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
Iron(Fe)nanoparticles and graphite(Gr)with different masses of bismuth trisulfide(Bi_(2)S_(3))were mixed by high-energy ball milling treatment to fabricate the corresponding composite iron anodes Bi_(2)S_(3)@Fe-Gr.The...Iron(Fe)nanoparticles and graphite(Gr)with different masses of bismuth trisulfide(Bi_(2)S_(3))were mixed by high-energy ball milling treatment to fabricate the corresponding composite iron anodes Bi_(2)S_(3)@Fe-Gr.The hydrogen evolution reaction and iron passivation process on these iron electrodes were investigated in alkaline and neutral solutions.The iron electrode Bi_(2)S_(3)-3@Fe-Gr(The additional amount of Bi_(2)S_(3)was 3 mg)revealed the strongest ability to inhibit hydrogen evolution among the iron electrodes of the present investigation,while the Bi_(2)S_(3)-6@Fe-Gr electrode(The additional amount of Bi_(2)S_(3)was 6 mg)delivered significant performance in inhibiting anodic passivation.This is because the high-energy ball milling process leads to the well-dispersion of Bi_(2)S_(3)and the changes in the surface of Fe nanoparticles,thereby slowing down the passivation of the iron electrode surface.展开更多
Traditional polymeric photocatalysts are typically constructed using aromatic building blocks to enhanceπ-conjugation.However,their inherent hydrophobicity and rigid structure lead to poor dispersibility in aqueous s...Traditional polymeric photocatalysts are typically constructed using aromatic building blocks to enhanceπ-conjugation.However,their inherent hydrophobicity and rigid structure lead to poor dispersibility in aqueous solutions,resulting in significant optical losses and exciton recombination.In this study,two series of six novel polymer photocatalysts(FLUSO,FLUSO-PEG10,FLUSO-PEG30;CPDTSO,CPDTSO-PEG10,CPDTSO-PEG30)are designed and synthesized by incorporating the hydrophilic,non-conjugated polyethylene glycol(PEG)chain,into both the main and side chains of polymers.By precisely optimizing the ratio of hydrophilic PEG segments,the water dispersibility is significantly improved while the light absorption capability of the polymer photocatalysts is well maintained.The experimental results confirm that the optimized FLUSO-PEG10 exhibits excellent photocatalytic hydrogen evolution rate,reaching up to 33.9 mmol/(g·h),which is nearly three times higher than that of fullyπ-conjugated counterparts.Water contact angles and particle size analyses reveal that incorporating non-conjugated segments into the main chains enhances the capacitance of the polymer/water interface and reduces particle aggregation,leading to improved photocatalyst dispersion and enhanced charge generation.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
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
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
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
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
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 hydrazine oxidation reaction(HzOR)has garnered significant attention as a feasible approach to replace sluggish anodic reactions to save energy.Nevertheless,there are still difficulties in developing highly effici...The hydrazine oxidation reaction(HzOR)has garnered significant attention as a feasible approach to replace sluggish anodic reactions to save energy.Nevertheless,there are still difficulties in developing highly efficient catalysts for the HzOR.Herein,we report amorphous ruthenium nanosheets(a-Ru NSs)with a thickness of approximately 9.6 nm.As a superior bifunctional electrocatalyst,a-Ru NSs exhibited enhanced electrocatalytic performance toward both the HzOR and hydrogen evolution reaction(HER),outperforming benchmark Pt/C catalysts,where the a-Ru NSs achieved a work-ing potential of merely-76 mV and a low overpotential of only 17 mV to attain a current density of 10 mA·cm^(-2) for the HzOR and HER,respectively.Furthermore,a-Ru NSs displayed a low cell voltage of 28 mV at 10 mA·cm^(-2) for overall hy-drazine splitting in a two-electrode electrolyzer.In situ Raman spectra revealed that the a-Ru NSs can efficiently promote N‒N bond cleavage,thereby producing more*NH_(2)and accelerating the progress of the reaction.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
This study investigates the instability characteristics of dynamic disasters resulting from disruption caused by extracting resources underground. Utilizing the split Hopkinson pressure bar (SHPB) system, the dynamic ...This study investigates the instability characteristics of dynamic disasters resulting from disruption caused by extracting resources underground. Utilizing the split Hopkinson pressure bar (SHPB) system, the dynamic response mechanism of coal energy evolution is examined, and the energy instability criterion is established. The validity of the instability criterion is explored from the standpoint of damage progression. The results demonstrate that the energy conversion mechanism undergoes a fundamental alternation under impact disturbance. Moreover, the energy release rate as well as the energy dissipation rate undergo comparable changes across distinct levels of impact disturbance. The distinction between the energy release rate and the energy dissipation rate (DRD) increases as coal mass deformation grows. Prior to coal facing instability and failure, the DRD experienced an inflection point followed by a sharp decrease. In conjunction with the discussion on the damage evolution, the physical and mechanical significance of DRD remains clear, which can essentially describe the whole impact loading process. The phenomenon that the inflection point appears and DRD subsequently suddenly decreases can be employed as the energy criterion prior to the failure of instability. Furthermore, this paper provides significant reference for the prediction of dynamic instability of coal under dynamic disturbance.展开更多
