knowledge,for the first time-on concentrated oligoarginines R9,which,unlike nona-lysines K9,exhibit aggregation in water.These results point to like charge pairing of the guanidinium side chain groups,as corroborated also by MD simulations and free energy calculations.展开更多
THE mechanical response and deformation mechanisms of pure nickel under nanoindentation were systematically investigated using molecular dynamics(MD)simulations,with a particular focus on the novel interplay between c...THE mechanical response and deformation mechanisms of pure nickel under nanoindentation were systematically investigated using molecular dynamics(MD)simulations,with a particular focus on the novel interplay between crystallographic orientation,grain boundary(GB)proximity,and pore characteristics(size/location).This study compares single-crystal nickel models along[100],[110],and[111]orientations with equiaxed polycrystalline models containing 0,1,and 2.5 nm pores in surface and subsurface configurations.Our results reveal that crystallographic anisotropy manifests as a 24.4%higher elastic modulus and 22.2%greater hardness in[111]-oriented single crystals compared to[100].Pore-GB synergistic effects are found to dominate the deformation behavior:2.5 nm subsurface pores reduce hardness by 25.2%through stress concentration and dislocation annihilation at GBs,whereas surface pores enable mechanical recovery via accelerated dislocation generation post-collapse.Additionally,size-dependent deformation regimes were identified,with 1 nm pores inducing negligible perturbation due to rapid atomic rearrangement,in contrast with persistent softening in 2.5 nm pores.These findings establish atomic-scale design principles for defect engineering in nickel-based aerospace components,demonstrating how crystallographic orientation,pore configuration,and GB interactions collectively govern nanoindentation behavior.展开更多
In this study,we perform particle-resolved simulations of settling spheroidal particles,considering oblate and prolate spheroids and spheres,and investigate the shape effect on the particle dynamics in suspensions wit...In this study,we perform particle-resolved simulations of settling spheroidal particles,considering oblate and prolate spheroids and spheres,and investigate the shape effect on the particle dynamics in suspensions with volume fraction 1%and 5%.We first examine the single-point statistics of the translational and rotational motion of the settling particles.The horizontal velocity has a symmetrical distribution with standard deviation dependent on the particle shape.The greater horizontal velocity fluctuations of the non-spherical particles,compared to that of spheres,are attributed to the horizontal drift of settling spheroids with oblique orientations induced by the fluid-particle and particle-particle interactions.The fluctuation of particle vertical velocity,instead,is skewed under the effect of wake-induced hydrodynamic interactions.Further,we explore the particle pair statistics,which demonstrate the formation of column-like particle micro-structures for the lowest volume fraction considered.This clustering is more pronounced for spheroidal particles than spheres,due to the stronger attractions among vertically-aligned settling spheroids.Moreover,the particle pair statistics are directly related to the collision rate among the dispersed particles.The local accumulation of oblate/prolate spheroids serves as the major mechanism to promote the particle-particle collisions in dilute suspensions.展开更多
This paper presents an adaptive multi-agent coordination(AMAC)strategy suitable for complex scenarios,which only requires information exchange between neighbouring robots.Unlike traditional multi-agent coordination me...This paper presents an adaptive multi-agent coordination(AMAC)strategy suitable for complex scenarios,which only requires information exchange between neighbouring robots.Unlike traditional multi-agent coordination methods that are solved by neural dynamics,the proposed strategy displays greater flexibility,adaptability and scalability.Furthermore,the proposed AMAC strategy is reconstructed as a time-varying complex-valued matrix equation.By introducing a dynamic error function,a fixed-time convergent zeroing neural network(FTCZNN)model is designed for the online solution of the AMAC strategy,with its convergence time upper bound derived theoretically.Finally,the effectiveness and applicability of the coordination control method are demonstrated by numerical simulations and physical experiments.Numerical results indicate that this method can reduce the formation error to the order of 10^(-6)within 1.8 s.展开更多
Ionic liquids(ILs)have exhibited great application potential in many fields due to their unique properties.Molecular dynamics(MD)simulation has been widely employed to investigate their microscopic structure.However,c...Ionic liquids(ILs)have exhibited great application potential in many fields due to their unique properties.Molecular dynamics(MD)simulation has been widely employed to investigate their microscopic structure.However,classical molecular dynamics simulations struggle to accurately describe the complex interactions in ILs using the existing parameterized force fields.Recently,the MD simulations based on machine learning force fields(MLFFs)trained by first-principles calculations have attracted considerable attentions due to their abilities to balance computational accuracy and efficiency.Herein,we report the Bayesian-based MLFFs which can be successfully applied in IL systems and accelerate MD simulation.The calculated atomic forces,structures,and vibrational behaviors were validated to match the accuracy of firstprinciples calculations.Properties of the imidazolium-based ILs,including density,self-diffusion coefficients,viscosity,and radial distribution functions were predicted at the extended scales.Z-bonds that describe the unique structures in ILs were analyzed and the influences of Cpositions,temperature,and solvent H2O on Z-bonding configurations were systematically investigated.Our results confirmed that MLFFs presented the strong feasibility to investigate the large and complex systems,especially to predict structures and properties of the ILs.And the procedure described for MLFFs provides valuable guidance for researchers who are studying ILs.展开更多
Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implem...Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implementation remains a significant challenge.Herein,we construct a free-standing polymer–inorganic hybrid photoelectrode with a direct Z-scheme heterostructure to develop high-efficiency PALSBs.Specifically,polypyrrole(PPy)is in situ vapor-phase polymerized on the surface of N-doped TiO_(2) nanorods supported on carbon cloth(N-TiO_(2)/CC),thereby forming a well-defined p–n heterojunction.This architecture efficiently facilitates the carrier separation of photo-generated electron–hole pairs and significantly enhances carrier transport by creating a built-in electric field.Thus,the PPy@N-TiO_(2)/CC can simultaneously act as a photocatalyst and an electrocatalyst to accelerate the reduction and evolution of sulfur,enabling ultrafast sulfur redox dynamics,as convincingly validated by both theoretical simulations and experimental results.Consequently,the PPy@N-TiO_(2)/CC PALSB achieves a high discharge capacity of 1653 mAh g^(−1),reaching 98.7%of the theoretical value.Furthermore,5 h of photo-charging without external voltage enables the PALSB to deliver a discharge capacity of 333 mAh g^(−1),achieving dual-mode energy harvesting capabilities.This work successfully integrates solar energy conversion and storage within a rechargeable battery system,providing a promising strategy for sustainable energy storage technologies.展开更多
SalicS1 is a genetically encoded,ratiometric FRET biosensor that brings salicylic acid(SA)research to the same real-time imaging standard long available for ABA and GA.Built through a modular Golden Gate platform and ...SalicS1 is a genetically encoded,ratiometric FRET biosensor that brings salicylic acid(SA)research to the same real-time imaging standard long available for ABA and GA.Built through a modular Golden Gate platform and informed by NPR-NIMIN structural biology,SalicS1 achieves SA specificity,tunable affinity,reversibility,and non-perturbing expression in Arabidopsis.Using this sensor,pathogen infection,non-adapted fungal challenge,and aphid feeding are shown to elicit spatially propagating SA surges rather than purely local accumulation,revealing a tissue-level organization of immune signaling that bulk assays could not resolve.SalicS1 therefore provides a broadly deployable tool for dissecting the geometry,timing,and genotype dependence of SA-mediated plant defense.展开更多
The structural changes in the CaO-SiO_(2)-Al_(2)O_(3)-MgO slag system with varying CaO contents were investigated through molecular dynamics(MD)simulations,and its effect on the dissolution behavior of alumina inclusi...The structural changes in the CaO-SiO_(2)-Al_(2)O_(3)-MgO slag system with varying CaO contents were investigated through molecular dynamics(MD)simulations,and its effect on the dissolution behavior of alumina inclusions was characterized by the Kullback-Leibler(KL)divergence.The slag structure analysis revealed that the[AlO]tetrahedral structure was the primary network structure in the slag.With increasing the CaO content,the non-bridge oxygen(NBO)content in the slag structure increases,and the bridge oxygen(BO)content decreases,thereby reducing the complexity of the slag network structure.Raman spectroscopy detection verifies the results of the MD simulations.The results indicated that the dissolution rate of alumina inclusions accelerates with increasing the CaO content in the slag,owing to the reduced complexity of the slag network structure and the enhanced interatomic interactions.The simulation results for the dissolution of alumina inclusions were consistent with theoretical calculations based on the slag inclusion capacity and the dimensionless dissolution rate of inclusions.Radial distribution function analysis demonstrated that the interaction between atoms in the slag system and alumina inclusions strengthens,increasing the dissolution rate of alumina inclusions.The[AlO_(6)]octahedral structure of the alumina inclusions is disrupted,forming BO structures,which in turn enhances the complexity of the slag network structure,slowing the dissolution rate of alumina inclusions.In contrast,the slag system with a higher CaO content has a relatively simpler network structure,promoting faster alumina inclusion dissolution.展开更多
This study investigates the influence of hydrogen concentration at grain boundaries on the sensitivity of polycrystalline iron to hydrogen embrittlement using molecular dynamics simulations.These simulations reveal th...This study investigates the influence of hydrogen concentration at grain boundaries on the sensitivity of polycrystalline iron to hydrogen embrittlement using molecular dynamics simulations.These simulations reveal the diffusion behavior of hydrogen atoms at grain boundaries and their consequential impact on the hydrogen embrittlement sensitivity of iron alloys.The findings indicate that as the hydrogen concentration increases,both the yield strength and ultimate tensile strength of Fe-H alloys exhibit a declining trend.Moreover,the capture of hydrogen atoms at the grain boundaries significantly influences the fracture toughness of the material and promotes the formation and propagation of cracks.This study provides a novel theoretical basis for understanding and predicting the hydrogen embrittlement behavior of iron-based materials in hydrogen-rich environments,offering valuable insights for the design and development of Fe alloys with enhanced resistance to hydrogen embrittlement.展开更多
Atomic vacancies in oxides induce deviations from ideal stoichiometry,critically influencing their functional properties in applications such as energy storage-conversion,catalysis,and electronic devices.The dynamic b...Atomic vacancies in oxides induce deviations from ideal stoichiometry,critically influencing their functional properties in applications such as energy storage-conversion,catalysis,and electronic devices.The dynamic behavior of these vacancies as main mass transport mediums to exchange chemical species with surroundings under operating conditions is central to oxide redox reactions running with the Mars-van Krevelen(MvK)mechanism;yet in-situ atomic-scale monitoring of the vacancy dynamics and vacancy-induced secondary defects within oxides remains challenging due to both their rapid transport kinetics at buried subsurface/interface and characterization difficulties,arising from the insulating nature of bulk oxides and the spatial-resolution requirement in reaction conditions.These challenges hinder precise defect engineering for the performance optimization of functional oxides.In this review,recent advancements in tracking oxygen vacancy and vacancyinduced secondary defects dynamics in oxides,including surface steps,cation vacancies,interfacial dislocations,ledges,and interfaces,have been summarized.The dynamic interconversion of defects and their synergistic effects on surface/subsurface/interface evolution are mainly discussed.The aim of this review is to enhance understanding of defect dynamics and their pivotal role in modulating structural dynamics and surface reaction reactivity,which is highly relevant to the catalyst activity/selectivity/stability evaluation of functional oxide catalysts for electroreduction and catalytic oxidation reactions.Finally,strategies to control buried subsurface and interfacial defects(interface engineering)through tailored surface reactions are proposed,offering new pathways to customize the performance of advanced oxide-based materials.展开更多
