Traumatic brain injury involves complex pathophysiological mechanisms,among which oxidative stress significantly contributes to the occurrence of secondary injury.In this study,we evaluated hypidone hydrochloride(YL-0...Traumatic brain injury involves complex pathophysiological mechanisms,among which oxidative stress significantly contributes to the occurrence of secondary injury.In this study,we evaluated hypidone hydrochloride(YL-0919),a self-developed antidepressant with selective sigma-1 receptor agonist properties,and its associated mechanisms and targets in traumatic brain injury.Behavioral experiments to assess functional deficits were followed by assessment of neuronal damage through histological analyses and examination of blood-brain barrier permeability and brain edema.Next,we investigated the antioxidative effects of YL-0919 by assessing the levels of traditional markers of oxidative stress in vivo in mice and in vitro in HT22 cells.Finally,the targeted action of YL-0919 was verified by employing a sigma-1 receptor antagonist(BD-1047).Our findings demonstrated that YL-0919 markedly improved deficits in motor function and spatial cognition on day 3 post traumatic brain injury,while also decreasing neuronal mortality and reversing blood-brain barrier disruption and brain edema.Furthermore,YL-0919 effectively combated oxidative stress both in vivo and in vitro.The protective effects of YL-0919 were partially inhibited by BD-1047.These results indicated that YL-0919 relieved impairments in motor and spatial cognition by restraining oxidative stress,a neuroprotective effect that was partially reversed by the sigma-1 receptor antagonist BD-1047.YL-0919 may have potential as a new treatment for traumatic brain injury.展开更多
A high thrust-to-weight ratio poses challenges to the high-temperature performance of Ni-based superalloys. The oxidation behavior of GH4738 at extreme temperatures has been investigated by isothermal and non-isotherm...A high thrust-to-weight ratio poses challenges to the high-temperature performance of Ni-based superalloys. The oxidation behavior of GH4738 at extreme temperatures has been investigated by isothermal and non-isothermal experiments. As a result of the competitive diffusion of alloying elements, the oxide scale included an outermost porous oxide layer (OOL), an inner relatively dense oxide layer (IOL), and an internal oxide zone (IOZ), depending on the temperature and time. A high temperature led to the formation of large voids at the IOL/IOZ interface. At 1200℃, the continuity of the Cr-rich oxide layer in the IOL was destroyed, and thus, spallation occurred. Extension of oxidation time contributed to the size of Al-rich oxide particles with the increase in the IOZ. Based on this finding,the oxidation kinetics of GH4738 was discussed, and the corresponding oxidation behavior at 900-1100℃ was predicted.展开更多
The trade-off between efficiency and stability has limited the application of TiO_(2)as a catalyst due to its poor surface reactivity.Here,we present a modification of a TiO_(2)layer with highly stable Sub-5 nm Fe_(2)...The trade-off between efficiency and stability has limited the application of TiO_(2)as a catalyst due to its poor surface reactivity.Here,we present a modification of a TiO_(2)layer with highly stable Sub-5 nm Fe_(2)O_(3)nanoparticles(NP)by modulating its structure-surface reactivity relationship to attain efficiency-stability balance via a voltage-assisted oxidation approach.In situ simultaneous oxidation of the Ti substrate and Fe precursor using high-energy plasma driven by high voltage resulted in uniform distribution of Fe_(2)O_(3)NP embedded within porous TiO_(2)layer.Comprehensive surface characterizations with density functional theory demonstrated an improved electronic transition in TiO_(2)due to the presence of surface defects from reactive oxygen species and possible charge transfer from Ti to Fe;it also unexpectedly increased the active site in the TiO_(2)layer due to uncoordinated electrons in Sub-5 nm Fe_(2)O_(3)NP/TiO_(2)catalyst,thereby enhancing the adsorption of chemical functional groups on the catalyst.This unique embedded structure exhibited remarkable improvement in reducing 4-nitrophenol to 4-aminophenol,achieving approximately 99%efficiency in 20 min without stability decay after 20 consecutive cycles,outperforming previously reported TiO_(2)-based catalysts.This finding proposes a modified-electrochemical strategy enabling facile construction of TiO_(2)with nanoscale oxides extandable to other metal oxide systems.展开更多
Owing to the advantages of simple structure,low power consumption and high-density integration,memristors or memristive devices are attracting increasing attention in the fields such as next generation non-volatile me...Owing to the advantages of simple structure,low power consumption and high-density integration,memristors or memristive devices are attracting increasing attention in the fields such as next generation non-volatile memories,neuromorphic computation and data encryption.However,the deposition of memristive films often requires expensive equipment,strict vacuum conditions,high energy consumption,and extended processing times.In contrast,electrochemical anodizing can produce metal oxide films quickly(e.g.10 s) under ambient conditions.By means of the anodizing technique,oxide films,oxide nanotubes,nanowires and nanodots can be fabricated to prepare memristors.Oxide film thickness,nanostructures,defect concentrations,etc,can be varied to regulate device performances by adjusting oxidation parameters such as voltage,current and time.Thus memristors fabricated by the anodic oxidation technique can achieve high device consistency,low variation,and ultrahigh yield rate.This article provides a comprehensive review of the research progress in the field of anodic oxidation assisted fabrication of memristors.Firstly,the principle of anodic oxidation is introduced;then,different types of memristors produced by anodic oxidation and their applications are presented;finally,features and challenges of anodic oxidation for memristor production are elaborated.展开更多
