A composite electrocatalyst,CoMoNiO-S/NF-110(NF is nickel foam),was synthesized through electrodeposition,followed by pyrolysis and then the vulcanization process.CoMoNiO-S/NF-110 exhibited a structure where Ni3S2 and...A composite electrocatalyst,CoMoNiO-S/NF-110(NF is nickel foam),was synthesized through electrodeposition,followed by pyrolysis and then the vulcanization process.CoMoNiO-S/NF-110 exhibited a structure where Ni3S2 and Mo2S3 nanoparticles were integrated at the edges of Co3O4 nanosheets,creating a rich,heterogeneous interface that enhances the synergistic effects of each component.In an alkaline electrolyte,the synthesized CoMoNiO-S/NF-110 exhibited superior electrocatalytic performance for oxygen evolution reaction(OER),achieving current densities of 100 and 200 mA·cm^(-2) with low overpotentials of 199.4 and 224.4 mV,respectively,outperforming RuO2 and several high-performance Mo and Ni-based catalysts.This excellent performance is attributed to the rich interface formed between the components and active sites exposed by the defect structure.展开更多
The poor electrical conductivity of metal-organic frameworks(MOFs)limits their electrocatalytic performance in the oxygen evolution reaction(OER).In this study,a Py@Co-MOF composite material based on pyrene(Py)molecul...The poor electrical conductivity of metal-organic frameworks(MOFs)limits their electrocatalytic performance in the oxygen evolution reaction(OER).In this study,a Py@Co-MOF composite material based on pyrene(Py)molecules and{[Co2(BINDI)(DMA)_(2)]·DMA}_(n)(Co-MOF,H4BINDI=N,N'-bis(5-isophthalic acid)naphthalenediimide,DMA=N,N-dimethylacetamide)was synthesized via a one-pot method,leveragingπ-πinteractions between pyrene and Co-MOF to modulate electrical conductivity.Results demonstrate that the Py@Co-MOF catalyst exhibited significantly enhanced OER performance compared to pure Co-MOF or pyrene-based electrodes,achieving an overpotential of 246 mV at a current density of 10 mA·cm^(-2) along with excellent stability.Density functional theory(DFT)calculations reveal that the formation of O*in the second step is the rate-determining step(RDS)during the OER process on Co-MOF,with an energy barrier of 0.85 eV due to the weak adsorption affinity of the OH*intermediate for Co sites.CCDC:2419276.展开更多
The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor ...The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor featuring a broad spectral absorption range,is successfully employed as the electron acceptor to combine with CdS for constructing a S-scheme heterojunction.The optimized photocatalyst(CdSCuO2∶1)delivers an exceptional hydrogen evolution rate of 18.89 mmol/(g·h),4.15-fold higher compared with bare CdS.X-ray photoelectron spectroscopy(XPS)and ultraviolet-visible diffuse reflection absorption spectroscopy(UV-vis DRS)confirmed the S-scheme band structure of the composites.Moreover,the surface photovoltage(SPV)and electron paramagnetic resonance(EPR)indicated that the photogenerated electrons and photogenerated holes of CdS-CuO2∶1 were respectively transferred to the conduction band(CB)of CdS with a higher reduction potential and the valence band(VB)of CuO with a higher oxidation potential under illumination,as expected for the S-scheme mechanism.Density-functional-theory calculations of the electron density difference(EDD)disclose an interfacial electric field oriented from CdS to CuO.This built-in field suppresses charge recombination and accelerates carrier migration,rationalizing the markedly enhanced PHE activity.This study offers a novel strategy for designing S-scheme heterojunctions with high light harvesting and charge utilization toward sustainable solar-tohydrogen conversion.展开更多
Binary composites(ZIF-67/rGO)were synthesized by one-step precipitation method using cobalt nitrate hexahydrate as metal source,2-methylimidazole as organic ligand,and reduced graphene oxide(rGO)as carbon carrier.Then...Binary composites(ZIF-67/rGO)were synthesized by one-step precipitation method using cobalt nitrate hexahydrate as metal source,2-methylimidazole as organic ligand,and reduced graphene oxide(rGO)as carbon carrier.Then Ru3+was introduced for ion exchange,and the porous Ru-doped Co_(3)O_(4)/rGO(Ru-Co_(3)O_(4)/rGO)composite electrocatalyst was prepared by annealing.The phase structure,morphology,and valence state of the catalyst were analyzed by X-ray powder diffraction(XRD),scanning electron microscope(SEM),transmission electron microscopy(TEM),and X-ray photoelectron spectroscopy(XPS).In 1 mol·L^(-1)KOH,the oxygen evolution reaction(OER)performance of the catalyst was measured by linear sweep voltammetry,cyclic voltammetry,and chronoamperometry.The results show that the combination of Ru doping and rGO provides a fast channel for collaborative electron transfer.At the same time,rGO as a carbon carrier can improve the electrical conductivity of Ru-Co_(3)O_(4)particles,and the uniformly dispersed nanoparticles enable the reactants to diffuse freely on the catalyst.The results showed that the electrochemical performance of Ru-Co_(3)O_(4)/rGO was much better than that of Co_(3)O_(4)/rGO,and the overpotential of Ru-Co_(3)O_(4)/rGO was 363.5 mV at the current density of 50 mA·cm^(-2).展开更多
The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alka...The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alkaline water.Precise control of the electronic structure by heteroatom doping has proven to be efficient for increasing catalytic activity.Nevertheless,both the structural characteristics and the underlying mechanism are not well understood,especially for doping with two different atoms,thus limiting the use of these catalysts.We report the production of phosphorus and nitrogen co-doped hollow carbon nanospheres(HCNs)by the copolymerization of pyrrole and aniline at a Triton X-100 micelle-interface,followed by doping with phytic acid and carbonization.The unique pore structure and defect-rich framework of the HCNs expose numerous active sites.Crucially,the combined effect of graphitic nitrogen and phosphorus-carbon bonds modulate the local electronic structure of adjacent C atoms and facilitates electron transfer.As a res-ult,the HCN carbonized at 1100°C exhibited superior HER activity and an outstanding stability(70 h at a current density of 10 mA cm^(−2))in alkaline water,because of the large number of graphitic nitrogen and phosphorus-carbon bonds.展开更多
