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
Effective lattice oxygen(Olatt)activation at low temperatures has long been a challenge in catalytic oxidation reactions.Traditional thermal catalytic soot combustion,even with Pt/Pd catalysts,is inefficient at exhaus...Effective lattice oxygen(Olatt)activation at low temperatures has long been a challenge in catalytic oxidation reactions.Traditional thermal catalytic soot combustion,even with Pt/Pd catalysts,is inefficient at exhaust temperatures below 200℃,particularly under conditions of frequent idling.Herein,we report an effective strategy utilizing non-thermal plasma(NTP)to activate Olatt in Ce_(1–x)Co_(x)O_(2–δ)catalysts,achieving dramatic enhancement of the soot combustion rate at low temperatures.At 200℃ and 4.3 W(discharge power,P_(dis)),NTP-Ce_(0.8)Co_(0.2)O_(2–δ)achieved 96.9%soot conversion(X_(C)),99.0%CO_(2) selectivity(S(CO_(2)))and a maximum energy conversion efficiency(Emax)of 14.7 g kWh^(–1).Compared with previously reported results,NTP-Ce_(0.8)Co_(0.2)O_(2–δ)exhibits the highest S(CO_(2))and Emax values.Remarkably,even without heating,X_(C),Emax,and S(CO_(2))reached 92.1%,6.1 g kWh–1,and 97.5%,respectively,at 6.3 W(P_(dis)).The results of characterization and theoretical calculation demonstrated that Co dopes into the CeO_(2) crystal lattice and forms an asymmetric Ce–O–Co structure,making oxygen“easy come,easy go”,thereby enabling the rapid combustion of soot over NTP-Ce_(0.8)Co_(0.2)O_(2–δ).This study highlights the great potential of NTP for activating Olatt and provides valuable insights into the design of efficient NTP-adapted catalysts for oxidation reactions.展开更多
Knowing the optimal operating parameters of Stirling engines is important for efficient combustion through adaptability to changed pressures and oxygen atmospheres. In this study, the optimum operating conditions for ...Knowing the optimal operating parameters of Stirling engines is important for efficient combustion through adaptability to changed pressures and oxygen atmospheres. In this study, the optimum operating conditions for efficient combustion in a singular Stirling engine combustor at different oxygen atmospheres were investigated and determined. Numerical simulations were performed to investigate the effects of ejection ratio and pressure on combustion performance. In an oxygen/carbon dioxide atmosphere, the results show that increasing the ejection ratio substantially alters the flame distribution in the Stirling engine combustor, increasing heat transfer and external combustion efficiency. In contrast, increasing the ejection ratio reduces the average and maximum temperatures of the Stirling engine combustor. Increased pressure affects the flame distribution in the Stirling engine combustor and impedes the flow and convective heat transfer in the combustor, reducing the overall external combustion efficiency at pressures above 6.5 MPa. In an air/carbon dioxide atmosphere, an increased ejection ratio reduces the average and maximum temperatures in the Stirling engine combustor. However, the overall flame distribution does not change substantially. The external combustion efficiency tends to increase and then decrease because of two opposing factors: the increase in the convective heat transfer coefficient and the decrease in the temperature difference. Increasing pressure inhibits forced convection heat transfer in the Stirling engine combustor, reducing external combustion efficiency, which drops from 78% to 65% when pressure increases from 0.2 MPa to 0.5 MPa.展开更多
Coal-direct chemical looping(CDCL) is a promising CO_(2) capture technology with low costs.Potassium modification can significantly enhance the reactivity of iron-based oxygen carriers and coal.However,potassium loss ...Coal-direct chemical looping(CDCL) is a promising CO_(2) capture technology with low costs.Potassium modification can significantly enhance the reactivity of iron-based oxygen carriers and coal.However,potassium loss causes a decline in cyclic stability.To address this,we prepared a potassium hexatitanate-modified iron-based OC and conducted CDCL experiments in a fixed-bed reactor using Zhundong coal coke as fuel.The study examined the impact of potassium hexatitanate on carbon conversion,OC activity stability,and potassium maintenance.Additionally,Fact Sage was used to calculate potassium fugacity patterns at different temperatures,Fe_(2)O_(3)/C molar ratios,and OC reduction degrees.Results showed that potassium hexatitanate increased carbon conversion,achieving 50%conversion at 40% potassium addition.In multi-cycle tests,carbon conversion rose with increased cycle times,reaching 84%.This improvement is attributed to ion exchange between Fe^(3+) and Ti^(4+),which induces lattice distortion and creates oxygen vacancies,enhancing OC reactivity.Potassium content remained stable during multi-cycle tests,indicating the effective potassium retention capacity of potassium hexatitanate.展开更多
Catalyzed gasoline particulate filters(cGPFs)are being developed to enable compliance with the particulate number limits for passenger cars equipped with gasoline direct injection(GDI)engines in China and Europe,It is...Catalyzed gasoline particulate filters(cGPFs)are being developed to enable compliance with the particulate number limits for passenger cars equipped with gasoline direct injection(GDI)engines in China and Europe,It is appealing to build catalysts with ceria—an irreplaceable"reducible"component in three-way converters—to help eliminate the soot particles trapped in cGPFs via O_(2)-assisted combustion.While research aiming at understanding how these recipes function has continued for more than two decades,a universal model elucidating the roles of different"active oxygen"species is yet to be realized.In this perspective,by critically assessing the reported data about gasoline soot catalytic combustion over ceria catalysts,it is suggested that ceria ignites soot through contributing its lattice oxygen,giving rise to a"hot ring"region at the periphery of soot-catalyst interface.During the"re-oxidation"semi-cycles,electrophilic superoxides and/or peroxides(O_(x)^(n-))are produced at the Ce^(3+)and oxygen vacancy sites enriched in this collar-like region,and then work as key reactive phases for soot deep oxidation.Based on this"O_(x)^(n-)assisted"Mars-van Krevelen mechanism,several guidelines for ceria catalyst designing are proposed,ending with a summary about where future opportunities and challenges may lie in developing efficient and practical cGPF catalysts.展开更多