Electrocatalytic glucose oxidation reaction(GOR)has attracted much attention owing to its crucial role in biofuel cell fabrication.Herein,we load MoO_(3)nanoparticles on carbon nanotubes(CNTs)and use a discharge proce...Electrocatalytic glucose oxidation reaction(GOR)has attracted much attention owing to its crucial role in biofuel cell fabrication.Herein,we load MoO_(3)nanoparticles on carbon nanotubes(CNTs)and use a discharge process to prepare a noblemetal-free MC-60 catalyst containing MoO_(3),Mo_(2)C,and a Mo_(2)C–MoO_(3)interface.In the GOR,MC-60 shows activity as high as 745μA/(mmol/L cm^(2)),considerably higher than those of the Pt/CNT(270μA/(mmol/L cm^(2)))and Au/CNT catalysts(110μA/(mmol/L cm^(2))).In the GOR,the response minimum on MC-60 is as low as 8μmol/L,with a steady-state response time of only 3 s.Moreover,MC-60 has superior stability and anti-interference ability to impurities in the GOR.The better performance of MC-60 in the GOR is attributed to the abundant Mo sites bonding to C and O atoms at the MoO_(3)–Mo_(2)C interface.These Mo sites create active sites for promoting glucose adsorption and oxidation,enhancing MC-60 performance in the GOR.Thus,these results help to fabricate more effi cient noble-metal-free catalysts for the fabrication of glucose-based biofuel cells.展开更多
In order to better understand the specific substituent effects on the electrochemical oxidation process of β-O-4 bond, a series of methoxyphenyl type β-O-4 dimer model compounds with different localized methoxyl gro...In order to better understand the specific substituent effects on the electrochemical oxidation process of β-O-4 bond, a series of methoxyphenyl type β-O-4 dimer model compounds with different localized methoxyl groups, including 2-(2-methoxyphenoxy)-1-phenylethanone, 2-(2-methoxyphenoxy)-1-phenylethanol, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanol, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanol have been selected and their electrochemical properties have been studied experimentally by cyclic voltammetry, and FT-IR spectroelectrochemistry. Combining with electrolysis products distribution analysis and density functional theory calculations, oxidation mechanisms of all six model dimers have been explored. In particular, a total effect from substituents of both para-methoxy(on the aryl ring closing to Cα) and Cα-OH on the oxidation mechanisms has been clearly observed, showing a significant selectivity on the Cα-Cβbond cleavage induced by electrochemical oxidations.展开更多
The scarcity,high cost and susceptibility to CO of Platinum severely restrict its application in alkaline hydrogen oxidation reaction(HOR).Hybridizing Pt with other transition metals provides an effective strategy to ...The scarcity,high cost and susceptibility to CO of Platinum severely restrict its application in alkaline hydrogen oxidation reaction(HOR).Hybridizing Pt with other transition metals provides an effective strategy to modulate its catalytic HOR performance,but at the cost of mass activity due to the coverage of modifiers on Pt surface.Herein,we constructed dual junctions'Pt/nitrogen-doped carbon(Pt/NC)andδ-MoC/NC to modify electronic structure of Pt via interfacial electron transfer to acquire Pt-MoC@NC catalyst with electron-deficient Pt nanoparticles,simultaneously endowing it with high mass activity and durability of alkaline HOR.Moreover,the unique structure of Pt-MoC@NC endows Pt with a high COtolerance at 1,000 ppm CO/H_(2),a quality that commercial Pt-C catalyst lacks.The theoretical calculations not only confirm the diffusion of electrons from Pt/NC to Mo C/NC could occur,but also demonstrate the negative shift of Pt d-band center for the optimized binding energies of*H,*OH and CO.展开更多
Owing to the intrinsically sluggish kinetics of urea oxidation reaction(UOR)involving a six-electron transfer process,developing efficient UOR electrocatalyst is a great challenge remained to be overwhelmed.Herein,by ...Owing to the intrinsically sluggish kinetics of urea oxidation reaction(UOR)involving a six-electron transfer process,developing efficient UOR electrocatalyst is a great challenge remained to be overwhelmed.Herein,by taking advantage of 2-Methylimidazole,of which is a kind of alkali in water and owns strong coordination ability to Co^(2+)in methanol,trace Co(1.0 mol%)addition was found to induce defect engineering onα-Ni(OH)_(2)in a dual-solvent system of water and methanol.Physical characterization results revealed that the synthesized electrocatalyst(WM-Ni_(0.99)Co_(0.01)(OH)_(2))was a kind of defective nanosheet with thickness around 5-6 nm,attributing to the synergistic effect of Co doping and defect engineering,its electron structure was finely altered,and its specific surface a rea was tremendously enlarged from 68 to 172.3 m^(2)g^(-1).With all these merits,its overpotential to drive 10 mA cm^(-2)was reduced by 110 mV.Besides,the interfacial behavior of UOR was also well deciphered by operando electrochemical impedance spectroscopy.展开更多
Urea holds promise as an alternative water-oxidation substrate in electrolytic cells.High-valence nickelbased spinel,especially after heteroatom doping,excels in urea oxidation reactions(UOR).However,traditional spine...Urea holds promise as an alternative water-oxidation substrate in electrolytic cells.High-valence nickelbased spinel,especially after heteroatom doping,excels in urea oxidation reactions(UOR).However,traditional spinel synthesis methods with prolonged high-temperature reactions lack kinetic precision,hindering the balance between controlled doping and highly active two-dimensional(2D)porous structures design.This significantly impedes the identification of electron configuration-dependent active sites in doped 2D nickel-based spinels.Herein,we present a microwave shock method for the preparation of 2D porous NiCo_(2)O_(4)spinel.Utilizing the transient on-off property of microwave pulses for precise heteroatom doping and 2D porous structural design,non-metal doping(boron,phosphorus,and sulfur)with distinct extranuclear electron disparities serves as straightforward examples for investigation.Precise tuning of lattice parameter reveals the impact of covalent bond strength on NiCo_(2)O_(4)structural stability.The introduced defect levels induce unpaired d-electrons in transition metals,enhancing the adsorption of electron-donating amino groups in urea molecules.Simultaneously,Bode plots confirm the impact mechanism of rapid electron migration caused by reduced band gaps on UOR activity.The prepared phosphorus-doped 2D porous NiCo_(2)O_(4),with optimal electron configuration control,outperforms most reported spinels.This controlled modification strategy advances understanding theoretical structure-activity mechanisms of high-performance 2D spinels in UOR.展开更多
