Designing the specific crystal phase with better intrinsic activity and more active sites is a very promising strategy for earth-abundant electrocatalysts for oxygen evolution reaction(OER).Herein,a facile two-step me...Designing the specific crystal phase with better intrinsic activity and more active sites is a very promising strategy for earth-abundant electrocatalysts for oxygen evolution reaction(OER).Herein,a facile two-step method including the high-pressure microwave and the hydrothermal sulfurization is adopted to prepare the WS_(x)/Ni_(9)S_(8) hetero-catalyst on nickel foam(WS_(x)/Ni_(9)S_(8)/NF).Firstly,WO3 polyhedrons homogeneously cover the surface of NF through the high-pressure microwave hydrothermal process.Secondly,WS_(x)/Ni_(9)S_(8) nanoparticles on the surface of NF can be synthesized after a hydrothermal sulfurization,which has been confirmed by scanning electron microscopy(SEM) elemental mapping and high-resolution transmission electron microscopy(HRTEM).The amorphous WSx and Ni9 S8 phase may provide the dual active sites for OER.The electrochemical measurements show that WS_(x)/Ni_(9)S_(8)/NF has superior OER activity with a low overpotential of 320 mV at the current density of 100 mA·cm^(-2),better than those of other samples.The enhanced OER performance may be due to the synergistic catalysis from Ni9 S8 phase and high valence of W.Owing to the stable structure of Ni9 S8,the long-term stability of WS_(x)/Ni_(9)S_(8)/NF for at least 10 h can be obtained.This work may provide a new approach for the doped nickel sulfides crystal phase through high-pressure microwave hydrothermal assistance for OER.展开更多
High pressure die casting(HPDC)AlSi10Mn Mg alloy castings are widely used in the automobile industry.Mg can optimize the mechanical properties of castings through heat treatment,while the release of thermal stress aro...High pressure die casting(HPDC)AlSi10Mn Mg alloy castings are widely used in the automobile industry.Mg can optimize the mechanical properties of castings through heat treatment,while the release of thermal stress arouses the deformation of large integrated die-castings.Herein,the development of non-heat treatment Al alloys is becoming the hot topic.In addition,HPDC contains externally solidified crystals(ESCs),which are detrimental to the mechanical properties of castings.To achieve high strength and toughness of non-heat treatment die-casting Al-Si alloy,we used AlSi9Mn alloy as matrix with the introduction of Zr,Ti,Nb,and Ce.Their influences on ESCs and mechanical properties were systematically investigated through three-dimensional reconstruction and thermodynamic simulation.Our results reveal that the addition of Ti increased ESCs'size and porosity,while the introduction of Nb refined ESCs and decreased porosity.Meanwhile,large-sized Al_3(Zr,Ti)phases formed and degraded the mechanical properties.Subsequent introduction of Ce resulted in the poisoning effect and reduced mechanical properties.展开更多
Burial dissolution is a critical diagenetic process influencing ultra-deep carbonate reservoir development and preservation.Artificial carbonate samples with different internal structures were prepared,and high-temper...Burial dissolution is a critical diagenetic process influencing ultra-deep carbonate reservoir development and preservation.Artificial carbonate samples with different internal structures were prepared,and high-temperature and highpressure dissolution kinetic simulations were conducted.The results demonstrate that the intensity of burial dissolution is controlled by temperature and pressure,while tectonic-fluid activity influences the development pattern of burial dissolution,ultimately determining the direction of its differential modification.Extensive burial dissolution is likely to occur primarily at relatively shallow depths,significantly influencing reservoir formation,preservation,modification,and adjustment.The development of faults facilitates the maintenance of the intensity of burial dissolution.The maximum intensity of burial dissolution occurs at the tips and overlap zones of faults and intersections of multiple faults.The larger the scale of the faults,the more conducive it is to the development of burial dissolution.Burial dissolution fosters the formation of fault networks characterized by enhanced reservoir capacity and permeability.Burial dissolution controlled by episodic tectonic-fluid activity is a plausible explanation for forming the Tarim Basin's ultra-deep fault-controlled“stringbead-like”reservoirs.展开更多
Degradable metals,represented by magnesium and magnesium alloys,have attracted significant attention as fracture internal fixation and bone defect repairing materials due to their good biocompatibility,suitable elasti...Degradable metals,represented by magnesium and magnesium alloys,have attracted significant attention as fracture internal fixation and bone defect repairing materials due to their good biocompatibility,suitable elastic modulus and degradable properties.The Mg-3Zn-1Ca-0.5Sr(wt%)alloy is considered a competitor in the biomaterial field thanks to its unique composition of essential nutrients and excellent mechanical properties.However,the presence of coarse second-phase particles in the alloy accelerates its degradation rate and causes excessive gas formation during implantation,which restricts the alloy's potential for clinical device applications.In order to further optimize the properties of the alloy,extrusion combined with high-pressure torsion(HPT)was adopted for deformation processing.The results show that by optimizing the material processing means,the grain can be refined and broken,and the second-phase distribution can be improved,thus improving the microstructure,mechanical properties,and corrosion resistance of the alloy.After 15 cycles of HPT processing,the grains of the alloy are significantly refined to the nanometer scale,reaching approximately 98 nm.Additionally,the second-phase distribution is greatly improved,transforming the original streamlined structure into a more dispersed distribution.This change in microstructure leads to a significant strengthening effect on the alloy,with a noticeable increase in hardness from 60.3 HV in the as-extruded state to 98.5 HV.展开更多
A rotary sealing device that automatically compensates for wear is designed to address the issues of easy wear and the short service life of the rotary sealing device with automatic wear compensation in mining machine...A rotary sealing device that automatically compensates for wear is designed to address the issues of easy wear and the short service life of the rotary sealing device with automatic wear compensation in mining machinery.After the end face of the guide sleeve wears out,it still tightly adheres to the sealing valve seat under the pressure difference,achieving automatic wear compensation.Based on fluid-solid coupling technology,the structural strength of the rotary sealing device was checked.The influence of factors on the sealing performance of rotary sealing devices was studied using the control variable method.The results show that as the pressure of water increases,the leakage rate of the sealing device decreases,and after 30 MPa,the leakage rate is almost 0 mL/h.The temperature of the rotating sealing device increases with the increase of rotation speed or pressure,and the temperature is more affected by the rotation speed factor.The frictional torque increases with increasing pressure and is independent of rotational speed.Comprehensive analysis shows that the wear resistance and reliability level of the sealing guide sleeve material is PVDF>PEEK>PE>PA.This study designs a high-pressure automatic compensation wear rotary sealing device and selects the optimal sealing material,providing technical support for the application of high-pressure water jet in mining machinery.展开更多