In igneous-intruded coal seams,coal undergoes significant metamorphism,which critically alters its pore structure and oxygen consumption dynamics,thereby elevating its spontaneous combustion tendency.This study invest...In igneous-intruded coal seams,coal undergoes significant metamorphism,which critically alters its pore structure and oxygen consumption dynamics,thereby elevating its spontaneous combustion tendency.This study investigates the specific surface area,pore volume,structure complexity/connectivity,heterogeneity/local features of pore size distribution,and oxygen consumption dynamics of igneous metamorphic coal through N_(2)/CO_(2) isothermal adsorption tests and low-temperature oxidation experiments,and elucidates the influence mechanisms of pore structure evolution on oxygen consumption dynamics during low-temperature oxidation.With increasing metamorphic degree,igneous metamorphic coal exhibits a more pronounced reduction in specific surface area during oxidation,while the increase in structure complexity due to coal-oxygen reactions is suppressed.Thermally metamorphic coal demonstrates accelerated oxygen consumption,with oxidation amplifying the difference in reaction rates compared to raw coal.Key mechanisms include oxidation-induced reduction in mesopore complexity and micropore volume,decreased dominance of small-pore-volume apertures,and increased heterogeneity,collectively leading to a lower half-oxygen-consuming temperature and steeper oxygen consumption curves.Simultaneously,increased pore volume/complexity and reduced uniformity/connectivity act synergistically to enhance oxygen consumption capacity,highlighting the coupling between pore structure evolution and oxidation behavior in igneous metamorphic coal.This study provides theoretical insights into the pore-oxygen coupling mechanisms governing coal spontaneous combustion in igneous intrusion areas.展开更多
The von Hippel-Lindau tumor suppressor(VHL)has been extensively used to develop degraders targeting numerous proteins of interest.However,studies on the rational design of VHL-proteolysis-targeting chimeras(PROTACs)re...The von Hippel-Lindau tumor suppressor(VHL)has been extensively used to develop degraders targeting numerous proteins of interest.However,studies on the rational design of VHL-proteolysis-targeting chimeras(PROTACs)remain scarce.This study aimed to develop strategies to investigate VHL-recruiting PROTACs connecting with varying attachment sites on VHL ligands,which could be utilized for KRAS^(G12C) degraders development and expanded to additional targets.We developed a molecular dynamics(MD)-based strategy to explore the stability of ternary complexes induced by KRAS^(G12C) PROTACs with four distinct attachment sites of VH032.We found a potent degrader namely YN14-H,linked to hydroxyl group on VH032 benzene ring,exhibited the most superior ability of inducing ternary complexes,reflected by the lowest dissociation constant(Kd)for ternary complex induction and the highest AlphaScreen(AS)-based interaction.YN14-H inhibited cell growth with low nanomolar half maximal inhibitory concentration(IC_(50))and half maximal degradation concentration(DC_(50))values as well as>98%of maximum degradation(D_(max))in NCI-H358 and MIA PaCa-2 cells harboring KRAS^(G12C)-mutation.Mechanistically,YN14-H significantly induced apoptosis and inhibited the migratory capacity.Notably,YN14-H demonstrated favorable pharmacokinetic properties and excellent antitumor activity in vivo.Furthermore,bromodomain-containing protein 7(BRD7)and Bruton tyrosine kinase(BTK)degraders attached to distinct sites on VH032 further verified the rationality and universality of our MD-based strategies.Our findings demonstrated that YN14-H could serve as a promising candidate for the treatment of tumors with KRAS^(G12C)-mutation and present a strategy for the rational design of VHL-recruiting PROTACs that target additional proteins at distinct attachment sites.展开更多
Nonconvex optimisation plays a crucial role in science and industry.However,existing methods often encounter local optima or provide inferior solutions when solving nonconvex optimisation problems,lacking robustness i...Nonconvex optimisation plays a crucial role in science and industry.However,existing methods often encounter local optima or provide inferior solutions when solving nonconvex optimisation problems,lacking robustness in noise scenarios.To address these limitations,we aim to develop a robust,efficient and globally convergent solver for nonconvex optimisation.This is achieved by combining the efficient local exploitation ability of a parameter-learnt neural dynamics(PLND)model with the global search capability of the coevolutionary mechanism.We combine their characteristics to design a coevolutionary neural dynamics with learnable parameters(CNDLP)model.The gradient information is used to find the optimal solution more effectively,and neural dynamics models have robustness,which ensures that the influence of noise can be effectively suppressed in the calculation process.Theoretical analyses show the global convergence and robustness of the designed CNDLP model.Numerical experiments on 9 benchmark functions and a practical engineering design example are conducted with five existing meta-heuristic algorithms.Benchmarks cover diverse problems,from classical landscapes like benchmark Shubert to high-dimensional cases such as 30-dimensional Rosenbrock.Results confirm CNDLP's excellent performance in both solution quality and convergence speed under noise.展开更多
CdS-based photocatalysts offer an efficient route for simultaneous photocatalytic hydrogen evolution and benzyl alcohol oxidation to value-added chemicals.However,the rapid charge recombination,poor oxidation capabili...CdS-based photocatalysts offer an efficient route for simultaneous photocatalytic hydrogen evolution and benzyl alcohol oxidation to value-added chemicals.However,the rapid charge recombination,poor oxidation capabilities,and strong photocorrosion of CdS,when used alone,can lead to low productivity of H2 and benzaldehyde.Herein,we present a novel S-scheme heterojunction through coupling CdS with Fluorenone-COF as the promising oxidation end.The suitable band level and active center of the fluorenone moiety impart strong oxidative capabilities to the fluorenone-based COFs,enabling them to efficiently catalyze the oxidation of benzyl alcohol with a low reaction energy barrier.Furthermore,the intrinsic electric field of the S-scheme heterojunction significantly improves the separation and mobility of photoinduced charge carriers,while effectively suppressing charge recombination,which in turn reduces the corrosive effect of photogenerated holes on CdS.Consequently,the heterojunction significantly improved the yield of both benzaldehyde and hydrogen.In the presence of Pt as a cocatalyst,the production rates of H2 and benzaldehyde reached 23.38 and 17.36 mmol g^(-1) h^(-1),respectively.This work not only addresses the challenges associated with the utilization of electron holes but also provides an effective green and low-carbon pathway to overcome the challenges of low efficiency and high cost in photocatalytic hydrogen production.展开更多