Exploitation of oxygen evolution reaction(OER)and urea oxidation reaction(UOR)catalysts with high activity and stability at large current density is a major challenge for energy-saving H_(2) production in water electr...Exploitation of oxygen evolution reaction(OER)and urea oxidation reaction(UOR)catalysts with high activity and stability at large current density is a major challenge for energy-saving H_(2) production in water electrolysis.Herein,we use the pyridinic-N doping carbon layers coupled with tensile strain of FeNi alloy activated by NiFe_(2)O_(4)(FeNi/NiFe_(2)O_(4)@NC)for efficiently increasing the performance of water and urea oxidation.Due to the tensile strain effect on FeNi/NiFe_(2)O_(4)@NC,it provides a favorable modulation on the electronic properties of the active center,thus enabling amazing OER(η_(100)=196 mV)and UOR(E_(10)=1.32 V)intrinsic activity.Besides,the carbon-coated layers can be used as armor to prevent FeNi alloy from being corroded by the electrolyte for enhancing the OER/UOR stability at large current density,showing high industrial practicability.This work thus provides a simple way to prepare high-efficiency catalyst for activating water and urea oxidation.展开更多
Surface ozone(O_(3))poses significant threats to public health,agricultural crops,and plants in natural ecosystems.Global warming is likely to increase future O_(3)mainly by altering atmospheric photochemical reaction...Surface ozone(O_(3))poses significant threats to public health,agricultural crops,and plants in natural ecosystems.Global warming is likely to increase future O_(3)mainly by altering atmospheric photochemical reactions and enhancing biogenic volatile organic compound(BVOC)emissions.To assess the impacts of the future 1.5 K climate target on O_(3)concentrations and ecological O_(3)exposure in China,numerical simulations were conducted using the CMAQ(Community Multiscale Air Quality)model during April-October 2018.Ecological O_(3)exposure was estimated using six indices(i.e.,M7,M24,N100,SUM60,W126,and AOT40f).The results show that the temperature rise increases the MDA8 O_(3)(maximum daily eight-hour average O_(3))concentrations by∼3 ppb and the number of O_(3)exceedance days by 10-20 days in the North China Plain(NCP),Yangtze River Delta(YRD),and Sichuan Basin(SCB)regions.All O_(3)exposure indices show substantial increases.M24 and M7 in eastern and southern China will rise by 1-3 ppb and 2-4 ppb,respectively.N100 increases by more than 120 h in the surrounding regions of Beijing.SUM60 increases by greater than 9 ppm h^(−1),W126 increases by greater than 15 ppm h^(−1)in Shaanxi and SCB,and AOT40f increases by 6 ppm h^(−1)in NCP and SCB.The temperature increase also promotes atmospheric oxidation capacity(AOC)levels,with the higher AOC contributed by OH radicals in southern China but by NO_(3)radicals in northern China.The change in the reaction rate caused by the temperature increase has a greater influence on O_(3)exposure and AOC than the change in BVOC emissions.展开更多
RuO_(2) has been considered a potential alternative to commercial IrO_(2) for the oxygen evolution reaction(OER)due to its superior intrinsic activity.However,its inherent structure dissolution in acidic environments ...RuO_(2) has been considered a potential alternative to commercial IrO_(2) for the oxygen evolution reaction(OER)due to its superior intrinsic activity.However,its inherent structure dissolution in acidic environments restricts its commercial applications.In this study,we report a novel Pd-doped ruthenium oxide(Pd–RuO_(2))nanosheet catalyst that exhibits improved activity and stability through a synergistic effect of Pd modulation of Ru electronic structure and the two-dimensional structure.The catalyst exhibits excellent performance,achieving an overpotential of only 204 mVat a current density of 10 mA cm^(-2).Impressively,after undergoing 8000 cycles of cyclic voltammetry testing,the overpotential merely decreased by 5 mV.The PEM electrolyzer with Pd0.08Ru0.92O_(2) as an anode catalyst survived an almost 130 h operation at 200 mA cm^(-2).To elucidate the underlying mechanisms responsible for the enhanced stability,we conducted an X-ray photoelectron spectroscopy(XPS)analysis,which reveals that the electron transfer from Pd to Ru effectively circumvents the over-oxidation of Ru,thus playing a crucial role in enhancing the catalyst's stability.Furthermore,density functional theory(DFT)calculations provide compelling evidence that the introduction of Pd into RuO_(2) effectively modulates electron correlations and facilitates the electron transfer from Pd to Ru,thereby preventing the overoxidation of Ru.Additionally,the application of the two-dimensional structure effectively inhibited the aggregation and growth of nanoparticles,further bolstering the structural integrity of the catalyst.展开更多
Exploring noble metal-free catalyst materials for high efficient electrochemical water splitting to produce hydrogen is strongly desired for renewable energy development.In this article,a novel bifunctional catalytic ...Exploring noble metal-free catalyst materials for high efficient electrochemical water splitting to produce hydrogen is strongly desired for renewable energy development.In this article,a novel bifunctional catalytic electrode of insitu-grown type for alkaline water splitting based on FeCoNi alloy substrate has been successfully prepared via a facile one-step hydrothermal oxidation route in an alkaline hydrogen peroxide medium.It shows that the matrix alloy with the atom ratio 4∶3∶3 of Fe∶Co∶Ni can obtain the best catalytic performance when hydrothermally treated at 180℃for 18 h in the solution containing 1.8 M hydrogen peroxide and 3.6 M sodium hydroxide.The as-prepared Fe_(0.4)Co_(0.3)Ni_(0.3)-1.8 electrode exhibits small overpotentials of only 184 and 175 mV at electrolysis current density of 10 mA cm^(-2)for alkaline OER and HER processes,respectively.The overall water splitting at electrolysis current density of 10 mA cm^(-2)can be stably delivered at a low cell voltage of 1.62 V.These characteristics including the large specific surface area,the high surface nickel content,the abundant catalyst species,the balanced distribution between bivalent and trivalent metal ions,and the strong binding of in-situ naturally growed catalytic layer to matrix are responsible for the prominent catalytic performance of the Fe_(0.4)Co_(0.3)Ni_(0.3)-1.8 electrode,which can act as a possible replacement for expensive noble metal-based materials.展开更多