Sulfur-doped iron-cobalt tannate nanorods(S-FeCoTA)derived from metal-organic frameworks(MOFs)as electrocatalysts were synthesized via a one-step hydrothermal method.The optimized S-FeCoTA was interlaced by loose nano...Sulfur-doped iron-cobalt tannate nanorods(S-FeCoTA)derived from metal-organic frameworks(MOFs)as electrocatalysts were synthesized via a one-step hydrothermal method.The optimized S-FeCoTA was interlaced by loose nanorods,which had many voids.The S-FeCoTA catalysts exhibited excellent electrochemical oxygen evolution reaction(OER)performance with a low overpotential of 273 mV at 10 mA·cm^(-2)and a small Tafel slope of 36 mV·dec^(-1)in 1 mol·L^(-1)KOH.The potential remained at 1.48 V(vs RHE)at 10 mA·cm^(-2)under continuous testing for 15 h,implying that S-FeCoTA had good stability.The Faraday efficiency of S-FeCoTA was 94%.The outstanding OER activity of S-FeCoTA is attributed to the synergistic effects among S,Fe,and Co,thus promoting electron transfer,reducing the reaction kinetic barrier,and enhancing the OER performance.展开更多
Several tritylodontid taxa have been reported from the Upper Jurassic of the Wucaiwan area in the Junggar Basin of Xinjiang,northwestern China,including Yuanotherium minor.The original study described the partially pr...Several tritylodontid taxa have been reported from the Upper Jurassic of the Wucaiwan area in the Junggar Basin of Xinjiang,northwestern China,including Yuanotherium minor.The original study described the partially preserved postcanine teeth in the middle of the left upper maxilla.After detailed re-examination of the specimen and by CT scanning,3D reconstruction,and scanning electron microscopy observations,we provided a more detailed description of the osteology,neurosensory,and tooth wear pattern for all the bones preserved in this specimen and clarified some characters.Based on new information about the cusp wear pattern,the chewing movement pattern of the dentition and detailed cusp morphology,we discussed the cuspal homology of upper cheek teeth of tritylodontids and postulate a standardized method for cusp identification.We hypothesize that the unique maxilla characteristics furnish the evidence for transitional stages about the evolution of the upper jaw-palate structure in tritylodontids.展开更多
The performance of a material is directly affected by its microstructural development during the solidification phase. Discrete cellular automaton (CA) models are widelyused in materials science to simulate and predic...The performance of a material is directly affected by its microstructural development during the solidification phase. Discrete cellular automaton (CA) models are widelyused in materials science to simulate and predict microstructural growth. This review comprehensively explains the developments and applications of CA in solidification structure simulation, including the theoretical underpinnings, computational procedures, software development, and recent advances. Summarizes the potential and limitations of cellular automata in understanding microstructure evolution during solidification, explores the evolution of microstructures during solidification, and adds to our existing knowledge of cellular automaton theory. Finally, the research trend in simulating the evolution of the solidification microstructure using cellular automaton theory is explored.展开更多
Transition metal dichalcogenides(TMDs)recently attracted widespread attention due to their potential application to the electrocatalysis of the hydrogen evolution reaction(HER).However,their HER performance is far inf...Transition metal dichalcogenides(TMDs)recently attracted widespread attention due to their potential application to the electrocatalysis of the hydrogen evolution reaction(HER).However,their HER performance is far inferior to that of platinum(Pt)metal.Preparation of multi-elemental alloy and construction of heterostructure are considered as highly effective methods to enhance hydrogen production activity.Herein,a novel quaternary CoMoSSe alloy with heterostructure was synthesized on the surface of carbon black(CB)particles(CoMoSSe@CB)by a simple Sol-Gel process and thereafter served as HER catalyst.Compared to CoSe@CB and MoS2@CB electrocatalysts,CoMoSSe@CB exhibits superior HER activity with a low overpotential of 190 mV at-10 mA·cm^(-2) and a Tafel slope of 62 mV·dec^(-1).This improvement is attributed to the alloying effects among Co,Mo,S and Se,as well as the heterogeneous structure in the composite material,which regulate the electronic structure and intermediate free energy,thereby increasing the number of active sites and enhancing charge-transfer ability.This work can provide new ideas and concepts for designing novel and efficient TMD electrocatalysts.展开更多
With the urgent need to resolve complex behaviors in nonlinear evolution equations,this study makes a contribution by establishing the local existence of solutions for Cauchy problems associated with equations of mixe...With the urgent need to resolve complex behaviors in nonlinear evolution equations,this study makes a contribution by establishing the local existence of solutions for Cauchy problems associated with equations of mixed types.Our primary contribution is the establishment of solution existence,illuminating the dynamics of these complex equations.To tackle this challenging problem,we construct an approximate solution sequence and apply the contraction mapping principle to rigorously prove local solution existence.Our results significantly advance the understanding of nonlinear evolution equations of mixed types.Furthermore,they provide a versatile,powerful approach for tackling analogous challenges across physics,engineering,and applied mathematics,making this work a valuable reference for researchers in these fields.展开更多
An evolution inequality of Sobolev type involving a nonlinear convolution term is considered.By using the nonlinear capacity method and the contradiction argument,the non-existence of the nontrivial local weak solutio...An evolution inequality of Sobolev type involving a nonlinear convolution term is considered.By using the nonlinear capacity method and the contradiction argument,the non-existence of the nontrivial local weak solution is proved.展开更多