Molecular dynamics simulations were conducted at temperatures of 298.15,273.15,253.15,and 233.15 K on three organic electrolytes,composed of 1 M NaPF6 dissolved in strongly coordinating diglyme(DG),a mixture of DG and...Molecular dynamics simulations were conducted at temperatures of 298.15,273.15,253.15,and 233.15 K on three organic electrolytes,composed of 1 M NaPF6 dissolved in strongly coordinating diglyme(DG),a mixture of DG and weakly coordinating Tetrahydrofuran(THF)with a 2:8 volume ratio,and a mixture of DG,THF,and weakly coordinating 1,3-dioxolane(DOL)with a 2:4:4 volume ratio,respectively,hereafter denoted as ND,NDT,and NDTD electrolytes for sodium-ion batteries.The studies indicate strong Na^(+)-DG coordination that leads to a vehicular mechanism,in the sense that Na+persists in migrating together with strongly coordinating DG in the first coordination shell at all the temperature ranges.Such a vehicular mechanism hinders Na+migration in the ND electrolyte.In contrast,the introduction of weakly coordinating molecules,such as THF in the NDT electrolyte and THF/DOL in the NDTD electrolyte,considerably perturbs Na+solvation with various coordinating configurations that include Na^(+)-THF and/or Na^(+)-DOL as well as Na^(+)-PF^(-)_(6) contact-ion pairs.Such diversity of the coordinating configurations significantly improves Na+migration,especially in the NDTD electrolyte,which has the highest ionic conductivity as well as the fractional ionic conductivity of Na+of 3.680.36 and 1.320.11 mS·cm^(-1),respectively,even at a low temperature of 233.15 K.展开更多
基金financed jointly by the National Major Science and Technology Special Project on Deep Earth Exploration(2024ZD1001701-5)the National Natural Science Foundation of China(42472127,42172086)+2 种基金the Yunnan Major Project of Basic Research(202401BN070001-002)Yunnan Mineral Resources Prediction and Evaluation Engineering Research Center(2011)Innovation Team Program of Kunming University of Science and Technology,Yunnan Province。
文摘The migration mechanisms of ore-forming fluids have long been a focus in the field of ore deposit studies.Calcite is ubiquitously present in various types of rocks in the lithosphere,and the underlying mechanisms of its influence on fluid migration are of crucial importance.While previous studies have revealed that salinity changes can modulate fluid migration,the underlying mechanisms remain poorly understood.We employ molecular dynamics simulations to elucidate how salinity variations in ore-forming fluids modulate the adsorption onto calcite nanopore walls,thereby revealing the microscopic mechanisms governing ore fluid transport through calcite nano-fractures.The results show that the adsorption energy Eint of the solution on the calcite surface increased from -14,948.84±182.48 kcal/mol to -12,144.08±118.2 kcal/mol as salinity increased,which is conducive to the long-range transport of the fluid in the calcite nanopore.
基金financially supported by the National Natural Science Foundation of China(Nos.22341304,22303100 and 12205270)the National Key R&D Program of China(Nos.2023YFA1008800 and 2020YFA0713601)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDC0180303)。
文摘The equilibrium dynamics and nonlinear rheology of unentangled polymer blends remain inadequately understood,especially regarding the influence of short-chain matrix length N_(S) on the structure and rheological behavior of dispersed long chains.Using molecular dynamics simulations based on the Kremer-Grest model,we systematically explore the N_(S)-dependence of static conformations,equilibrium dynamics,and nonlinear shear responses in unentangled long-chain/short-chain polymer blends.Our results demonstrate a decoupling between the static and dynamic sensitivity to N_(S):while the static chain size,R_g,follows Flory theory with slight swelling at small N_(S) due to incomplete excluded volume screening,the diffusion coefficient,D,and the relaxation time,τ_(0),exhibit a strong,non-monotonic N_(S)-dependence,transitioning from monomeric friction dominance at small N_(S) to collective segmental rearrangement at large N_(S).Additionally,we observe partial decoupling between the viscous and normal stress responses:while the zero-shear viscosity,η,is strongly N_(S)-dependent,the first and second normal stress coefficients,Ψ_(1) and Ψ_(2),collapse onto universal curves when scaled by the dimensionless shear rate,γτ_(0),suggesting a common mechanism of orientation and stretching.Under shear,long chains compress in the vorticity direction λ_(z)~Wi^(-0.2),which reduces collision frequency and contributes to shear thinning,while the scaling of weaker orientation resistance m_(G)~Wi^(0.35)reflects hydrodynamic screening by the short-chain matrix.These findings highlight the limitations of single-chain models and emphasize the necessity of considering N_(S)-dependent matrix dynamics and flow-induced structural changes in understanding the rheology of unentangled polymer blends.
文摘The study presents an analysis of the spatiotemporal evolution of vegetation cover in the Izarene forest,using LANDSAT satellite images collected for the years 1984,2003,and 2022.The methodological approach is based on the use of ArcGIS 10.8 software for processing multispectral images,as well as the calculation of the Normalized Difference Vegetation Index(NDVI),which enables the observation of variations in vegetation cover over time.The findings show that biodiversity is pretty abundant,but they also show that some places with low vegetation density are under a lot of stress.Due in large part to overuse of natural resources,uncontrolled human activity,and environmental factors,these regions seem to be more vulnerable to degradation.However,a decrease in deforestation over the past 20 years is revealed by comparing the two periods(1984–2003 and 2003–2022).The participation of governmental agencies,especially the Department of Water and Forests,through concrete projects like reforestation,forest fire prevention,and awareness-raising campaigns among local communities,is responsible for this progress.In several areas,these measures have stabilized or even improved the state of the vegetation.The analysis emphasizes how crucial sustainable,integrated,and participatory management is to protecting the Izarene forest,which is a significant resource for maintaining the region’s ecological balance.