Normal diffusion flame(NDF)of acid gas with a H_(2)S concentration below 50.0%(vol)generally exhibits a low flame temperature in a low-level oxygen enrichment atmosphere under Claus conditions,resulting in flame insta...Normal diffusion flame(NDF)of acid gas with a H_(2)S concentration below 50.0%(vol)generally exhibits a low flame temperature in a low-level oxygen enrichment atmosphere under Claus conditions,resulting in flame instability.This research proposed that inverse diffusion flame(IDF)was applied to acid gas combustion for enhancing flame temperature.IDF of acid gas was compared with fuel gas cocombustion(FGC),split flow of acid gas(SFAG)and high-level oxygen enrichment combustion(OEC).Additionally,the effect of CO_(2)addition on the IDF of H_(2)S was investigated.The results indicated that a stable flame could be observed in the IDF of acid gas,its peak flame temperature was about 801.0 K,which was higher than that in the OEC,FGC and SFAG with a value of about 591.0,684.0 and 734.0 K,respectively.IDF of acid gas was contributed to the formation of sulfur and H_(2),and mainly involved the oxidation zone and the chemical decomposition and oxidation zone in sequence.In the IDF,CO_(2)exhibited a better oxidation performance,and the peak flame temperature was decreased by about 21.0 K with an increase in CO_(2)addition from 50.8%to 59.5%(vol),whereas significantly enhanced the oxidation reaction rate of H_(2)S,and the peak volume fraction of SO_(2)was increased from 5.812%to 7.075%.The application of IDF to acid gas combustion achieved the objective for improving flame temperature in low-level oxygen enrichment atmosphere under Claus conditions,providing a new perspective in the sulfur recovery and hydrogen production from acid gas.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
Electrically controlled solid propellant(ECSP)offers multiple ignition and adjustable burning rate,serving as fuel for next-generation intelligent propulsion systems.To further enhance the combustion performance of EC...Electrically controlled solid propellant(ECSP)offers multiple ignition and adjustable burning rate,serving as fuel for next-generation intelligent propulsion systems.To further enhance the combustion performance of ECSP,a method utilizing electrochemical and thermal decomposition catalysts has been proposed.In this work,we investigated the combustion characteristics of hydroxylamine nitrate(HAN)-based ECSP incorporating cerium oxide(CeO_(2))and graphene oxide(GO)by using an electrically controlled combustion test system.Electrochemical impedance spectroscopy(EIS)and linear sweep voltammetry(LSV)were used to measure the electrical conductibility and overpotential of ECSP with various additives,and Tafel curves were calculated.Thermogravimetric analysis coupled with differential scanning calorimetry(TG-DSC)was employed to investigate the thermal decomposition behavior of ECSP.While the addition of CeO_(2) and GO reduced the conductivity of ECSP,both catalysts exhibited strong electrocatalytic properties and facilitated the thermal decomposition of ECSP.Between two catalysts,GO demonstrated superior electrochemical catalytic performance but weaker thermal decomposition catalytic ability than CeO_(2).The addition of catalysts significantly enhanced the combustion performance of HAN-based ECSP.Specifically,the ignition delay time was shortened by 10%~20%.CeO_(2) raised the burning rate by approximately 20%but GO exhibited a remarkable boost of 40%in burning rate at high voltage.The combination of GO and PVA produced a flame-retardant substance that negatively impacted the ignition delay of ECSP and resulted in a smaller increase in the burning rate of ECSP at low ignition voltages.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
Coal cinder is an abundant byproduct of the extensive consumption of coal in industrial production and daily life.Making full use of the cinder is conducive to a low-carbon economy.In this study,inspired by the burnin...Coal cinder is an abundant byproduct of the extensive consumption of coal in industrial production and daily life.Making full use of the cinder is conducive to a low-carbon economy.In this study,inspired by the burning of coal,a new method for constructing a silica-based composite porous material(SiO_(2)-CPM)was developed by combusting a siloxane-modified anthracite coal gel(CSiO_(2) gel).During this process,the combustion product was directly converted into a porous material,and the calorific value of the coal remained nearly unchanged(~98%of the original calorific value was retained),demonstrating the viability of this method for energy-efficient applications.The SiO_(2)-CPM exhibited an ultra-low thermal conductivity(0.036 W/(m·K)at room temperature),outperforming conventional insulation materials(e.g.,cotton~0.05 W/(m·K)).Additionally,it showed enhanced mechanical strength(fracture stress of 41.8 kPa)compared to the powder state of the coal cinder.Experimental results indicate that the amount of siloxane,structure-directing agent,and an acidic environment were critical for mechanical enhancement.The SiO_(2)-CPM showed good dimensional stability against thermal expansion and exhibited excellent thermal insulation and fire resistance even at 900℃.Meanwhile,the SiO_(2)-CPM with complex geometry could be easily fabricated using this method owing to the excellent shaping ability of the CSiO_(2) gel.Compared to conventional methods such as sol-gel synthesis or freeze-drying,this approach for fabricating SiO_(2)-CPM is simpler and cost-effective and allows the direct utilization of coal cinder post-combustion.展开更多