With the global oil and gas industry increasingly targeting ultra-deep well development,the demand for wear resistance in polycrystalline diamond compact(PDC)bits is increasing.However,further improvement of the mecha...With the global oil and gas industry increasingly targeting ultra-deep well development,the demand for wear resistance in polycrystalline diamond compact(PDC)bits is increasing.However,further improvement of the mechanical properties of PDC incurs prohibitively elevated costs and stringent technological challenges.Here,we present a two-stage high-pressure infiltration(HPI)methodology involving cobalt removal pretreatment followed by lubricant infiltration.The successful infiltration of lubricants into diamond micropores has been systematically verified,and the effects of lubricant phase composition,infiltration pressure,and temperature on infiltration depth have been thoroughly investigated.Fractal dimension analysis characterizes the pore structure of cobalt-removed diamonds,revealing a strong correlation between the fractal dimension and friction coefficient reduction.Tribological testing confirms the formation of lubricating films at friction interfaces,achieving a 71.5%reduction in the coefficient of friction for lubricant-containing diamond materials.This straightforward strategy opens a gate to developing the next generation of self-lubricating diamond materials.展开更多
Perovskite oxynitrides AB(N,O)_(3), a crucial class in materials science, have attracted much attention. By precisely controlling A-and B-site ions and tuning the N/O ratio, new materials with exotic charge states and...Perovskite oxynitrides AB(N,O)_(3), a crucial class in materials science, have attracted much attention. By precisely controlling A-and B-site ions and tuning the N/O ratio, new materials with exotic charge states and intriguing electronic behaviors can be designed and synthesized. In this work, a novel oxynitride perovskite, CeNbO_(2)N, was prepared under high-temperature and high-pressure conditions. The compound crystallizes in an orthorhombic perovskite structure in Pnma symmetry with disordered N/O distribution. The x-ray absorption spectroscopy confirms the presence of a Nb^(4+) state with 4d^(1) electronic configuration in CeNbO_(2)N. As a result, the resistivity of CeNbO_(2)N is sharply reduced compared to its counterpart CeTa^(5+)ON_(2) and other Nb^(5+) compounds. No long-range spin order is found to occur with the temperature down to 2 K in CeNbO_(2)N, while a remarkable negative magnetoresistance effect shows up at lower temperatures, probably due to the magnetic scattering arising from short-range spin correlations.展开更多
Iron nitride(Fe_(x)N_y) is a promising candidate for the next generation of ferromagnetic materials. However, synthesizing high-quality bulk iron nitride with tuned structure and magnetic properties remains a challeng...Iron nitride(Fe_(x)N_y) is a promising candidate for the next generation of ferromagnetic materials. However, synthesizing high-quality bulk iron nitride with tuned structure and magnetic properties remains a challenge. Currently, experimental and theoretical results regarding the magnetic property of iron nitrides remain controversial. With the recent advancements in high-pressure technology, new synthetic pathways to iron nitrides have been proposed. High-pressure synthesis technology provides multidimensional possibilities for tuning the structure and magnetic properties of iron nitrides. This review summarizes recent progress in high-pressure synthesis of iron nitrides, especially the high-pressure solid-state metathesis reaction synthesis(HSM). We have summarized the reaction characteristics of HSM. The HSM reaction exhibits vector synthesis characteristics and promotes nitrogen disorder diffusion at high temperature. Due to this, the HSM reaction can achieve the synthesis of multinary iron-based metal nitrides and regulate the local magnetic moments. It serves as a powerful means for tuning the structure and magnetic properties of iron nitrides. Taking advantage of neutron diffraction in characterizing local magnetic moment and nitrogen disorder in iron nitrides, the relationship between iron local magnetic moment and nitrogen content has been elucidated. Moreover, the development of high-pressure in-situ imaging technology based on large-volume press allows the real-time observation of HSM reaction process. In this review, we also report our latest experiments on neutron diffraction and high-pressure in-situ image for the study of iron nitrides.展开更多
The Suizhou meteorite is a heavily shock-met-amorphosed L6 chondrite which contains thin shock melt veins.So far,26 high-pressure phases have been identified from the meteorite.Among the high-pressure phases,ten of th...The Suizhou meteorite is a heavily shock-met-amorphosed L6 chondrite which contains thin shock melt veins.So far,26 high-pressure phases have been identified from the meteorite.Among the high-pressure phases,ten of them were approved as new minerals which include tuite,xieite,wangdaodeite,chenmingite,hemleyite,poirierite,asimowite,hiroseite,elgoresyite,and ohtaniite,by the Commission on New Minerals,Nomenclature and Classification of the International Mineralogical Association.Other high-pressure phases identified from the meteorite are ahrensite,akimotoite,bridgmanite,lingunite,magnesiowüstite,majorite,majorite-pyrope_(ss),maskelynite,riesite,ringwoodite,wadsleyite,and 5 other phases including phase A,vitrified phase B and phase C,phase D(Ca-rich majorite),and partly inverted ringwoodite.The occurrence and abundance of high-pressure phases makes this meteorite the one with the richest variety of high-pressure minerals to date.展开更多
The 304 austenitic stainless steel was processed by high-pressure torsion(HPT)at room temperature with 10,20,and 30 rotations under a pressure of 3 GPa and a rotation speed of 1 r/min.The phase transformation and micr...The 304 austenitic stainless steel was processed by high-pressure torsion(HPT)at room temperature with 10,20,and 30 rotations under a pressure of 3 GPa and a rotation speed of 1 r/min.The phase transformation and microstructural evolution of 304 stainless steel after HPT were investigated by X-ray diffraction(XRD)analysis,electron backscatter diffraction(EBSD)analysis,transmission electron microscopy(TEM),nanoindentation test and differential scanning calorimetry(DSC)analysis.The experimental results show that HPT causes elongated nanocrystalline grains of 25 nm width along the torsion direction.After 10 turns of HPT,the deformation-induced martensitic transformation is completed and the hardness increases from 3 GPa to 8.5 GPa at the edge of the disc.However,a local reverse phase transformation from martensite to austenite is observed in the peripheral regions of the sample after 30 turns of HPT,leading to a higher volume fraction of austenite,and the hardness of the sample also decreases accordingly.展开更多
