The experiment explored the Fe_(2)O_(3) reduction process with H_(2)/CO mixed gas and confirmed a promoting effect from CO when its volume proportion in mixed gas is 20% at 850℃.The ReaxFF molecular dynamics(MD)simul...The experiment explored the Fe_(2)O_(3) reduction process with H_(2)/CO mixed gas and confirmed a promoting effect from CO when its volume proportion in mixed gas is 20% at 850℃.The ReaxFF molecular dynamics(MD)simulation method was used to observe the reduction process and provide an atomic-level explanation.The accuracy of the parameters used in the simulation was verified by the density functional theory(DFT)calculation.The simulation shows that the initial reduction rate of H_(2) is much faster than that of CO(from 800 to 950℃).As the reduction proceeds,cementite,obtained after CO participates in the reduction at 850℃,will appear on the iron surface.Due to the active properties of C atoms in cementite,they are easy to further react with the O atoms in Fe_(2)O_(3).The generation of internal CO may destroy the dense structure of the surface layer,thereby affecting the overall reduction swelling of Fe_(2)O_(3).However,excess CO is detrimental to the reaction rate,mainly because of the poor thermodynamic conditions of CO in the temperature range and the molecular diffusion capacity is not as good as that of H_(2).Furthermore,the surface structures obtained after H_(2) and CO reduction have been compared,and it was found that the structure obtained by CO reduction has a larger surface area,thus promoting the sub sequent reaction of H_(2).展开更多
We propose a theoretical framework,based on the two-component Gross-Pitaevskii equation(GPE),for the investigation of vortex solitons(VSs)in hybrid atomic-molecular Bose-Einstein condensates under the action of the st...We propose a theoretical framework,based on the two-component Gross-Pitaevskii equation(GPE),for the investigation of vortex solitons(VSs)in hybrid atomic-molecular Bose-Einstein condensates under the action of the stimulated Raman-induced photoassociation and square-optical-lattice potential.Stationary solutions of the coupled GPE system are obtained by means of the imaginary-time integration,while the temporal dynamics are simulated using the fourth-order Runge-Kutta algorithm.The analysis reveals stable rhombus-shaped VS shapes with topological charges m=1 and 2 of the atomic component.The stability domains and spatial structure of these VSs are governed by three key parameters:the parametric-coupling strength(χ),atomicmolecular interaction strength(g_(12)),and the optical-lattice potential depth(V_(0)).By varyingχand g_(12),we demonstrate a structural transition where four-core rhombus-shaped VSs evolve into eight-core square-shaped modes,highlighting the nontrivial nonlinear dynamics of the system.This work establishes a connection between interactions of cold atoms and topologically structured matter waves in hybrid quantum systems.展开更多
The T_(1)(Al_(2) CuLi)phase is one of the most effective strengthening nanoscale-precipitate in Al-Cu alloys with Li.However,its formation and evolution still need to be further clarified during aging due to the compl...The T_(1)(Al_(2) CuLi)phase is one of the most effective strengthening nanoscale-precipitate in Al-Cu alloys with Li.However,its formation and evolution still need to be further clarified during aging due to the complex precipitation sequences.Here,a detailed investigation has been carried out on the atomic struc-tural evolution of T_(1) precipitate in an aged Al-Cu-Li-Mg-Ag alloy using state-of-the-art Cs-corrected high-angle annular dark field(HAADF)-coupled with integrated differential phase contrast(iDPC)-scanning transmission electron microscopy(STEM)and energy-dispersive X-ray spectroscopy(EDXS)techniques.An intermediate T_(1)’phase between T_(1p) and T_(1) phase,with a crystal structure and orientation rela-tionship consistent with T_(1),but exhibiting different atomic occupancy and chemical composition was found.We observed the atomic structural transformation from T_(1p) to T_(1)’phase(fcc→hcp),involving only 1/12<112>Al shear component.DFT calculation results validated our proposed structural models and the precipitation sequence.Besides,the distributions of minor solute elements(Ag,Mg,and Zn)in the pre-cipitates exhibited significant differences.These findings may contribute to a further understanding of the nucleation mechanism of T_(1) precipitate.展开更多
This study aims to clarify the mechanisms for the grain boundary(GB)segregation through investigating the absorption of excess solute atoms at GBs in Al−Cu alloys by using the hybrid molecular dynamics/Monte Carlo sim...This study aims to clarify the mechanisms for the grain boundary(GB)segregation through investigating the absorption of excess solute atoms at GBs in Al−Cu alloys by using the hybrid molecular dynamics/Monte Carlo simulations.Two segregation mechanisms,substitutional and interstitial mechanisms,are observed.The intergranular defects,including dislocations,steps and vacancies,and the intervals in structural units are conductive to the prevalence of interstitial mechanism.And substitutional mechanism is favored by the highly ordered twin GBs.Furthermore,the two mechanisms affect the GB structure differently.It is quantified that interstitial mechanism is less destructive to GB structure than substitutional one,and often leads to a segregation level being up to about 6 times higher than the latter.These findings contribute to atomic scale insights into the microscopic mechanisms about how solute atoms are absorbed by GB structures,and clarify the correlation among intergranular structures,segregation mechanisms and kinetics.展开更多
Broadband transparent films play a pivotal role in various applications such as lenses and solar cells,particularly porous structured transparent films exhibit significant potential.This study investigates a porous Si...Broadband transparent films play a pivotal role in various applications such as lenses and solar cells,particularly porous structured transparent films exhibit significant potential.This study investigates a porous SiO_(2) refractive index gradient anti-reflective film prepared by atomic layer deposition(ALD).A porous SiO_(2) film with gradual porosity was obtained by phosphoric acid etching of Al_(2)O_(3)/SiO_(2) multilayers with gradient Al2O3 ratios,achieving a gradual decrease in refractive index from the substrate to the surface.The film exhibited an average transmittance as high as 97.8%within the wavelength range from 320 nm to 1200 nm.The environmental adaptability was further enhanced by surface modification using rare earth oxide(REO)La_(2)O_(3),resulting in formation of a lotus leaf-like structure and achieving a water contact angle of 100.0°.These data proved that the modification significantly improved hydrophobic self-cleaning capability while maintaining exceptional transparency of the film.The surface structure of the modified film remained undamaged even after undergoing wipe testing,demonstrating its excellent surface durability.展开更多
Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Her...Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Herein,with crystal and atomic structures of the self-assembled PDI revealed from the X-ray diffraction pattern,the electronic structure is theoretically illustrated by the first-principles density functional theory calculations,suggesting the suitable band structure and the direct electronic transition for efficient photocatalytic oxygen evolution over PDI.It is confirmed that the carbonyl O atoms on the conjugation structure serve as the active sites for oxygen evolution reaction by the crystal orbital Hamiltonian group analysis.The calculations of reaction free energy changes indicate that the oxygen evolution reaction should follow the reaction pathway of H_(2)O→^(*)OH→^(*)O→^(*)OOH→^(*)O_(2)with an overpotential of 0.81 V.Through an in-depth theoretical computational analysis in the atomic and electronic structures,the origin of photocatalytic oxygen evolution activity for PDI is well illustrated,which would help the rational design and modification of polymeric photocatalysts for efficient oxygen evolution.展开更多