Through employing zeolitic imidazolate framework-67(ZIF-67)templates,the straightforward hydrother-mal and electrodeposition methods were applied to synthesize FeOOH@CoMoO_(4)heterostructure attached to the sur-face o...Through employing zeolitic imidazolate framework-67(ZIF-67)templates,the straightforward hydrother-mal and electrodeposition methods were applied to synthesize FeOOH@CoMoO_(4)heterostructure attached to the sur-face of nickel foam(NF).The specific structure of the as-prepared FeOOH@CoMoO_(4)/NF-400s provided pronounced porosity and extensive surface area,enhancing rapid electron transport and exposing abundant active sites to improve catalytic reactions.Furthermore,the introduction of FeOOH,which induces electron transfer from FeOOH to CoMoO_(4),confirms their strong electronic interaction,thereby leading to an accelerated surface catalytic reaction.Consequently,the constructed FeOOH@CoMoO_(4)/NF-400s heterostructure demonstrated exceptional oxygen evolu-tion reaction(OER)activity,requiring an overpotential of 199 mV to deliver the current density of 10 mA·cm^(-2),cou-pled with the superior Tafel slope value of 49.56 mV·dec^(-1)and outstanding stability over 20 h under the current densities of both 10 and 100 mA·cm^(-2).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
The utilization of nickel-based catalysts as alternatives to expensive platinum-based(Pt-based)materials for the hydrogen evolution reaction in acidic electrolytes has attracted considerable attention due to their pot...The utilization of nickel-based catalysts as alternatives to expensive platinum-based(Pt-based)materials for the hydrogen evolution reaction in acidic electrolytes has attracted considerable attention due to their potential for enabling cost-effective industrial applications.However,the unsatisfied cyclic stability and electrochemical activity limit their further application.In this work,nickel-molybdenum(Ni-Mo)alloy catalysts were successfully synthesized through a comprehensive process including electrodeposition,thermal annealing,and electrochemical activation.Owing to the synergistic interaction of molybdenum trinickelide(Ni_(3)Mo)and molybdenum dioxide(MoO_(2))in Ni-Mo alloy,the catalyst display superior overall electrochemical properties.A low overpotential of 86 mV at 10 mA/cm^(2)and a Tafel slope of 74.0 mV/dec in 0.5 mol/L H_(2)SO_(4)solution can be achieved.Notably,remarkable stability with negligible performance degradation even after 100 h could be maintained.This work presents a novel and effective strategy for the design and fabrication of high-performance,non-precious metal electrocatalysts for acidic water electrolysis.展开更多
Elemental doping is an effective strategy for tuning the band structure of graphite carbon nitride(CN)to enhance its photocatalytic performance.In this study,sodium(Na)and oxygen(O)co-doped carbon nitride(Na/O-CN_(x),...Elemental doping is an effective strategy for tuning the band structure of graphite carbon nitride(CN)to enhance its photocatalytic performance.In this study,sodium(Na)and oxygen(O)co-doped carbon nitride(Na/O-CN_(x),x=1.0,2.0,3.0,4.0)was synthesized via solid-phase reaction of sodium citrate(NaCA)and pure CN powder in the Teflon-sealed autoclave under air conditions at 180℃.Surface area of Na/O-CN_(3.0) is measured to be 18.8 m^(2)/g,increasing by 60.7%compared to that of pure CN(11.7 m^(2)/g).Bandgap energy of Na/O-CN_(3.0) is determined to be 2.68 eV,marginally lower than that of pure CN(2.70 eV),thereby enhancing its capacity for sunlight absorption.Meanwhile,the incorporation of Na and O atoms into Na/O-CN_(x) is found to effectively reduce recombination rates of photogenerated electron-hole pairs.As a result,Na/O-CN_(x) samples exhibit markedly enhanced photocatalytic hydrogen evolution activity under visible light irradiation.Notably,the optimal Na/O-CN_(3.0) sample achieves a photocatalytic hydrogen production rate of 103.2μmol·g^(–1)·h^(–1),which is 8.2 times greater than that of pure CN(11.2μmol·g^(–1)·h^(–1)).Furthermore,a series of Na/O-CN_(x)-yO_(2)(y=0,20%,40%,60%,80%,100%)samples were prepared by modulating the oxygen content within reaction atmosphere.The catalytic performance evaluations reveal that the incorporation of both Na and O atoms in Na/O-CN_(3.0) enhances photocatalytic activity.This study also introduces novel methodologies for synthesis of metal atom-doped CN materials at lower temperature,highlighting the synergistic effect of Na and O atoms in photocatalytic hydrogen production of Na/O-CN_(x) samples.展开更多
The development of highly active catalyst in pH-neutral media for oxygen evolution reaction(OER)is critical in the field of renewable energy storage and conversion.Nevertheless,the slow kinetics of proton-coupled elec...The development of highly active catalyst in pH-neutral media for oxygen evolution reaction(OER)is critical in the field of renewable energy storage and conversion.Nevertheless,the slow kinetics of proton-coupled electron transfer(PCET)hinders the overall OER efficiency.Herein,we report an ionic liquid(IL)modified CoSn(OH)_(6)nanocubes(denoted as CoS-n(OH)_(6)-IL),which could be prepared through a facile strategy.The modified IL would not change the structural character-istics of CoSn(OH)_(6),but could effectively regulate the local proton activity near the active sites.The CoSn(OH)_(6)-IL exhibited higher intrinsic OER performances than the pristine CoSn(OH)_(6)in neutral media.For example,the current density of CoS-n(OH)_(6)-IL at 1.8 V versus reversible hydrogen electrode(RHE)was about 4 times higher than that of CoSn(OH)_(6).According to the pH-dependent kinetic investigations,operando electrochemical impedance spectroscopic,chemical probe tests,and deuterium kinetic isotope effects,the interfacial layer of IL could be utilized as a proton transfer mediator to promote the proton transfer,which enhances the surface coverage of OER intermediates and reduces the activation barrier.Consequent-ly,the sluggish OER kinetics would be efficiently accelerated.This study provides a facile and effective strategy to facilitate the PCET processes and is beneficial to guide the rational design of OER electrocatalysts.展开更多