Developing efficient,durable,and precious metal-free electrocatalysts is currently a huge challenge.In this article,through a simple one-step high-temperature pyrolysis method,by incorporating various non-metallic ele...Developing efficient,durable,and precious metal-free electrocatalysts is currently a huge challenge.In this article,through a simple one-step high-temperature pyrolysis method,by incorporating various non-metallic element atoms,we prepared four different NiX(X=Cl_(2),(CH_(3)COO)_(2),(NO_(3))2,SO_(4))@CNT catalysts.Additionally,by adjusting the temperature,these four materials were expanded into twelve catalyst materials for comparative optimization of hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)activity.Ultimately,Ni(NO_(3))2@CNT-900 typically exhibits superior OER and HER activity.In 1 mol/L KOH solution with a current density of 10 mA/cm^(2),the overpotentials of HER and OER of Ni(NO_(3))2@CNT-900 are only 145 mV and 300 mV,respectively.Furthermore,the Ni(NO_(3))2@CNT-900 shows excellent durability in both HER and OER.展开更多
To weaken the basal texture and in-plane anisotropy of magnesium alloy, non-basal slips are pre-enhanced by pre-rolling with a single pass larger strain reduction at elevated temperatures. Then Mg alloy sheets with th...To weaken the basal texture and in-plane anisotropy of magnesium alloy, non-basal slips are pre-enhanced by pre-rolling with a single pass larger strain reduction at elevated temperatures. Then Mg alloy sheets with the thickness of 1 mm are achieved after five passes rolling at 300 ℃. A double peak and disperse basal texture is generated after pre- rolling at higher temperatures when the non-basal slips are more active. So, the texture intensity of pre-rolled samples is reduced. Moreover, the distribution condition of in-grain misorientation axes (a method to analyze the activation of slips) shows that the pyramidal slip is quite active during deformation. After annealing on final rolled sheets, the texture distributions are changed and the intensity of texture reduces obviously due to static recrystallization. In particular, the r-value and in-plane anisotropy of pre-rolled samples are obviously lower than those of sample without pre-rolling.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
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.
文摘Iron(Fe)nanoparticles and graphite(Gr)with different masses of bismuth trisulfide(Bi_(2)S_(3))were mixed by high-energy ball milling treatment to fabricate the corresponding composite iron anodes Bi_(2)S_(3)@Fe-Gr.The hydrogen evolution reaction and iron passivation process on these iron electrodes were investigated in alkaline and neutral solutions.The iron electrode Bi_(2)S_(3)-3@Fe-Gr(The additional amount of Bi_(2)S_(3)was 3 mg)revealed the strongest ability to inhibit hydrogen evolution among the iron electrodes of the present investigation,while the Bi_(2)S_(3)-6@Fe-Gr electrode(The additional amount of Bi_(2)S_(3)was 6 mg)delivered significant performance in inhibiting anodic passivation.This is because the high-energy ball milling process leads to the well-dispersion of Bi_(2)S_(3)and the changes in the surface of Fe nanoparticles,thereby slowing down the passivation of the iron electrode surface.
文摘Traditional polymeric photocatalysts are typically constructed using aromatic building blocks to enhanceπ-conjugation.However,their inherent hydrophobicity and rigid structure lead to poor dispersibility in aqueous solutions,resulting in significant optical losses and exciton recombination.In this study,two series of six novel polymer photocatalysts(FLUSO,FLUSO-PEG10,FLUSO-PEG30;CPDTSO,CPDTSO-PEG10,CPDTSO-PEG30)are designed and synthesized by incorporating the hydrophilic,non-conjugated polyethylene glycol(PEG)chain,into both the main and side chains of polymers.By precisely optimizing the ratio of hydrophilic PEG segments,the water dispersibility is significantly improved while the light absorption capability of the polymer photocatalysts is well maintained.The experimental results confirm that the optimized FLUSO-PEG10 exhibits excellent photocatalytic hydrogen evolution rate,reaching up to 33.9 mmol/(g·h),which is nearly three times higher than that of fullyπ-conjugated counterparts.Water contact angles and particle size analyses reveal that incorporating non-conjugated segments into the main chains enhances the capacitance of the polymer/water interface and reduces particle aggregation,leading to improved photocatalyst dispersion and enhanced charge generation.
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 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 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.
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.
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 Key R&D Program of China(2018YFA0702001)National Natural Science Foundation of China(22371268,22301287)+3 种基金Fundamental Research Funds for the Central Universities(WK2060000016)Anhui Provincial Natural Science Foundation(2208085J09,2208085QB33)Collaborative Innovation Program of Hefei Science Center,CAS(2022HSC-CIP020)Youth Innovation Promotion Association of the Chinese Academy of Science(2018494)and USTC Tang Scholar.