Single-atom catalysts(SACs),in which isolated metal atoms such as palladium(Pd)are anchored on solid supports,promise breakthroughs in energy conversion and catalysis.However,balancing their activity(reaction speed)an...Single-atom catalysts(SACs),in which isolated metal atoms such as palladium(Pd)are anchored on solid supports,promise breakthroughs in energy conversion and catalysis.However,balancing their activity(reaction speed)and stability(longevity)remains challenging,as the interplay between metal atoms,supports,and reactants is poorly understood.展开更多
Heat dissipation highly relies on the thermal conductivity(κ)of materials.Materials with large bandgaps and signifcant atomic mass ratios,such as BAs,SiC,andθ-TaN,have attracted considerable attention due to their p...Heat dissipation highly relies on the thermal conductivity(κ)of materials.Materials with large bandgaps and signifcant atomic mass ratios,such as BAs,SiC,andθ-TaN,have attracted considerable attention due to their potential for achieving ultra-highκ,with BAs serving as a particularly representative example due to its unique combination of large bandgap and high thermal conductivity.In this paper,the efects of atomic mass modifcation on phonon bandgap andκare systematically investigated using a BAs model,accounting for both three-and four-phonon scattering processes.A 20%increase inκcan be obtained by substituting B,achieved through widening the phonon bandgap,which suppresses phonon scattering.Notably,the AAOO four-phonon scattering channel is more suppressed than the AAO three-phonon channel,leading to an increased phonon lifetime(τ).For As,κcan also be enhanced by 5%when replaced by lighter atoms,such as^(69)As,primarily due to the increased phonon group velocity(υ).We systematically clarify how atomic-mass-induced bandgap variations afectτ,υ,and thereforeκin wide-bandgap systems.Our work provides a specifc scheme for further improving the ultra-highκof materials with large bandgaps,which possesses great guiding signifcance.展开更多
For atoms in external electric fields,the hyperpolarizabilities are the coefficients describing the nonlinear interactions contributing to the induced energies at the fourth power of the applied electric fields.Accura...For atoms in external electric fields,the hyperpolarizabilities are the coefficients describing the nonlinear interactions contributing to the induced energies at the fourth power of the applied electric fields.Accurate evaluations of these coefficients for various systems are crucial for improving precision in advanced atom-based optical lattice clocks and for estimating field-induced effects in atoms for quantum information applications.However,there is a notable scarcity of research on atomic hyperpolarizabilities,especially in the relativistic realm.Our work addresses this gap by establishing a novel set of alternative formulas for the hyperpolarizability based on the fourth-order perturbation theory.These formulas offer a more reasonable regrouping of scalar and tensor components compared to previous formulas,thereby enhancing their correctness and applicability.To validate our formulas,we perform the calculations for the ground and low-lying excited pure states of few-electron atoms H,Li,and Be^(+).The highly accurate results obtained for the H atom could serve as benchmarks for further development of other theoretical methods.展开更多
Photocatalytic oxygen reduction for hydrogen peroxide(H_(2)O_(2))synthesis presents a green and costeffective production method.However,achieving highly selective H_(2)O_(2)synthesis remains challenging,necessitating ...Photocatalytic oxygen reduction for hydrogen peroxide(H_(2)O_(2))synthesis presents a green and costeffective production method.However,achieving highly selective H_(2)O_(2)synthesis remains challenging,necessitating precise control over free radical reaction pathways and minimizing undesirable oxidative by-products.Herein,we report for the visible light-driven simultaneous co-photocatalytic reduction of O2to H_(2)O_(2)and oxidation of biomass using the atomic rubidium-nitride modified carbon nitride(CNRb).The optimized CNRb catalyst demonstrates a record photoreduction rate of 8.01 mM h^(-1)for H_(2)O_(2)generation and photooxidation rate of 3.75 mM h^(-1)for furfuryl alcohol to furoic acid,achieving a remarkable solar-to-chemical conversion(SCC)efficiency of up to 2.27%.Experimental characterizations and DFT calculation disclosed that the introducing atomic Rb–N configurations allows for the high-selective generation of superoxide radicals while suppressing hydroxyl free radical formation.This is because the Rb–N serves as the new alternative site to perceive a stronger connection position for O2adsorption and reinforce the capability to extract protons,thereby triggering a high selective redox product formation.This study holds great potential in precisely regulating reactive radical processes at the atomic level,thereby paving the way for efficient synthesis of H_(2)O_(2)coupled with biomass valorization.展开更多
The bismuth-telluride-based alloy is the only thermoelectric material commercialized for the applications of refrigeration and energy harvesting,but its low cost-effectiveness severely restricts its large-scale ap-pli...The bismuth-telluride-based alloy is the only thermoelectric material commercialized for the applications of refrigeration and energy harvesting,but its low cost-effectiveness severely restricts its large-scale ap-plication.The introduction of a porous structure in bulk thermoelectric materials has been theoretically proven to effectively reduce thermal conductivity and cost.However,the electrical properties of highly porous materials are considerably suppressed due to the strong carrier scattering at the interface be-tween the matrix and pores,ultimately leading to decreased figure of merit,ZT.Here,we use an atomic layer deposition strategy to introduce some hollow glass bubbles with nano-oxide layers into commercial Bi_(0.5)Sb_(1.5)Te_(3)for preparing high-performance porous thermoelectric materials.Experimental results indi-cate that the nano-oxide layers weaken carrier scattering at the interface between pores and matrix while maintaining high-strength phonon scattering,thereby optimizing carrier/phonon transport behaviors,and effectively increasing the ZT by 23.2%(from 0.99 to 1.22 at 350 K).Besides,our strategy has excellent universality confirmed by its effectiveness in improving the ZT of Bi_(2)Te_(2.7)Se_(0.3),therefore demonstrating great potential for developing low-cost and high-performance thermoelectric materials.展开更多