The pore structure of rocks significantly influences the porosity and permeability of reservoirs and the migration ability of oil and gas,and being the key task on the development of volcanic gas reservoirs.Nine volca...The pore structure of rocks significantly influences the porosity and permeability of reservoirs and the migration ability of oil and gas,and being the key task on the development of volcanic gas reservoirs.Nine volcanic rock samples from the Yingcheng Formation and Huoshiling Formation in the Longfengshan area of the Changling Fault Depression in the Songliao Basin were selected for this study.The pore structures of the volcanic rocks in the study area were investigated using high-pressure mercury injection,X-ray diffraction combined with fractal theory.The relationships between the fractal dimension and physical properties characteristics,pore structure parameters,and mineral content were analyzed to provide guidance for the development of volcanic rock gas reservoirs.The results show that the reservoir can be divided into 3 types(I,II,and III)based on the shape of the capillary pressure curve,and the physical properties deteriorate successively.Different types of reservoirs exhibit different fractal characteristics.For typesⅠ,ⅡandⅢ,the average total fractal dimensions were 2.3418,2.6850,and 2.9203,respectively.The larger the fractal dimension,the stronger the heterogeneity of reservoir.A small number of macro-pores primarily contributed to permeability.The fractal dimension was negatively correlated with porosity and permeability.The fractal dimension of the rock was strongly correlated with quartz and feldspar contents,and the mineral composition and content are closely related to the pore evolution of the reservoir,which are the internal factors affecting the fractal dimension of volcanic rock.展开更多
Achieving optimal mechanical performance in high-pressure die-cast(HPDC)Mg-based alloys through experimental methods is both costly and time-intensive due to significant variations in composition.This study leverages ...Achieving optimal mechanical performance in high-pressure die-cast(HPDC)Mg-based alloys through experimental methods is both costly and time-intensive due to significant variations in composition.This study leverages machine learning(ML)techniques to accelerate the development of high-performance Mg-based alloys.Data on alloy composition and mechanical properties were collected from literature sources,focusing on HPDC Mg-based alloys.Six ML models—extra trees,CatBoost,k-nearest neighbors,random forest,gradient boosting,and decision tree—were trained to predict mechanical behavior.Cat Boost yielded the highest prediction accuracy with R^(2) scores of 0.95 for ultimate tensile strength(UTS)and 0.92 for yield strength(YS).Further validation using published datasets reaffirmed its reliability,demonstrating R^(2) values of 0.956(UTS)and 0.936(YS),MAE of 1%and 2.8%,and RMSE of 1%and 3.5%,respectively.Among these,the CatBoost model demonstrated the highest predictive accuracy,outperforming other ML techniques across multiple optimization metrics.展开更多
High-pressure water jet technology has emerged as a highly effective method for removing industrial-scale deposits from pipelines,offering a clean,efficient,and environmentally sustainable alternative to conventional ...High-pressure water jet technology has emerged as a highly effective method for removing industrial-scale deposits from pipelines,offering a clean,efficient,and environmentally sustainable alternative to conventional mechanical or chemical cleaning techniques.Among the many parameters influencing its performance,the geometry of the nozzle plays a decisive role in governing jet coherence,impact pressure distribution,and overall cleaning efficiency.In this study,a comprehensive numerical and experimental investigation is conducted to elucidate the influence of nozzle geometry on the behavior of high-pressure water jets.Using Computational Fluid Dynamics(CFD)simulations based on the Volume of Fluid(VOF)approach,the jet dynamics and impingement characteristics of three representative nozzle configurations—flat,conical,and tapered—are systematically analyzed.Particular attention is devoted to the tapered nozzle,where variations in the outlet diameter are explored to determine their effect on flow structure,jet stability,and impact performance.The numerical predictions are rigorously validated against experimental measurements,demonstrating excellent quantitative agreement and confirming the robustness of the computational model.Results show that the tapered nozzle,characterized by its elongated conical transition section,promotes a more stable jet core and superior efflux performance compared to flat and conical geometries.Furthermore,the exit diameter is found to exert a profound influence on jet development.At an inlet pressure of 130 MPa,increasing the tapered nozzle's outlet diameter from 0.8 mm to 1.2 mm enlarges the coherent core region,enhances jet stability,and improves hydraulic energy utilization.Under these conditions,the total impact pressure on the target surface increases by 33.14%,while the overall cleaning efficiency improves by 40.44%.展开更多
The utilization of ironsand for preparing oxidized pellets poses challenges,including slow oxidation and low consolidation strength.The effects and function mechanisms of high-pressure grinding roll(HPGR)pretreatment ...The utilization of ironsand for preparing oxidized pellets poses challenges,including slow oxidation and low consolidation strength.The effects and function mechanisms of high-pressure grinding roll(HPGR)pretreatment on the oxidation and consolidation of ironsand pellets were investigated,and the energy utilization efficiency of HPGR with different roller pressure intensities was evaluated.The results indicate that HPGR pretreatment at 8 MPa improves the ironsand properties,with the specific surface area increasing by 740 cm^(2) g^(-1) and mechanical energy storage increasing by 2.5 kJ mol^(-1),which is conducive to oxidation and crystalline connection of particles.As roller pressure intensity increases to 16 MPa,more mechanical energy of HPGR is applied for crystal activation,with mechanical energy storage further rising by 18.1 kJ mol^(-1).The apparent activation energy for pellet oxidation initially decreases and then increases,reaching a minimum at 12 MPa.Simultaneously,the roasted pellets porosity decreases by 2.8%,while the compressive strength increases by 789 N.At higher roller pressure intensity,the densely connected structure between particles impedes gas diffusion within the pellets,diminishing the beneficial effects of HPGR on pellet oxidation.Moreover,excessive roller pressure intensity decreases the HPGR energy utilization efficiency.The optimal HPGR roller pressure intensity for ironsand is 12 MPa,at which the specific surface area increases by 790 cm^(2) g^(-1),mechanical energy storage increases by 10.6 kJ mol^(-1),the compressive strength of roasted pellets rises to 2816 N,and the appropriate preheating and roasting temperatures decrease by 250 and 125°C,respectively.展开更多