Co-Ni-based superalloys are known for their capability to function at elevated temperatures and superior hot corrosion and thermal fatigue resistance.Therefore,these alloys show potential as crucial high-temperature s...Co-Ni-based superalloys are known for their capability to function at elevated temperatures and superior hot corrosion and thermal fatigue resistance.Therefore,these alloys show potential as crucial high-temperature structural materials for aeroengine and gas turbine hot-end components.Our previous work elucidated the influence of Ti and Ta on the high-temperature mechanical properties of alloys.However,the intricate interaction among elements considerably affects the oxidation resistance of alloys.In this paper,Co-35Ni-10Al-2W-5Cr-2Mo-1Nb-xTi-(5−x)Ta alloys(x=1,2,3,4)with varying Ti and Ta contents were designed and compounded,and their oxidation resistance was investigated at the temperature range from 800 to 1000℃.After oxidation at three test conditions,namely,800℃for 200 h,900℃for 200 h,and 1000℃for 50 h,the main structure of the oxide layer of the alloy consisted of spinel,Cr_(2)O_(3),and Al_(2)O_(3)from outside to inside.Oxides consisting of Ta,W,and Mo formed below the Cr_(2)O_(3)layer.The interaction of Ti and Ta imparted the highest oxidation resistance to 3Ti2Ta alloy.Conversely,an excessive amount of Ti or Ta resulted in an adverse effect on the oxidation resistance of the alloys.This study reports the volatilization of W and Mo oxides during the oxidation process of Co-Ni-based cast superalloys with a high Al content for the first time and explains the formation mechanism of holes in the oxide layer.The results provide a basis for gaining insights into the effects of the interaction of alloying elements on the oxidation resistance of the alloys they form.展开更多
Currently,there is a lack of effective medicines capable of halting or reve rsing the progression of neurodegenerative disorde rs,including amyotrophic lateral sclerosis,Parkinson s disease,multiple sclerosis,or Alzhe...Currently,there is a lack of effective medicines capable of halting or reve rsing the progression of neurodegenerative disorde rs,including amyotrophic lateral sclerosis,Parkinson s disease,multiple sclerosis,or Alzheimer s disease.Given the unmet medical need,it is necessary to reevaluate the existing para digms of how to to rget these diseases.When considering neurodegenerative diseases from a systemic neurometabolic perspective,it becomes possible to explain the shared pathological features.This innovative approach presented in this paper draws upon exte nsive research conducted by the authors and researchers worldwide.In this review,we highlight the importance of metabolic mitochondrial dysfunction in the context of neurodegenerative diseases.We provide an overview of the risk factors associated with developing neurodegenerative disorders,including genetic,epigenetic,and environmental fa ctors.Additionally,we examine pathological mechanisms implicated in these diseases such as oxidative stress,accumulation of misfolded proteins,inflammation,demyelination,death of neurons,insulin resistance,dysbiosis,and neurotransmitter disturbances.Finally,we outline a proposal for the restoration of mitochondrial metabolism,a crucial aspect that may hold the key to facilitating curative therapeutic interventions for neurodegenerative disorders in forthcoming advancements.展开更多
Laser powder bed fusion(L-PBF)has been employed to additively manufacture WE43 magnesium(Mg)alloy biodegradable implants,but WE43 L-PBF samples exhibit excessively rapid corrosion.In this work,dense WE43 L-PBF samples...Laser powder bed fusion(L-PBF)has been employed to additively manufacture WE43 magnesium(Mg)alloy biodegradable implants,but WE43 L-PBF samples exhibit excessively rapid corrosion.In this work,dense WE43 L-PBF samples were built with the relativity density reaching 99.9%.High temperature oxidation was performed on the L-PBF samples in circulating air via various heating temperatures and holding durations.The oxidation and diffusion at the elevated temperature generated a gradient structure composed of an oxide layer at the surface,a transition layer in the middle and the matrix.The oxide layer consisted of rare earth(RE)oxides,and became dense and thick with increasing the holding duration.The matrix was composed ofα-Mg,RE oxides and Mg_(24)RE_(5) precipitates.The precipitates almost disappeared in the transition layer.Enhanced passivation effect was observed in the samples treated by a suitable high temperature oxidation.The original L-PBF samples lost 40%weight after 3-day immersion in Hank’s solution,and broke into fragments after 7-day immersion.The casted and solution treated samples lost roughly half of the weight after 28-day immersion.The high temperature oxidation samples,which were heated at 525℃ for 8 h,kept the structural integrity,and lost only 6.88%weight after 28-day immersion.The substantially improved corrosion resistance was contributed to the gradient structure at the surface.On one hand,the outmost dense layer of RE oxides isolated the corrosive medium;on the other hand,the transition layer considerably inhibited the corrosion owing to the lack of precipitates.Overall,high temperature oxidation provides an efficient,economic and safe approach to inhibit the corrosion of WE43 L-PBF samples,and has promising prospects for future clinical applications.展开更多
Electrocatalytic hydrogen production from seawater holds enormous promise for clean energy generation.Nevertheless,the direct electrolysis of seawater encounters significant challenges due to poor anodic stability cau...Electrocatalytic hydrogen production from seawater holds enormous promise for clean energy generation.Nevertheless,the direct electrolysis of seawater encounters significant challenges due to poor anodic stability caused by detrimental chlorine chemistry.Herein,we present our recent discovery that the incorporation of Ce into Ni Fe layered double hydroxide nanosheet array on Ni foam(Ce-Ni Fe LDH/NF)emerges as a robust electrocatalyst for seawater oxidation.During the seawater oxidation process,CeO_(2)is generated,effectively repelling Cl^(-)and inhibiting the formation of Cl O-,resulting in a notable enhancement in the oxidation activity and stability of alkaline seawater.The prepared Ce-Ni Fe LDH/NF requires only overpotential of 390 m V to achieve the current density of 1 A cm^(-2),while maintaining long-term stability for 500 h,outperforming the performance of Ni Fe LDH/NF(430 m V,150 h)by a significant margin.This study highlights the effectiveness of a Ce-doping strategy in augmenting the activity and stability of materials based on Ni Fe LDH in seawater electrolysis for oxygen evolution.展开更多