When performing tasks,unmanned clusters often face a variety of strategy choices.One of the key issues in unmanned cluster tasks is the method through which to design autonomous collaboration and cooperative evolution...When performing tasks,unmanned clusters often face a variety of strategy choices.One of the key issues in unmanned cluster tasks is the method through which to design autonomous collaboration and cooperative evolution mechanisms that allow for unmanned clusters to maximize their overall task effective-ness under the condition of strategic diversity.This paper ana-lyzes these task requirements from three perspectives:the diver-sity of the decision space,information network construction,and the autonomous collaboration mechanism.Then,this paper pro-poses a method for solving the problem of strategy selection diversity under two network structures.Next,this paper presents a Moran-rule-based evolution dynamics model for unmanned cluster strategies and a vision-driven-mechanism-based evolu-tion dynamics model for unmanned cluster strategy in the con-text of strategy selection diversity according to various unmanned cluster application scenarios.Finally,this paper pro-vides a simulation analysis of the effects of relevant parameters such as the payoff factor and cluster size on cooperative evolu-tion in autonomous cluster collaboration for the two types of models.On this basis,this paper presents advice for effectively addressing diverse choices in unmanned cluster tasks,thereby providing decision support for practical applications of unmanned cluster tasks.展开更多
The ultrafine copper wire with a diameter of 18μm is prepared via cold drawing process from the single crystal downcast billet(Φ8 mm),taking a drawing strain to 12.19.In this paper,in-depth investigation of the micr...The ultrafine copper wire with a diameter of 18μm is prepared via cold drawing process from the single crystal downcast billet(Φ8 mm),taking a drawing strain to 12.19.In this paper,in-depth investigation of the microstructure feature,texture evolution,mechanical properties,and electrical conductivity of ultrafine wires ranging fromΦ361μm toΦ18μm is performed.Specially,the microstructure feature and texture type covering the whole longitudinal section of ultrafine wires are elaborately characterized.The results show that the average lamella thickness decreases from 1.63μm to 102 nm during the drawing process.Whereas,inhomogeneous texture evolution across different wire sections was observed.The main texture types of copper wires are comprised of<111>,<001>and<112>orientations.Specifically,the peripheral region is primarily dominated by<111>and<112>,while the central region is dominated by<001>and<111>.As the drawing strain increases,the volume fraction of hard orientation<111>with low Schmid factor increases,where notably higher fraction of<111>is resulted from the consumption of<112>and<001>for the wire ofΦ18μm.For drawn copper wire of 18μm,superior properties are obtained with a tensile strength of 729.8 MPa and an electrical conductivity of 86.9%IACS.Furthermore,it is found that grain strengthening,dislocation strengthening,and texture strengthening are three primary strengthening mechanisms of drawn copper wire,while the dislocation density is the main factor on the reducing of conductivity.展开更多
In this study,a series of triaxial tests are conducted on sandstone specimens to investigate the evolution of their mechanics and permeability characteristics under the combined action of immersion corrosion and seepa...In this study,a series of triaxial tests are conducted on sandstone specimens to investigate the evolution of their mechanics and permeability characteristics under the combined action of immersion corrosion and seepage of different chemical solutions.It is observed that with the increase of confining pressure,the peak stress,dilatancy stress,dilatancy stress ratio,peak strain,and elastic modulus of the sandstone increase while the Poisson ratio decreases and less secondary cracks are produced when the samples are broken.The pore pressure and confining pressure have opposite influences on the mechanical properties.With the increase of the applied axial stress,three stages are clearly identified in the permeability evolution curves:initial compaction stage,linear elasticity stage and plastic deformation stage.The permeability reaches the maximum value when the highest volumetric dilatancy is obtained.In addition,the hydrochemical action of salt solution with pH=7 and 4 has an obvious deteriorating effect on the mechanical properties and induces the increase of permeability.The obtained results will be useful in engineering to understand the mechanical and seepage properties of sandstone under the coupled chemical-seepage-stress multiple fields.展开更多
Friction stir additive manufacturing(FSAM)is an innovative additive manufacturing(AM)method.The various heat treatment conditions of aluminum-lithium alloys using this method have not been widely discussed.In this stu...Friction stir additive manufacturing(FSAM)is an innovative additive manufacturing(AM)method.The various heat treatment conditions of aluminum-lithium alloys using this method have not been widely discussed.In this study,the microstructure evolution and mechanical properties of FSAM 2195 aluminum-lithium alloy in different heat treatment conditions(T3 and T8)were investigated.The results demonstrated that the heat treatment state of 2195 Al-Li alloys was minimally influenced by FSAM as the FSAM temperature exceeded the solid solution temperature.After conducting a single-pass FSAM experiment,a notable grain refinement was observed in the nugget zone(NZ)region compared to the base material(BM).The average grain size of the 2195-T3 alloy decreased from 6.1 to 2.9µm,while the proportion of high-angle grain boundaries increased from 16.5%to 43.9%.Similarly,the average grain size of the 2195-T8 alloy decreased from 8.9 to 2.8µm,with an increase in high-angle grain boundary from 37.6%to 59.2%.The tensile strength of the 2195-T3 Al-Li alloy reached 466 and 478 MPa in the NZ of single-pass and lap experiments,respectively.In comparison,the tensile strength of the 2195-T8 Al-Li alloy in the NZ could reach 452 and 481 MPa in single-pass and lap experiments,respectively.These results demonstrate the significant improvements in microstructure and mechanical properties were achieved through the FSAM process.展开更多
文摘A composite electrocatalyst,CoMoNiO-S/NF-110(NF is nickel foam),was synthesized through electrodeposition,followed by pyrolysis and then the vulcanization process.CoMoNiO-S/NF-110 exhibited a structure where Ni3S2 and Mo2S3 nanoparticles were integrated at the edges of Co3O4 nanosheets,creating a rich,heterogeneous interface that enhances the synergistic effects of each component.In an alkaline electrolyte,the synthesized CoMoNiO-S/NF-110 exhibited superior electrocatalytic performance for oxygen evolution reaction(OER),achieving current densities of 100 and 200 mA·cm^(-2) with low overpotentials of 199.4 and 224.4 mV,respectively,outperforming RuO2 and several high-performance Mo and Ni-based catalysts.This excellent performance is attributed to the rich interface formed between the components and active sites exposed by the defect structure.