Al_(65)Cu_(20)Fe_(15)bulk is synthesized with the high-pressure synthesis(HPS)method.Various analytical techniques,such as single crystal x-ray diffraction(SXRD),scanning electron microscopy equipped with energy-dispe...Al_(65)Cu_(20)Fe_(15)bulk is synthesized with the high-pressure synthesis(HPS)method.Various analytical techniques,such as single crystal x-ray diffraction(SXRD),scanning electron microscopy equipped with energy-dispersive x-ray spectroscopy,and transmission electron microscopy,are employed to characterize the sintered bulk and confirmed its quasicrystalline structure.The electrical resistivity of the HPS quasicrystal specimen is measured from 2 K to 300 K,revealing a significantly elevated value in comparison to samples prepared via alternative methods.Nanoindentation testing demonstrates exceptional hardness and elastic modulus of our Al_(65)Cu_(20)Fe_(15)quasicrystal,consistent with existing results.The ratio of hardness to elastic modulus further highlight the potential superior wear resistance of the Al_(65)Cu_(20)Fe_(15)quasicrystal.Differential scanning calorimetry measurement conducted on the HPS Al_(65)Cu_(20)Fe_(15)quasicrystals reveal a high melting point of 877℃.展开更多
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
Developing efficient and durable electrocatalysts for acidic oxygen evolution reaction(OER)is pivotal for advancing proton exchange membrane water electrolysis(PEMWEs),yet balancing activity and stability remains a fo...Developing efficient and durable electrocatalysts for acidic oxygen evolution reaction(OER)is pivotal for advancing proton exchange membrane water electrolysis(PEMWEs),yet balancing activity and stability remains a formidable challenge.Herein,we propose a dual-engineering strategy to stabilize Ru-based catalysts by synergizing the oxygen vacancy site-synergized mechanism-lattice oxygen mechanism(OVSM-LOM)with Ru-N bond stabilization.The engineered RuO_(2)@NCC catalyst exhibits exceptional OER performance in 0.5 M H2SO4,achieving an ultralow overpotential of 215 mV at 10 mA cm^(-2) and prolonged stability for over 327 h.The catalyst delivers 300 h of continuous operation at 1 A cm^(-2),with a negligible degradation rate of only 0.067 mV h-1,further demonstrating its potential for practical application.Oxygen vacancies unlock the OVSM-LOM pathway,bypassing the sluggish adsorbate evolution mechanism(AEM)and accelerating reaction kinetics,while the Ru-N bonds suppress Ru dissolution by anchoring low-valent Ru centers.Quasi-in situ X-ray photoelectron spectroscopy(XPS),X-ray absorption spectroscopy(XAS),and isotopic labeling experiments confirm the lattice oxygen participation with *O formation as the rate-determining step.The Ru-N bonds reinforce the structural integrity by stabilizing low-valent Ru centers and inhibiting overoxidation.Theoretical calculations further verify that the synergistic interaction between OVs and Ru-O(N)active sites optimizes the Ru d-band center and stabilizes intermediates,while Ru-N coordination enhances structural integrity.This study establishes a novel paradigm for designing robust acidic OER catalysts through defect and coordination engineering,bridging the gap between activity and stability for sustainable energy technologies.展开更多
Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and of...Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and offering the highest theoretical energy density(~3.5 k Wh kg^(-1))among discussed candidates.Contributing to the poor cycle life of currently reported Li-O_(2)cells is singlet oxygen(1O_(2))formation,inducing parasitic reactions,degrading key components,and severely deteriorating cell performance.Here,we harness the chirality-induced spin selectivity effect of chiral cobalt oxide nanosheets(Co_(3)O_(4)NSs)as cathode materials to suppress 1O_(2)in Li-O_(2)batteries for the first time.Operando photoluminescence spectroscopy reveals a 3.7-fold and 3.23-fold reduction in 1O_(2)during discharge and charge,respectively,compared to conventional carbon paperbased cells,consistent with differential electrochemical mass spectrometry results,which indicate a near-theoretical charge-to-O_(2)ratio(2.04 e-/O_(2)).Density functional theory calculations demonstrate that chirality induces a peak shift near the Fermi level,enhancing Co 3d-O 2p hybridization,stabilizing reaction intermediates,and lowering activation barriers for Li_(2)O_(2)formation and decomposition.These findings establish a new strategy for improving the stability and energy efficiency of sustainable Li-O_(2)batteries,abridging the current gap to commercialization.展开更多
The development of Pt-free catalysts for the oxygen reduction reaction(ORR)is a great issue for meeting the cost challenges of proton exchange membrane fuel cells(PEMFCs)in commercial applications.In this work,a serie...The development of Pt-free catalysts for the oxygen reduction reaction(ORR)is a great issue for meeting the cost challenges of proton exchange membrane fuel cells(PEMFCs)in commercial applications.In this work,a series of RuCo/C catalysts were synthesized by NaBH4 reduction method under the premise that the total metal mass percentage was 20%.X-ray diffraction(XRD)patterns and scanning electron microscopy(SEM)confirmed the formation of single-phase nanoparticles with an average size of 33 nm.Cyclic voltammograms(CV)and linear sweep voltammograms(LSV)tests indicated that RuCo(2:1)/C catalyst had the optimal ORR properties.Additionally,the RuCo(2:1)/C catalyst remarkably sustained 98.1% of its activity even after 3000 cycles,surpassing the performance of Pt/C(84.8%).Analysis of the elemental state of the catalyst surface after cycling using X-ray photoelectron spectroscopy(XPS)revealed that the Ru^(0) percentage of RuCo(2:1)/C decreased by 2.2%(from 66.3% to 64.1%),while the Pt^(0) percentage of Pt/C decreased by 7.1%(from 53.3% to 46.2%).It is suggested that the synergy between Ru and Co holds the potential to pave the way for future low-cost and highly stable ORR catalysts,offering significant promise in the context of PEMFCs.展开更多
基金financially supported by Qingdao Science and Technology Benefiting People Special Project (No. 20-3-4-8-nsh)the Fundamental Research Funds for the Central Universities (No.20CX02212A)the Development Fund of State Key Laboratory of Heavy Oil Processing and China University of Petroleum Training Program of Innovation and Entrepreneurship for Undergraduates (No.201910425018)。
文摘Designing the specific crystal phase with better intrinsic activity and more active sites is a very promising strategy for earth-abundant electrocatalysts for oxygen evolution reaction(OER).Herein,a facile two-step method including the high-pressure microwave and the hydrothermal sulfurization is adopted to prepare the WS_(x)/Ni_(9)S_(8) hetero-catalyst on nickel foam(WS_(x)/Ni_(9)S_(8)/NF).Firstly,WO3 polyhedrons homogeneously cover the surface of NF through the high-pressure microwave hydrothermal process.Secondly,WS_(x)/Ni_(9)S_(8) nanoparticles on the surface of NF can be synthesized after a hydrothermal sulfurization,which has been confirmed by scanning electron microscopy(SEM) elemental mapping and high-resolution transmission electron microscopy(HRTEM).The amorphous WSx and Ni9 S8 phase may provide the dual active sites for OER.The electrochemical measurements show that WS_(x)/Ni_(9)S_(8)/NF has superior OER activity with a low overpotential of 320 mV at the current density of 100 mA·cm^(-2),better than those of other samples.The enhanced OER performance may be due to the synergistic catalysis from Ni9 S8 phase and high valence of W.Owing to the stable structure of Ni9 S8,the long-term stability of WS_(x)/Ni_(9)S_(8)/NF for at least 10 h can be obtained.This work may provide a new approach for the doped nickel sulfides crystal phase through high-pressure microwave hydrothermal assistance for OER.