基金Project co-funded by European Union in the context of the precommercial public procurement of RD services managed by CDTI E.P.Eco-funded by the European Regional Development Fund(ERDF)as part of the project for the development of a Compact Linear Accelerator for Hadrontherapy,Exp.CPP 03/2023 AB(DCCPI/OCPI)。
文摘In response to the increasing demand for hadron therapy facilities,significant efforts have been directed toward enhancing the performance of high-gradient and high-transmission injectors for light ion beams.For carbon ion irradiations,which offer greater radiobiological efficiency in tumor treatment,recent research has focused on developing high-production sources of fully stripped C^(6+)ions and highly compact,high-frequency RFQ cavities.This study explores the design possibilities of a carbon ion acceleration section using 750 MHz Interdigital H-mode Drift Tube Linacs(IH-DTLs)as a high-efficiency solution for accelerating ions in the 5-10 MeV per nucleon energy range.A particle-tracking routine based on the TRAVEL code was developed to design the acceleration line through a tailored KONUS-type configuration.Three design solutions were proposed and compared,exploring different alternatives regarding the use of a MEBT to match the output beam phase space of the RFQ to the optics of the line,as well as varying considerations for magnetic systems to focus the beam.Additionally,the compatibility of the proposed solutions with the existing design of the carbon ion bent-linac for hadron therapy was assessed.
基金support from the project“National Institute of Virology and Bacteriology(Program EXCELES,ID Project No.LX22NPO5103)Funded by the European Union-Next Generation EU".D.B.also acknowledges VSB-Technical University of Ostrava,IT4Innovations National Supercomputing Center,Czech Republic,for awarding this project access to the LUMI supercomputer,owned by the EuroHPC Joint Undertaking,hosted by CSC(Finland)and the LUMI consortium through the Ministry of Education,Youth and Sports of the Czech Republic through the e-INFRA CZ(Grant ID:90254)+4 种基金project OPEN-35-3.M.V.and J.H.acknowledge the Czech Science Foundation for support via grant number 25-16117S and the project"The Energy Conversion and Storage"funded as project No.CZ.02.01.01/00/22_008/0004617 by Programme Johannes Amos Comeniuscall Excellent Research.M.V.also acknowledges support by the Ministry of Education,Youth and Sports of the Czech Republic through the e-INFRA CZ(ID:90254)Project OPEN-30-53.P.J.acknowledges support from the European Research Council via an ERC Advanced Grant no.101095957The authors would like to acknowledge the contribution of COST Action CA21169,supported by COST(European Cooperation in Science and Technology).
文摘Like-charge pairing is a physical manifestation of the unique solvation properties of certain ion pairs in water.Water's high dielectric constant and related charge screening capability significantly influence the interaction between like-charged ions,with the possibility to transform it-in exceptional cases when noncovalent interactions are involved-from repulsion to attraction.Guanidinium cations(Gdm^(+))represent a quintessential example of such like-charge pairing due to their specific geometry and electronic structure.In this work,we present experimental validation and quantification of Gdm^(+)-Gdm contact ion pairing in water utilizing nuclear magnetic resonance(NMR)spectroscopy complemented by molecular dynamics(MD)simulations and density functional theory(DFT)calculations.The observed Gdm^(+)-Gdm^(+)interaction is attractive albeit weak-about 0.5 kJ·mol^(-1)-which aligns with theoretical estimation from MD simulations.We contrast the behavior of Gdm^(+) with that of NH_(4)^(+) cations,which exhibit no contact ion pairing in water.DFT calculations predict that the NMR chemical shift of Gdm^(+) dimers is different than that of monomers,in agreement with NMR titration curves that display a nonlinear Langmuir-like behavior.Additionally,we conducted cryo-electron microscopy-to our knowledge,for the first time-on concentrated oligoarginines R9,which,unlike nona-lysines K9,exhibit aggregation in water.These results point to like charge pairing of the guanidinium side chain groups,as corroborated also by MD simulations and free energy calculations.
基金The National Natural Science Foundation of China(Grant No.12462006)Beijing Institute of Structure and Environment Engineering Joint Innovation Fund(No.BQJJ202414).
文摘THE mechanical response and deformation mechanisms of pure nickel under nanoindentation were systematically investigated using molecular dynamics(MD)simulations,with a particular focus on the novel interplay between crystallographic orientation,grain boundary(GB)proximity,and pore characteristics(size/location).This study compares single-crystal nickel models along[100],[110],and[111]orientations with equiaxed polycrystalline models containing 0,1,and 2.5 nm pores in surface and subsurface configurations.Our results reveal that crystallographic anisotropy manifests as a 24.4%higher elastic modulus and 22.2%greater hardness in[111]-oriented single crystals compared to[100].Pore-GB synergistic effects are found to dominate the deformation behavior:2.5 nm subsurface pores reduce hardness by 25.2%through stress concentration and dislocation annihilation at GBs,whereas surface pores enable mechanical recovery via accelerated dislocation generation post-collapse.Additionally,size-dependent deformation regimes were identified,with 1 nm pores inducing negligible perturbation due to rapid atomic rearrangement,in contrast with persistent softening in 2.5 nm pores.These findings establish atomic-scale design principles for defect engineering in nickel-based aerospace components,demonstrating how crystallographic orientation,pore configuration,and GB interactions collectively govern nanoindentation behavior.
基金supported by the National Natural Science Foundation of China(Grant Nos.92252104,12388101,and 12472224).
文摘In this study,we perform particle-resolved simulations of settling spheroidal particles,considering oblate and prolate spheroids and spheres,and investigate the shape effect on the particle dynamics in suspensions with volume fraction 1%and 5%.We first examine the single-point statistics of the translational and rotational motion of the settling particles.The horizontal velocity has a symmetrical distribution with standard deviation dependent on the particle shape.The greater horizontal velocity fluctuations of the non-spherical particles,compared to that of spheres,are attributed to the horizontal drift of settling spheroids with oblique orientations induced by the fluid-particle and particle-particle interactions.The fluctuation of particle vertical velocity,instead,is skewed under the effect of wake-induced hydrodynamic interactions.Further,we explore the particle pair statistics,which demonstrate the formation of column-like particle micro-structures for the lowest volume fraction considered.This clustering is more pronounced for spheroidal particles than spheres,due to the stronger attractions among vertically-aligned settling spheroids.Moreover,the particle pair statistics are directly related to the collision rate among the dispersed particles.The local accumulation of oblate/prolate spheroids serves as the major mechanism to promote the particle-particle collisions in dilute suspensions.