文摘The poor electrical conductivity of metal-organic frameworks(MOFs)limits their electrocatalytic performance in the oxygen evolution reaction(OER).In this study,a Py@Co-MOF composite material based on pyrene(Py)molecules and{[Co2(BINDI)(DMA)_(2)]·DMA}_(n)(Co-MOF,H4BINDI=N,N'-bis(5-isophthalic acid)naphthalenediimide,DMA=N,N-dimethylacetamide)was synthesized via a one-pot method,leveragingπ-πinteractions between pyrene and Co-MOF to modulate electrical conductivity.Results demonstrate that the Py@Co-MOF catalyst exhibited significantly enhanced OER performance compared to pure Co-MOF or pyrene-based electrodes,achieving an overpotential of 246 mV at a current density of 10 mA·cm^(-2) along with excellent stability.Density functional theory(DFT)calculations reveal that the formation of O*in the second step is the rate-determining step(RDS)during the OER process on Co-MOF,with an energy barrier of 0.85 eV due to the weak adsorption affinity of the OH*intermediate for Co sites.CCDC:2419276.
文摘The efficiency and stability of catalysts for photocatalytic hydrogen evolution(PHE)are largely governed by the charge transfer behaviors across the heterojunction interfaces.In this study,CuO,a typical semiconductor featuring a broad spectral absorption range,is successfully employed as the electron acceptor to combine with CdS for constructing a S-scheme heterojunction.The optimized photocatalyst(CdSCuO2∶1)delivers an exceptional hydrogen evolution rate of 18.89 mmol/(g·h),4.15-fold higher compared with bare CdS.X-ray photoelectron spectroscopy(XPS)and ultraviolet-visible diffuse reflection absorption spectroscopy(UV-vis DRS)confirmed the S-scheme band structure of the composites.Moreover,the surface photovoltage(SPV)and electron paramagnetic resonance(EPR)indicated that the photogenerated electrons and photogenerated holes of CdS-CuO2∶1 were respectively transferred to the conduction band(CB)of CdS with a higher reduction potential and the valence band(VB)of CuO with a higher oxidation potential under illumination,as expected for the S-scheme mechanism.Density-functional-theory calculations of the electron density difference(EDD)disclose an interfacial electric field oriented from CdS to CuO.This built-in field suppresses charge recombination and accelerates carrier migration,rationalizing the markedly enhanced PHE activity.This study offers a novel strategy for designing S-scheme heterojunctions with high light harvesting and charge utilization toward sustainable solar-tohydrogen conversion.
文摘Binary composites(ZIF-67/rGO)were synthesized by one-step precipitation method using cobalt nitrate hexahydrate as metal source,2-methylimidazole as organic ligand,and reduced graphene oxide(rGO)as carbon carrier.Then Ru3+was introduced for ion exchange,and the porous Ru-doped Co_(3)O_(4)/rGO(Ru-Co_(3)O_(4)/rGO)composite electrocatalyst was prepared by annealing.The phase structure,morphology,and valence state of the catalyst were analyzed by X-ray powder diffraction(XRD),scanning electron microscope(SEM),transmission electron microscopy(TEM),and X-ray photoelectron spectroscopy(XPS).In 1 mol·L^(-1)KOH,the oxygen evolution reaction(OER)performance of the catalyst was measured by linear sweep voltammetry,cyclic voltammetry,and chronoamperometry.The results show that the combination of Ru doping and rGO provides a fast channel for collaborative electron transfer.At the same time,rGO as a carbon carrier can improve the electrical conductivity of Ru-Co_(3)O_(4)particles,and the uniformly dispersed nanoparticles enable the reactants to diffuse freely on the catalyst.The results showed that the electrochemical performance of Ru-Co_(3)O_(4)/rGO was much better than that of Co_(3)O_(4)/rGO,and the overpotential of Ru-Co_(3)O_(4)/rGO was 363.5 mV at the current density of 50 mA·cm^(-2).