基金financially supported by the National Natural Science Foundation of China(Nos.52175284 and 52474396)the National Key Research and Development Program of China(No.2022YFB3404201)。
文摘High pressure die casting(HPDC)AlSi10Mn Mg alloy castings are widely used in the automobile industry.Mg can optimize the mechanical properties of castings through heat treatment,while the release of thermal stress arouses the deformation of large integrated die-castings.Herein,the development of non-heat treatment Al alloys is becoming the hot topic.In addition,HPDC contains externally solidified crystals(ESCs),which are detrimental to the mechanical properties of castings.To achieve high strength and toughness of non-heat treatment die-casting Al-Si alloy,we used AlSi9Mn alloy as matrix with the introduction of Zr,Ti,Nb,and Ce.Their influences on ESCs and mechanical properties were systematically investigated through three-dimensional reconstruction and thermodynamic simulation.Our results reveal that the addition of Ti increased ESCs'size and porosity,while the introduction of Nb refined ESCs and decreased porosity.Meanwhile,large-sized Al_3(Zr,Ti)phases formed and degraded the mechanical properties.Subsequent introduction of Ce resulted in the poisoning effect and reduced mechanical properties.
基金supported by the National Natural Science Foundation of China(Grant No.U21B2062)supported by the Key Laboratory for Carbonate Reservoirs of China National Petroleum Corporation。
文摘Burial dissolution is a critical diagenetic process influencing ultra-deep carbonate reservoir development and preservation.Artificial carbonate samples with different internal structures were prepared,and high-temperature and highpressure dissolution kinetic simulations were conducted.The results demonstrate that the intensity of burial dissolution is controlled by temperature and pressure,while tectonic-fluid activity influences the development pattern of burial dissolution,ultimately determining the direction of its differential modification.Extensive burial dissolution is likely to occur primarily at relatively shallow depths,significantly influencing reservoir formation,preservation,modification,and adjustment.The development of faults facilitates the maintenance of the intensity of burial dissolution.The maximum intensity of burial dissolution occurs at the tips and overlap zones of faults and intersections of multiple faults.The larger the scale of the faults,the more conducive it is to the development of burial dissolution.Burial dissolution fosters the formation of fault networks characterized by enhanced reservoir capacity and permeability.Burial dissolution controlled by episodic tectonic-fluid activity is a plausible explanation for forming the Tarim Basin's ultra-deep fault-controlled“stringbead-like”reservoirs.
基金National Key Research and Development Program of China(2021YFB3701004)。
文摘Degradable metals,represented by magnesium and magnesium alloys,have attracted significant attention as fracture internal fixation and bone defect repairing materials due to their good biocompatibility,suitable elastic modulus and degradable properties.The Mg-3Zn-1Ca-0.5Sr(wt%)alloy is considered a competitor in the biomaterial field thanks to its unique composition of essential nutrients and excellent mechanical properties.However,the presence of coarse second-phase particles in the alloy accelerates its degradation rate and causes excessive gas formation during implantation,which restricts the alloy's potential for clinical device applications.In order to further optimize the properties of the alloy,extrusion combined with high-pressure torsion(HPT)was adopted for deformation processing.The results show that by optimizing the material processing means,the grain can be refined and broken,and the second-phase distribution can be improved,thus improving the microstructure,mechanical properties,and corrosion resistance of the alloy.After 15 cycles of HPT processing,the grains of the alloy are significantly refined to the nanometer scale,reaching approximately 98 nm.Additionally,the second-phase distribution is greatly improved,transforming the original streamlined structure into a more dispersed distribution.This change in microstructure leads to a significant strengthening effect on the alloy,with a noticeable increase in hardness from 60.3 HV in the as-extruded state to 98.5 HV.
基金Supported by Jiangsu Provincial Natural Science Foundation(Grant No.BK20231497)Jiangsu Provincial Post graduate Research&Practice Innovation Program(Grant No.KYCX25_2982)+3 种基金China University of Mining and Technology Graduate Innovation Program(Grant No.2025WLKXJ094)National Natural Science Foundation of China(Grant No.51975573)National Key R&D Program of China(Grant No.2022YFC2905600)Priority Academic Program Development of Jiangsu Higher Education Institute of China.
文摘A rotary sealing device that automatically compensates for wear is designed to address the issues of easy wear and the short service life of the rotary sealing device with automatic wear compensation in mining machinery.After the end face of the guide sleeve wears out,it still tightly adheres to the sealing valve seat under the pressure difference,achieving automatic wear compensation.Based on fluid-solid coupling technology,the structural strength of the rotary sealing device was checked.The influence of factors on the sealing performance of rotary sealing devices was studied using the control variable method.The results show that as the pressure of water increases,the leakage rate of the sealing device decreases,and after 30 MPa,the leakage rate is almost 0 mL/h.The temperature of the rotating sealing device increases with the increase of rotation speed or pressure,and the temperature is more affected by the rotation speed factor.The frictional torque increases with increasing pressure and is independent of rotational speed.Comprehensive analysis shows that the wear resistance and reliability level of the sealing guide sleeve material is PVDF>PEEK>PE>PA.This study designs a high-pressure automatic compensation wear rotary sealing device and selects the optimal sealing material,providing technical support for the application of high-pressure water jet in mining machinery.
