To mitigate the impact of interdiffusion reactions between the silicide slurry and Ta12W alloy substrate during vacuum sintering process on the oxidation resistance of the silicide coating,a micro-arc oxidation pretre...To mitigate the impact of interdiffusion reactions between the silicide slurry and Ta12W alloy substrate during vacuum sintering process on the oxidation resistance of the silicide coating,a micro-arc oxidation pretreatment was employed to construct a Ta_(2)O_(5)ceramic layer on the Ta12W alloy surface.Subsequently,a slurry spraying-vacuum sintering method was used to prepare a Si-Cr-Ti-Zr coating on the pretreated substrate.Comparative studies were conducted on the microstructure,phase composition,and isothermal oxidation resistance(at 1600℃)of the as-prepared coatings with and without the micro-arc oxidation ceramic layer.The results show that the Ta_(2)O_(5)layer prepared at 400 V is more continuous and has smaller pores than that prepared at 350 V.After microarc oxidation pretreatment,the Si-Cr-Ti-Zr coating on Ta12W alloy consists of three distinct layers:an upper layer dominated by Ti_(5)Si_(3),Ta_(5)Si_(3),and ZrSi;a middle layer dominated by TaSi_(2);a coating/substrate interfacial reaction layer dominated by Ta_(5)Si_(3).Both the Si-Cr-Ti-Zr coatings with and without the Ta_(2)O_(5)ceramic layer do not fail after isothermal oxidation at 1600℃for 5 h.Notably,the addition of the Ta2O5 ceramic layer reduces the high-temperature oxidation rate of the coating.展开更多
It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,...It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,and FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbents were prepared by coupling fly ash-based Si-Al carriers.The active components Fe-Ce-La oxides and Si-Al carriers were characterized by TPD,TG,XRF,BET and XPS,respectively.The effects of temperature,Si/Al ratio and FeCeLaO loading rate on the sulfur resistance were investigated.Results show that the SO_(2) promotes the arsenic removal of Fe_(2)O_(3),CeLaO and FeCeLaO.At 400℃,the arsenic removal efficiencies of the three oxides increase from 45.3%,72.5% and 81.3% without SO_(2) to 62.6%,80.5%and 91.0%,respectively.The SO_(2) inhibits the arsenic removal of La_(2)O_(2)CO_(3) and FeLaO,and the inhibition effect is pronounced at high temperatures.The sulfur poisoning resistance of Si-Al carriers increases with the increase of Si/Al ratio.When the Si/Al ratio is increased to 9.74,the arsenic removal efficiency in the SO_(2) environment is 13.9% higher than that in the absence of SO_(2).Introducing FeCeLaO active components is beneficial for enhancing the SO_(2) poisoning resistance of Si-Al carriers.The strong sulfur resistance of the FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbent results from multiple factors:protective effects of Ce on Fe,La and Al;sulfation-induced generation of Ce^(3+)and surface-adsorbed oxygen;and strong surface acidity of SiO_(2).展开更多
The limited high-temperature oxidation resistance of Mg alloys is a key factor restricting their development and application.The addition of some rare earth elements(REs),owing to their unique physical and chemical pr...The limited high-temperature oxidation resistance of Mg alloys is a key factor restricting their development and application.The addition of some rare earth elements(REs),owing to their unique physical and chemical properties,can significantly enhance the oxidation resistance of Mg alloys.Based on our previous study,we conclude that REs such as Gd,Y,and Ce enhance the oxidation resistance of Mg-RE alloys.This article comprehensively reviews recent research progress on high-temperature oxidation behavior and the potential mechanism in Mg-RE alloys.Based on the thermodynamic and kinetic analyses,the evolution of the complex oxide system formed during the high-temperature oxidation of Mg-RE alloys is first summarized.The diffusion behavior and concentration control mechanisms of REs during the oxidation process and how these mechanisms affect the sustained growth of the oxide film and antioxidant properties were elucidated.Moreover,the different structures of the oxide films were classified,and their properties were discussed.Finally,this paper introduces the applications of commonly used REs in Mg alloys and frontier research on their oxidation mechanisms.Based on the above review,we propose that future research perspectives can be explored in terms of expanding the experimental temperature range for oxidation tests,optimizing the chemical composition by adding trace REs to study their synergistic mechanism,revealing the underlying oxidation mechanism through advanced in situ microscopic characterization methods,and investigating the mechanical properties of oxide films using diverse approaches.展开更多
Platinum group metals have high melting points,strong corrosion resistance,stable chemical properties,and low oxygen permeability in high-temperature oxygen-containing environments.As thermal protective coating materi...Platinum group metals have high melting points,strong corrosion resistance,stable chemical properties,and low oxygen permeability in high-temperature oxygen-containing environments.As thermal protective coating materials,they have gained essential applications in the aerospace field and have excellent prospects for application in frontier military fields,such as protecting hot-end components of hypersonic aircraft.This research reviewed the latest research progress of platinum group metal coatings with hightemperature oxidation resistance,including coating preparation techniques,oxidation failure,and alloying modification.The leading preparation techniques of current platinum group metal coatings were discussed,as well as the advantages and disadvantages of various existing preparation techniques.Besides,the intrinsic properties,failure forms,and failure mechanisms of coatings of single platinum group metal in high-temperature oxygen-containing environments were analyzed.On this basis,the necessity,main methods,and main achievements of alloying modification of platinum group metals were summarized.Finally,the future development of platinum group coatings with high-temperature oxidation resistance was discussed and prospected.展开更多
Peroxymonosulfate(PMS)-based Fenton-like technologies have been increasingly employed in the upgrading of biomass,but they are commonly limited by the trade-off between conversion and selectivity due to the short life...Peroxymonosulfate(PMS)-based Fenton-like technologies have been increasingly employed in the upgrading of biomass,but they are commonly limited by the trade-off between conversion and selectivity due to the short lifetime of reactive oxygen species(ROS)and uncontrollable oxidation pathways.Herein,we show that single-atom Co supported on carbon nitride enables the high-valent-oxo cobalt species(Co(IV)O)mediated oxidation of glucose into value-added products in acetonitrile.This photocatalytic Fenton-like system achieved an overall selectivity of gluconic acid,glucaric acid,arabinose,and formic acid up to 90.3%at glucose conversion of 69.6%,outperforming most of previously reported catalytic systems.The small amount(0.72 wt%)of single-atom Co could not only elevate the optical absorption and the efficiency of photo-generated carriers separation but also induce the efficient generation of Co(IV)O with reduced ROS to enable efficient and selective oxidation.These findings prove the great promise of high-valent metal-oxo species in biomass conversions.展开更多