文摘The hydrazine oxidation reaction(HzOR)has garnered significant attention as a feasible approach to replace sluggish anodic reactions to save energy.Nevertheless,there are still difficulties in developing highly efficient catalysts for the HzOR.Herein,we report amorphous ruthenium nanosheets(a-Ru NSs)with a thickness of approximately 9.6 nm.As a superior bifunctional electrocatalyst,a-Ru NSs exhibited enhanced electrocatalytic performance toward both the HzOR and hydrogen evolution reaction(HER),outperforming benchmark Pt/C catalysts,where the a-Ru NSs achieved a work-ing potential of merely-76 mV and a low overpotential of only 17 mV to attain a current density of 10 mA·cm^(-2) for the HzOR and HER,respectively.Furthermore,a-Ru NSs displayed a low cell voltage of 28 mV at 10 mA·cm^(-2) for overall hy-drazine splitting in a two-electrode electrolyzer.In situ Raman spectra revealed that the a-Ru NSs can efficiently promote N‒N bond cleavage,thereby producing more*NH_(2)and accelerating the progress of the reaction.
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Projects(51934007,12072363,52004268) supported by the National Natural Science Foundation of ChinaProject(22KJD440002) supported by the Natural Science Fund for Colleges and Universities in Jiangsu Province,China。
文摘This study investigates the instability characteristics of dynamic disasters resulting from disruption caused by extracting resources underground. Utilizing the split Hopkinson pressure bar (SHPB) system, the dynamic response mechanism of coal energy evolution is examined, and the energy instability criterion is established. The validity of the instability criterion is explored from the standpoint of damage progression. The results demonstrate that the energy conversion mechanism undergoes a fundamental alternation under impact disturbance. Moreover, the energy release rate as well as the energy dissipation rate undergo comparable changes across distinct levels of impact disturbance. The distinction between the energy release rate and the energy dissipation rate (DRD) increases as coal mass deformation grows. Prior to coal facing instability and failure, the DRD experienced an inflection point followed by a sharp decrease. In conjunction with the discussion on the damage evolution, the physical and mechanical significance of DRD remains clear, which can essentially describe the whole impact loading process. The phenomenon that the inflection point appears and DRD subsequently suddenly decreases can be employed as the energy criterion prior to the failure of instability. Furthermore, this paper provides significant reference for the prediction of dynamic instability of coal under dynamic disturbance.
基金Project(145209113)supported by the Basic Research Expenses of Department of Education of Heilongjiang Province,China。
文摘Developing efficient,durable,and precious metal-free electrocatalysts is currently a huge challenge.In this article,through a simple one-step high-temperature pyrolysis method,by incorporating various non-metallic element atoms,we prepared four different NiX(X=Cl_(2),(CH_(3)COO)_(2),(NO_(3))2,SO_(4))@CNT catalysts.Additionally,by adjusting the temperature,these four materials were expanded into twelve catalyst materials for comparative optimization of hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)activity.Ultimately,Ni(NO_(3))2@CNT-900 typically exhibits superior OER and HER activity.In 1 mol/L KOH solution with a current density of 10 mA/cm^(2),the overpotentials of HER and OER of Ni(NO_(3))2@CNT-900 are only 145 mV and 300 mV,respectively.Furthermore,the Ni(NO_(3))2@CNT-900 shows excellent durability in both HER and OER.
基金Project(52374395) supported by the National Natural Science Foundations of ChinaProjects(20210302123135,20210302123163) supported by the Natural Science Foundation of Shanxi Province,China+2 种基金Projects(YDZJSX20231B003,YDZJSX2021A010) supported by the Central Government Guided Local Science and Technology Development Projects,ChinaProject(2022M710541) supported by the China Postdoctoral Science FoundationProjects(202104021301022,202204021301009) supported by the Scientific and Technological Achievements Transformation Guidance Special Project of Shanxi Province,China。
文摘To weaken the basal texture and in-plane anisotropy of magnesium alloy, non-basal slips are pre-enhanced by pre-rolling with a single pass larger strain reduction at elevated temperatures. Then Mg alloy sheets with the thickness of 1 mm are achieved after five passes rolling at 300 ℃. A double peak and disperse basal texture is generated after pre- rolling at higher temperatures when the non-basal slips are more active. So, the texture intensity of pre-rolled samples is reduced. Moreover, the distribution condition of in-grain misorientation axes (a method to analyze the activation of slips) shows that the pyramidal slip is quite active during deformation. After annealing on final rolled sheets, the texture distributions are changed and the intensity of texture reduces obviously due to static recrystallization. In particular, the r-value and in-plane anisotropy of pre-rolled samples are obviously lower than those of sample without pre-rolling.
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.