基金supported by the National Natural Science Foundation of China under Grants 61962023,61562029 and 62466019.
文摘This paper presents an adaptive multi-agent coordination(AMAC)strategy suitable for complex scenarios,which only requires information exchange between neighbouring robots.Unlike traditional multi-agent coordination methods that are solved by neural dynamics,the proposed strategy displays greater flexibility,adaptability and scalability.Furthermore,the proposed AMAC strategy is reconstructed as a time-varying complex-valued matrix equation.By introducing a dynamic error function,a fixed-time convergent zeroing neural network(FTCZNN)model is designed for the online solution of the AMAC strategy,with its convergence time upper bound derived theoretically.Finally,the effectiveness and applicability of the coordination control method are demonstrated by numerical simulations and physical experiments.Numerical results indicate that this method can reduce the formation error to the order of 10^(-6)within 1.8 s.
基金supported by the National Natural Science Foundation of China(Nos.22278397)the Fundamental Research Funds for the Central Universities(2024SMECP01).
文摘Ionic liquids(ILs)have exhibited great application potential in many fields due to their unique properties.Molecular dynamics(MD)simulation has been widely employed to investigate their microscopic structure.However,classical molecular dynamics simulations struggle to accurately describe the complex interactions in ILs using the existing parameterized force fields.Recently,the MD simulations based on machine learning force fields(MLFFs)trained by first-principles calculations have attracted considerable attentions due to their abilities to balance computational accuracy and efficiency.Herein,we report the Bayesian-based MLFFs which can be successfully applied in IL systems and accelerate MD simulation.The calculated atomic forces,structures,and vibrational behaviors were validated to match the accuracy of firstprinciples calculations.Properties of the imidazolium-based ILs,including density,self-diffusion coefficients,viscosity,and radial distribution functions were predicted at the extended scales.Z-bonds that describe the unique structures in ILs were analyzed and the influences of Cpositions,temperature,and solvent H2O on Z-bonding configurations were systematically investigated.Our results confirmed that MLFFs presented the strong feasibility to investigate the large and complex systems,especially to predict structures and properties of the ILs.And the procedure described for MLFFs provides valuable guidance for researchers who are studying ILs.
基金the financial support from the National Natural Science Foundation of China (22109127)the Chinese Postdoctoral Science Foundation (2021M702666)+2 种基金the Research Fund of the State Key Laboratory of Solidification Processing (NPU),China (Grant No.2023-TS-02)The financial support from the Youth Project of"Shaanxi High-level Talents Introduction Plan"the Key Laboratory of Advanced Energy Materials Chemistry (Ministry of Education) are also sincerely appreciated
文摘Photo-assisted lithium–sulfur batteries(PALSBs)offer an eco-friendly solution to address the issue of sluggish reaction kinetics of conventional LSBs.However,designing an efficient photoelectrode for practical implementation remains a significant challenge.Herein,we construct a free-standing polymer–inorganic hybrid photoelectrode with a direct Z-scheme heterostructure to develop high-efficiency PALSBs.Specifically,polypyrrole(PPy)is in situ vapor-phase polymerized on the surface of N-doped TiO_(2) nanorods supported on carbon cloth(N-TiO_(2)/CC),thereby forming a well-defined p–n heterojunction.This architecture efficiently facilitates the carrier separation of photo-generated electron–hole pairs and significantly enhances carrier transport by creating a built-in electric field.Thus,the PPy@N-TiO_(2)/CC can simultaneously act as a photocatalyst and an electrocatalyst to accelerate the reduction and evolution of sulfur,enabling ultrafast sulfur redox dynamics,as convincingly validated by both theoretical simulations and experimental results.Consequently,the PPy@N-TiO_(2)/CC PALSB achieves a high discharge capacity of 1653 mAh g^(−1),reaching 98.7%of the theoretical value.Furthermore,5 h of photo-charging without external voltage enables the PALSB to deliver a discharge capacity of 333 mAh g^(−1),achieving dual-mode energy harvesting capabilities.This work successfully integrates solar energy conversion and storage within a rechargeable battery system,providing a promising strategy for sustainable energy storage technologies.
基金supported by the Anhui Province Tongxin Science and Technology Innovation Project(202523b11020014)the Anhui Province Higher Education Quality Engineering Program(2024fwxx003).
文摘SalicS1 is a genetically encoded,ratiometric FRET biosensor that brings salicylic acid(SA)research to the same real-time imaging standard long available for ABA and GA.Built through a modular Golden Gate platform and informed by NPR-NIMIN structural biology,SalicS1 achieves SA specificity,tunable affinity,reversibility,and non-perturbing expression in Arabidopsis.Using this sensor,pathogen infection,non-adapted fungal challenge,and aphid feeding are shown to elicit spatially propagating SA surges rather than purely local accumulation,revealing a tissue-level organization of immune signaling that bulk assays could not resolve.SalicS1 therefore provides a broadly deployable tool for dissecting the geometry,timing,and genotype dependence of SA-mediated plant defense.
基金supported by Special Funding Projects for Local Science and Technology Development guided by the Central Committee(No.YDZJSX2022C028)the Fundamental Research Program of Shanxi Province(Nos.20210302123218 and 202203021211187)+4 种基金Innovation and Entrepreneurship Training Program for College Students in Shanxi Province(202210109006)the National Natural Science Foundation(52474367)the Key Research and Development for University-Local Government Collaboration of Lvliang City(2024XDHZ01)the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi(2025Q022)the Foundation of State Key Laboratory of Advanced Metallurgy,USTB(K22-10).