High-entropy oxides(HEOs)derive their exceptional properties from the atomic-level homogenization of multiple constituent elements within the crystal lattice,which induces a sophisticated local environment that fundam...High-entropy oxides(HEOs)derive their exceptional properties from the atomic-level homogenization of multiple constituent elements within the crystal lattice,which induces a sophisticated local environment that fundamentally reconfigures electron density distributions and coordination environment at active sites.However,the mechanisms by which multi-component systems in HEOs precisely regulate high-activity catalytic sites remain poorly understood.This work addresses this gap by designing medium-entropy perovskite oxides through the strategic incorporation of transition metals with distinct electronegativities and ionic radii,aiming to unravel how local environmental modifications impact the energy band location,coordination states,and adsorption behavior of the Co site.A family of A_(4)BO_(4)-type medium-entropy oxides PrSr(Fe_(0.2)Co_(0.2)Ni_(0.2)Cu_(0.2)M_(0.2))O_(4)(M=Sc,Cr,Mn)was successfully synthesized.Divergent atomic properties among Sc,Cr,and Mn(electronegativity,ionic size,and metal-oxygen bond strength)triggered pronounced electron redistribution,effectively tuning the d-band center of Co.Remarkably,Cr substitution significantly enhanced O_(4) adsorption at Co-active sites,as indicated by an elongated O-O bond length(1.234Å→1.279Å).Concurrently,Cr doping destabilized the M'-O-Cr bonds(M'=Fe,Co,Ni,Cu)and lowered the thermodynamic barrier for oxygen vacancy formation.Electrochemical tests revealed that PrSr(Fe_(0.2)Co_(0.2)Ni_(0.2)Cu_(0.2)Cr_(0.2))O_(4)(PSMO-Cr)exhibited the highest electrical conductivity and fastest oxygen surface exchange kinetics.At 700℃,the area-specific resistance(ASR)of the PSMO-Cr cathode was 0.07Ωcm^(2).Corresponding fuel cells achieved a maximum power density of 0.76 W cm^(-2).In electrolysis mode,the maximum current density reached 0.56 A cm^(-2) under 1.3 V at 700℃using PSMO-Cr as the anode.These results demonstrate that PSMO-Cr is a promising bifunctional catalyst for energy conversion applications.展开更多
Magnetic field-driven spin polarization modulation has emerged as an effective way to boost the electrocatalytic oxygen evolution reaction(OER).However,the correlation among catalyst structure,magnetic property,and ma...Magnetic field-driven spin polarization modulation has emerged as an effective way to boost the electrocatalytic oxygen evolution reaction(OER).However,the correlation among catalyst structure,magnetic property,and magnetic field enhanced-electrochemical activity remains to be fully elucidated.Herein,single-domain CoFe_(2)O_(4) catalysts with tunable oxygen vacancies(CFO-V_(O)) were synthesized to probe how V_(O) mediates magnetism and OER activity under magnetic field.The introduction of V_(O) can simultaneously modulate saturation magnetization(M_(s)) and coercivity(H_(c)),where the increased M_(s) dominates the magnetic field-enhanced OER activity.Under a 14,000 G magnetic field,the optimized CFO-V_(O) exhibits up to 16.1 % reduction in overpotential and 365 % enhancement in magnetocurrent(MC).Electrochemical analyses and post-OER characterization reveal that the magnetic field synergistically improves OER kinetics through lattice distortion induction,magnetohydrodynamic effect,and spin charge transfer effect.Importantly,the magnetic field promotes additional Co^(3+) generation to compensate for charge imbalance caused by V_(O) filling,maintaining dynamic equilibrium of V_(O) and effective reactant adsorption-conversion processes.This work unveils the synergistic mechanism of V_(O) and magnetic parameters for enhancing OER performance under the magnetic field,providing new insights into the design of high-efficiency spinregulated OER catalysts.展开更多
Silica nanoparticles-stabilized cobalt and nitrogen-doped carbon materials were synthesized through pyrolysis of metal-organic-framework of ZIF-67 supported by silica nanoparticles.The experimental results reveal that...Silica nanoparticles-stabilized cobalt and nitrogen-doped carbon materials were synthesized through pyrolysis of metal-organic-framework of ZIF-67 supported by silica nanoparticles.The experimental results reveal that the introduction of the silica nanoparticles can stabilize the microstructure of the derived CoN-C materials,which in turn exhibits the promising electrocatalytic activity towards both oxygen reduction and oxygen evolution reactions.The optimized sample exhibits a better oxygen reduction activity than commercial Pt/C catalyst as confirmed by the positive shift of half-wave potential by 20 mV while it has a low overpotential of 273 mV for oxygen evolution reactions with the retained performance over 80%after 25,000 s of continuous operation.It is demonstrated that the introduction of support frame might be an effective way to improve the activity and stability of metal-organic-framework derived electrocatalyst with stabilized microstructure.展开更多
In composite solid propellants with high aluminum(Al)content and low burning rate,incomplete combustion of the Al powder may occur.In this study,varying lithium(Li)content in Al-Li alloy powder was utilized instead of...In composite solid propellants with high aluminum(Al)content and low burning rate,incomplete combustion of the Al powder may occur.In this study,varying lithium(Li)content in Al-Li alloy powder was utilized instead of pure aluminum particles to mitigate agglomeration and enhance the combustion efficiency of solid propellants(Combustion efficiency herein refers to the completeness of metallic fuel oxidation,quantified as the ratio of actual-to-theoretical energy released during combustion)with high Al content and low burning rates.The impact of Al-Li alloy with different Li contents on combustion and agglomeration of solid propellant was investigated using explosion heat,combustion heat,differential thermal analysis(DTA),thermos-gravimetric analysis(TG),dynamic high-pressure combustion test,ignition experiment of small solid rocket motor(SRM)tests,condensation combustion product collection,and X-ray diffraction techniques(XRD).Compared with pure Al,Al-Li alloys exhibit higher combustion heat,which contributes to improved combustion efficiency in Al-Li alloy-containing propellants.DTA and TG analyses demonstrated higher reactivity and lower ignition temperatures for Al-Li alloys.High-pressure combustion experiments at 5 MPa showed that Al-Li alloy fuel significantly decreases combustion agglomeration.The results from theφ75 mm andφ165 mm SRM and XRD tests further support this finding.This study provides novel insights into the combustion and agglomeration behaviors of high-Al,low-burning-rate composite solid propellants and supports the potential application of Al-Li alloys in advanced propellant formulations.展开更多