Nitric oxide(NO)is a key vasodilator that regulates vascular pressure and blood flow.Tibetans have developed a"blunted"mechanism for regulating NO levels at high altitude,with GTP cyclohydrolase 1(GCH1)ident...Nitric oxide(NO)is a key vasodilator that regulates vascular pressure and blood flow.Tibetans have developed a"blunted"mechanism for regulating NO levels at high altitude,with GTP cyclohydrolase 1(GCH1)identified as a key candidate gene.Here,we present comprehensive genetic and functional analyses of GCH1,which exhibits strong Darwinian positive selection in Tibetans.We show that Tibetan-enriched GCH1 variants down-regulate its expression in the blood of Tibetans.Based on this observation,we generate the heterozygous Gch1 knockout(Gch1^(+/-))mouse model to simulate its downregulation in Tibetans.We find that under prolonged hypoxia,the Gch1^(+/-)mice have relatively higher blood NO and blood oxygen saturation levels compared with the wild-type(WT)controls,providing better oxygen supplies to the cardiovascular and pulmonary systems.Markedly,hypoxia-induced cardiac hypertrophy and pulmonary remodeling are significantly attenuated in the Gch1^(^(+/-))mice compared with the WT controls,likely due to the adaptive changes in molecular regulations related to metabolism,inflammation,circadian rhythm,extracellular matrix,and oxidative stress.This study sheds light on the role of GCH1 in regulating blood NO,contributing to the physiological adaptation of the cardiovascular and pulmonary systems in Tibetans at high altitude.展开更多
High-entropy oxides(HEOs)have emerged as a promising class of memristive materials,characterized by entropy-stabilized crystal structures,multivalent cation coordination,and tunable defect landscapes.These intrinsic f...High-entropy oxides(HEOs)have emerged as a promising class of memristive materials,characterized by entropy-stabilized crystal structures,multivalent cation coordination,and tunable defect landscapes.These intrinsic features enable forming-free resistive switching,multilevel conductance modulation,and synaptic plasticity,making HEOs attractive for neuromorphic computing.This review outlines recent progress in HEO-based memristors across materials engineering,switching mechanisms,and synaptic emulation.Particular attention is given to vacancy migration,phase transitions,and valence-state dynamics—mechanisms that underlie the switching behaviors observed in both amorphous and crystalline systems.Their relevance to neuromorphic functions such as short-term plasticity and spike-timing-dependent learning is also examined.While encouraging results have been achieved at the device level,challenges remain in conductance precision,variability control,and scalable integration.Addressing these demands a concerted effort across materials design,interface optimization,and task-aware modeling.With such integration,HEO memristors offer a compelling pathway toward energy-efficient and adaptable brain-inspired electronics.展开更多
The high-temperature compressive deformation behavior of medium manganese steel using a four-roll reversible rolling mill is investigated,revealing the effects of different Mn contents on the thermal deformation behav...The high-temperature compressive deformation behavior of medium manganese steel using a four-roll reversible rolling mill is investigated,revealing the effects of different Mn contents on the thermal deformation behavior of oxidation products in the alloy.It is found that within the experimental temperature range,the higher the deformation temperature,the better the plasticity of the oxidation products.It was observed that increasing the Mn content refines the grains,enhances the deformation ability of the oxidation products,and improves the flatness of the interfaces.Since(Fe,Mn)O has a similar crystal structure to FeO,the addition of Mn refines the grains of(Fe,Mn)O,causing the deformation to be distributed across more grains under the same deformation amount,and thereby improving its plasticity.At the interface between Fe-Mn alloy oxidation products and the matrix,there exists a spinel-phase solid solution,which can deform together with the oxidation products and the matrix at high temperatures.It was found that with increasing the Mn content,the size and number of pores between the spinel phases increased.First-principles simulation calculations were used to verify this,showing that Mn promotes the generation of vacancies.The greater number of pores in the spinel phase can effectively relieve the compressive stress caused by rolling deformation,thereby improving the deformation capability of the oxidation products at the interface.展开更多
The production of vanadium-titanium magnetite(VTM)pellets has the problems of low consolidation strength and high energy consumption in the preheating and roasting process.High-pressure grinding roll(HPGR)pretreatment...The production of vanadium-titanium magnetite(VTM)pellets has the problems of low consolidation strength and high energy consumption in the preheating and roasting process.High-pressure grinding roll(HPGR)pretreatment process was used to increase the fine-grained content and specific surface area of VTM concentrates,to strengthen the oxidation consolidation process of VTM pellets,and oxidation kinetic experiments were carried out.The results showed that the specific surface area of VTM concentrates was increased from 872 to 1457 cm^(2)/g by HPGR and then pelletising and roasting.With preheating at 1000℃ for 10 min and roasting at 1260℃ for 10 min,the strengths of preheated pellets were increased from 329 to 535 N,and the strengths of roasted pellets were increased from 1010 to 2591 N.The limiting link in the early stage of VTM pellets oxidation was the control of chemical reaction,while the limiting link in the later stage of oxidation was the mixed control of chemical reaction and gas diffusion.The activation energies of VTM pellets before and after HPGR pretreatment were 53.07 and 40.03 kJ/mol in the early stage of oxidation reaction,while the activation energies in the later stage of oxidation were 29.24 and 22.75 kJ/mol,respectively.展开更多
Carbon coatings for silicon(Si)-based anode materials are essential for designing high-performance Li-ion batteries(LIBs).The coatings prevent direct contact with the electrolyte and enhance anode performance.However,...Carbon coatings for silicon(Si)-based anode materials are essential for designing high-performance Li-ion batteries(LIBs).The coatings prevent direct contact with the electrolyte and enhance anode performance.However,conventional carbon coatings are limited by their volume expansion and structural degradation,which lead to capacity fading and reduced durability.This study introduces a scalable and practical one-step carbon-coating strategy for directly coating silicon suboxide(SiO_(x))-based materials using aqueous quasi-defect-free reduced graphene oxide(QrGO)without post-treatment,unlike conventional graphene oxide(GO)-based coating methods.This simple process enables uniform encapsulation with QrGO for a highly adhesive and conductive coating.The QrGO-based composite anode material has several advantages,including reduced cracking due to volume expansion and enhanced charge carrier transport,as well as an increased Si content of 20 wt.%compared to the 5 wt.%in typical commercial Si-based active materials.In particular,the capacity retention of the QrGO-coated Si electrodes dramatically increases at high C-rate.The full cell exhibited long-term stability and capacity that were twice that of commercial SiO_(x)-based cells.Therefore,the QrGO-based one-step coating process represents a scalable,transformative,and commercially viable strategy for developing high-performance LIBs.展开更多
This study explored the impact of sintering time and temperature on the synthesis and formation of high-entropy rare earth oxides(HEOs).By systematically varying the sintering conditions,a series of Lu_(2)Yb_(2)Tm_(2)...This study explored the impact of sintering time and temperature on the synthesis and formation of high-entropy rare earth oxides(HEOs).By systematically varying the sintering conditions,a series of Lu_(2)Yb_(2)Tm_(2)Er_(2)O_(12) samples was synthesized and their structural and chemical properties were analyzed using scanning electron microscopy(SEM)with energy-dispersive X-ray spectroscopy(EDS)elemental mapping,X-ray diffraction(XRD),high-resolution transmission electron microscopy(HRTEM),and X-ray photoelectron spectroscopy(XPS).According to XRD patterns,a single-phase cubic C-type structure is easier to form at higher sintering temperatures(1400-1500℃),with sharper peaks signifying better crystallinity.With longer sintering times improving grain development and homogeneity,SEM research reveals a change in morphology from spherical grains at lower temperatures(1100-1200℃)to blocky grains at higher temperatures(1300-1500℃).HRTEM pictures verified the nanoparticles'strong crystallinity,and at higher temperatures,the lattice fringes widen and become more distinct,indicating better atomic ordering and diffusion.Stable and uniform high-entropy oxide production is indicated by the XPS spectra,which shows uniform elemental distribution and consistent chemical states of the constituent elements with very slight variations in the oxygen peaks.The findings highlight how important the sintering temperature is for reaching the intended high-entropy phase,with higher temperatures promoting improved atomic diffusion and compositional homogeneity.The results open the door for the use of high-entropy rare earth oxides in sophisticated functional materials by offering insightful information on how to best synthesize them.展开更多