Transition metal chalcogenides(TMCs)are recognized as pre-catalysts,and their(oxy)hydroxides derived from electrochemical reconstruction are the active species in the water oxidation.However,understanding the role of ...Transition metal chalcogenides(TMCs)are recognized as pre-catalysts,and their(oxy)hydroxides derived from electrochemical reconstruction are the active species in the water oxidation.However,understanding the role of the residual chalcogen in the reconstructed layer is lacking in detail,and the corresponding catalytic mechanism remains controversial.Here,taking Cu_(1-x)Co_(x)S as a platform,we explore the regulating effect and existence form of the residual S doped into the reconstructive layer for oxygen evolution reaction(OER),where a dual-path OER mechanism is proposed.First-principles calculations and operando~(18)O isotopic labeling experiments jointly reveal that the residual S in the reconstructive layer of Cu_(1-x)Co_(x)S can wisely balance the adsorbate evolution mechanism(AEM)and lattice oxygen oxidation mechanism(LOM)by activating lattice oxygen and optimizing the adsorption/desorption behaviors at metal active sites,rather than change the reaction mechanism from AEM to LOM.Following such a dual-path OER mechanism,Cu_(0.4)Co_(0.6)S-derived Cu_(0.4)Co_(0.6)OSH not only overcomes the restriction of linear scaling relationship in AEM,but also avoids the structural collapse caused by lattice oxygen migration in LOM,so as to greatly reduce the OER potential and improved stability.展开更多
The surface properties of oxidic supports and their interaction with the supported metals play critical roles in governing the catalytic activities of oxide‐supported metal catalysts.When metals are supported on redu...The surface properties of oxidic supports and their interaction with the supported metals play critical roles in governing the catalytic activities of oxide‐supported metal catalysts.When metals are supported on reducible oxides,dynamic surface reconstruction phenomena,including strong metal–support interaction(SMSI)and oxygen vacancy formation,complicate the determination of the structural–functional relationship at the active sites.Here,we performed a systematic investigation of the dynamic behavior of Au nanocatalysts supported on flame‐synthesized TiO_(2),which takes predominantly a rutile phase,using CO oxidation above room temperature as a probe reaction.Our analysis conclusively elucidated a negative correlation between the catalytic activity of Au/TiO_(2) and the oxygen vacancy at the Au/TiO_(2) interface.Although the reversible formation and retracting of SMSI overlayers have been ubiquitously observed on Au/TiO_(2) samples,the catalytic consequence of SMSI remains inconclusive.Density functional theory suggests that the electron transfer from TiO_(2) to Au is correlated to the presence of the interfacial oxygen vacancies,retarding the catalytic activation of CO oxidation.展开更多
Vegetable oils are a source of energy, essential fatty acids, antioxidants and fat-soluble vitamins useful for human health care and development. These oils also contribute to organoleptic quality of their products’ ...Vegetable oils are a source of energy, essential fatty acids, antioxidants and fat-soluble vitamins useful for human health care and development. These oils also contribute to organoleptic quality of their products’ derivatives. However, their chemical and physical properties can be modified by the mode of their extraction, storage and distribution. These modifications might negatively affect the nutritional quality of the oils. The goals of this study were to: sample different vegetable oils for cosmetic or dietary use marketed in Cameroon, and verify purity and oxidation states of each kind of oil through determination of its acidity, iodine, peroxide, saponification, refractive indexes and the conformity of the labeling. The carotene content, the level of polar components and specific absorbance were also determined. As the result, six oils namely palm, palm kernel, coconut, black cumin, peanut and shea butter were collected. Apart from labeling, chemicals and physicals parameters analyzed were generally in accordance with the Cameroonian and Codex Alimentarius standard. This study suggests that vegetable oils sampled in the Cameroonian market may not expose consumers to lipid oxidation products generating pathological oxidative stress and inflammation. However, efforts in application of existing standard need to be done as far as labeling are concerned.展开更多
基金supported by the National Natural Science Foundation of China,Nos.82204360(to HM)and 82270411(to GW)National Science and Technology Innovation 2030 Major Program,No.2021ZD0200900(to YL)。
文摘Traumatic brain injury involves complex pathophysiological mechanisms,among which oxidative stress significantly contributes to the occurrence of secondary injury.In this study,we evaluated hypidone hydrochloride(YL-0919),a self-developed antidepressant with selective sigma-1 receptor agonist properties,and its associated mechanisms and targets in traumatic brain injury.Behavioral experiments to assess functional deficits were followed by assessment of neuronal damage through histological analyses and examination of blood-brain barrier permeability and brain edema.Next,we investigated the antioxidative effects of YL-0919 by assessing the levels of traditional markers of oxidative stress in vivo in mice and in vitro in HT22 cells.Finally,the targeted action of YL-0919 was verified by employing a sigma-1 receptor antagonist(BD-1047).Our findings demonstrated that YL-0919 markedly improved deficits in motor function and spatial cognition on day 3 post traumatic brain injury,while also decreasing neuronal mortality and reversing blood-brain barrier disruption and brain edema.Furthermore,YL-0919 effectively combated oxidative stress both in vivo and in vitro.The protective effects of YL-0919 were partially inhibited by BD-1047.These results indicated that YL-0919 relieved impairments in motor and spatial cognition by restraining oxidative stress,a neuroprotective effect that was partially reversed by the sigma-1 receptor antagonist BD-1047.YL-0919 may have potential as a new treatment for traumatic brain injury.