基金supported by the National Natural Science Foundation of China(grant number:52203375 and 52073254)。
文摘With the global oil and gas industry increasingly targeting ultra-deep well development,the demand for wear resistance in polycrystalline diamond compact(PDC)bits is increasing.However,further improvement of the mechanical properties of PDC incurs prohibitively elevated costs and stringent technological challenges.Here,we present a two-stage high-pressure infiltration(HPI)methodology involving cobalt removal pretreatment followed by lubricant infiltration.The successful infiltration of lubricants into diamond micropores has been systematically verified,and the effects of lubricant phase composition,infiltration pressure,and temperature on infiltration depth have been thoroughly investigated.Fractal dimension analysis characterizes the pore structure of cobalt-removed diamonds,revealing a strong correlation between the fractal dimension and friction coefficient reduction.Tribological testing confirms the formation of lubricating films at friction interfaces,achieving a 71.5%reduction in the coefficient of friction for lubricant-containing diamond materials.This straightforward strategy opens a gate to developing the next generation of self-lubricating diamond materials.
基金Project supported by the National Key R&D Program of China (Grant No. 2021YFA1400300)the National Natural Science Foundation of China (Grant Nos. 12425403, 12261131499, 12304268, 12304159, 11934017, and 11921004)+1 种基金the China Postdoctoral Science Foundation (Grant No. 2023M743741)The synchrotron x-ray diffraction experiments were performed at SPring-8 with the approval of the Japan Synchrotron Radiation Research Institute (Grant Nos. 2023B1575, 2023B1976, 2024A1506, and 2024A1695)。
文摘Perovskite oxynitrides AB(N,O)_(3), a crucial class in materials science, have attracted much attention. By precisely controlling A-and B-site ions and tuning the N/O ratio, new materials with exotic charge states and intriguing electronic behaviors can be designed and synthesized. In this work, a novel oxynitride perovskite, CeNbO_(2)N, was prepared under high-temperature and high-pressure conditions. The compound crystallizes in an orthorhombic perovskite structure in Pnma symmetry with disordered N/O distribution. The x-ray absorption spectroscopy confirms the presence of a Nb^(4+) state with 4d^(1) electronic configuration in CeNbO_(2)N. As a result, the resistivity of CeNbO_(2)N is sharply reduced compared to its counterpart CeTa^(5+)ON_(2) and other Nb^(5+) compounds. No long-range spin order is found to occur with the temperature down to 2 K in CeNbO_(2)N, while a remarkable negative magnetoresistance effect shows up at lower temperatures, probably due to the magnetic scattering arising from short-range spin correlations.
基金financially supported by the National Natural Science Foundation of China (Grant Nos. 12374013 and U2030107)the Fundamental Research Funds for the Central University (Grant No. 2020SCUNL107)+1 种基金The high-pressure in-situ imaging experiments were conducted at BL12SW of SSRF (Proposal No. 2024-SSRF-PT-505499)The NPD experiments were supported by Chinese Academy of Engineering Physics。
文摘Iron nitride(Fe_(x)N_y) is a promising candidate for the next generation of ferromagnetic materials. However, synthesizing high-quality bulk iron nitride with tuned structure and magnetic properties remains a challenge. Currently, experimental and theoretical results regarding the magnetic property of iron nitrides remain controversial. With the recent advancements in high-pressure technology, new synthetic pathways to iron nitrides have been proposed. High-pressure synthesis technology provides multidimensional possibilities for tuning the structure and magnetic properties of iron nitrides. This review summarizes recent progress in high-pressure synthesis of iron nitrides, especially the high-pressure solid-state metathesis reaction synthesis(HSM). We have summarized the reaction characteristics of HSM. The HSM reaction exhibits vector synthesis characteristics and promotes nitrogen disorder diffusion at high temperature. Due to this, the HSM reaction can achieve the synthesis of multinary iron-based metal nitrides and regulate the local magnetic moments. It serves as a powerful means for tuning the structure and magnetic properties of iron nitrides. Taking advantage of neutron diffraction in characterizing local magnetic moment and nitrogen disorder in iron nitrides, the relationship between iron local magnetic moment and nitrogen content has been elucidated. Moreover, the development of high-pressure in-situ imaging technology based on large-volume press allows the real-time observation of HSM reaction process. In this review, we also report our latest experiments on neutron diffraction and high-pressure in-situ image for the study of iron nitrides.
基金Science and Technology Planning Project of Guangdong Province(2023B1212060048).
文摘The Suizhou meteorite is a heavily shock-met-amorphosed L6 chondrite which contains thin shock melt veins.So far,26 high-pressure phases have been identified from the meteorite.Among the high-pressure phases,ten of them were approved as new minerals which include tuite,xieite,wangdaodeite,chenmingite,hemleyite,poirierite,asimowite,hiroseite,elgoresyite,and ohtaniite,by the Commission on New Minerals,Nomenclature and Classification of the International Mineralogical Association.Other high-pressure phases identified from the meteorite are ahrensite,akimotoite,bridgmanite,lingunite,magnesiowüstite,majorite,majorite-pyrope_(ss),maskelynite,riesite,ringwoodite,wadsleyite,and 5 other phases including phase A,vitrified phase B and phase C,phase D(Ca-rich majorite),and partly inverted ringwoodite.The occurrence and abundance of high-pressure phases makes this meteorite the one with the richest variety of high-pressure minerals to date.
基金Funded by the National Natural Science Foundation of China(No.51905215)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.SJCX231233)。
文摘The 304 austenitic stainless steel was processed by high-pressure torsion(HPT)at room temperature with 10,20,and 30 rotations under a pressure of 3 GPa and a rotation speed of 1 r/min.The phase transformation and microstructural evolution of 304 stainless steel after HPT were investigated by X-ray diffraction(XRD)analysis,electron backscatter diffraction(EBSD)analysis,transmission electron microscopy(TEM),nanoindentation test and differential scanning calorimetry(DSC)analysis.The experimental results show that HPT causes elongated nanocrystalline grains of 25 nm width along the torsion direction.After 10 turns of HPT,the deformation-induced martensitic transformation is completed and the hardness increases from 3 GPa to 8.5 GPa at the edge of the disc.However,a local reverse phase transformation from martensite to austenite is observed in the peripheral regions of the sample after 30 turns of HPT,leading to a higher volume fraction of austenite,and the hardness of the sample also decreases accordingly.