Molecular dynamics(MD)simulation is employed to investigate the deformation behavior under various loading paths and strain rates of nanocrystalline magnesium(NC Mg)with[0001]texture.Atomic-scale structural evolution ...Molecular dynamics(MD)simulation is employed to investigate the deformation behavior under various loading paths and strain rates of nanocrystalline magnesium(NC Mg)with[0001]texture.Atomic-scale structural evolution of NC Mg was performed under uniaxial and biaxial loadings.In tension process,compression twins and basal slip dominate,while the compression process is dominated by tension twins.The activation mechanism of twinning is highly sensitive to the loading path and grain orientation.Meanwhile,the effect of strain rate on the structural evolution of NC Mg was investigated.It is found that the effect of strain rate on the plastic deformation of NC Mg is reflected through the plasticity delays and the way to release the stress.As the strain rate decreases,the plastic deformation mechanism gradually changes from intragranular to grain boundary.Some significant potential deformation mechanisms in the loading process were studied.It is observed that{1121}twins nucleated inside the grains,and the thickening process is completed by basal〈a〉slip of the twin boundary.The strain compatibility between twins is automatically optimized with loading.Moreover,the detwinning mechanism caused by the interaction between twins and basal stacking faults is clarified.展开更多
Carbon electrocatalyst materials based on lignocellulosic biomass with multi-components,various dimensions,high carbon content,and hierarchical morphology structures have gained great popularity in electrocatalytic ap...Carbon electrocatalyst materials based on lignocellulosic biomass with multi-components,various dimensions,high carbon content,and hierarchical morphology structures have gained great popularity in electrocatalytic applications recently.Due to the catalytic deficiency of neutral carbon atoms,the usage of single lignocellulosic-based carbon materials in electrocatalysis involving energy storage and conversion presents unsatisfactory applicability.However,atomic-level modulation of lignocellulose-based carbon materials can optimize the electronic structures,charge separation,transfer processes,and so forth,which results in substantially enhanced electrocatalytic performance of carbon-based catalysts.This paper reviews the recent advances in the rational design of lignocellulosic-based carbon materials as electrocatalysts from an atomic-level perspective,such as self/external heteroatom doping and metal modification.Then,through systematic discussion of the design principles and reaction mechanisms of the catalysts,the applications of the prepared lignocellulosic-based catalysts in rechargeable batteries and electrocatalysis are reviewed.Finally,the challenges in improving the catalytic performance of lignocellulosic-based carbon materials as electrocatalysts and the prospects in diverse applications are reviewed.This review contributes to the synthesis strategy of lignocellulose-based carbon electrocatalysts via atomic-level modulation,which in turn promotes the lignocellulose valorization for energy storage and conversion.展开更多
Atomic-scale strain mapping has become increasingly vital for investigating deformation mechanisms and the governing principles of solid materials.This is due to the significant impact of atomic-scale strain on the ph...Atomic-scale strain mapping has become increasingly vital for investigating deformation mechanisms and the governing principles of solid materials.This is due to the significant impact of atomic-scale strain on the physical,chemical,and mechanical properties of nanomaterials that comprise functional devices such as nanoelectronics,communication devices,electromechanical systems,and sensors.The advent of advanced electron microscopes has enabled the acquisition of high-magnification images with atomic resolution,providing an exceptional platform for measuring the atomic-scale strain of solid materials.However,accurate and unified strain mapping methods and standards for evaluating atomic-scale strain distribution remain scarce.Consequently,a unified strain mapping framework is proposed for atomic-scale strain measurement.Utilizing finite deformation analysis and the least-squares mathematical method,two types of atomic-scale strain field mapping methods have been developed,including the phase analysis-based methods(PAD and PAS)and the peak matching-based strain mapping method(PMS)for high-resolution scanning transmission electron microscope images.The prototypical 2D materials,graphene and molybdenum disulfide,serve as the subjects for the strain field mapping research,conducted through both simulation and experimentation.Upon comparing the theoretical strain mapping results of single-layer graphene and molybdenum disulfide with and without defects,it is demonstrated that the proposed strain mapping methods,particularly the PMS method,can accurately describe the large deformation surrounding a significant strain gradient.展开更多
To mitigate the harmful effects of Al_(2)O_(3) inclusions in steel,it is necessary to conduct comprehensive research on the mechanisms and kinetic laws of Al_(2)O_(3) inclusion modification by Ce.Combined with laborat...To mitigate the harmful effects of Al_(2)O_(3) inclusions in steel,it is necessary to conduct comprehensive research on the mechanisms and kinetic laws of Al_(2)O_(3) inclusion modification by Ce.Combined with laboratory experiments,first-principles calculations,and molecular dynamics simulations,the kinetic model of Ce modification for Al_(2)O_(3) inclusions was established.Based on first-principles calculations,differential charge analysis,density of states analysis,and adsorption energy analysis were performed on the transformation process from Al_(2)O_(3) to CeAlO_(3) at the atomic scale,and the microscopic transformation mechanism of inclusions at the atomic scale was obtained.Molecular dynamics simulations and the solution of mean square displacement function show that the diffusion coefficient for Ce atoms was 2.169×10^(−4) cm^(2)/s,which agreed well with experimental results.In this model,the rate-determining step is the diffusion of Ce atoms across Ce–Al–O inclusions.The relationship between the conversion rate,refining time,and initial radius was discussed.A refining time of 60 s can completely transform Al_(2)O_(3) inclusions less than 2.56μm into CeAlO_(3) inclusions,while refining time of 1200 s is sufficient to modify inclusions size below 11.47μm.展开更多
Novel and promising chloride ion batteries(CIBs)that can operate at room temperature have attracted great attentions,due to the sustainable chloride-containing resources and high theoretical energy density.To achieve ...Novel and promising chloride ion batteries(CIBs)that can operate at room temperature have attracted great attentions,due to the sustainable chloride-containing resources and high theoretical energy density.To achieve the superior electrochemical properties of CIBs,the structure design of electrode materials is essential.Herein,2D NiAl-layered double hydroxide(NiAl-LDH)nanoarrays derived from Al2O3 are in-situ grafted to graphene(G)by atomic layer deposition(ALD)and hydrothermal method.The achieved NiAl-LDH@G hybrids with 2D NiAl-LDH arrays grown perpendicularly on graphene surface,can efficiently prevent the stacking of LDHs and enlarge specific surface area to provide more active sites.The NiAl-LDH@G cathode exhibits a maximum discharge capacity of 223.3 mA h g^(-1)and an excellent reversible capacity of 107 mA h g^(-1)over 500 cycles at 100 mA g^(-1)with a high coulombic efficiency around 96%,whereas pure NiAl-LDH has a discharge capacity of only 48.8 mA h g^(-1)and a coulombic efficiency(CE)of about 78%.More importantly,the NiAl-LDH@G electrode has a stable voltage at 1.9 V and an outstanding discharge capacity of higher than 72 mA h g^(-1)after 120 days.Additionally,XRD,XPS,and EDS have been employed to unveil the electrochemical reaction and Cl-storage mechanism of the NiAlLDH@G cathode in CIBs.This work opens a facile and reasonable way for improving electrochemical performance at anion-type rechargeable batteries in terms of cathode material design and mechanism interpretation.展开更多