This paper investigates the reliability of internal marine combustion engines using an integrated approach that combines Fault Tree Analysis(FTA)and Bayesian Networks(BN).FTA provides a structured,top-down method for ...This paper investigates the reliability of internal marine combustion engines using an integrated approach that combines Fault Tree Analysis(FTA)and Bayesian Networks(BN).FTA provides a structured,top-down method for identifying critical failure modes and their root causes,while BN introduces flexibility in probabilistic reasoning,enabling dynamic updates based on new evidence.This dual methodology overcomes the limitations of static FTA models,offering a comprehensive framework for system reliability analysis.Critical failures,including External Leakage(ELU),Failure to Start(FTS),and Overheating(OHE),were identified as key risks.By incorporating redundancy into high-risk components such as pumps and batteries,the likelihood of these failures was significantly reduced.For instance,redundant pumps reduced the probability of ELU by 31.88%,while additional batteries decreased the occurrence of FTS by 36.45%.The results underscore the practical benefits of combining FTA and BN for enhancing system reliability,particularly in maritime applications where operational safety and efficiency are critical.This research provides valuable insights for maintenance planning and highlights the importance of redundancy in critical systems,especially as the industry transitions toward more autonomous vessels.展开更多
Al/NH_(4)CoF_(3)-Φ(Φ=0.5,1.0,1.5,2.0,and 3.0)binary composites and Al-NH_(4)CoF_(3)@P(VDF-HFP)ternary composites are fabricated via ultrasonication-assisted blending and electrostatic spraying.The effect of equivale...Al/NH_(4)CoF_(3)-Φ(Φ=0.5,1.0,1.5,2.0,and 3.0)binary composites and Al-NH_(4)CoF_(3)@P(VDF-HFP)ternary composites are fabricated via ultrasonication-assisted blending and electrostatic spraying.The effect of equivalence ratio(Φ)on the reaction properties is systematically investigated in the binary Al/NH_(4)CoF_(3)system.For ternary systems,electrostatic spraying allows both components to be efficiently encapsulated by P(VDF-HFP)and to achieve structural stabilization and enhanced reactivity through synergistic interfacial interactions.Morphological analysis using SEM/TEM revealed that P(VDF-HFP)formed a protective layer on Al and NH_(4)CoF_(3)particles,improving dispersion,hydrophobicity(water contact angle increased by 80.5%compared to physically mixed composites),and corrosion resistance.Thermal decomposition of NH_(4)CoF_(3)occurred at 265℃,releasing NH_(3)and HF,which triggered exothermic reactions with Al.The ternary composites exhibited a narrowed main reaction temperature range and concentrated heat release,attributed to improved interfacial contact and polymer decomposition.Combustion tests demonstrated that Al-NH_(4)CoF_(3)@P(VDF-HFP)achieved self-sustaining combustion.In addition,a simple validation was done by replacing the Al component in the aluminium-containing propellant,demonstrating its potential application in the propellant field.This work establishes a novel strategy for designing stable,high-energy composites with potential applications in advanced propulsion systems.展开更多
Early prevention and control of coal spontaneous combustion have emerged as a critical research area in coal mine safety.Due to their sustainability and environmental friendliness,microorganisms have gained attention....Early prevention and control of coal spontaneous combustion have emerged as a critical research area in coal mine safety.Due to their sustainability and environmental friendliness,microorganisms have gained attention.A filamentous fungus was collected in the coal mine and identified as Absidia spinosa.Results indicated that the mycelium effectively covered and repaired many coal pores.The oxygen consumption ratio of A.spinosa was higher in coal-containing environments than in coal-free conditions.The fungus significantly impacted aliphatic functional groups,disrupting bridging bonds and side chains connected to aromatic structures and reducing the relative content of C—O bonds.Additionally,A.spinosa increases the ignition temperature by 25.34℃.The total heat release was decreased by approximately 32.58%,and the activation energies were increased.The genome of Absidia spinosa revealed genes related to oxygen consumption,small molecule degradation,and secretion of metabolic products,such as those annotated under GO ID:0140657,etc.The pathways involved in the degradation of small organic molecules(e.g.,ko00626,etc.),carbon fixation,and nitrogen cycling,all linked to coal decomposition.Through oxygen consumption and the alteration of coal-active structures,A.spinosa effectively inhibits CSC,providing an experimental basis for exploring eco-friendly biological control methods in the goaf.展开更多
Naphthalene,anthracene and pyridone endoperoxides are known to thermally release singlet oxygen.However,in the cycloreversion reaction,singlet oxygen is produced stoichiometrically;therefore,multiple singlet oxygen re...Naphthalene,anthracene and pyridone endoperoxides are known to thermally release singlet oxygen.However,in the cycloreversion reaction,singlet oxygen is produced stoichiometrically;therefore,multiple singlet oxygen releasing modules are expected to be very useful in inducing apoptosis of cancer cells.Herein,we present a potential therapeutic agent presenting three-pyridone endoperoxide modules and a mitochondria targeting group.Compared to previously reported pyridone-based monofunctional endoperoxides,the triple endoperoxide is highly effective as evidenced by assays and fluorescence microscopy.展开更多
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.