High-capacity O3-type layered NiFeMn-based oxides are promising cathodes for sodium-ion batteries,though their practical deployment is constrained by the inherent limitations of Fe redox chemistry.Traditional designs ...High-capacity O3-type layered NiFeMn-based oxides are promising cathodes for sodium-ion batteries,though their practical deployment is constrained by the inherent limitations of Fe redox chemistry.Traditional designs generally enforcing stoichiometric symmetry(Ni=Mn)yield low Fe redox activity.Herein,we propose a valence engineering strategy that breaks conventional Ni/Mn stoichiometry to reconfigure Fe's local chemical environment and unlock unprecedented redox depth.Density functional theory(DFT)calculations reveal that the designed NaNi_(0.35)Fe_(0.225)Mn_(0.425)O_(2)cathode exhibits a reduced Bader charge on Fe(1.598 vs.1.638 in NaNi_(1/3)Fe_(1/3)Mn_(1/3)O_(2))and elevated Fe 3d orbital energy,signifying enhanced Fe redox activity.This configuration enables an exceptional Fe^(2.60+)/Fe^(3.88+)redox(1.28 e~-per Fe),delivering a reversible capacity of184.3 mAh g^(-1)within 2-4.2 V at 0.2 C,markedly exceeding the benchmark NaNi_(1/3)Fe_(1/3)Mn_(1/3)O_(2)(161.3 mAh g^(-1))with low reaction depth of Fe^(3.01+)/Fe^(3.61+).The intensified cationic redox reaction enables an ultrahigh energy density of 596 Whkg-1.The NaNi_(0.35)Fe_(0.225)Mn_(0.425)O_(2)cathode demonstrates robust performance over a broad temperature range from-15℃to 60℃.In situ and ex situ characterizations unveil a reversible O3■P3■OP2 phase transition with minimal volume change(1.88%)that circumvents detrimental deleterious O'3 intermediates and intragranular cracking.This work establishes valence engineering as a paradigm to consolidate cationic redox reaction in high-energy layered sodium oxide cathodes.展开更多
The methanol oxidation reaction(MOR)to formic acid offers a promising alternative to the anodic oxygen evolution reaction(OER)in water electrolysis.However,the development of efficient and cost-effective catalysts rem...The methanol oxidation reaction(MOR)to formic acid offers a promising alternative to the anodic oxygen evolution reaction(OER)in water electrolysis.However,the development of efficient and cost-effective catalysts remains a primary challenge.In this study,an enhancement in catalytic MOR performance is achieved through the incorporation of Mn atoms with unsaturated t_(2g)orbitals into Ni_(3)Se_(4).Comprehensive experimental analyses and theoretical calculations reveal that substituting Ni with Mn induces strong electron-withdrawing effects,effectively modulating the local coordination environment of the metal centers.The presence of Mn also elongates Ni–Se(O)bonds,which reduces eg orbital occupancy and modifies the spin state of the material.Electrochemical measurements demonstrate that electrodes based on this optimized material exhibit a high spin state and deliver excellent catalytic activity,achieving a MOR current density up to∼190 mA cm^(−2)at 1.6 V.This performance enhancement is attributed to the favorable electronic configuration and reduced reaction energy barriers associated with the high-spin state.展开更多
Atomic vacancies in oxides induce deviations from ideal stoichiometry,critically influencing their functional properties in applications such as energy storage-conversion,catalysis,and electronic devices.The dynamic b...Atomic vacancies in oxides induce deviations from ideal stoichiometry,critically influencing their functional properties in applications such as energy storage-conversion,catalysis,and electronic devices.The dynamic behavior of these vacancies as main mass transport mediums to exchange chemical species with surroundings under operating conditions is central to oxide redox reactions running with the Mars-van Krevelen(MvK)mechanism;yet in-situ atomic-scale monitoring of the vacancy dynamics and vacancy-induced secondary defects within oxides remains challenging due to both their rapid transport kinetics at buried subsurface/interface and characterization difficulties,arising from the insulating nature of bulk oxides and the spatial-resolution requirement in reaction conditions.These challenges hinder precise defect engineering for the performance optimization of functional oxides.In this review,recent advancements in tracking oxygen vacancy and vacancyinduced secondary defects dynamics in oxides,including surface steps,cation vacancies,interfacial dislocations,ledges,and interfaces,have been summarized.The dynamic interconversion of defects and their synergistic effects on surface/subsurface/interface evolution are mainly discussed.The aim of this review is to enhance understanding of defect dynamics and their pivotal role in modulating structural dynamics and surface reaction reactivity,which is highly relevant to the catalyst activity/selectivity/stability evaluation of functional oxide catalysts for electroreduction and catalytic oxidation reactions.Finally,strategies to control buried subsurface and interfacial defects(interface engineering)through tailored surface reactions are proposed,offering new pathways to customize the performance of advanced oxide-based materials.展开更多
Solid oxide cells(SOCs)have emerged as one of the key technologies for low-carbon energy transition due to their fuel flexibility and high system efficiency.However,their long-term deployment remains hindered by mater...Solid oxide cells(SOCs)have emerged as one of the key technologies for low-carbon energy transition due to their fuel flexibility and high system efficiency.However,their long-term deployment remains hindered by material degradation and interfacial instability under high-temperature and multi-atmospheric operating conditions.In particular,achieving a balance between catalytic activity and structural stability presents a major bottleneck in material design.High-entropy materials(HEMs),with their unique configurational entropy effect,multi-principal element synergy,and tunable local defect chemistry,offer a promising pathway to overcome these limitations.This perspective reviews recent advances in the application of HEMs in SOCs,including element selection and structure tuning,machine-learning-assisted design,in situ leaching and self-assembly engineering,and high-entropy coating strategies.Special attention is paid to how HEMs leverage their multi-elemental composition and defect regulation to enhance electrode performance,stabilize interfaces,and improve tolerance to poisoning species.We further highlight the potential of data-driven approaches for accelerating HEM screening and performance optimization,and discuss the integration of high-throughput experimentation with computational modeling to enable efficient exploration of the vast compositional space.Despite the remarkable progress,key challenges remain in achieving long-term stability and reliability across diverse operating scenarios.Future research should focus on precise control of non-equimolar compositions,development of cross-scale dynamic characterization techniques,and establishment of closed-loop frameworks that couple data-driven models with experimental feedback.These efforts will pave the way toward the rational design of high-performance,durable SOC systems.展开更多