Liquefied natural gas storage and transportation as well as space propulsion systems have sparked inter-est in the martensitic transformation and behaviours of 316 L stainless steels(SS)under ultra-cryogenic deformati...Liquefied natural gas storage and transportation as well as space propulsion systems have sparked inter-est in the martensitic transformation and behaviours of 316 L stainless steels(SS)under ultra-cryogenic deformation.In this study,high-resolution transmission electron microscopy(HRTEM)and molecular dy-namics(MD)simulations were used to investigate the atomic arrangements and crystalline defects of deformation-induced γ-austenite→ε-martensite→α'-martensite and γ→α'martensitic transforma-tions in 316 L SS at 15 and 173 K.Theγ→εtransformation involves the glide of Shockley partial dislocations on(111)γplanes without a change in atomic spacing.The formation of anα'inclusion in a singleε-band is achieved by a continuous lattice distortion,accompanied by the formation of a tran-sition zone ofα'and the expansion of the average atomic spacings due to dislocation shuffling.Asα'grows further intoγ,the orientation relationship(OR)of theα'changes by lattice bending.This pro-cess follows the Bogers-Burgers-Olson-Cohen model despite it not occurring on intersecting shear bands.Stacking faults and twins can also serve as nucleation sites forα'at 173 K.We also found that direct transformation of γ→α'occurs by the glide of √6aγ[11(2)]/12 dislocations on every(111)γplane with misfit dislocations.Overall,this study provides,for the first time,insights into the atomic-scale mech-anisms of various two-step and one-step martensitic transformations induced by cryogenic deformation and corresponding local strain,enhancing our understanding of the role of martensitic transformation under ultra-cryogenic-temperature deformation in controlling the properties.展开更多
Efficient water dissociation catalysts are important for reducing the activation energy barrier of water molecules in the field of energy conversio n.Herein,symmetry-bro ken Rh ensemble induced by mandated charge was ...Efficient water dissociation catalysts are important for reducing the activation energy barrier of water molecules in the field of energy conversio n.Herein,symmetry-bro ken Rh ensemble induced by mandated charge was established to boost the catalytic activity toward water dissociation.As an experimental verification,the turnover frequency of 1.0-RTO_(V4)in hydrogen generation from ammonia borane hydrolysis reaches up to 2838 min-1(24828 min^(-1)depend on Rh dispersion),exceeding the benchmark set up by state-of-the-art catalysts.The transfer of mandated charge from O_(V)to Rh near O_(V)breaks the local symmetry of Rh nanoparticle and forms Rh^(γ-)(electron-aggregation Rh)-Rh interfacial atomic ensemble.This symmetry-broken Rh ensemble is the reason for the high activity of the catalyst.This work provides an effective electronic regulation strategy based on symmetry-broken atomic ensemble induced by mandated charge,designed to stimulate the limiting activity of metal catalyst in the field of next generation energy chemistry.展开更多
The exploitation of durable and highly active Pt-based electrocatalysts for the oxygen reduction reaction(ORR)is essential for the commercialization of proton exchange membrane fuel cells(PEMFCs).Herein,we designed Pt...The exploitation of durable and highly active Pt-based electrocatalysts for the oxygen reduction reaction(ORR)is essential for the commercialization of proton exchange membrane fuel cells(PEMFCs).Herein,we designed Pt@Pt_(3)Ti core-shell nanoparticles with atomic-controllable shells through precise thermal diffusing Ti into Pt nanoparticles for effective and durable ORR.Combining theoretical and experiment analysis,we found that the lattice strain of Pt_(3)Ti shells can be tailored by precisely controlling the thick-ness of Pt_(3)Ti shell in atomic-scale on account of the lattice constant difference between Pt and Pt_(3)Ti to optimize adsorption properties of Pt_(3)Ti for ORR intermediates,thus enhancing its performance.The Pt@Pt_(3)Ti catalyst with one-atomic Pt_(3)Ti shell(Pt@1L-Pt_(3)Ti/TiO_(2)-C)demonstrates excellent performance with mass activity of 592 mA mgpt-1 and durability nearly 19.5-fold that of commercial Pt/C with negligible decay(2%)after 30,000 potential cycles(0.6-1.0 V vs.RHE).Notably,at higher potential cycles(1.0 V-1.5 V vs.RHE),Pt@1L-Pt_(3)Ti/TiO_(2)-C also showed far superior durability than Pt/C(9.6%decayed while 54.8% for commercial Pt/C).This excellent stability is derived from the intrinsic stability of Pt_(3)Ti alloy and the confinement effect of TiO_(2)-C.The catalyst's enhancement was further confirmed in PEMFC configuration.展开更多
Laboratory and field observations have suggested a correlation between contact dynamics and slow dynamics.The underlying mechanical mechanisms at the contact level require investigation at the nanoscale.This study use...Laboratory and field observations have suggested a correlation between contact dynamics and slow dynamics.The underlying mechanical mechanisms at the contact level require investigation at the nanoscale.This study uses molecular dynamics(MD)simulations to investigate the interactions between two quartz plates separated by a water film,focusing on the relationship between adhesion force and separation distance.The density and orientation angle profiles were calculated from simulation data to investigate the relationship between the interfacial structure of the water film and contact potential.The simulations reveal multiple metastable states of the contact potential,consistent with existing theoretical models.The results show that the contact force is influenced by the structure of the water film,including oscillation forces and stratification.This provided verification and development for existing theoretical models based on metastable contacts.展开更多
基金financial support from the National Natural Science Foundation of China(Nos.52204335 and 52374319)the National Nature Science Foundation of China(No.52174291)the Central Universities Foundation of China(No.06500170)。
文摘The experiment explored the Fe_(2)O_(3) reduction process with H_(2)/CO mixed gas and confirmed a promoting effect from CO when its volume proportion in mixed gas is 20% at 850℃.The ReaxFF molecular dynamics(MD)simulation method was used to observe the reduction process and provide an atomic-level explanation.The accuracy of the parameters used in the simulation was verified by the density functional theory(DFT)calculation.The simulation shows that the initial reduction rate of H_(2) is much faster than that of CO(from 800 to 950℃).As the reduction proceeds,cementite,obtained after CO participates in the reduction at 850℃,will appear on the iron surface.Due to the active properties of C atoms in cementite,they are easy to further react with the O atoms in Fe_(2)O_(3).The generation of internal CO may destroy the dense structure of the surface layer,thereby affecting the overall reduction swelling of Fe_(2)O_(3).However,excess CO is detrimental to the reaction rate,mainly because of the poor thermodynamic conditions of CO in the temperature range and the molecular diffusion capacity is not as good as that of H_(2).Furthermore,the surface structures obtained after H_(2) and CO reduction have been compared,and it was found that the structure obtained by CO reduction has a larger surface area,thus promoting the sub sequent reaction of H_(2).