文摘Effective lattice oxygen(Olatt)activation at low temperatures has long been a challenge in catalytic oxidation reactions.Traditional thermal catalytic soot combustion,even with Pt/Pd catalysts,is inefficient at exhaust temperatures below 200℃,particularly under conditions of frequent idling.Herein,we report an effective strategy utilizing non-thermal plasma(NTP)to activate Olatt in Ce_(1–x)Co_(x)O_(2–δ)catalysts,achieving dramatic enhancement of the soot combustion rate at low temperatures.At 200℃ and 4.3 W(discharge power,P_(dis)),NTP-Ce_(0.8)Co_(0.2)O_(2–δ)achieved 96.9%soot conversion(X_(C)),99.0%CO_(2) selectivity(S(CO_(2)))and a maximum energy conversion efficiency(Emax)of 14.7 g kWh^(–1).Compared with previously reported results,NTP-Ce_(0.8)Co_(0.2)O_(2–δ)exhibits the highest S(CO_(2))and Emax values.Remarkably,even without heating,X_(C),Emax,and S(CO_(2))reached 92.1%,6.1 g kWh–1,and 97.5%,respectively,at 6.3 W(P_(dis)).The results of characterization and theoretical calculation demonstrated that Co dopes into the CeO_(2) crystal lattice and forms an asymmetric Ce–O–Co structure,making oxygen“easy come,easy go”,thereby enabling the rapid combustion of soot over NTP-Ce_(0.8)Co_(0.2)O_(2–δ).This study highlights the great potential of NTP for activating Olatt and provides valuable insights into the design of efficient NTP-adapted catalysts for oxidation reactions.
基金Supported by the Shanghai Rising Star Program (Grant No. 21QB1403900)the Shanghai Municipal Commission of Science and Technology (Grant No. 22170712600)。
文摘Knowing the optimal operating parameters of Stirling engines is important for efficient combustion through adaptability to changed pressures and oxygen atmospheres. In this study, the optimum operating conditions for efficient combustion in a singular Stirling engine combustor at different oxygen atmospheres were investigated and determined. Numerical simulations were performed to investigate the effects of ejection ratio and pressure on combustion performance. In an oxygen/carbon dioxide atmosphere, the results show that increasing the ejection ratio substantially alters the flame distribution in the Stirling engine combustor, increasing heat transfer and external combustion efficiency. In contrast, increasing the ejection ratio reduces the average and maximum temperatures of the Stirling engine combustor. Increased pressure affects the flame distribution in the Stirling engine combustor and impedes the flow and convective heat transfer in the combustor, reducing the overall external combustion efficiency at pressures above 6.5 MPa. In an air/carbon dioxide atmosphere, an increased ejection ratio reduces the average and maximum temperatures in the Stirling engine combustor. However, the overall flame distribution does not change substantially. The external combustion efficiency tends to increase and then decrease because of two opposing factors: the increase in the convective heat transfer coefficient and the decrease in the temperature difference. Increasing pressure inhibits forced convection heat transfer in the Stirling engine combustor, reducing external combustion efficiency, which drops from 78% to 65% when pressure increases from 0.2 MPa to 0.5 MPa.
基金fnancially supported by the Open Research Fund Program of Anhui Provincial Institute of Modern Coal Processing Technology,Anhui University of Science and Technology (MTY202201)。
文摘Coal-direct chemical looping(CDCL) is a promising CO_(2) capture technology with low costs.Potassium modification can significantly enhance the reactivity of iron-based oxygen carriers and coal.However,potassium loss causes a decline in cyclic stability.To address this,we prepared a potassium hexatitanate-modified iron-based OC and conducted CDCL experiments in a fixed-bed reactor using Zhundong coal coke as fuel.The study examined the impact of potassium hexatitanate on carbon conversion,OC activity stability,and potassium maintenance.Additionally,Fact Sage was used to calculate potassium fugacity patterns at different temperatures,Fe_(2)O_(3)/C molar ratios,and OC reduction degrees.Results showed that potassium hexatitanate increased carbon conversion,achieving 50%conversion at 40% potassium addition.In multi-cycle tests,carbon conversion rose with increased cycle times,reaching 84%.This improvement is attributed to ion exchange between Fe^(3+) and Ti^(4+),which induces lattice distortion and creates oxygen vacancies,enhancing OC reactivity.Potassium content remained stable during multi-cycle tests,indicating the effective potassium retention capacity of potassium hexatitanate.
基金supported by the National Natural Science Foundation of China(22076176,22276106)the Natural Science Foundation of Shandong Province(ZR2021YQ14)+3 种基金the Innovation Ability Improvement Project for Technology-based Small-and Medium-sized Enterprises of Shandong Province(2022TSGC1345)Jiangsu Province Science and Technology Plan Special Fund(BZ2022053)Key Research and Development Program of Anhui Province(202104g01020006)the Fundamental Research Funds for the Central Universities(202141008)。
文摘Catalyzed gasoline particulate filters(cGPFs)are being developed to enable compliance with the particulate number limits for passenger cars equipped with gasoline direct injection(GDI)engines in China and Europe,It is appealing to build catalysts with ceria—an irreplaceable"reducible"component in three-way converters—to help eliminate the soot particles trapped in cGPFs via O_(2)-assisted combustion.While research aiming at understanding how these recipes function has continued for more than two decades,a universal model elucidating the roles of different"active oxygen"species is yet to be realized.In this perspective,by critically assessing the reported data about gasoline soot catalytic combustion over ceria catalysts,it is suggested that ceria ignites soot through contributing its lattice oxygen,giving rise to a"hot ring"region at the periphery of soot-catalyst interface.During the"re-oxidation"semi-cycles,electrophilic superoxides and/or peroxides(O_(x)^(n-))are produced at the Ce^(3+)and oxygen vacancy sites enriched in this collar-like region,and then work as key reactive phases for soot deep oxidation.Based on this"O_(x)^(n-)assisted"Mars-van Krevelen mechanism,several guidelines for ceria catalyst designing are proposed,ending with a summary about where future opportunities and challenges may lie in developing efficient and practical cGPF catalysts.