基金Supported by Key Scientific and Technological Projects of Sinopec(No.P21104-2).
文摘The pore structure of rocks significantly influences the porosity and permeability of reservoirs and the migration ability of oil and gas,and being the key task on the development of volcanic gas reservoirs.Nine volcanic rock samples from the Yingcheng Formation and Huoshiling Formation in the Longfengshan area of the Changling Fault Depression in the Songliao Basin were selected for this study.The pore structures of the volcanic rocks in the study area were investigated using high-pressure mercury injection,X-ray diffraction combined with fractal theory.The relationships between the fractal dimension and physical properties characteristics,pore structure parameters,and mineral content were analyzed to provide guidance for the development of volcanic rock gas reservoirs.The results show that the reservoir can be divided into 3 types(I,II,and III)based on the shape of the capillary pressure curve,and the physical properties deteriorate successively.Different types of reservoirs exhibit different fractal characteristics.For typesⅠ,ⅡandⅢ,the average total fractal dimensions were 2.3418,2.6850,and 2.9203,respectively.The larger the fractal dimension,the stronger the heterogeneity of reservoir.A small number of macro-pores primarily contributed to permeability.The fractal dimension was negatively correlated with porosity and permeability.The fractal dimension of the rock was strongly correlated with quartz and feldspar contents,and the mineral composition and content are closely related to the pore evolution of the reservoir,which are the internal factors affecting the fractal dimension of volcanic rock.
基金supported by Basic Science Research Program through the National Research Foundation of Korea(NRF)funded by the Ministry of Education(2021R1A6A1A10044950)。
文摘Achieving optimal mechanical performance in high-pressure die-cast(HPDC)Mg-based alloys through experimental methods is both costly and time-intensive due to significant variations in composition.This study leverages machine learning(ML)techniques to accelerate the development of high-performance Mg-based alloys.Data on alloy composition and mechanical properties were collected from literature sources,focusing on HPDC Mg-based alloys.Six ML models—extra trees,CatBoost,k-nearest neighbors,random forest,gradient boosting,and decision tree—were trained to predict mechanical behavior.Cat Boost yielded the highest prediction accuracy with R^(2) scores of 0.95 for ultimate tensile strength(UTS)and 0.92 for yield strength(YS).Further validation using published datasets reaffirmed its reliability,demonstrating R^(2) values of 0.956(UTS)and 0.936(YS),MAE of 1%and 2.8%,and RMSE of 1%and 3.5%,respectively.Among these,the CatBoost model demonstrated the highest predictive accuracy,outperforming other ML techniques across multiple optimization metrics.
基金the Natural Science Foundation of Shandong Province,China(No.ZR2021QE157).
文摘High-pressure water jet technology has emerged as a highly effective method for removing industrial-scale deposits from pipelines,offering a clean,efficient,and environmentally sustainable alternative to conventional mechanical or chemical cleaning techniques.Among the many parameters influencing its performance,the geometry of the nozzle plays a decisive role in governing jet coherence,impact pressure distribution,and overall cleaning efficiency.In this study,a comprehensive numerical and experimental investigation is conducted to elucidate the influence of nozzle geometry on the behavior of high-pressure water jets.Using Computational Fluid Dynamics(CFD)simulations based on the Volume of Fluid(VOF)approach,the jet dynamics and impingement characteristics of three representative nozzle configurations—flat,conical,and tapered—are systematically analyzed.Particular attention is devoted to the tapered nozzle,where variations in the outlet diameter are explored to determine their effect on flow structure,jet stability,and impact performance.The numerical predictions are rigorously validated against experimental measurements,demonstrating excellent quantitative agreement and confirming the robustness of the computational model.Results show that the tapered nozzle,characterized by its elongated conical transition section,promotes a more stable jet core and superior efflux performance compared to flat and conical geometries.Furthermore,the exit diameter is found to exert a profound influence on jet development.At an inlet pressure of 130 MPa,increasing the tapered nozzle's outlet diameter from 0.8 mm to 1.2 mm enlarges the coherent core region,enhances jet stability,and improves hydraulic energy utilization.Under these conditions,the total impact pressure on the target surface increases by 33.14%,while the overall cleaning efficiency improves by 40.44%.
基金financially supported by the General Program of National Natural Science Foundation of China(No.52174330)Hunan Provincial Innovation Foundation for Postgraduate(No.QL20220069)Postgraduate Innovative Project of Central South University(No.1053320214756).
文摘The utilization of ironsand for preparing oxidized pellets poses challenges,including slow oxidation and low consolidation strength.The effects and function mechanisms of high-pressure grinding roll(HPGR)pretreatment on the oxidation and consolidation of ironsand pellets were investigated,and the energy utilization efficiency of HPGR with different roller pressure intensities was evaluated.The results indicate that HPGR pretreatment at 8 MPa improves the ironsand properties,with the specific surface area increasing by 740 cm^(2) g^(-1) and mechanical energy storage increasing by 2.5 kJ mol^(-1),which is conducive to oxidation and crystalline connection of particles.As roller pressure intensity increases to 16 MPa,more mechanical energy of HPGR is applied for crystal activation,with mechanical energy storage further rising by 18.1 kJ mol^(-1).The apparent activation energy for pellet oxidation initially decreases and then increases,reaching a minimum at 12 MPa.Simultaneously,the roasted pellets porosity decreases by 2.8%,while the compressive strength increases by 789 N.At higher roller pressure intensity,the densely connected structure between particles impedes gas diffusion within the pellets,diminishing the beneficial effects of HPGR on pellet oxidation.Moreover,excessive roller pressure intensity decreases the HPGR energy utilization efficiency.The optimal HPGR roller pressure intensity for ironsand is 12 MPa,at which the specific surface area increases by 790 cm^(2) g^(-1),mechanical energy storage increases by 10.6 kJ mol^(-1),the compressive strength of roasted pellets rises to 2816 N,and the appropriate preheating and roasting temperatures decrease by 250 and 125°C,respectively.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.52173231 and 51925105)the Natural Science Foundation of Hebei Province,China(Grant No.E2022203182)+1 种基金The Innovation Ability Promotion Project of Hebei supported by Hebei Key Laboratory for Optimizing Metal Product Technology and Performance(Grant No.22567609H)supported by the grants from Slovak National Agencies(Grant Nos.VEGA 2/0144/21,APVV19-0369,and APVV-20-0124)。
文摘Al_(65)Cu_(20)Fe_(15)bulk is synthesized with the high-pressure synthesis(HPS)method.Various analytical techniques,such as single crystal x-ray diffraction(SXRD),scanning electron microscopy equipped with energy-dispersive x-ray spectroscopy,and transmission electron microscopy,are employed to characterize the sintered bulk and confirmed its quasicrystalline structure.The electrical resistivity of the HPS quasicrystal specimen is measured from 2 K to 300 K,revealing a significantly elevated value in comparison to samples prepared via alternative methods.Nanoindentation testing demonstrates exceptional hardness and elastic modulus of our Al_(65)Cu_(20)Fe_(15)quasicrystal,consistent with existing results.The ratio of hardness to elastic modulus further highlight the potential superior wear resistance of the Al_(65)Cu_(20)Fe_(15)quasicrystal.Differential scanning calorimetry measurement conducted on the HPS Al_(65)Cu_(20)Fe_(15)quasicrystals reveal a high melting point of 877℃.