Tetrahydrofuran-2,5-dicarboxylic acid(THFDCA)is a bio-based cyclic dicarboxylic acid with greater flexibility and biosafety than the renowned 2,5-furandicarboxylic acid(FDCA),but its synthesis is limited to thermochem...Tetrahydrofuran-2,5-dicarboxylic acid(THFDCA)is a bio-based cyclic dicarboxylic acid with greater flexibility and biosafety than the renowned 2,5-furandicarboxylic acid(FDCA),but its synthesis is limited to thermochemical methods with only several reports.This study pioneers an electrocatalytic strategy for the efficient synthesis of THFDCA via the oxidation of tetrahydrofuran dimethanol(THFDM).By constructing NiCo bimetallic oxides micron sheets on nickel foam(NiCoMS/NF)through controlled pyrolysis of a metal-organic framework(MOF)-like precursor,we achieved a remarkable THFDM conversion of 99.0%and THFDCA yield up to 98.2%,surpassing all reports on thermocatalytic oxidation as we know.In-depth analysis revealed that the synergistic effect between NiO and Co_(3)O_(4) contributes to the high catalytic performance.In-situ Raman and rotating ring-disk electrode(RRDE)techniques were employed to discuss the reaction mechanism and the inhibitory effect on oxygen evolution reaction(OER).This study not only provides a paradigm-shifting,groundbreaking strategy for the synthesis of the flexible cyclic dicarboxylic acid derived from furanic biomass but also offers deep insights into the synergistic effects of electrocatalysts.展开更多
TiB_(2)coatings can significantly enhance the high-temperature oxidation resistance of molybdenum,which would broaden the application range of molybdenum and alloys thereof.However,traditional methods for preparing Ti...TiB_(2)coatings can significantly enhance the high-temperature oxidation resistance of molybdenum,which would broaden the application range of molybdenum and alloys thereof.However,traditional methods for preparing TiB_(2)coatings have disadvantages such as high equipment costs,complicated processes,and highly toxic gas emissions.This paper proposes an environmentally friendly method,which requires inexpensive equipment and simple processing,for preparing TiB_(2)coating on molybdenum via electrophoretic deposition within Na3AlF6-based molten salts.The produced TiB_(2)layer had an approximate thickness of 60μm and exhibited high density,outstanding hardness(38.2 GPa)and robust adhesion strength(51 N).Additionally,high-temperature oxidation experiments revealed that,at900℃,the TiB_(2)coating provided effective protection to the molybdenum substrate against oxidation for 3 h.This result indicates that the TiB_(2)coating prepared on molybdenum using molten salt electrophoretic deposition possesses good high-temperature oxidation resistance.展开更多
Enhancing the oxidation resistance of Co-based superalloys by adding a high content of Cr,while simultaneously ensuring the stability of theγ/γ′phases,presents a significant challenge.This study evaluated the alloy...Enhancing the oxidation resistance of Co-based superalloys by adding a high content of Cr,while simultaneously ensuring the stability of theγ/γ′phases,presents a significant challenge.This study evaluated the alloying potential of Co–30Ni–10Al–5V–4Ta using the CALPHAD method,revealing promising characteristics.The developed Co–30Ni–10Al–5V–4Ta–12Cr alloy characterized by high Cr content andγ/γ′two-phase structure,demonstrating highγ′solvus temperature of 1139℃,low density of 8.48 g/cm^(3),minimalγ/γ′lattice misfit of +0.28%,high compressive yield strength of 651 MPa at 800℃,and excellent oxidation resistance with a weight gain of 6.5 mg/cm^(3)after 200 h at 1000℃.Examination of the oxidation behavior at 1000℃ revealed an oxide layer consisting of a porous outer CoO,NiO,and V_(3)O_(4)(CNV)oxide and a denser inner mixed oxide layer comprising CoO,NiO,and V_(3)O_(4)(CNV)oxide,Al_(2)O_(3),Cr_(2)O_(3),CoO,and NiO(CNAC)oxide,and TaO_(2),CoO,and NiO(CNT)oxide.展开更多
Fenton technology has garnered significant attention for the deep removal of low-concentration emerging contaminants due to its remarkable oxidation performance.However,the traditional mineralization process for emerg...Fenton technology has garnered significant attention for the deep removal of low-concentration emerging contaminants due to its remarkable oxidation performance.However,the traditional mineralization process for emerging contaminants requires a substantial amount of hydroxyl radicals(HO˙),leading to excessive consumption of H_(2)O_(2).Through interfacial engineering of Fe-Zr bimetallic catalysts(FeZrO_(x)),this study demonstrates synergistic enhancement of phenolic pollutant removal at heterojunction interfaces while achieving an 80%reduction in H_(2)O_(2)dosage compared to traditional Fe_(2)O_(3)systems.The chemical states of Fe and Zr at the(104)/(111)heterojunction interface in FeZrO_(x)exhibit marked modifications relative to their monometallic Fe_(2)O_(3)and ZrO_(2)counterparts.The elevated charge density at interfacial Fe sites in FeZrO_(x)promotes HO˙generation,while optimized antibonding orbital composition below the Fermi level in bisphenol A adsorbed on Zr sites enhances hydrogen abstraction and subsequent polymerization.This Fe-Zr synergy at the(104)/(111)heterojunction concurrently suppresses HO˙diffusion losses and directs phenolic pollutant(e.g.,phenol and bisphenol A)polymerization within the reactive interface,thereby reducing H_(2)O_(2)consumption compared to monometallic systems.展开更多
Transition metal oxides(TMOs)are widely explored as electrode materials for electrochemical energy storage owing to their rich redox activity,tunable oxidation states,and high theoretical capacitance.However,conventio...Transition metal oxides(TMOs)are widely explored as electrode materials for electrochemical energy storage owing to their rich redox activity,tunable oxidation states,and high theoretical capacitance.However,conventional synthesis routes often rely on toxic chemicals,high-temperature processing,and energy-intensive steps,limiting their sustainability and large-scale applicability.This review highlights recent progress in green synthesis approaches,particularly plant-mediated,microbial,and agro-waste-derived methods that use environmentally benign reducing and stabilizing agents to produce nanostructured TMOs.These green routes enable controlled morphology,enhanced porosity,and defect-rich architectures,resulting in improved charge storage,rate capability,and cycling stability.A comparative assessment of green-synthesized and conventionally prepared TMOs is provided,along with insights into synthesis mechanisms,advantages,limitations,and performance trends.Green chemistry-based strategies show strong potential for developing high-performance,scalable,and eco-friendly electrode materials for next-generation supercapacitors and batteries.展开更多
基金National Natural Science Foundation of China(52071274)Key Research and Development Projects of Shaanxi Province(2023-YBGY-442)Science and Technology Nova Project-Innovative Talent Promotion Program of Shaanxi Province(2020KJXX-062)。
文摘To mitigate the impact of interdiffusion reactions between the silicide slurry and Ta12W alloy substrate during vacuum sintering process on the oxidation resistance of the silicide coating,a micro-arc oxidation pretreatment was employed to construct a Ta_(2)O_(5)ceramic layer on the Ta12W alloy surface.Subsequently,a slurry spraying-vacuum sintering method was used to prepare a Si-Cr-Ti-Zr coating on the pretreated substrate.Comparative studies were conducted on the microstructure,phase composition,and isothermal oxidation resistance(at 1600℃)of the as-prepared coatings with and without the micro-arc oxidation ceramic layer.The results show that the Ta_(2)O_(5)layer prepared at 400 V is more continuous and has smaller pores than that prepared at 350 V.After microarc oxidation pretreatment,the Si-Cr-Ti-Zr coating on Ta12W alloy consists of three distinct layers:an upper layer dominated by Ti_(5)Si_(3),Ta_(5)Si_(3),and ZrSi;a middle layer dominated by TaSi_(2);a coating/substrate interfacial reaction layer dominated by Ta_(5)Si_(3).Both the Si-Cr-Ti-Zr coatings with and without the Ta_(2)O_(5)ceramic layer do not fail after isothermal oxidation at 1600℃for 5 h.Notably,the addition of the Ta2O5 ceramic layer reduces the high-temperature oxidation rate of the coating.