基金financially supported by the project of the National Natural Science Foundation of China(52322203)the Key Research and Development Program of Shaanxi Province(2024GHZDXM-21)。
文摘The design of cost-effective and efficient metal-free carbon-based catalysts for the hydrogen evolution reaction(HER)is of great significance for increasing the production of clean hydrogen by the electrolysis of alkaline water.Precise control of the electronic structure by heteroatom doping has proven to be efficient for increasing catalytic activity.Nevertheless,both the structural characteristics and the underlying mechanism are not well understood,especially for doping with two different atoms,thus limiting the use of these catalysts.We report the production of phosphorus and nitrogen co-doped hollow carbon nanospheres(HCNs)by the copolymerization of pyrrole and aniline at a Triton X-100 micelle-interface,followed by doping with phytic acid and carbonization.The unique pore structure and defect-rich framework of the HCNs expose numerous active sites.Crucially,the combined effect of graphitic nitrogen and phosphorus-carbon bonds modulate the local electronic structure of adjacent C atoms and facilitates electron transfer.As a res-ult,the HCN carbonized at 1100°C exhibited superior HER activity and an outstanding stability(70 h at a current density of 10 mA cm^(−2))in alkaline water,because of the large number of graphitic nitrogen and phosphorus-carbon bonds.
文摘Sulfur-doped iron-cobalt tannate nanorods(S-FeCoTA)derived from metal-organic frameworks(MOFs)as electrocatalysts were synthesized via a one-step hydrothermal method.The optimized S-FeCoTA was interlaced by loose nanorods,which had many voids.The S-FeCoTA catalysts exhibited excellent electrochemical oxygen evolution reaction(OER)performance with a low overpotential of 273 mV at 10 mA·cm^(-2)and a small Tafel slope of 36 mV·dec^(-1)in 1 mol·L^(-1)KOH.The potential remained at 1.48 V(vs RHE)at 10 mA·cm^(-2)under continuous testing for 15 h,implying that S-FeCoTA had good stability.The Faraday efficiency of S-FeCoTA was 94%.The outstanding OER activity of S-FeCoTA is attributed to the synergistic effects among S,Fe,and Co,thus promoting electron transfer,reducing the reaction kinetic barrier,and enhancing the OER performance.
文摘Several tritylodontid taxa have been reported from the Upper Jurassic of the Wucaiwan area in the Junggar Basin of Xinjiang,northwestern China,including Yuanotherium minor.The original study described the partially preserved postcanine teeth in the middle of the left upper maxilla.After detailed re-examination of the specimen and by CT scanning,3D reconstruction,and scanning electron microscopy observations,we provided a more detailed description of the osteology,neurosensory,and tooth wear pattern for all the bones preserved in this specimen and clarified some characters.Based on new information about the cusp wear pattern,the chewing movement pattern of the dentition and detailed cusp morphology,we discussed the cuspal homology of upper cheek teeth of tritylodontids and postulate a standardized method for cusp identification.We hypothesize that the unique maxilla characteristics furnish the evidence for transitional stages about the evolution of the upper jaw-palate structure in tritylodontids.
文摘The performance of a material is directly affected by its microstructural development during the solidification phase. Discrete cellular automaton (CA) models are widelyused in materials science to simulate and predict microstructural growth. This review comprehensively explains the developments and applications of CA in solidification structure simulation, including the theoretical underpinnings, computational procedures, software development, and recent advances. Summarizes the potential and limitations of cellular automata in understanding microstructure evolution during solidification, explores the evolution of microstructures during solidification, and adds to our existing knowledge of cellular automaton theory. Finally, the research trend in simulating the evolution of the solidification microstructure using cellular automaton theory is explored.
基金Scientific Research and Innovation Team Program of Sichuan University of Science and Engineering(SUSE652B004,2024RC13)Special Basic Cooperative Research Programs of Yunnan Provincial Undergraduate Universities Association(202101BA070001-085)。
文摘Transition metal dichalcogenides(TMDs)recently attracted widespread attention due to their potential application to the electrocatalysis of the hydrogen evolution reaction(HER).However,their HER performance is far inferior to that of platinum(Pt)metal.Preparation of multi-elemental alloy and construction of heterostructure are considered as highly effective methods to enhance hydrogen production activity.Herein,a novel quaternary CoMoSSe alloy with heterostructure was synthesized on the surface of carbon black(CB)particles(CoMoSSe@CB)by a simple Sol-Gel process and thereafter served as HER catalyst.Compared to CoSe@CB and MoS2@CB electrocatalysts,CoMoSSe@CB exhibits superior HER activity with a low overpotential of 190 mV at-10 mA·cm^(-2) and a Tafel slope of 62 mV·dec^(-1).This improvement is attributed to the alloying effects among Co,Mo,S and Se,as well as the heterogeneous structure in the composite material,which regulate the electronic structure and intermediate free energy,thereby increasing the number of active sites and enhancing charge-transfer ability.This work can provide new ideas and concepts for designing novel and efficient TMD electrocatalysts.
基金Supported by the National Natural Science Foundation of China(12201368,62376252)Key Project of Natural Science Foundation of Zhejiang Province(LZ22F030003)Zhejiang Province Leading Geese Plan(2024C02G1123882,2024C01SA100795).
文摘With the urgent need to resolve complex behaviors in nonlinear evolution equations,this study makes a contribution by establishing the local existence of solutions for Cauchy problems associated with equations of mixed types.Our primary contribution is the establishment of solution existence,illuminating the dynamics of these complex equations.To tackle this challenging problem,we construct an approximate solution sequence and apply the contraction mapping principle to rigorously prove local solution existence.Our results significantly advance the understanding of nonlinear evolution equations of mixed types.Furthermore,they provide a versatile,powerful approach for tackling analogous challenges across physics,engineering,and applied mathematics,making this work a valuable reference for researchers in these fields.
基金Supported by Scientific Research Fund of Hunan Provincial Education Departmen(t23A0361)。
文摘An evolution inequality of Sobolev type involving a nonlinear convolution term is considered.By using the nonlinear capacity method and the contradiction argument,the non-existence of the nontrivial local weak solution is proved.