基金supported by the National Natural Science Foundation of China(22178114,U23A20131)the social development science and technology tackling project of 2021"Scientific and Innovative Action Plan of Shanghai"(21DZ1209000)。
文摘Normal diffusion flame(NDF)of acid gas with a H_(2)S concentration below 50.0%(vol)generally exhibits a low flame temperature in a low-level oxygen enrichment atmosphere under Claus conditions,resulting in flame instability.This research proposed that inverse diffusion flame(IDF)was applied to acid gas combustion for enhancing flame temperature.IDF of acid gas was compared with fuel gas cocombustion(FGC),split flow of acid gas(SFAG)and high-level oxygen enrichment combustion(OEC).Additionally,the effect of CO_(2)addition on the IDF of H_(2)S was investigated.The results indicated that a stable flame could be observed in the IDF of acid gas,its peak flame temperature was about 801.0 K,which was higher than that in the OEC,FGC and SFAG with a value of about 591.0,684.0 and 734.0 K,respectively.IDF of acid gas was contributed to the formation of sulfur and H_(2),and mainly involved the oxidation zone and the chemical decomposition and oxidation zone in sequence.In the IDF,CO_(2)exhibited a better oxidation performance,and the peak flame temperature was decreased by about 21.0 K with an increase in CO_(2)addition from 50.8%to 59.5%(vol),whereas significantly enhanced the oxidation reaction rate of H_(2)S,and the peak volume fraction of SO_(2)was increased from 5.812%to 7.075%.The application of IDF to acid gas combustion achieved the objective for improving flame temperature in low-level oxygen enrichment atmosphere under Claus conditions,providing a new perspective in the sulfur recovery and hydrogen production from acid gas.
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supported by the National Natural Science Foundation of China(Grant No.12074187).
文摘Electrically controlled solid propellant(ECSP)offers multiple ignition and adjustable burning rate,serving as fuel for next-generation intelligent propulsion systems.To further enhance the combustion performance of ECSP,a method utilizing electrochemical and thermal decomposition catalysts has been proposed.In this work,we investigated the combustion characteristics of hydroxylamine nitrate(HAN)-based ECSP incorporating cerium oxide(CeO_(2))and graphene oxide(GO)by using an electrically controlled combustion test system.Electrochemical impedance spectroscopy(EIS)and linear sweep voltammetry(LSV)were used to measure the electrical conductibility and overpotential of ECSP with various additives,and Tafel curves were calculated.Thermogravimetric analysis coupled with differential scanning calorimetry(TG-DSC)was employed to investigate the thermal decomposition behavior of ECSP.While the addition of CeO_(2) and GO reduced the conductivity of ECSP,both catalysts exhibited strong electrocatalytic properties and facilitated the thermal decomposition of ECSP.Between two catalysts,GO demonstrated superior electrochemical catalytic performance but weaker thermal decomposition catalytic ability than CeO_(2).The addition of catalysts significantly enhanced the combustion performance of HAN-based ECSP.Specifically,the ignition delay time was shortened by 10%~20%.CeO_(2) raised the burning rate by approximately 20%but GO exhibited a remarkable boost of 40%in burning rate at high voltage.The combination of GO and PVA produced a flame-retardant substance that negatively impacted the ignition delay of ECSP and resulted in a smaller increase in the burning rate of ECSP at low ignition voltages.
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supported by the National Natural Science Foundation of China(No.52573220)the National Key R&D Program of China(No.2023YFC3404201)+1 种基金the Fundamental Research Funds for the Central Universities(No.FRF-IDRY-GD24-005)the State Key Laboratory of Solid Waste Reuse for Building Materials(No.SWR-2022-009).
文摘Coal cinder is an abundant byproduct of the extensive consumption of coal in industrial production and daily life.Making full use of the cinder is conducive to a low-carbon economy.In this study,inspired by the burning of coal,a new method for constructing a silica-based composite porous material(SiO_(2)-CPM)was developed by combusting a siloxane-modified anthracite coal gel(CSiO_(2) gel).During this process,the combustion product was directly converted into a porous material,and the calorific value of the coal remained nearly unchanged(~98%of the original calorific value was retained),demonstrating the viability of this method for energy-efficient applications.The SiO_(2)-CPM exhibited an ultra-low thermal conductivity(0.036 W/(m·K)at room temperature),outperforming conventional insulation materials(e.g.,cotton~0.05 W/(m·K)).Additionally,it showed enhanced mechanical strength(fracture stress of 41.8 kPa)compared to the powder state of the coal cinder.Experimental results indicate that the amount of siloxane,structure-directing agent,and an acidic environment were critical for mechanical enhancement.The SiO_(2)-CPM showed good dimensional stability against thermal expansion and exhibited excellent thermal insulation and fire resistance even at 900℃.Meanwhile,the SiO_(2)-CPM with complex geometry could be easily fabricated using this method owing to the excellent shaping ability of the CSiO_(2) gel.Compared to conventional methods such as sol-gel synthesis or freeze-drying,this approach for fabricating SiO_(2)-CPM is simpler and cost-effective and allows the direct utilization of coal cinder post-combustion.