文摘It is crucial to develop arsenic removal adsorbents with strong sulfur resistance under middle-low-temperature flue gas conditions(<400℃).In this work,five Fe-Ce-La oxides were prepared by co-precipitation method,and FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbents were prepared by coupling fly ash-based Si-Al carriers.The active components Fe-Ce-La oxides and Si-Al carriers were characterized by TPD,TG,XRF,BET and XPS,respectively.The effects of temperature,Si/Al ratio and FeCeLaO loading rate on the sulfur resistance were investigated.Results show that the SO_(2) promotes the arsenic removal of Fe_(2)O_(3),CeLaO and FeCeLaO.At 400℃,the arsenic removal efficiencies of the three oxides increase from 45.3%,72.5% and 81.3% without SO_(2) to 62.6%,80.5%and 91.0%,respectively.The SO_(2) inhibits the arsenic removal of La_(2)O_(2)CO_(3) and FeLaO,and the inhibition effect is pronounced at high temperatures.The sulfur poisoning resistance of Si-Al carriers increases with the increase of Si/Al ratio.When the Si/Al ratio is increased to 9.74,the arsenic removal efficiency in the SO_(2) environment is 13.9% higher than that in the absence of SO_(2).Introducing FeCeLaO active components is beneficial for enhancing the SO_(2) poisoning resistance of Si-Al carriers.The strong sulfur resistance of the FeCeLaO/SiO_(2)-Al_(2)O_(3) composite adsorbent results from multiple factors:protective effects of Ce on Fe,La and Al;sulfation-induced generation of Ce^(3+)and surface-adsorbed oxygen;and strong surface acidity of SiO_(2).
基金supported by the Key R&D Program of Shandong Province,China(No.2025CXGC 010412)the National Key Research and Development Program of China(No.2022YFB3709300)the National Natural Science Foundation of China(No.U21A2048).
文摘The limited high-temperature oxidation resistance of Mg alloys is a key factor restricting their development and application.The addition of some rare earth elements(REs),owing to their unique physical and chemical properties,can significantly enhance the oxidation resistance of Mg alloys.Based on our previous study,we conclude that REs such as Gd,Y,and Ce enhance the oxidation resistance of Mg-RE alloys.This article comprehensively reviews recent research progress on high-temperature oxidation behavior and the potential mechanism in Mg-RE alloys.Based on the thermodynamic and kinetic analyses,the evolution of the complex oxide system formed during the high-temperature oxidation of Mg-RE alloys is first summarized.The diffusion behavior and concentration control mechanisms of REs during the oxidation process and how these mechanisms affect the sustained growth of the oxide film and antioxidant properties were elucidated.Moreover,the different structures of the oxide films were classified,and their properties were discussed.Finally,this paper introduces the applications of commonly used REs in Mg alloys and frontier research on their oxidation mechanisms.Based on the above review,we propose that future research perspectives can be explored in terms of expanding the experimental temperature range for oxidation tests,optimizing the chemical composition by adding trace REs to study their synergistic mechanism,revealing the underlying oxidation mechanism through advanced in situ microscopic characterization methods,and investigating the mechanical properties of oxide films using diverse approaches.
文摘Platinum group metals have high melting points,strong corrosion resistance,stable chemical properties,and low oxygen permeability in high-temperature oxygen-containing environments.As thermal protective coating materials,they have gained essential applications in the aerospace field and have excellent prospects for application in frontier military fields,such as protecting hot-end components of hypersonic aircraft.This research reviewed the latest research progress of platinum group metal coatings with hightemperature oxidation resistance,including coating preparation techniques,oxidation failure,and alloying modification.The leading preparation techniques of current platinum group metal coatings were discussed,as well as the advantages and disadvantages of various existing preparation techniques.Besides,the intrinsic properties,failure forms,and failure mechanisms of coatings of single platinum group metal in high-temperature oxygen-containing environments were analyzed.On this basis,the necessity,main methods,and main achievements of alloying modification of platinum group metals were summarized.Finally,the future development of platinum group coatings with high-temperature oxidation resistance was discussed and prospected.
基金supported by the National Natural Science Foundation of China(22478202,22208169,U23A20125,22478203)China Postdoctoral Science Foundation(2022M721703).
文摘Peroxymonosulfate(PMS)-based Fenton-like technologies have been increasingly employed in the upgrading of biomass,but they are commonly limited by the trade-off between conversion and selectivity due to the short lifetime of reactive oxygen species(ROS)and uncontrollable oxidation pathways.Herein,we show that single-atom Co supported on carbon nitride enables the high-valent-oxo cobalt species(Co(IV)O)mediated oxidation of glucose into value-added products in acetonitrile.This photocatalytic Fenton-like system achieved an overall selectivity of gluconic acid,glucaric acid,arabinose,and formic acid up to 90.3%at glucose conversion of 69.6%,outperforming most of previously reported catalytic systems.The small amount(0.72 wt%)of single-atom Co could not only elevate the optical absorption and the efficiency of photo-generated carriers separation but also induce the efficient generation of Co(IV)O with reduced ROS to enable efficient and selective oxidation.These findings prove the great promise of high-valent metal-oxo species in biomass conversions.
基金funded by grants from the National Natural Science Foundation of China(32288101 and 91631306 to B.S32170632 and 32000390 to Y.H.32400503 to Y.G.)Major Scientific Project of Yunnan Province(202305AH340007 to B.S.)+4 种基金Yunnan Revitalization Talent Support Program Science&Technology Champion Project(202005AB160004 to B.S.)Yunnan Revitalization Talent Support Program Innovation Team(202405AS350008)Yunnan Scientist Workshops(to B.S.)the Youth Innovation Promotion Association of CAS(to Y.H.),the Science and Technology General Program of Yunnan Province(202301AW070010 and 202001AT070110 to Y.H.)and the Provincial Key Research,Development,and Translational Program(XZ202101ZY0009G to Baima.).