文摘Through employing zeolitic imidazolate framework-67(ZIF-67)templates,the straightforward hydrother-mal and electrodeposition methods were applied to synthesize FeOOH@CoMoO_(4)heterostructure attached to the sur-face of nickel foam(NF).The specific structure of the as-prepared FeOOH@CoMoO_(4)/NF-400s provided pronounced porosity and extensive surface area,enhancing rapid electron transport and exposing abundant active sites to improve catalytic reactions.Furthermore,the introduction of FeOOH,which induces electron transfer from FeOOH to CoMoO_(4),confirms their strong electronic interaction,thereby leading to an accelerated surface catalytic reaction.Consequently,the constructed FeOOH@CoMoO_(4)/NF-400s heterostructure demonstrated exceptional oxygen evolu-tion reaction(OER)activity,requiring an overpotential of 199 mV to deliver the current density of 10 mA·cm^(-2),cou-pled with the superior Tafel slope value of 49.56 mV·dec^(-1)and outstanding stability over 20 h under the current densities of both 10 and 100 mA·cm^(-2).
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.
基金supported by the National Natural Science Foundation of China(22179138).
文摘The utilization of nickel-based catalysts as alternatives to expensive platinum-based(Pt-based)materials for the hydrogen evolution reaction in acidic electrolytes has attracted considerable attention due to their potential for enabling cost-effective industrial applications.However,the unsatisfied cyclic stability and electrochemical activity limit their further application.In this work,nickel-molybdenum(Ni-Mo)alloy catalysts were successfully synthesized through a comprehensive process including electrodeposition,thermal annealing,and electrochemical activation.Owing to the synergistic interaction of molybdenum trinickelide(Ni_(3)Mo)and molybdenum dioxide(MoO_(2))in Ni-Mo alloy,the catalyst display superior overall electrochemical properties.A low overpotential of 86 mV at 10 mA/cm^(2)and a Tafel slope of 74.0 mV/dec in 0.5 mol/L H_(2)SO_(4)solution can be achieved.Notably,remarkable stability with negligible performance degradation even after 100 h could be maintained.This work presents a novel and effective strategy for the design and fabrication of high-performance,non-precious metal electrocatalysts for acidic water electrolysis.
基金National Natural Science Foundation of China(21806023)Natural Science Foundation of Hunan Province(2021JJ40199)+2 种基金Education Department Foundation of Hunan Province(20C0813)Hunan University of Science and Technology Fundamental Research FundsPostgraduate Scientific Research Innovation Project of Hunan Province(CX20240877)。
文摘Elemental doping is an effective strategy for tuning the band structure of graphite carbon nitride(CN)to enhance its photocatalytic performance.In this study,sodium(Na)and oxygen(O)co-doped carbon nitride(Na/O-CN_(x),x=1.0,2.0,3.0,4.0)was synthesized via solid-phase reaction of sodium citrate(NaCA)and pure CN powder in the Teflon-sealed autoclave under air conditions at 180℃.Surface area of Na/O-CN_(3.0) is measured to be 18.8 m^(2)/g,increasing by 60.7%compared to that of pure CN(11.7 m^(2)/g).Bandgap energy of Na/O-CN_(3.0) is determined to be 2.68 eV,marginally lower than that of pure CN(2.70 eV),thereby enhancing its capacity for sunlight absorption.Meanwhile,the incorporation of Na and O atoms into Na/O-CN_(x) is found to effectively reduce recombination rates of photogenerated electron-hole pairs.As a result,Na/O-CN_(x) samples exhibit markedly enhanced photocatalytic hydrogen evolution activity under visible light irradiation.Notably,the optimal Na/O-CN_(3.0) sample achieves a photocatalytic hydrogen production rate of 103.2μmol·g^(–1)·h^(–1),which is 8.2 times greater than that of pure CN(11.2μmol·g^(–1)·h^(–1)).Furthermore,a series of Na/O-CN_(x)-yO_(2)(y=0,20%,40%,60%,80%,100%)samples were prepared by modulating the oxygen content within reaction atmosphere.The catalytic performance evaluations reveal that the incorporation of both Na and O atoms in Na/O-CN_(3.0) enhances photocatalytic activity.This study also introduces novel methodologies for synthesis of metal atom-doped CN materials at lower temperature,highlighting the synergistic effect of Na and O atoms in photocatalytic hydrogen production of Na/O-CN_(x) samples.
基金supported by the National Natural Science Foundation of China(22209040,22202063).
文摘The development of highly active catalyst in pH-neutral media for oxygen evolution reaction(OER)is critical in the field of renewable energy storage and conversion.Nevertheless,the slow kinetics of proton-coupled electron transfer(PCET)hinders the overall OER efficiency.Herein,we report an ionic liquid(IL)modified CoSn(OH)_(6)nanocubes(denoted as CoS-n(OH)_(6)-IL),which could be prepared through a facile strategy.The modified IL would not change the structural character-istics of CoSn(OH)_(6),but could effectively regulate the local proton activity near the active sites.The CoSn(OH)_(6)-IL exhibited higher intrinsic OER performances than the pristine CoSn(OH)_(6)in neutral media.For example,the current density of CoS-n(OH)_(6)-IL at 1.8 V versus reversible hydrogen electrode(RHE)was about 4 times higher than that of CoSn(OH)_(6).According to the pH-dependent kinetic investigations,operando electrochemical impedance spectroscopic,chemical probe tests,and deuterium kinetic isotope effects,the interfacial layer of IL could be utilized as a proton transfer mediator to promote the proton transfer,which enhances the surface coverage of OER intermediates and reduces the activation barrier.Consequent-ly,the sluggish OER kinetics would be efficiently accelerated.This study provides a facile and effective strategy to facilitate the PCET processes and is beneficial to guide the rational design of OER electrocatalysts.
基金supported by the National Natural Science Foundation of China(72471240).