文摘The structural changes in the CaO-SiO_(2)-Al_(2)O_(3)-MgO slag system with varying CaO contents were investigated through molecular dynamics(MD)simulations,and its effect on the dissolution behavior of alumina inclusions was characterized by the Kullback-Leibler(KL)divergence.The slag structure analysis revealed that the[AlO]tetrahedral structure was the primary network structure in the slag.With increasing the CaO content,the non-bridge oxygen(NBO)content in the slag structure increases,and the bridge oxygen(BO)content decreases,thereby reducing the complexity of the slag network structure.Raman spectroscopy detection verifies the results of the MD simulations.The results indicated that the dissolution rate of alumina inclusions accelerates with increasing the CaO content in the slag,owing to the reduced complexity of the slag network structure and the enhanced interatomic interactions.The simulation results for the dissolution of alumina inclusions were consistent with theoretical calculations based on the slag inclusion capacity and the dimensionless dissolution rate of inclusions.Radial distribution function analysis demonstrated that the interaction between atoms in the slag system and alumina inclusions strengthens,increasing the dissolution rate of alumina inclusions.The[AlO_(6)]octahedral structure of the alumina inclusions is disrupted,forming BO structures,which in turn enhances the complexity of the slag network structure,slowing the dissolution rate of alumina inclusions.In contrast,the slag system with a higher CaO content has a relatively simpler network structure,promoting faster alumina inclusion dissolution.
基金supported by the National Science Fund for Distinguished Young Scholars(No.52425404).
文摘This study investigates the influence of hydrogen concentration at grain boundaries on the sensitivity of polycrystalline iron to hydrogen embrittlement using molecular dynamics simulations.These simulations reveal the diffusion behavior of hydrogen atoms at grain boundaries and their consequential impact on the hydrogen embrittlement sensitivity of iron alloys.The findings indicate that as the hydrogen concentration increases,both the yield strength and ultimate tensile strength of Fe-H alloys exhibit a declining trend.Moreover,the capture of hydrogen atoms at the grain boundaries significantly influences the fracture toughness of the material and promotes the formation and propagation of cracks.This study provides a novel theoretical basis for understanding and predicting the hydrogen embrittlement behavior of iron-based materials in hydrogen-rich environments,offering valuable insights for the design and development of Fe alloys with enhanced resistance to hydrogen embrittlement.
基金supported by the funding support from the National Key R&D Program of China(2024YFA1509400)the Beijing Natural Science Foundation(F251001)+2 种基金the National Natural Science Foundation of China(No.22479148)the Institute of Weiqiao UCAS Science and Technology(GYY-GDHX-2024-ZY-007)supported by the U.S.National Science Foundation Under Grant No.DMR 2303712。
文摘Atomic vacancies in oxides induce deviations from ideal stoichiometry,critically influencing their functional properties in applications such as energy storage-conversion,catalysis,and electronic devices.The dynamic behavior of these vacancies as main mass transport mediums to exchange chemical species with surroundings under operating conditions is central to oxide redox reactions running with the Mars-van Krevelen(MvK)mechanism;yet in-situ atomic-scale monitoring of the vacancy dynamics and vacancy-induced secondary defects within oxides remains challenging due to both their rapid transport kinetics at buried subsurface/interface and characterization difficulties,arising from the insulating nature of bulk oxides and the spatial-resolution requirement in reaction conditions.These challenges hinder precise defect engineering for the performance optimization of functional oxides.In this review,recent advancements in tracking oxygen vacancy and vacancyinduced secondary defects dynamics in oxides,including surface steps,cation vacancies,interfacial dislocations,ledges,and interfaces,have been summarized.The dynamic interconversion of defects and their synergistic effects on surface/subsurface/interface evolution are mainly discussed.The aim of this review is to enhance understanding of defect dynamics and their pivotal role in modulating structural dynamics and surface reaction reactivity,which is highly relevant to the catalyst activity/selectivity/stability evaluation of functional oxide catalysts for electroreduction and catalytic oxidation reactions.Finally,strategies to control buried subsurface and interfacial defects(interface engineering)through tailored surface reactions are proposed,offering new pathways to customize the performance of advanced oxide-based materials.
基金supported by the National Natural Science Foundation of China(No.52374247)the Joint Funds of the National Natural Science Foundation of China(No.U24B2042).
文摘In igneous-intruded coal seams,coal undergoes significant metamorphism,which critically alters its pore structure and oxygen consumption dynamics,thereby elevating its spontaneous combustion tendency.This study investigates the specific surface area,pore volume,structure complexity/connectivity,heterogeneity/local features of pore size distribution,and oxygen consumption dynamics of igneous metamorphic coal through N_(2)/CO_(2) isothermal adsorption tests and low-temperature oxidation experiments,and elucidates the influence mechanisms of pore structure evolution on oxygen consumption dynamics during low-temperature oxidation.With increasing metamorphic degree,igneous metamorphic coal exhibits a more pronounced reduction in specific surface area during oxidation,while the increase in structure complexity due to coal-oxygen reactions is suppressed.Thermally metamorphic coal demonstrates accelerated oxygen consumption,with oxidation amplifying the difference in reaction rates compared to raw coal.Key mechanisms include oxidation-induced reduction in mesopore complexity and micropore volume,decreased dominance of small-pore-volume apertures,and increased heterogeneity,collectively leading to a lower half-oxygen-consuming temperature and steeper oxygen consumption curves.Simultaneously,increased pore volume/complexity and reduced uniformity/connectivity act synergistically to enhance oxygen consumption capacity,highlighting the coupling between pore structure evolution and oxidation behavior in igneous metamorphic coal.This study provides theoretical insights into the pore-oxygen coupling mechanisms governing coal spontaneous combustion in igneous intrusion areas.
基金supported by National Natural Science Foundation of China(No.82404417)State Key Laboratory of National Security Specially Needed Medicines Program(No.LTMC2022Zz006).