基金supported by the National Natural Science Foundation of China(Grant No.62275075)the Natural Science Foundation of Hubei Soliton Research Association(Grant No.2025HBSRA09)+1 种基金joint supported by Hubei Provincial Natural Science Foundation and Xianning of China(Grant Nos.2025AFD401 and 2025AFD405)Israel Science Foundation(Grant No.1695/22).
文摘We propose a theoretical framework,based on the two-component Gross-Pitaevskii equation(GPE),for the investigation of vortex solitons(VSs)in hybrid atomic-molecular Bose-Einstein condensates under the action of the stimulated Raman-induced photoassociation and square-optical-lattice potential.Stationary solutions of the coupled GPE system are obtained by means of the imaginary-time integration,while the temporal dynamics are simulated using the fourth-order Runge-Kutta algorithm.The analysis reveals stable rhombus-shaped VS shapes with topological charges m=1 and 2 of the atomic component.The stability domains and spatial structure of these VSs are governed by three key parameters:the parametric-coupling strength(χ),atomicmolecular interaction strength(g_(12)),and the optical-lattice potential depth(V_(0)).By varyingχand g_(12),we demonstrate a structural transition where four-core rhombus-shaped VSs evolve into eight-core square-shaped modes,highlighting the nontrivial nonlinear dynamics of the system.This work establishes a connection between interactions of cold atoms and topologically structured matter waves in hybrid quantum systems.
基金supported by the Pre-research fund(No.412130024).
文摘The T_(1)(Al_(2) CuLi)phase is one of the most effective strengthening nanoscale-precipitate in Al-Cu alloys with Li.However,its formation and evolution still need to be further clarified during aging due to the complex precipitation sequences.Here,a detailed investigation has been carried out on the atomic struc-tural evolution of T_(1) precipitate in an aged Al-Cu-Li-Mg-Ag alloy using state-of-the-art Cs-corrected high-angle annular dark field(HAADF)-coupled with integrated differential phase contrast(iDPC)-scanning transmission electron microscopy(STEM)and energy-dispersive X-ray spectroscopy(EDXS)techniques.An intermediate T_(1)’phase between T_(1p) and T_(1) phase,with a crystal structure and orientation rela-tionship consistent with T_(1),but exhibiting different atomic occupancy and chemical composition was found.We observed the atomic structural transformation from T_(1p) to T_(1)’phase(fcc→hcp),involving only 1/12<112>Al shear component.DFT calculation results validated our proposed structural models and the precipitation sequence.Besides,the distributions of minor solute elements(Ag,Mg,and Zn)in the pre-cipitates exhibited significant differences.These findings may contribute to a further understanding of the nucleation mechanism of T_(1) precipitate.
基金supported by grants from the National Natural Science Foundation of China(Nos.52031017,51801237)the National Key Laboratory of Science and Technology on High-strength Structural Materials in Central South University,China(No.6142912200106).
文摘This study aims to clarify the mechanisms for the grain boundary(GB)segregation through investigating the absorption of excess solute atoms at GBs in Al−Cu alloys by using the hybrid molecular dynamics/Monte Carlo simulations.Two segregation mechanisms,substitutional and interstitial mechanisms,are observed.The intergranular defects,including dislocations,steps and vacancies,and the intervals in structural units are conductive to the prevalence of interstitial mechanism.And substitutional mechanism is favored by the highly ordered twin GBs.Furthermore,the two mechanisms affect the GB structure differently.It is quantified that interstitial mechanism is less destructive to GB structure than substitutional one,and often leads to a segregation level being up to about 6 times higher than the latter.These findings contribute to atomic scale insights into the microscopic mechanisms about how solute atoms are absorbed by GB structures,and clarify the correlation among intergranular structures,segregation mechanisms and kinetics.
文摘Broadband transparent films play a pivotal role in various applications such as lenses and solar cells,particularly porous structured transparent films exhibit significant potential.This study investigates a porous SiO_(2) refractive index gradient anti-reflective film prepared by atomic layer deposition(ALD).A porous SiO_(2) film with gradual porosity was obtained by phosphoric acid etching of Al_(2)O_(3)/SiO_(2) multilayers with gradient Al2O3 ratios,achieving a gradual decrease in refractive index from the substrate to the surface.The film exhibited an average transmittance as high as 97.8%within the wavelength range from 320 nm to 1200 nm.The environmental adaptability was further enhanced by surface modification using rare earth oxide(REO)La_(2)O_(3),resulting in formation of a lotus leaf-like structure and achieving a water contact angle of 100.0°.These data proved that the modification significantly improved hydrophobic self-cleaning capability while maintaining exceptional transparency of the film.The surface structure of the modified film remained undamaged even after undergoing wipe testing,demonstrating its excellent surface durability.
基金supported by National Natural Science Foundation of China(No.523B2070,No.52225606).
文摘Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Herein,with crystal and atomic structures of the self-assembled PDI revealed from the X-ray diffraction pattern,the electronic structure is theoretically illustrated by the first-principles density functional theory calculations,suggesting the suitable band structure and the direct electronic transition for efficient photocatalytic oxygen evolution over PDI.It is confirmed that the carbonyl O atoms on the conjugation structure serve as the active sites for oxygen evolution reaction by the crystal orbital Hamiltonian group analysis.The calculations of reaction free energy changes indicate that the oxygen evolution reaction should follow the reaction pathway of H_(2)O→^(*)OH→^(*)O→^(*)OOH→^(*)O_(2)with an overpotential of 0.81 V.Through an in-depth theoretical computational analysis in the atomic and electronic structures,the origin of photocatalytic oxygen evolution activity for PDI is well illustrated,which would help the rational design and modification of polymeric photocatalysts for efficient oxygen evolution.
文摘Single-atom catalysts(SACs),in which isolated metal atoms such as palladium(Pd)are anchored on solid supports,promise breakthroughs in energy conversion and catalysis.However,balancing their activity(reaction speed)and stability(longevity)remains challenging,as the interplay between metal atoms,supports,and reactants is poorly understood.