基金financially supported by the National Key R&D Program of China (No.2021YFB3700400)the National Natural Science Foundation of China (Nos.52074030,51904021,and 52174294)。
文摘A high thrust-to-weight ratio poses challenges to the high-temperature performance of Ni-based superalloys. The oxidation behavior of GH4738 at extreme temperatures has been investigated by isothermal and non-isothermal experiments. As a result of the competitive diffusion of alloying elements, the oxide scale included an outermost porous oxide layer (OOL), an inner relatively dense oxide layer (IOL), and an internal oxide zone (IOZ), depending on the temperature and time. A high temperature led to the formation of large voids at the IOL/IOZ interface. At 1200℃, the continuity of the Cr-rich oxide layer in the IOL was destroyed, and thus, spallation occurred. Extension of oxidation time contributed to the size of Al-rich oxide particles with the increase in the IOZ. Based on this finding,the oxidation kinetics of GH4738 was discussed, and the corresponding oxidation behavior at 900-1100℃ was predicted.
基金supported by the National Projects of the National Research Foundation(NRF)funded by Republic of Korea(#2022R1F1A1072739 and#2022R1A2C1004392)Prof.Nashrah is also grateful for financial supports by the YU Infra-Project in conjunction with BK21 FOUR National Program(#222A251009)by the Nano-Fab-NRF grant funded by Republic of Korea(#2009-0082580).
文摘The trade-off between efficiency and stability has limited the application of TiO_(2)as a catalyst due to its poor surface reactivity.Here,we present a modification of a TiO_(2)layer with highly stable Sub-5 nm Fe_(2)O_(3)nanoparticles(NP)by modulating its structure-surface reactivity relationship to attain efficiency-stability balance via a voltage-assisted oxidation approach.In situ simultaneous oxidation of the Ti substrate and Fe precursor using high-energy plasma driven by high voltage resulted in uniform distribution of Fe_(2)O_(3)NP embedded within porous TiO_(2)layer.Comprehensive surface characterizations with density functional theory demonstrated an improved electronic transition in TiO_(2)due to the presence of surface defects from reactive oxygen species and possible charge transfer from Ti to Fe;it also unexpectedly increased the active site in the TiO_(2)layer due to uncoordinated electrons in Sub-5 nm Fe_(2)O_(3)NP/TiO_(2)catalyst,thereby enhancing the adsorption of chemical functional groups on the catalyst.This unique embedded structure exhibited remarkable improvement in reducing 4-nitrophenol to 4-aminophenol,achieving approximately 99%efficiency in 20 min without stability decay after 20 consecutive cycles,outperforming previously reported TiO_(2)-based catalysts.This finding proposes a modified-electrochemical strategy enabling facile construction of TiO_(2)with nanoscale oxides extandable to other metal oxide systems.
基金supported by the National Key Research and Development Program of China (Grant No.2018YFE0203802)Natural Science Foundation of Hubei Province, China (Grant No.2022CFA031)Dongguan Innovative Research Team Program (2020607101007)。
文摘Owing to the advantages of simple structure,low power consumption and high-density integration,memristors or memristive devices are attracting increasing attention in the fields such as next generation non-volatile memories,neuromorphic computation and data encryption.However,the deposition of memristive films often requires expensive equipment,strict vacuum conditions,high energy consumption,and extended processing times.In contrast,electrochemical anodizing can produce metal oxide films quickly(e.g.10 s) under ambient conditions.By means of the anodizing technique,oxide films,oxide nanotubes,nanowires and nanodots can be fabricated to prepare memristors.Oxide film thickness,nanostructures,defect concentrations,etc,can be varied to regulate device performances by adjusting oxidation parameters such as voltage,current and time.Thus memristors fabricated by the anodic oxidation technique can achieve high device consistency,low variation,and ultrahigh yield rate.This article provides a comprehensive review of the research progress in the field of anodic oxidation assisted fabrication of memristors.Firstly,the principle of anodic oxidation is introduced;then,different types of memristors produced by anodic oxidation and their applications are presented;finally,features and challenges of anodic oxidation for memristor production are elaborated.
基金supported by the National Natural Science Foundation of China(Nos.82170426 and 22078193)Double Thousand Plan of Jiangxi Province(Nos.461654,jxsq2019102052).
文摘Electrocatalytic glucose oxidation reaction(GOR)has attracted much attention owing to its crucial role in biofuel cell fabrication.Herein,we load MoO_(3)nanoparticles on carbon nanotubes(CNTs)and use a discharge process to prepare a noblemetal-free MC-60 catalyst containing MoO_(3),Mo_(2)C,and a Mo_(2)C–MoO_(3)interface.In the GOR,MC-60 shows activity as high as 745μA/(mmol/L cm^(2)),considerably higher than those of the Pt/CNT(270μA/(mmol/L cm^(2)))and Au/CNT catalysts(110μA/(mmol/L cm^(2))).In the GOR,the response minimum on MC-60 is as low as 8μmol/L,with a steady-state response time of only 3 s.Moreover,MC-60 has superior stability and anti-interference ability to impurities in the GOR.The better performance of MC-60 in the GOR is attributed to the abundant Mo sites bonding to C and O atoms at the MoO_(3)–Mo_(2)C interface.These Mo sites create active sites for promoting glucose adsorption and oxidation,enhancing MC-60 performance in the GOR.Thus,these results help to fabricate more effi cient noble-metal-free catalysts for the fabrication of glucose-based biofuel cells.
基金The authors gratefully acknowledge the financial support of the Natural Science Foundation of China,China(Grant No.21975082 and 21736003)the Guangdong Basic and Applied Basic Research Foundation(Grant Number:2019A1515011472 and 2022A1515011341)the Science and Technology Program of Guangzhou(Grant Number:202102080479).