文摘The von Hippel-Lindau tumor suppressor(VHL)has been extensively used to develop degraders targeting numerous proteins of interest.However,studies on the rational design of VHL-proteolysis-targeting chimeras(PROTACs)remain scarce.This study aimed to develop strategies to investigate VHL-recruiting PROTACs connecting with varying attachment sites on VHL ligands,which could be utilized for KRAS^(G12C) degraders development and expanded to additional targets.We developed a molecular dynamics(MD)-based strategy to explore the stability of ternary complexes induced by KRAS^(G12C) PROTACs with four distinct attachment sites of VH032.We found a potent degrader namely YN14-H,linked to hydroxyl group on VH032 benzene ring,exhibited the most superior ability of inducing ternary complexes,reflected by the lowest dissociation constant(Kd)for ternary complex induction and the highest AlphaScreen(AS)-based interaction.YN14-H inhibited cell growth with low nanomolar half maximal inhibitory concentration(IC_(50))and half maximal degradation concentration(DC_(50))values as well as>98%of maximum degradation(D_(max))in NCI-H358 and MIA PaCa-2 cells harboring KRAS^(G12C)-mutation.Mechanistically,YN14-H significantly induced apoptosis and inhibited the migratory capacity.Notably,YN14-H demonstrated favorable pharmacokinetic properties and excellent antitumor activity in vivo.Furthermore,bromodomain-containing protein 7(BRD7)and Bruton tyrosine kinase(BTK)degraders attached to distinct sites on VH032 further verified the rationality and universality of our MD-based strategies.Our findings demonstrated that YN14-H could serve as a promising candidate for the treatment of tumors with KRAS^(G12C)-mutation and present a strategy for the rational design of VHL-recruiting PROTACs that target additional proteins at distinct attachment sites.
基金supported by the Leading Talent of the Qinghai Province Kunlun Talents Programme・High-Level Innovative and Entrepreneurial Talents(QHKLYC-GDCXCY-2024-359).
文摘Nonconvex optimisation plays a crucial role in science and industry.However,existing methods often encounter local optima or provide inferior solutions when solving nonconvex optimisation problems,lacking robustness in noise scenarios.To address these limitations,we aim to develop a robust,efficient and globally convergent solver for nonconvex optimisation.This is achieved by combining the efficient local exploitation ability of a parameter-learnt neural dynamics(PLND)model with the global search capability of the coevolutionary mechanism.We combine their characteristics to design a coevolutionary neural dynamics with learnable parameters(CNDLP)model.The gradient information is used to find the optimal solution more effectively,and neural dynamics models have robustness,which ensures that the influence of noise can be effectively suppressed in the calculation process.Theoretical analyses show the global convergence and robustness of the designed CNDLP model.Numerical experiments on 9 benchmark functions and a practical engineering design example are conducted with five existing meta-heuristic algorithms.Benchmarks cover diverse problems,from classical landscapes like benchmark Shubert to high-dimensional cases such as 30-dimensional Rosenbrock.Results confirm CNDLP's excellent performance in both solution quality and convergence speed under noise.
基金National Natural Science Foundation of China(22378148,52472110,22308113)Natural Science Foundation of Guangdong Province(2024A1515012433)for their support.
文摘CdS-based photocatalysts offer an efficient route for simultaneous photocatalytic hydrogen evolution and benzyl alcohol oxidation to value-added chemicals.However,the rapid charge recombination,poor oxidation capabilities,and strong photocorrosion of CdS,when used alone,can lead to low productivity of H2 and benzaldehyde.Herein,we present a novel S-scheme heterojunction through coupling CdS with Fluorenone-COF as the promising oxidation end.The suitable band level and active center of the fluorenone moiety impart strong oxidative capabilities to the fluorenone-based COFs,enabling them to efficiently catalyze the oxidation of benzyl alcohol with a low reaction energy barrier.Furthermore,the intrinsic electric field of the S-scheme heterojunction significantly improves the separation and mobility of photoinduced charge carriers,while effectively suppressing charge recombination,which in turn reduces the corrosive effect of photogenerated holes on CdS.Consequently,the heterojunction significantly improved the yield of both benzaldehyde and hydrogen.In the presence of Pt as a cocatalyst,the production rates of H2 and benzaldehyde reached 23.38 and 17.36 mmol g^(-1) h^(-1),respectively.This work not only addresses the challenges associated with the utilization of electron holes but also provides an effective green and low-carbon pathway to overcome the challenges of low efficiency and high cost in photocatalytic hydrogen production.
基金supported by the National Natural Science Foundation of China(22273040)。
文摘Molecular dynamics simulations were conducted at temperatures of 298.15,273.15,253.15,and 233.15 K on three organic electrolytes,composed of 1 M NaPF6 dissolved in strongly coordinating diglyme(DG),a mixture of DG and weakly coordinating Tetrahydrofuran(THF)with a 2:8 volume ratio,and a mixture of DG,THF,and weakly coordinating 1,3-dioxolane(DOL)with a 2:4:4 volume ratio,respectively,hereafter denoted as ND,NDT,and NDTD electrolytes for sodium-ion batteries.The studies indicate strong Na^(+)-DG coordination that leads to a vehicular mechanism,in the sense that Na+persists in migrating together with strongly coordinating DG in the first coordination shell at all the temperature ranges.Such a vehicular mechanism hinders Na+migration in the ND electrolyte.In contrast,the introduction of weakly coordinating molecules,such as THF in the NDT electrolyte and THF/DOL in the NDTD electrolyte,considerably perturbs Na+solvation with various coordinating configurations that include Na^(+)-THF and/or Na^(+)-DOL as well as Na^(+)-PF^(-)_(6) contact-ion pairs.Such diversity of the coordinating configurations significantly improves Na+migration,especially in the NDTD electrolyte,which has the highest ionic conductivity as well as the fractional ionic conductivity of Na+of 3.680.36 and 1.320.11 mS·cm^(-1),respectively,even at a low temperature of 233.15 K.