基金supported by the National Key Research and Development Program of China(Grant No.2023YFA1407001)the Department of Science and Technology of Jiangsu Province(Grant No.BK20220032)+1 种基金support from the Guang Dong Basic and Applied Basic Research Foundation(Grant No.2023A1515010365)support from the Postgraduate Research and Practice Innovation Program of Jiangsu Province under Grant No.KYCX25_1934。
文摘Heat dissipation highly relies on the thermal conductivity(κ)of materials.Materials with large bandgaps and signifcant atomic mass ratios,such as BAs,SiC,andθ-TaN,have attracted considerable attention due to their potential for achieving ultra-highκ,with BAs serving as a particularly representative example due to its unique combination of large bandgap and high thermal conductivity.In this paper,the efects of atomic mass modifcation on phonon bandgap andκare systematically investigated using a BAs model,accounting for both three-and four-phonon scattering processes.A 20%increase inκcan be obtained by substituting B,achieved through widening the phonon bandgap,which suppresses phonon scattering.Notably,the AAOO four-phonon scattering channel is more suppressed than the AAO three-phonon channel,leading to an increased phonon lifetime(τ).For As,κcan also be enhanced by 5%when replaced by lighter atoms,such as^(69)As,primarily due to the increased phonon group velocity(υ).We systematically clarify how atomic-mass-induced bandgap variations afectτ,υ,and thereforeκin wide-bandgap systems.Our work provides a specifc scheme for further improving the ultra-highκof materials with large bandgaps,which possesses great guiding signifcance.
基金supported by the National Natural Science Foundation of China(Grant Nos.12174402 and 12393821)the Strategic Priority Research Program of the Chinese Academy of Sciences(Grant Nos.XDB0920100 and XDB0920101)+2 种基金the Nature Science Foundation of Hubei Province(Grant Nos.2019CFA058 and 2022CFA013)supported by the Natural Sciences and Engineering Research Council of Canada(NSERC)supported in part by NSF grant PHY-2116679.All the calculations are finished on the APM-Theoretical Computing Cluster(APMTCC)。
文摘For atoms in external electric fields,the hyperpolarizabilities are the coefficients describing the nonlinear interactions contributing to the induced energies at the fourth power of the applied electric fields.Accurate evaluations of these coefficients for various systems are crucial for improving precision in advanced atom-based optical lattice clocks and for estimating field-induced effects in atoms for quantum information applications.However,there is a notable scarcity of research on atomic hyperpolarizabilities,especially in the relativistic realm.Our work addresses this gap by establishing a novel set of alternative formulas for the hyperpolarizability based on the fourth-order perturbation theory.These formulas offer a more reasonable regrouping of scalar and tensor components compared to previous formulas,thereby enhancing their correctness and applicability.To validate our formulas,we perform the calculations for the ground and low-lying excited pure states of few-electron atoms H,Li,and Be^(+).The highly accurate results obtained for the H atom could serve as benchmarks for further development of other theoretical methods.
基金National Natural Science Foundation of China(22309032,22109120,and 62104170)Guangdong Basic and Applied Basic Research Foundation(2022A1515011737)+2 种基金Science and Technology Program of Guangzhou(2023A04J1395)GDAS’Project of Science and Technology Development(2021GDASYL-20210102010)Zhejiang Provincial Natural Science Foundation of China(LY23F040001)。
文摘Photocatalytic oxygen reduction for hydrogen peroxide(H_(2)O_(2))synthesis presents a green and costeffective production method.However,achieving highly selective H_(2)O_(2)synthesis remains challenging,necessitating precise control over free radical reaction pathways and minimizing undesirable oxidative by-products.Herein,we report for the visible light-driven simultaneous co-photocatalytic reduction of O2to H_(2)O_(2)and oxidation of biomass using the atomic rubidium-nitride modified carbon nitride(CNRb).The optimized CNRb catalyst demonstrates a record photoreduction rate of 8.01 mM h^(-1)for H_(2)O_(2)generation and photooxidation rate of 3.75 mM h^(-1)for furfuryl alcohol to furoic acid,achieving a remarkable solar-to-chemical conversion(SCC)efficiency of up to 2.27%.Experimental characterizations and DFT calculation disclosed that the introducing atomic Rb–N configurations allows for the high-selective generation of superoxide radicals while suppressing hydroxyl free radical formation.This is because the Rb–N serves as the new alternative site to perceive a stronger connection position for O2adsorption and reinforce the capability to extract protons,thereby triggering a high selective redox product formation.This study holds great potential in precisely regulating reactive radical processes at the atomic level,thereby paving the way for efficient synthesis of H_(2)O_(2)coupled with biomass valorization.
基金supported by the National Natural Science Foundation of China(Nos.U21A2054,21905007)the Key Discipline of Materials Science and Engineering,Bureau of Education of Guangzhou(Grant No.202255464).
文摘The bismuth-telluride-based alloy is the only thermoelectric material commercialized for the applications of refrigeration and energy harvesting,but its low cost-effectiveness severely restricts its large-scale ap-plication.The introduction of a porous structure in bulk thermoelectric materials has been theoretically proven to effectively reduce thermal conductivity and cost.However,the electrical properties of highly porous materials are considerably suppressed due to the strong carrier scattering at the interface be-tween the matrix and pores,ultimately leading to decreased figure of merit,ZT.Here,we use an atomic layer deposition strategy to introduce some hollow glass bubbles with nano-oxide layers into commercial Bi_(0.5)Sb_(1.5)Te_(3)for preparing high-performance porous thermoelectric materials.Experimental results indi-cate that the nano-oxide layers weaken carrier scattering at the interface between pores and matrix while maintaining high-strength phonon scattering,thereby optimizing carrier/phonon transport behaviors,and effectively increasing the ZT by 23.2%(from 0.99 to 1.22 at 350 K).Besides,our strategy has excellent universality confirmed by its effectiveness in improving the ZT of Bi_(2)Te_(2.7)Se_(0.3),therefore demonstrating great potential for developing low-cost and high-performance thermoelectric materials.
基金supports from the projects by the NSFC[51771166]the Hebei Natural Science Foundation[E2019203452,E2021203011]+3 种基金the key project of department of education of Hebei province[ZD2021107]project of the central government guiding local science and technology development[216Z1001G]Cultivation Project for Basic Research and Innovation of Yanshan University[2021LGZD002]project of State Key Laboratory of Materials Processing and Die&Mould Technology[P2023-004]are gratefully acknowledged.