文摘In order to better understand the specific substituent effects on the electrochemical oxidation process of β-O-4 bond, a series of methoxyphenyl type β-O-4 dimer model compounds with different localized methoxyl groups, including 2-(2-methoxyphenoxy)-1-phenylethanone, 2-(2-methoxyphenoxy)-1-phenylethanol, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2-methoxyphenoxy)-1-(4-methoxyphenyl)ethanol, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanone, 2-(2,6-dimethoxyphenoxy)-1-(4-methoxyphenyl)ethanol have been selected and their electrochemical properties have been studied experimentally by cyclic voltammetry, and FT-IR spectroelectrochemistry. Combining with electrolysis products distribution analysis and density functional theory calculations, oxidation mechanisms of all six model dimers have been explored. In particular, a total effect from substituents of both para-methoxy(on the aryl ring closing to Cα) and Cα-OH on the oxidation mechanisms has been clearly observed, showing a significant selectivity on the Cα-Cβbond cleavage induced by electrochemical oxidations.
基金supported by the National Natural Science Foundation of China (Grant Nos.52072272,52171145 and 22109120)the Zhejiang Provincial Natural Science Foundation of China (LQ21B030002)+1 种基金the Zhejiang Provincial Special Support Program for High-level Talents (2019R52042)the Key programs for Science and Technology Innovation of Wenzhou (ZG2022037)。
文摘The scarcity,high cost and susceptibility to CO of Platinum severely restrict its application in alkaline hydrogen oxidation reaction(HOR).Hybridizing Pt with other transition metals provides an effective strategy to modulate its catalytic HOR performance,but at the cost of mass activity due to the coverage of modifiers on Pt surface.Herein,we constructed dual junctions'Pt/nitrogen-doped carbon(Pt/NC)andδ-MoC/NC to modify electronic structure of Pt via interfacial electron transfer to acquire Pt-MoC@NC catalyst with electron-deficient Pt nanoparticles,simultaneously endowing it with high mass activity and durability of alkaline HOR.Moreover,the unique structure of Pt-MoC@NC endows Pt with a high COtolerance at 1,000 ppm CO/H_(2),a quality that commercial Pt-C catalyst lacks.The theoretical calculations not only confirm the diffusion of electrons from Pt/NC to Mo C/NC could occur,but also demonstrate the negative shift of Pt d-band center for the optimized binding energies of*H,*OH and CO.
基金supported by the Central South University Scientific Research Foundation for Post-doctor(Grant No.:140050052)the National Natural Science Foundation of China(Grant No.:52204325)
文摘Owing to the intrinsically sluggish kinetics of urea oxidation reaction(UOR)involving a six-electron transfer process,developing efficient UOR electrocatalyst is a great challenge remained to be overwhelmed.Herein,by taking advantage of 2-Methylimidazole,of which is a kind of alkali in water and owns strong coordination ability to Co^(2+)in methanol,trace Co(1.0 mol%)addition was found to induce defect engineering onα-Ni(OH)_(2)in a dual-solvent system of water and methanol.Physical characterization results revealed that the synthesized electrocatalyst(WM-Ni_(0.99)Co_(0.01)(OH)_(2))was a kind of defective nanosheet with thickness around 5-6 nm,attributing to the synergistic effect of Co doping and defect engineering,its electron structure was finely altered,and its specific surface a rea was tremendously enlarged from 68 to 172.3 m^(2)g^(-1).With all these merits,its overpotential to drive 10 mA cm^(-2)was reduced by 110 mV.Besides,the interfacial behavior of UOR was also well deciphered by operando electrochemical impedance spectroscopy.
基金financial support from the National Natural Science Foundation of China(52203070)the Open Fund of State Key Laboratory of New Textile Materials and Advanced Processing Technologies(FZ2022005)+2 种基金the Open Fund of Hubei Key Laboratory of Biomass Fiber and Ecological Dyeing and Finishing(STRZ202203)the financial support provided by the China Scholarship Council(CSC)Visiting Scholar Programfinancial support from Institute for Sustainability,Energy and Resources,The University of Adelaide,Future Making Fellowship。
文摘Urea holds promise as an alternative water-oxidation substrate in electrolytic cells.High-valence nickelbased spinel,especially after heteroatom doping,excels in urea oxidation reactions(UOR).However,traditional spinel synthesis methods with prolonged high-temperature reactions lack kinetic precision,hindering the balance between controlled doping and highly active two-dimensional(2D)porous structures design.This significantly impedes the identification of electron configuration-dependent active sites in doped 2D nickel-based spinels.Herein,we present a microwave shock method for the preparation of 2D porous NiCo_(2)O_(4)spinel.Utilizing the transient on-off property of microwave pulses for precise heteroatom doping and 2D porous structural design,non-metal doping(boron,phosphorus,and sulfur)with distinct extranuclear electron disparities serves as straightforward examples for investigation.Precise tuning of lattice parameter reveals the impact of covalent bond strength on NiCo_(2)O_(4)structural stability.The introduced defect levels induce unpaired d-electrons in transition metals,enhancing the adsorption of electron-donating amino groups in urea molecules.Simultaneously,Bode plots confirm the impact mechanism of rapid electron migration caused by reduced band gaps on UOR activity.The prepared phosphorus-doped 2D porous NiCo_(2)O_(4),with optimal electron configuration control,outperforms most reported spinels.This controlled modification strategy advances understanding theoretical structure-activity mechanisms of high-performance 2D spinels in UOR.
基金supported by the National Natural Science Foundation of China(21872040,22162004)the Excellent Scholars and Innovation Team of Guangxi Universities,the Innovation Project of Guangxi Graduate Education(YCBZ2022038)the High-performance Computing Platform of Guangxi University.