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.
基金support from the National Natural Science Foundation of China(Nos.12305373 and 52276220)the Guangzhou Basic Research Program(No.SL2024A04J00234).
文摘Developing efficient and durable electrocatalysts for acidic oxygen evolution reaction(OER)is pivotal for advancing proton exchange membrane water electrolysis(PEMWEs),yet balancing activity and stability remains a formidable challenge.Herein,we propose a dual-engineering strategy to stabilize Ru-based catalysts by synergizing the oxygen vacancy site-synergized mechanism-lattice oxygen mechanism(OVSM-LOM)with Ru-N bond stabilization.The engineered RuO_(2)@NCC catalyst exhibits exceptional OER performance in 0.5 M H2SO4,achieving an ultralow overpotential of 215 mV at 10 mA cm^(-2) and prolonged stability for over 327 h.The catalyst delivers 300 h of continuous operation at 1 A cm^(-2),with a negligible degradation rate of only 0.067 mV h-1,further demonstrating its potential for practical application.Oxygen vacancies unlock the OVSM-LOM pathway,bypassing the sluggish adsorbate evolution mechanism(AEM)and accelerating reaction kinetics,while the Ru-N bonds suppress Ru dissolution by anchoring low-valent Ru centers.Quasi-in situ X-ray photoelectron spectroscopy(XPS),X-ray absorption spectroscopy(XAS),and isotopic labeling experiments confirm the lattice oxygen participation with *O formation as the rate-determining step.The Ru-N bonds reinforce the structural integrity by stabilizing low-valent Ru centers and inhibiting overoxidation.Theoretical calculations further verify that the synergistic interaction between OVs and Ru-O(N)active sites optimizes the Ru d-band center and stabilizes intermediates,while Ru-N coordination enhances structural integrity.This study establishes a novel paradigm for designing robust acidic OER catalysts through defect and coordination engineering,bridging the gap between activity and stability for sustainable energy technologies.
基金supported by Basic Science Research Program(Priority Research Institute)through the NRF of Korea funded by the Ministry of Education(2021R1A6A1A10039823)by the Korea Basic Science Institute(National Research Facilities and Equipment Center)grant funded by the Ministry of Education(2020R1A6C101B194)。
文摘Lithium-oxygen(Li-O2)batteries are perceived as a promising breakthrough in sustainable electrochemical energy storage,utilizing ambient air as an energy source,eliminating the need for costly cathode materials,and offering the highest theoretical energy density(~3.5 k Wh kg^(-1))among discussed candidates.Contributing to the poor cycle life of currently reported Li-O_(2)cells is singlet oxygen(1O_(2))formation,inducing parasitic reactions,degrading key components,and severely deteriorating cell performance.Here,we harness the chirality-induced spin selectivity effect of chiral cobalt oxide nanosheets(Co_(3)O_(4)NSs)as cathode materials to suppress 1O_(2)in Li-O_(2)batteries for the first time.Operando photoluminescence spectroscopy reveals a 3.7-fold and 3.23-fold reduction in 1O_(2)during discharge and charge,respectively,compared to conventional carbon paperbased cells,consistent with differential electrochemical mass spectrometry results,which indicate a near-theoretical charge-to-O_(2)ratio(2.04 e-/O_(2)).Density functional theory calculations demonstrate that chirality induces a peak shift near the Fermi level,enhancing Co 3d-O 2p hybridization,stabilizing reaction intermediates,and lowering activation barriers for Li_(2)O_(2)formation and decomposition.These findings establish a new strategy for improving the stability and energy efficiency of sustainable Li-O_(2)batteries,abridging the current gap to commercialization.
基金Funded by the 111 Project(No.B17034)Open Project of Hubei Key Laboratory of Power System Design and Test for Electrical Vehicle(No.ZDSYS202212)+1 种基金Innovative Research Team Development Program of Ministry of Education of China(No.IRT_17R83)the Science and Technology Project of China Southern Power Grid Co.,Ltd.(No.GDKJXM20222546)。
文摘The development of Pt-free catalysts for the oxygen reduction reaction(ORR)is a great issue for meeting the cost challenges of proton exchange membrane fuel cells(PEMFCs)in commercial applications.In this work,a series of RuCo/C catalysts were synthesized by NaBH4 reduction method under the premise that the total metal mass percentage was 20%.X-ray diffraction(XRD)patterns and scanning electron microscopy(SEM)confirmed the formation of single-phase nanoparticles with an average size of 33 nm.Cyclic voltammograms(CV)and linear sweep voltammograms(LSV)tests indicated that RuCo(2:1)/C catalyst had the optimal ORR properties.Additionally,the RuCo(2:1)/C catalyst remarkably sustained 98.1% of its activity even after 3000 cycles,surpassing the performance of Pt/C(84.8%).Analysis of the elemental state of the catalyst surface after cycling using X-ray photoelectron spectroscopy(XPS)revealed that the Ru^(0) percentage of RuCo(2:1)/C decreased by 2.2%(from 66.3% to 64.1%),while the Pt^(0) percentage of Pt/C decreased by 7.1%(from 53.3% to 46.2%).It is suggested that the synergy between Ru and Co holds the potential to pave the way for future low-cost and highly stable ORR catalysts,offering significant promise in the context of PEMFCs.