文摘Molecular dynamics(MD)simulation is employed to investigate the deformation behavior under various loading paths and strain rates of nanocrystalline magnesium(NC Mg)with[0001]texture.Atomic-scale structural evolution of NC Mg was performed under uniaxial and biaxial loadings.In tension process,compression twins and basal slip dominate,while the compression process is dominated by tension twins.The activation mechanism of twinning is highly sensitive to the loading path and grain orientation.Meanwhile,the effect of strain rate on the structural evolution of NC Mg was investigated.It is found that the effect of strain rate on the plastic deformation of NC Mg is reflected through the plasticity delays and the way to release the stress.As the strain rate decreases,the plastic deformation mechanism gradually changes from intragranular to grain boundary.Some significant potential deformation mechanisms in the loading process were studied.It is observed that{1121}twins nucleated inside the grains,and the thickening process is completed by basal〈a〉slip of the twin boundary.The strain compatibility between twins is automatically optimized with loading.Moreover,the detwinning mechanism caused by the interaction between twins and basal stacking faults is clarified.
基金supported by the National Natural Science Foundation of China(32071721,32071720,32271814,32301530,32471806)Tianjin Excellent Special Commissioner for Agricultural Science and Technology Project(23ZYCGSN00580)+4 种基金Young Elite Scientist Sponsorship Program by Cast(No.YESS20230242)Natural Science Foundation of Tianjin(23JCZDJC00630)the China Postdoctoral Science Foundation under Grant Number(2023M741363,2023M740563)the Postdoctoral Innovation Project of Shandong Province(SDCX-ZG-202302031)China Scholarship Council(No.202408120091,No.202408120105).
文摘Carbon electrocatalyst materials based on lignocellulosic biomass with multi-components,various dimensions,high carbon content,and hierarchical morphology structures have gained great popularity in electrocatalytic applications recently.Due to the catalytic deficiency of neutral carbon atoms,the usage of single lignocellulosic-based carbon materials in electrocatalysis involving energy storage and conversion presents unsatisfactory applicability.However,atomic-level modulation of lignocellulose-based carbon materials can optimize the electronic structures,charge separation,transfer processes,and so forth,which results in substantially enhanced electrocatalytic performance of carbon-based catalysts.This paper reviews the recent advances in the rational design of lignocellulosic-based carbon materials as electrocatalysts from an atomic-level perspective,such as self/external heteroatom doping and metal modification.Then,through systematic discussion of the design principles and reaction mechanisms of the catalysts,the applications of the prepared lignocellulosic-based catalysts in rechargeable batteries and electrocatalysis are reviewed.Finally,the challenges in improving the catalytic performance of lignocellulosic-based carbon materials as electrocatalysts and the prospects in diverse applications are reviewed.This review contributes to the synthesis strategy of lignocellulose-based carbon electrocatalysts via atomic-level modulation,which in turn promotes the lignocellulose valorization for energy storage and conversion.
基金support from the National Natural Science Foundation of China through Grants 12172190,11872035,11632010,and 12302236。
文摘Atomic-scale strain mapping has become increasingly vital for investigating deformation mechanisms and the governing principles of solid materials.This is due to the significant impact of atomic-scale strain on the physical,chemical,and mechanical properties of nanomaterials that comprise functional devices such as nanoelectronics,communication devices,electromechanical systems,and sensors.The advent of advanced electron microscopes has enabled the acquisition of high-magnification images with atomic resolution,providing an exceptional platform for measuring the atomic-scale strain of solid materials.However,accurate and unified strain mapping methods and standards for evaluating atomic-scale strain distribution remain scarce.Consequently,a unified strain mapping framework is proposed for atomic-scale strain measurement.Utilizing finite deformation analysis and the least-squares mathematical method,two types of atomic-scale strain field mapping methods have been developed,including the phase analysis-based methods(PAD and PAS)and the peak matching-based strain mapping method(PMS)for high-resolution scanning transmission electron microscope images.The prototypical 2D materials,graphene and molybdenum disulfide,serve as the subjects for the strain field mapping research,conducted through both simulation and experimentation.Upon comparing the theoretical strain mapping results of single-layer graphene and molybdenum disulfide with and without defects,it is demonstrated that the proposed strain mapping methods,particularly the PMS method,can accurately describe the large deformation surrounding a significant strain gradient.
基金supported by the National Natural Science Foundation of China(Nos.52064011,52274331 and 52264041)Guizhou Provincial Basic Research Program(Natural Science)(Nos.ZK[2021]258 and ZK[2023]Zhongdian 020)+6 种基金Guizhou Provincial Key Technology R&D Program(No.[2021]342)Guizhou Provincial Program on Commercialization of Scientific and Technological Achievements(No.[2022]089)supported by Open Project of State Key Laboratory of Advanced Special Steel,Shanghai Key Laboratory of Advanced Ferrometallurgy,Shanghai University(No.SKLASS 2023-08)the Science and Technology Commission of Shanghai Municipality(No.19DZ2270200)supported by State Key Laboratory of Advanced Metallurgy(No.K23-04)China Postdoctoral Science Foundation(No.2023MD744232)Key Research Projects in Higher Education Institutions of Henan Province(No.24B450003).
文摘To mitigate the harmful effects of Al_(2)O_(3) inclusions in steel,it is necessary to conduct comprehensive research on the mechanisms and kinetic laws of Al_(2)O_(3) inclusion modification by Ce.Combined with laboratory experiments,first-principles calculations,and molecular dynamics simulations,the kinetic model of Ce modification for Al_(2)O_(3) inclusions was established.Based on first-principles calculations,differential charge analysis,density of states analysis,and adsorption energy analysis were performed on the transformation process from Al_(2)O_(3) to CeAlO_(3) at the atomic scale,and the microscopic transformation mechanism of inclusions at the atomic scale was obtained.Molecular dynamics simulations and the solution of mean square displacement function show that the diffusion coefficient for Ce atoms was 2.169×10^(−4) cm^(2)/s,which agreed well with experimental results.In this model,the rate-determining step is the diffusion of Ce atoms across Ce–Al–O inclusions.The relationship between the conversion rate,refining time,and initial radius was discussed.A refining time of 60 s can completely transform Al_(2)O_(3) inclusions less than 2.56μm into CeAlO_(3) inclusions,while refining time of 1200 s is sufficient to modify inclusions size below 11.47μm.
基金supported by the National Natural Science Foundation of China(Grant Nos.22278101,22068010,22168016,and 52365044)the Natural Science Foundation of Hainan Province(Grant Nos.2019RC142 and 519QN176)the Finance Science and Technology Project of Hainan Province(Grant No.ZDYF2020009).