文摘When performing tasks,unmanned clusters often face a variety of strategy choices.One of the key issues in unmanned cluster tasks is the method through which to design autonomous collaboration and cooperative evolution mechanisms that allow for unmanned clusters to maximize their overall task effective-ness under the condition of strategic diversity.This paper ana-lyzes these task requirements from three perspectives:the diver-sity of the decision space,information network construction,and the autonomous collaboration mechanism.Then,this paper pro-poses a method for solving the problem of strategy selection diversity under two network structures.Next,this paper presents a Moran-rule-based evolution dynamics model for unmanned cluster strategies and a vision-driven-mechanism-based evolu-tion dynamics model for unmanned cluster strategy in the con-text of strategy selection diversity according to various unmanned cluster application scenarios.Finally,this paper pro-vides a simulation analysis of the effects of relevant parameters such as the payoff factor and cluster size on cooperative evolu-tion in autonomous cluster collaboration for the two types of models.On this basis,this paper presents advice for effectively addressing diverse choices in unmanned cluster tasks,thereby providing decision support for practical applications of unmanned cluster tasks.
基金Project supported by“Unveiled the List of Commanders”Key Core Common Technology Projects of Ji’an,ChinaProject(LJKMZ20220591)supported by the Basic Scientific Research Project of the Education Department of Liaoning Province,ChinaProject(CSTB2023NSCQ-LZX0116)supported by the Natural Science Foundation Joint Fund for Innovation and Development Projects of Chongqing,China。
文摘The ultrafine copper wire with a diameter of 18μm is prepared via cold drawing process from the single crystal downcast billet(Φ8 mm),taking a drawing strain to 12.19.In this paper,in-depth investigation of the microstructure feature,texture evolution,mechanical properties,and electrical conductivity of ultrafine wires ranging fromΦ361μm toΦ18μm is performed.Specially,the microstructure feature and texture type covering the whole longitudinal section of ultrafine wires are elaborately characterized.The results show that the average lamella thickness decreases from 1.63μm to 102 nm during the drawing process.Whereas,inhomogeneous texture evolution across different wire sections was observed.The main texture types of copper wires are comprised of<111>,<001>and<112>orientations.Specifically,the peripheral region is primarily dominated by<111>and<112>,while the central region is dominated by<001>and<111>.As the drawing strain increases,the volume fraction of hard orientation<111>with low Schmid factor increases,where notably higher fraction of<111>is resulted from the consumption of<112>and<001>for the wire ofΦ18μm.For drawn copper wire of 18μm,superior properties are obtained with a tensile strength of 729.8 MPa and an electrical conductivity of 86.9%IACS.Furthermore,it is found that grain strengthening,dislocation strengthening,and texture strengthening are three primary strengthening mechanisms of drawn copper wire,while the dislocation density is the main factor on the reducing of conductivity.
基金Projects(12072102,12102129)supported by the National Natural Science Foundation of ChinaProject(DM2022B01)supported by the Key Laboratory of Safe Mining of Deep Metal Mines,Ministry of Education,ChinaProject(JZ-008)supported by the Six Talent Peaks Project in Jiangsu Province,China。
文摘In this study,a series of triaxial tests are conducted on sandstone specimens to investigate the evolution of their mechanics and permeability characteristics under the combined action of immersion corrosion and seepage of different chemical solutions.It is observed that with the increase of confining pressure,the peak stress,dilatancy stress,dilatancy stress ratio,peak strain,and elastic modulus of the sandstone increase while the Poisson ratio decreases and less secondary cracks are produced when the samples are broken.The pore pressure and confining pressure have opposite influences on the mechanical properties.With the increase of the applied axial stress,three stages are clearly identified in the permeability evolution curves:initial compaction stage,linear elasticity stage and plastic deformation stage.The permeability reaches the maximum value when the highest volumetric dilatancy is obtained.In addition,the hydrochemical action of salt solution with pH=7 and 4 has an obvious deteriorating effect on the mechanical properties and induces the increase of permeability.The obtained results will be useful in engineering to understand the mechanical and seepage properties of sandstone under the coupled chemical-seepage-stress multiple fields.
基金Project(U22A20190)supported by International Science and Technology Cooperation under the National Natural Science Foundation of ChinaProjects(U2241248,52205379)supported by the National Natural Science Foundation of ChinaProject(BE2023026)supported by Jiangsu Provincial Key Research and Development Program and Nanjing Science and Technology Innovation Project for Overseas Scholars,China。
文摘Friction stir additive manufacturing(FSAM)is an innovative additive manufacturing(AM)method.The various heat treatment conditions of aluminum-lithium alloys using this method have not been widely discussed.In this study,the microstructure evolution and mechanical properties of FSAM 2195 aluminum-lithium alloy in different heat treatment conditions(T3 and T8)were investigated.The results demonstrated that the heat treatment state of 2195 Al-Li alloys was minimally influenced by FSAM as the FSAM temperature exceeded the solid solution temperature.After conducting a single-pass FSAM experiment,a notable grain refinement was observed in the nugget zone(NZ)region compared to the base material(BM).The average grain size of the 2195-T3 alloy decreased from 6.1 to 2.9µm,while the proportion of high-angle grain boundaries increased from 16.5%to 43.9%.Similarly,the average grain size of the 2195-T8 alloy decreased from 8.9 to 2.8µm,with an increase in high-angle grain boundary from 37.6%to 59.2%.The tensile strength of the 2195-T3 Al-Li alloy reached 466 and 478 MPa in the NZ of single-pass and lap experiments,respectively.In comparison,the tensile strength of the 2195-T8 Al-Li alloy in the NZ could reach 452 and 481 MPa in single-pass and lap experiments,respectively.These results demonstrate the significant improvements in microstructure and mechanical properties were achieved through the FSAM process.