文摘Nitric oxide(NO)is a key vasodilator that regulates vascular pressure and blood flow.Tibetans have developed a"blunted"mechanism for regulating NO levels at high altitude,with GTP cyclohydrolase 1(GCH1)identified as a key candidate gene.Here,we present comprehensive genetic and functional analyses of GCH1,which exhibits strong Darwinian positive selection in Tibetans.We show that Tibetan-enriched GCH1 variants down-regulate its expression in the blood of Tibetans.Based on this observation,we generate the heterozygous Gch1 knockout(Gch1^(+/-))mouse model to simulate its downregulation in Tibetans.We find that under prolonged hypoxia,the Gch1^(+/-)mice have relatively higher blood NO and blood oxygen saturation levels compared with the wild-type(WT)controls,providing better oxygen supplies to the cardiovascular and pulmonary systems.Markedly,hypoxia-induced cardiac hypertrophy and pulmonary remodeling are significantly attenuated in the Gch1^(^(+/-))mice compared with the WT controls,likely due to the adaptive changes in molecular regulations related to metabolism,inflammation,circadian rhythm,extracellular matrix,and oxidative stress.This study sheds light on the role of GCH1 in regulating blood NO,contributing to the physiological adaptation of the cardiovascular and pulmonary systems in Tibetans at high altitude.
基金financially supported by the National Natural Science Foundation of China(Grant No.12172093)the Guangdong Basic and Applied Basic Research Foundation(Grant No.2021A1515012607)。
文摘High-entropy oxides(HEOs)have emerged as a promising class of memristive materials,characterized by entropy-stabilized crystal structures,multivalent cation coordination,and tunable defect landscapes.These intrinsic features enable forming-free resistive switching,multilevel conductance modulation,and synaptic plasticity,making HEOs attractive for neuromorphic computing.This review outlines recent progress in HEO-based memristors across materials engineering,switching mechanisms,and synaptic emulation.Particular attention is given to vacancy migration,phase transitions,and valence-state dynamics—mechanisms that underlie the switching behaviors observed in both amorphous and crystalline systems.Their relevance to neuromorphic functions such as short-term plasticity and spike-timing-dependent learning is also examined.While encouraging results have been achieved at the device level,challenges remain in conductance precision,variability control,and scalable integration.Addressing these demands a concerted effort across materials design,interface optimization,and task-aware modeling.With such integration,HEO memristors offer a compelling pathway toward energy-efficient and adaptable brain-inspired electronics.
基金supported by National Key Research and Development Program of China(Grant No.2022YFB3304800)the Reviving-Liaoning Excellence Plan(XLYC2203186).
文摘The high-temperature compressive deformation behavior of medium manganese steel using a four-roll reversible rolling mill is investigated,revealing the effects of different Mn contents on the thermal deformation behavior of oxidation products in the alloy.It is found that within the experimental temperature range,the higher the deformation temperature,the better the plasticity of the oxidation products.It was observed that increasing the Mn content refines the grains,enhances the deformation ability of the oxidation products,and improves the flatness of the interfaces.Since(Fe,Mn)O has a similar crystal structure to FeO,the addition of Mn refines the grains of(Fe,Mn)O,causing the deformation to be distributed across more grains under the same deformation amount,and thereby improving its plasticity.At the interface between Fe-Mn alloy oxidation products and the matrix,there exists a spinel-phase solid solution,which can deform together with the oxidation products and the matrix at high temperatures.It was found that with increasing the Mn content,the size and number of pores between the spinel phases increased.First-principles simulation calculations were used to verify this,showing that Mn promotes the generation of vacancies.The greater number of pores in the spinel phase can effectively relieve the compressive stress caused by rolling deformation,thereby improving the deformation capability of the oxidation products at the interface.
基金supports provided from Guangxi Science and Technology Major Project(AA24263047).
文摘The production of vanadium-titanium magnetite(VTM)pellets has the problems of low consolidation strength and high energy consumption in the preheating and roasting process.High-pressure grinding roll(HPGR)pretreatment process was used to increase the fine-grained content and specific surface area of VTM concentrates,to strengthen the oxidation consolidation process of VTM pellets,and oxidation kinetic experiments were carried out.The results showed that the specific surface area of VTM concentrates was increased from 872 to 1457 cm^(2)/g by HPGR and then pelletising and roasting.With preheating at 1000℃ for 10 min and roasting at 1260℃ for 10 min,the strengths of preheated pellets were increased from 329 to 535 N,and the strengths of roasted pellets were increased from 1010 to 2591 N.The limiting link in the early stage of VTM pellets oxidation was the control of chemical reaction,while the limiting link in the later stage of oxidation was the mixed control of chemical reaction and gas diffusion.The activation energies of VTM pellets before and after HPGR pretreatment were 53.07 and 40.03 kJ/mol in the early stage of oxidation reaction,while the activation energies in the later stage of oxidation were 29.24 and 22.75 kJ/mol,respectively.
基金supported by Korea Electrotechnology Research Institute(KERI)Primary research program through the National Research Council of Science&Technology(NST)funded by the Ministry of Science and ICT(MSIT)(No.25A01015)by the Technology Innovation Program(20019091)funded by the Ministry of Trade,Industry&Energy(MOTIE,Korea)by the National Research Council of Science&Technology(NST)grant from the Korea government(MSIT)(No.GTL24012-000).
文摘Carbon coatings for silicon(Si)-based anode materials are essential for designing high-performance Li-ion batteries(LIBs).The coatings prevent direct contact with the electrolyte and enhance anode performance.However,conventional carbon coatings are limited by their volume expansion and structural degradation,which lead to capacity fading and reduced durability.This study introduces a scalable and practical one-step carbon-coating strategy for directly coating silicon suboxide(SiO_(x))-based materials using aqueous quasi-defect-free reduced graphene oxide(QrGO)without post-treatment,unlike conventional graphene oxide(GO)-based coating methods.This simple process enables uniform encapsulation with QrGO for a highly adhesive and conductive coating.The QrGO-based composite anode material has several advantages,including reduced cracking due to volume expansion and enhanced charge carrier transport,as well as an increased Si content of 20 wt.%compared to the 5 wt.%in typical commercial Si-based active materials.In particular,the capacity retention of the QrGO-coated Si electrodes dramatically increases at high C-rate.The full cell exhibited long-term stability and capacity that were twice that of commercial SiO_(x)-based cells.Therefore,the QrGO-based one-step coating process represents a scalable,transformative,and commercially viable strategy for developing high-performance LIBs.
基金Project supported by Natural Science Foundation of Zhejiang Province(LD21E080001)Zhejiang Provincial Ten Thousand Talent Program(ZJWR0302055)。
文摘This study explored the impact of sintering time and temperature on the synthesis and formation of high-entropy rare earth oxides(HEOs).By systematically varying the sintering conditions,a series of Lu_(2)Yb_(2)Tm_(2)Er_(2)O_(12) samples was synthesized and their structural and chemical properties were analyzed using scanning electron microscopy(SEM)with energy-dispersive X-ray spectroscopy(EDS)elemental mapping,X-ray diffraction(XRD),high-resolution transmission electron microscopy(HRTEM),and X-ray photoelectron spectroscopy(XPS).According to XRD patterns,a single-phase cubic C-type structure is easier to form at higher sintering temperatures(1400-1500℃),with sharper peaks signifying better crystallinity.With longer sintering times improving grain development and homogeneity,SEM research reveals a change in morphology from spherical grains at lower temperatures(1100-1200℃)to blocky grains at higher temperatures(1300-1500℃).HRTEM pictures verified the nanoparticles'strong crystallinity,and at higher temperatures,the lattice fringes widen and become more distinct,indicating better atomic ordering and diffusion.Stable and uniform high-entropy oxide production is indicated by the XPS spectra,which shows uniform elemental distribution and consistent chemical states of the constituent elements with very slight variations in the oxygen peaks.The findings highlight how important the sintering temperature is for reaching the intended high-entropy phase,with higher temperatures promoting improved atomic diffusion and compositional homogeneity.The results open the door for the use of high-entropy rare earth oxides in sophisticated functional materials by offering insightful information on how to best synthesize them.