文摘Novel and promising chloride ion batteries(CIBs)that can operate at room temperature have attracted great attentions,due to the sustainable chloride-containing resources and high theoretical energy density.To achieve the superior electrochemical properties of CIBs,the structure design of electrode materials is essential.Herein,2D NiAl-layered double hydroxide(NiAl-LDH)nanoarrays derived from Al2O3 are in-situ grafted to graphene(G)by atomic layer deposition(ALD)and hydrothermal method.The achieved NiAl-LDH@G hybrids with 2D NiAl-LDH arrays grown perpendicularly on graphene surface,can efficiently prevent the stacking of LDHs and enlarge specific surface area to provide more active sites.The NiAl-LDH@G cathode exhibits a maximum discharge capacity of 223.3 mA h g^(-1)and an excellent reversible capacity of 107 mA h g^(-1)over 500 cycles at 100 mA g^(-1)with a high coulombic efficiency around 96%,whereas pure NiAl-LDH has a discharge capacity of only 48.8 mA h g^(-1)and a coulombic efficiency(CE)of about 78%.More importantly,the NiAl-LDH@G electrode has a stable voltage at 1.9 V and an outstanding discharge capacity of higher than 72 mA h g^(-1)after 120 days.Additionally,XRD,XPS,and EDS have been employed to unveil the electrochemical reaction and Cl-storage mechanism of the NiAlLDH@G cathode in CIBs.This work opens a facile and reasonable way for improving electrochemical performance at anion-type rechargeable batteries in terms of cathode material design and mechanism interpretation.
基金supported by the Henry Royce Institute for Advanced Materials,funded through Engineering and Physical Sciences Research Council(EPSRC)grants EP/R00661X/1,EP/S019367/1,EP/P025021/1,and EP/P025498/1.
文摘Liquefied natural gas storage and transportation as well as space propulsion systems have sparked inter-est in the martensitic transformation and behaviours of 316 L stainless steels(SS)under ultra-cryogenic deformation.In this study,high-resolution transmission electron microscopy(HRTEM)and molecular dy-namics(MD)simulations were used to investigate the atomic arrangements and crystalline defects of deformation-induced γ-austenite→ε-martensite→α'-martensite and γ→α'martensitic transforma-tions in 316 L SS at 15 and 173 K.Theγ→εtransformation involves the glide of Shockley partial dislocations on(111)γplanes without a change in atomic spacing.The formation of anα'inclusion in a singleε-band is achieved by a continuous lattice distortion,accompanied by the formation of a tran-sition zone ofα'and the expansion of the average atomic spacings due to dislocation shuffling.Asα'grows further intoγ,the orientation relationship(OR)of theα'changes by lattice bending.This pro-cess follows the Bogers-Burgers-Olson-Cohen model despite it not occurring on intersecting shear bands.Stacking faults and twins can also serve as nucleation sites forα'at 173 K.We also found that direct transformation of γ→α'occurs by the glide of √6aγ[11(2)]/12 dislocations on every(111)γplane with misfit dislocations.Overall,this study provides,for the first time,insights into the atomic-scale mech-anisms of various two-step and one-step martensitic transformations induced by cryogenic deformation and corresponding local strain,enhancing our understanding of the role of martensitic transformation under ultra-cryogenic-temperature deformation in controlling the properties.
基金supported by the National Natural Science Foundation of China(No.22279118,No.22309164)the China Postdoctoral Science Foundation(No.2023M733214)+1 种基金the Young Top Talent Program of Zhongyuan-Yingcai-Jihua(No.30602674)the Special Projects of Henan Province Key Research and Development and Promotion(Science and Technology Research)(No.232102241033)。
文摘Efficient water dissociation catalysts are important for reducing the activation energy barrier of water molecules in the field of energy conversio n.Herein,symmetry-bro ken Rh ensemble induced by mandated charge was established to boost the catalytic activity toward water dissociation.As an experimental verification,the turnover frequency of 1.0-RTO_(V4)in hydrogen generation from ammonia borane hydrolysis reaches up to 2838 min-1(24828 min^(-1)depend on Rh dispersion),exceeding the benchmark set up by state-of-the-art catalysts.The transfer of mandated charge from O_(V)to Rh near O_(V)breaks the local symmetry of Rh nanoparticle and forms Rh^(γ-)(electron-aggregation Rh)-Rh interfacial atomic ensemble.This symmetry-broken Rh ensemble is the reason for the high activity of the catalyst.This work provides an effective electronic regulation strategy based on symmetry-broken atomic ensemble induced by mandated charge,designed to stimulate the limiting activity of metal catalyst in the field of next generation energy chemistry.
基金supported by the National Natural Science Foundation of China(No.21875039)the Project on the Integration of Industry-Education-Research of Fujian Province(No.2021H6020)the State Key Laboratory of Advanced Technology for Materials Synthesis and Processing(Wuhan University of Technology).
文摘The exploitation of durable and highly active Pt-based electrocatalysts for the oxygen reduction reaction(ORR)is essential for the commercialization of proton exchange membrane fuel cells(PEMFCs).Herein,we designed Pt@Pt_(3)Ti core-shell nanoparticles with atomic-controllable shells through precise thermal diffusing Ti into Pt nanoparticles for effective and durable ORR.Combining theoretical and experiment analysis,we found that the lattice strain of Pt_(3)Ti shells can be tailored by precisely controlling the thick-ness of Pt_(3)Ti shell in atomic-scale on account of the lattice constant difference between Pt and Pt_(3)Ti to optimize adsorption properties of Pt_(3)Ti for ORR intermediates,thus enhancing its performance.The Pt@Pt_(3)Ti catalyst with one-atomic Pt_(3)Ti shell(Pt@1L-Pt_(3)Ti/TiO_(2)-C)demonstrates excellent performance with mass activity of 592 mA mgpt-1 and durability nearly 19.5-fold that of commercial Pt/C with negligible decay(2%)after 30,000 potential cycles(0.6-1.0 V vs.RHE).Notably,at higher potential cycles(1.0 V-1.5 V vs.RHE),Pt@1L-Pt_(3)Ti/TiO_(2)-C also showed far superior durability than Pt/C(9.6%decayed while 54.8% for commercial Pt/C).This excellent stability is derived from the intrinsic stability of Pt_(3)Ti alloy and the confinement effect of TiO_(2)-C.The catalyst's enhancement was further confirmed in PEMFC configuration.
文摘Laboratory and field observations have suggested a correlation between contact dynamics and slow dynamics.The underlying mechanical mechanisms at the contact level require investigation at the nanoscale.This study uses molecular dynamics(MD)simulations to investigate the interactions between two quartz plates separated by a water film,focusing on the relationship between adhesion force and separation distance.The density and orientation angle profiles were calculated from simulation data to investigate the relationship between the interfacial structure of the water film and contact potential.The simulations reveal multiple metastable states of the contact potential,consistent with existing theoretical models.The results show that the contact force is influenced by the structure of the water film,including oscillation forces and stratification.This provided verification and development for existing theoretical models based on metastable contacts.