基金supported by the National Natural Science Foundation of China(51872078,52272197,52572219)Heilongjiang Provincial Natural Science Foundation of China(LH2024E106)。
文摘High-entropy oxides(HEOs)derive their exceptional properties from the atomic-level homogenization of multiple constituent elements within the crystal lattice,which induces a sophisticated local environment that fundamentally reconfigures electron density distributions and coordination environment at active sites.However,the mechanisms by which multi-component systems in HEOs precisely regulate high-activity catalytic sites remain poorly understood.This work addresses this gap by designing medium-entropy perovskite oxides through the strategic incorporation of transition metals with distinct electronegativities and ionic radii,aiming to unravel how local environmental modifications impact the energy band location,coordination states,and adsorption behavior of the Co site.A family of A_(4)BO_(4)-type medium-entropy oxides PrSr(Fe_(0.2)Co_(0.2)Ni_(0.2)Cu_(0.2)M_(0.2))O_(4)(M=Sc,Cr,Mn)was successfully synthesized.Divergent atomic properties among Sc,Cr,and Mn(electronegativity,ionic size,and metal-oxygen bond strength)triggered pronounced electron redistribution,effectively tuning the d-band center of Co.Remarkably,Cr substitution significantly enhanced O_(4) adsorption at Co-active sites,as indicated by an elongated O-O bond length(1.234Å→1.279Å).Concurrently,Cr doping destabilized the M'-O-Cr bonds(M'=Fe,Co,Ni,Cu)and lowered the thermodynamic barrier for oxygen vacancy formation.Electrochemical tests revealed that PrSr(Fe_(0.2)Co_(0.2)Ni_(0.2)Cu_(0.2)Cr_(0.2))O_(4)(PSMO-Cr)exhibited the highest electrical conductivity and fastest oxygen surface exchange kinetics.At 700℃,the area-specific resistance(ASR)of the PSMO-Cr cathode was 0.07Ωcm^(2).Corresponding fuel cells achieved a maximum power density of 0.76 W cm^(-2).In electrolysis mode,the maximum current density reached 0.56 A cm^(-2) under 1.3 V at 700℃using PSMO-Cr as the anode.These results demonstrate that PSMO-Cr is a promising bifunctional catalyst for energy conversion applications.
基金supported by the “Climbing Plan” of Harbin Normal University (No.XKB202301)National Natural Science Foundation of China (Nos.21871065 and 22071038)。
文摘Magnetic field-driven spin polarization modulation has emerged as an effective way to boost the electrocatalytic oxygen evolution reaction(OER).However,the correlation among catalyst structure,magnetic property,and magnetic field enhanced-electrochemical activity remains to be fully elucidated.Herein,single-domain CoFe_(2)O_(4) catalysts with tunable oxygen vacancies(CFO-V_(O)) were synthesized to probe how V_(O) mediates magnetism and OER activity under magnetic field.The introduction of V_(O) can simultaneously modulate saturation magnetization(M_(s)) and coercivity(H_(c)),where the increased M_(s) dominates the magnetic field-enhanced OER activity.Under a 14,000 G magnetic field,the optimized CFO-V_(O) exhibits up to 16.1 % reduction in overpotential and 365 % enhancement in magnetocurrent(MC).Electrochemical analyses and post-OER characterization reveal that the magnetic field synergistically improves OER kinetics through lattice distortion induction,magnetohydrodynamic effect,and spin charge transfer effect.Importantly,the magnetic field promotes additional Co^(3+) generation to compensate for charge imbalance caused by V_(O) filling,maintaining dynamic equilibrium of V_(O) and effective reactant adsorption-conversion processes.This work unveils the synergistic mechanism of V_(O) and magnetic parameters for enhancing OER performance under the magnetic field,providing new insights into the design of high-efficiency spinregulated OER catalysts.
基金Funded by the National Natural Science Foundation of China Guangdong(No.22279096)。
文摘Silica nanoparticles-stabilized cobalt and nitrogen-doped carbon materials were synthesized through pyrolysis of metal-organic-framework of ZIF-67 supported by silica nanoparticles.The experimental results reveal that the introduction of the silica nanoparticles can stabilize the microstructure of the derived CoN-C materials,which in turn exhibits the promising electrocatalytic activity towards both oxygen reduction and oxygen evolution reactions.The optimized sample exhibits a better oxygen reduction activity than commercial Pt/C catalyst as confirmed by the positive shift of half-wave potential by 20 mV while it has a low overpotential of 273 mV for oxygen evolution reactions with the retained performance over 80%after 25,000 s of continuous operation.It is demonstrated that the introduction of support frame might be an effective way to improve the activity and stability of metal-organic-framework derived electrocatalyst with stabilized microstructure.