基金supported by the National Natural Science Foundation of China(Grant Nos.52202282,52402054,22471283,and 52202327)Natural Science Foundation of Tianjin City(Grant Nos.22JCYBJC00040,24JCQNJC00970)。
文摘High-capacity O3-type layered NiFeMn-based oxides are promising cathodes for sodium-ion batteries,though their practical deployment is constrained by the inherent limitations of Fe redox chemistry.Traditional designs generally enforcing stoichiometric symmetry(Ni=Mn)yield low Fe redox activity.Herein,we propose a valence engineering strategy that breaks conventional Ni/Mn stoichiometry to reconfigure Fe's local chemical environment and unlock unprecedented redox depth.Density functional theory(DFT)calculations reveal that the designed NaNi_(0.35)Fe_(0.225)Mn_(0.425)O_(2)cathode exhibits a reduced Bader charge on Fe(1.598 vs.1.638 in NaNi_(1/3)Fe_(1/3)Mn_(1/3)O_(2))and elevated Fe 3d orbital energy,signifying enhanced Fe redox activity.This configuration enables an exceptional Fe^(2.60+)/Fe^(3.88+)redox(1.28 e~-per Fe),delivering a reversible capacity of184.3 mAh g^(-1)within 2-4.2 V at 0.2 C,markedly exceeding the benchmark NaNi_(1/3)Fe_(1/3)Mn_(1/3)O_(2)(161.3 mAh g^(-1))with low reaction depth of Fe^(3.01+)/Fe^(3.61+).The intensified cationic redox reaction enables an ultrahigh energy density of 596 Whkg-1.The NaNi_(0.35)Fe_(0.225)Mn_(0.425)O_(2)cathode demonstrates robust performance over a broad temperature range from-15℃to 60℃.In situ and ex situ characterizations unveil a reversible O3■P3■OP2 phase transition with minimal volume change(1.88%)that circumvents detrimental deleterious O'3 intermediates and intragranular cracking.This work establishes valence engineering as a paradigm to consolidate cationic redox reaction in high-energy layered sodium oxide cathodes.
基金financially supported by the Sichuan Science and Technology Program (Grant No. 2025NSFSC0139)the China Postdoctoral Science Foundation (Grant No.2023MD734228)+10 种基金funding from Generalitat de Catalunya 2021SGR00457supported by MCIN with funding from European Union NextGenerationEU(PRTR-C17.I1)by Generalitat de Catalunya (In-CAEM Project)the support from the project AMaDE(PID2023-149158OB-C43)funded by MCIN/AEI/10.13039/501100011033/by “ERDF A way of making Europe”by the “European Union”supported by the Severo Ochoa program from Spanish MCIN/AEI (Grant No.:CEX2021-001214-S)funded by the CERCA Programme/Generalitat de Catalunyaperformed in the framework of Universitat Autònoma de Barcelona Materials Science PhD programfunding from the CSC-UAB PhD scholarship program. ICN2 is founding member of e-DREAM[87]
文摘The methanol oxidation reaction(MOR)to formic acid offers a promising alternative to the anodic oxygen evolution reaction(OER)in water electrolysis.However,the development of efficient and cost-effective catalysts remains a primary challenge.In this study,an enhancement in catalytic MOR performance is achieved through the incorporation of Mn atoms with unsaturated t_(2g)orbitals into Ni_(3)Se_(4).Comprehensive experimental analyses and theoretical calculations reveal that substituting Ni with Mn induces strong electron-withdrawing effects,effectively modulating the local coordination environment of the metal centers.The presence of Mn also elongates Ni–Se(O)bonds,which reduces eg orbital occupancy and modifies the spin state of the material.Electrochemical measurements demonstrate that electrodes based on this optimized material exhibit a high spin state and deliver excellent catalytic activity,achieving a MOR current density up to∼190 mA cm^(−2)at 1.6 V.This performance enhancement is attributed to the favorable electronic configuration and reduced reaction energy barriers associated with the high-spin state.
基金supported by the funding support from the National Key R&D Program of China(2024YFA1509400)the Beijing Natural Science Foundation(F251001)+2 种基金the National Natural Science Foundation of China(No.22479148)the Institute of Weiqiao UCAS Science and Technology(GYY-GDHX-2024-ZY-007)supported by the U.S.National Science Foundation Under Grant No.DMR 2303712。
文摘Atomic vacancies in oxides induce deviations from ideal stoichiometry,critically influencing their functional properties in applications such as energy storage-conversion,catalysis,and electronic devices.The dynamic behavior of these vacancies as main mass transport mediums to exchange chemical species with surroundings under operating conditions is central to oxide redox reactions running with the Mars-van Krevelen(MvK)mechanism;yet in-situ atomic-scale monitoring of the vacancy dynamics and vacancy-induced secondary defects within oxides remains challenging due to both their rapid transport kinetics at buried subsurface/interface and characterization difficulties,arising from the insulating nature of bulk oxides and the spatial-resolution requirement in reaction conditions.These challenges hinder precise defect engineering for the performance optimization of functional oxides.In this review,recent advancements in tracking oxygen vacancy and vacancyinduced secondary defects dynamics in oxides,including surface steps,cation vacancies,interfacial dislocations,ledges,and interfaces,have been summarized.The dynamic interconversion of defects and their synergistic effects on surface/subsurface/interface evolution are mainly discussed.The aim of this review is to enhance understanding of defect dynamics and their pivotal role in modulating structural dynamics and surface reaction reactivity,which is highly relevant to the catalyst activity/selectivity/stability evaluation of functional oxide catalysts for electroreduction and catalytic oxidation reactions.Finally,strategies to control buried subsurface and interfacial defects(interface engineering)through tailored surface reactions are proposed,offering new pathways to customize the performance of advanced oxide-based materials.
基金supported by National Natural Science Foundation of China(U24A20542,52472210)Natural Science Foundation of Jiangsu Province(No.BK20221312)Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX25_1706).