基金the National Natural Science Foundation of China(Grant No.U2441263)for financial support of this work。
文摘In composite solid propellants with high aluminum(Al)content and low burning rate,incomplete combustion of the Al powder may occur.In this study,varying lithium(Li)content in Al-Li alloy powder was utilized instead of pure aluminum particles to mitigate agglomeration and enhance the combustion efficiency of solid propellants(Combustion efficiency herein refers to the completeness of metallic fuel oxidation,quantified as the ratio of actual-to-theoretical energy released during combustion)with high Al content and low burning rates.The impact of Al-Li alloy with different Li contents on combustion and agglomeration of solid propellant was investigated using explosion heat,combustion heat,differential thermal analysis(DTA),thermos-gravimetric analysis(TG),dynamic high-pressure combustion test,ignition experiment of small solid rocket motor(SRM)tests,condensation combustion product collection,and X-ray diffraction techniques(XRD).Compared with pure Al,Al-Li alloys exhibit higher combustion heat,which contributes to improved combustion efficiency in Al-Li alloy-containing propellants.DTA and TG analyses demonstrated higher reactivity and lower ignition temperatures for Al-Li alloys.High-pressure combustion experiments at 5 MPa showed that Al-Li alloy fuel significantly decreases combustion agglomeration.The results from theφ75 mm andφ165 mm SRM and XRD tests further support this finding.This study provides novel insights into the combustion and agglomeration behaviors of high-Al,low-burning-rate composite solid propellants and supports the potential application of Al-Li alloys in advanced propellant formulations.
基金supported by Istanbul Technical University(Project No.45698)supported through the“Young Researchers’Career Development Project-training of doctoral students”of the Croatian Science Foundation.
文摘This paper investigates the reliability of internal marine combustion engines using an integrated approach that combines Fault Tree Analysis(FTA)and Bayesian Networks(BN).FTA provides a structured,top-down method for identifying critical failure modes and their root causes,while BN introduces flexibility in probabilistic reasoning,enabling dynamic updates based on new evidence.This dual methodology overcomes the limitations of static FTA models,offering a comprehensive framework for system reliability analysis.Critical failures,including External Leakage(ELU),Failure to Start(FTS),and Overheating(OHE),were identified as key risks.By incorporating redundancy into high-risk components such as pumps and batteries,the likelihood of these failures was significantly reduced.For instance,redundant pumps reduced the probability of ELU by 31.88%,while additional batteries decreased the occurrence of FTS by 36.45%.The results underscore the practical benefits of combining FTA and BN for enhancing system reliability,particularly in maritime applications where operational safety and efficiency are critical.This research provides valuable insights for maintenance planning and highlights the importance of redundancy in critical systems,especially as the industry transitions toward more autonomous vessels.
基金supported by the National Natural Science Foundation of China(No.51706105)。
文摘Al/NH_(4)CoF_(3)-Φ(Φ=0.5,1.0,1.5,2.0,and 3.0)binary composites and Al-NH_(4)CoF_(3)@P(VDF-HFP)ternary composites are fabricated via ultrasonication-assisted blending and electrostatic spraying.The effect of equivalence ratio(Φ)on the reaction properties is systematically investigated in the binary Al/NH_(4)CoF_(3)system.For ternary systems,electrostatic spraying allows both components to be efficiently encapsulated by P(VDF-HFP)and to achieve structural stabilization and enhanced reactivity through synergistic interfacial interactions.Morphological analysis using SEM/TEM revealed that P(VDF-HFP)formed a protective layer on Al and NH_(4)CoF_(3)particles,improving dispersion,hydrophobicity(water contact angle increased by 80.5%compared to physically mixed composites),and corrosion resistance.Thermal decomposition of NH_(4)CoF_(3)occurred at 265℃,releasing NH_(3)and HF,which triggered exothermic reactions with Al.The ternary composites exhibited a narrowed main reaction temperature range and concentrated heat release,attributed to improved interfacial contact and polymer decomposition.Combustion tests demonstrated that Al-NH_(4)CoF_(3)@P(VDF-HFP)achieved self-sustaining combustion.In addition,a simple validation was done by replacing the Al component in the aluminium-containing propellant,demonstrating its potential application in the propellant field.This work establishes a novel strategy for designing stable,high-energy composites with potential applications in advanced propulsion systems.
基金supported by the National Natural Science Foundation of China(No.51974128)the National Key Research and Development Program of China(No.2023YFC3009105)。
文摘Early prevention and control of coal spontaneous combustion have emerged as a critical research area in coal mine safety.Due to their sustainability and environmental friendliness,microorganisms have gained attention.A filamentous fungus was collected in the coal mine and identified as Absidia spinosa.Results indicated that the mycelium effectively covered and repaired many coal pores.The oxygen consumption ratio of A.spinosa was higher in coal-containing environments than in coal-free conditions.The fungus significantly impacted aliphatic functional groups,disrupting bridging bonds and side chains connected to aromatic structures and reducing the relative content of C—O bonds.Additionally,A.spinosa increases the ignition temperature by 25.34℃.The total heat release was decreased by approximately 32.58%,and the activation energies were increased.The genome of Absidia spinosa revealed genes related to oxygen consumption,small molecule degradation,and secretion of metabolic products,such as those annotated under GO ID:0140657,etc.The pathways involved in the degradation of small organic molecules(e.g.,ko00626,etc.),carbon fixation,and nitrogen cycling,all linked to coal decomposition.Through oxygen consumption and the alteration of coal-active structures,A.spinosa effectively inhibits CSC,providing an experimental basis for exploring eco-friendly biological control methods in the goaf.
基金supported by the National Natural Science Foundation of China(22007008,22178048).
文摘Naphthalene,anthracene and pyridone endoperoxides are known to thermally release singlet oxygen.However,in the cycloreversion reaction,singlet oxygen is produced stoichiometrically;therefore,multiple singlet oxygen releasing modules are expected to be very useful in inducing apoptosis of cancer cells.Herein,we present a potential therapeutic agent presenting three-pyridone endoperoxide modules and a mitochondria targeting group.Compared to previously reported pyridone-based monofunctional endoperoxides,the triple endoperoxide is highly effective as evidenced by assays and fluorescence microscopy.