文摘Solid oxide cells(SOCs)have emerged as one of the key technologies for low-carbon energy transition due to their fuel flexibility and high system efficiency.However,their long-term deployment remains hindered by material degradation and interfacial instability under high-temperature and multi-atmospheric operating conditions.In particular,achieving a balance between catalytic activity and structural stability presents a major bottleneck in material design.High-entropy materials(HEMs),with their unique configurational entropy effect,multi-principal element synergy,and tunable local defect chemistry,offer a promising pathway to overcome these limitations.This perspective reviews recent advances in the application of HEMs in SOCs,including element selection and structure tuning,machine-learning-assisted design,in situ leaching and self-assembly engineering,and high-entropy coating strategies.Special attention is paid to how HEMs leverage their multi-elemental composition and defect regulation to enhance electrode performance,stabilize interfaces,and improve tolerance to poisoning species.We further highlight the potential of data-driven approaches for accelerating HEM screening and performance optimization,and discuss the integration of high-throughput experimentation with computational modeling to enable efficient exploration of the vast compositional space.Despite the remarkable progress,key challenges remain in achieving long-term stability and reliability across diverse operating scenarios.Future research should focus on precise control of non-equimolar compositions,development of cross-scale dynamic characterization techniques,and establishment of closed-loop frameworks that couple data-driven models with experimental feedback.These efforts will pave the way toward the rational design of high-performance,durable SOC systems.
基金supported by the National Natural Science Foundation of China(22072170,U23A20125)the President Foundation of Ningbo Institute of Materials Technology and Engineering。
文摘Tetrahydrofuran-2,5-dicarboxylic acid(THFDCA)is a bio-based cyclic dicarboxylic acid with greater flexibility and biosafety than the renowned 2,5-furandicarboxylic acid(FDCA),but its synthesis is limited to thermochemical methods with only several reports.This study pioneers an electrocatalytic strategy for the efficient synthesis of THFDCA via the oxidation of tetrahydrofuran dimethanol(THFDM).By constructing NiCo bimetallic oxides micron sheets on nickel foam(NiCoMS/NF)through controlled pyrolysis of a metal-organic framework(MOF)-like precursor,we achieved a remarkable THFDM conversion of 99.0%and THFDCA yield up to 98.2%,surpassing all reports on thermocatalytic oxidation as we know.In-depth analysis revealed that the synergistic effect between NiO and Co_(3)O_(4) contributes to the high catalytic performance.In-situ Raman and rotating ring-disk electrode(RRDE)techniques were employed to discuss the reaction mechanism and the inhibitory effect on oxygen evolution reaction(OER).This study not only provides a paradigm-shifting,groundbreaking strategy for the synthesis of the flexible cyclic dicarboxylic acid derived from furanic biomass but also offers deep insights into the synergistic effects of electrocatalysts.
基金supported by the Original Exploratory Program of the National Natural Science Foundation of China(No.52450012)。
文摘TiB_(2)coatings can significantly enhance the high-temperature oxidation resistance of molybdenum,which would broaden the application range of molybdenum and alloys thereof.However,traditional methods for preparing TiB_(2)coatings have disadvantages such as high equipment costs,complicated processes,and highly toxic gas emissions.This paper proposes an environmentally friendly method,which requires inexpensive equipment and simple processing,for preparing TiB_(2)coating on molybdenum via electrophoretic deposition within Na3AlF6-based molten salts.The produced TiB_(2)layer had an approximate thickness of 60μm and exhibited high density,outstanding hardness(38.2 GPa)and robust adhesion strength(51 N).Additionally,high-temperature oxidation experiments revealed that,at900℃,the TiB_(2)coating provided effective protection to the molybdenum substrate against oxidation for 3 h.This result indicates that the TiB_(2)coating prepared on molybdenum using molten salt electrophoretic deposition possesses good high-temperature oxidation resistance.
基金supported by the National Natural ScienceFoundation of China(Nos.52371007 and 51831007).
文摘Enhancing the oxidation resistance of Co-based superalloys by adding a high content of Cr,while simultaneously ensuring the stability of theγ/γ′phases,presents a significant challenge.This study evaluated the alloying potential of Co–30Ni–10Al–5V–4Ta using the CALPHAD method,revealing promising characteristics.The developed Co–30Ni–10Al–5V–4Ta–12Cr alloy characterized by high Cr content andγ/γ′two-phase structure,demonstrating highγ′solvus temperature of 1139℃,low density of 8.48 g/cm^(3),minimalγ/γ′lattice misfit of +0.28%,high compressive yield strength of 651 MPa at 800℃,and excellent oxidation resistance with a weight gain of 6.5 mg/cm^(3)after 200 h at 1000℃.Examination of the oxidation behavior at 1000℃ revealed an oxide layer consisting of a porous outer CoO,NiO,and V_(3)O_(4)(CNV)oxide and a denser inner mixed oxide layer comprising CoO,NiO,and V_(3)O_(4)(CNV)oxide,Al_(2)O_(3),Cr_(2)O_(3),CoO,and NiO(CNAC)oxide,and TaO_(2),CoO,and NiO(CNT)oxide.
基金supported by the National Natural Science Foundation of China(Grant Nos.22476187 and 22206173)the Natural Science Foundation of Henan Province(Grant No.252300421179)+1 种基金the Foundation of Henan Educational Committee(Grant No.25A610001)the Science and Technology Innovation Leading Talent Support Program of Henan Province(Grant No.254000510035).
文摘Fenton technology has garnered significant attention for the deep removal of low-concentration emerging contaminants due to its remarkable oxidation performance.However,the traditional mineralization process for emerging contaminants requires a substantial amount of hydroxyl radicals(HO˙),leading to excessive consumption of H_(2)O_(2).Through interfacial engineering of Fe-Zr bimetallic catalysts(FeZrO_(x)),this study demonstrates synergistic enhancement of phenolic pollutant removal at heterojunction interfaces while achieving an 80%reduction in H_(2)O_(2)dosage compared to traditional Fe_(2)O_(3)systems.The chemical states of Fe and Zr at the(104)/(111)heterojunction interface in FeZrO_(x)exhibit marked modifications relative to their monometallic Fe_(2)O_(3)and ZrO_(2)counterparts.The elevated charge density at interfacial Fe sites in FeZrO_(x)promotes HO˙generation,while optimized antibonding orbital composition below the Fermi level in bisphenol A adsorbed on Zr sites enhances hydrogen abstraction and subsequent polymerization.This Fe-Zr synergy at the(104)/(111)heterojunction concurrently suppresses HO˙diffusion losses and directs phenolic pollutant(e.g.,phenol and bisphenol A)polymerization within the reactive interface,thereby reducing H_(2)O_(2)consumption compared to monometallic systems.
文摘Transition metal oxides(TMOs)are widely explored as electrode materials for electrochemical energy storage owing to their rich redox activity,tunable oxidation states,and high theoretical capacitance.However,conventional synthesis routes often rely on toxic chemicals,high-temperature processing,and energy-intensive steps,limiting their sustainability and large-scale applicability.This review highlights recent progress in green synthesis approaches,particularly plant-mediated,microbial,and agro-waste-derived methods that use environmentally benign reducing and stabilizing agents to produce nanostructured TMOs.These green routes enable controlled morphology,enhanced porosity,and defect-rich architectures,resulting in improved charge storage,rate capability,and cycling stability.A comparative assessment of green-synthesized and conventionally prepared TMOs is provided,along with insights into synthesis mechanisms,advantages,limitations,and performance trends.Green chemistry-based strategies show strong potential for developing high-performance,scalable,and eco-friendly electrode materials for next-generation supercapacitors and batteries.