文摘Exploitation of oxygen evolution reaction(OER)and urea oxidation reaction(UOR)catalysts with high activity and stability at large current density is a major challenge for energy-saving H_(2) production in water electrolysis.Herein,we use the pyridinic-N doping carbon layers coupled with tensile strain of FeNi alloy activated by NiFe_(2)O_(4)(FeNi/NiFe_(2)O_(4)@NC)for efficiently increasing the performance of water and urea oxidation.Due to the tensile strain effect on FeNi/NiFe_(2)O_(4)@NC,it provides a favorable modulation on the electronic properties of the active center,thus enabling amazing OER(η_(100)=196 mV)and UOR(E_(10)=1.32 V)intrinsic activity.Besides,the carbon-coated layers can be used as armor to prevent FeNi alloy from being corroded by the electrolyte for enhancing the OER/UOR stability at large current density,showing high industrial practicability.This work thus provides a simple way to prepare high-efficiency catalyst for activating water and urea oxidation.
基金supported by the National Natural Science Foundation of China[grant numbers 42277095 and 42021004].
文摘Surface ozone(O_(3))poses significant threats to public health,agricultural crops,and plants in natural ecosystems.Global warming is likely to increase future O_(3)mainly by altering atmospheric photochemical reactions and enhancing biogenic volatile organic compound(BVOC)emissions.To assess the impacts of the future 1.5 K climate target on O_(3)concentrations and ecological O_(3)exposure in China,numerical simulations were conducted using the CMAQ(Community Multiscale Air Quality)model during April-October 2018.Ecological O_(3)exposure was estimated using six indices(i.e.,M7,M24,N100,SUM60,W126,and AOT40f).The results show that the temperature rise increases the MDA8 O_(3)(maximum daily eight-hour average O_(3))concentrations by∼3 ppb and the number of O_(3)exceedance days by 10-20 days in the North China Plain(NCP),Yangtze River Delta(YRD),and Sichuan Basin(SCB)regions.All O_(3)exposure indices show substantial increases.M24 and M7 in eastern and southern China will rise by 1-3 ppb and 2-4 ppb,respectively.N100 increases by more than 120 h in the surrounding regions of Beijing.SUM60 increases by greater than 9 ppm h^(−1),W126 increases by greater than 15 ppm h^(−1)in Shaanxi and SCB,and AOT40f increases by 6 ppm h^(−1)in NCP and SCB.The temperature increase also promotes atmospheric oxidation capacity(AOC)levels,with the higher AOC contributed by OH radicals in southern China but by NO_(3)radicals in northern China.The change in the reaction rate caused by the temperature increase has a greater influence on O_(3)exposure and AOC than the change in BVOC emissions.
基金supported by the National Natural Science Foundation of China(No.22209035)the Major Science and Technology Projects of Yunnan Province(No.202302AH360001)the Natural Science Foundation of Hebei Province(No.E2020202091).
文摘RuO_(2) has been considered a potential alternative to commercial IrO_(2) for the oxygen evolution reaction(OER)due to its superior intrinsic activity.However,its inherent structure dissolution in acidic environments restricts its commercial applications.In this study,we report a novel Pd-doped ruthenium oxide(Pd–RuO_(2))nanosheet catalyst that exhibits improved activity and stability through a synergistic effect of Pd modulation of Ru electronic structure and the two-dimensional structure.The catalyst exhibits excellent performance,achieving an overpotential of only 204 mVat a current density of 10 mA cm^(-2).Impressively,after undergoing 8000 cycles of cyclic voltammetry testing,the overpotential merely decreased by 5 mV.The PEM electrolyzer with Pd0.08Ru0.92O_(2) as an anode catalyst survived an almost 130 h operation at 200 mA cm^(-2).To elucidate the underlying mechanisms responsible for the enhanced stability,we conducted an X-ray photoelectron spectroscopy(XPS)analysis,which reveals that the electron transfer from Pd to Ru effectively circumvents the over-oxidation of Ru,thus playing a crucial role in enhancing the catalyst's stability.Furthermore,density functional theory(DFT)calculations provide compelling evidence that the introduction of Pd into RuO_(2) effectively modulates electron correlations and facilitates the electron transfer from Pd to Ru,thereby preventing the overoxidation of Ru.Additionally,the application of the two-dimensional structure effectively inhibited the aggregation and growth of nanoparticles,further bolstering the structural integrity of the catalyst.
基金supported by the Overseas Expertise Introduction Center for Discipline Innovation(D18025)National Nature Science Foundation of China(Grant No.41931295)
文摘Exploring noble metal-free catalyst materials for high efficient electrochemical water splitting to produce hydrogen is strongly desired for renewable energy development.In this article,a novel bifunctional catalytic electrode of insitu-grown type for alkaline water splitting based on FeCoNi alloy substrate has been successfully prepared via a facile one-step hydrothermal oxidation route in an alkaline hydrogen peroxide medium.It shows that the matrix alloy with the atom ratio 4∶3∶3 of Fe∶Co∶Ni can obtain the best catalytic performance when hydrothermally treated at 180℃for 18 h in the solution containing 1.8 M hydrogen peroxide and 3.6 M sodium hydroxide.The as-prepared Fe_(0.4)Co_(0.3)Ni_(0.3)-1.8 electrode exhibits small overpotentials of only 184 and 175 mV at electrolysis current density of 10 mA cm^(-2)for alkaline OER and HER processes,respectively.The overall water splitting at electrolysis current density of 10 mA cm^(-2)can be stably delivered at a low cell voltage of 1.62 V.These characteristics including the large specific surface area,the high surface nickel content,the abundant catalyst species,the balanced distribution between bivalent and trivalent metal ions,and the strong binding of in-situ naturally growed catalytic layer to matrix are responsible for the prominent catalytic performance of the Fe_(0.4)Co_(0.3)Ni_(0.3)-1.8 electrode,which can act as a possible replacement for expensive noble metal-based materials.
基金the National Major Science and Technology Projects of China(Nos.J2019-VII-0010-0150 and J2019-VI-0009-0123)National Natural Science Foundation of China(Nos.52022011 and 52090041)+3 种基金Beijing Nova Program(No.Z211100002121170)Science Center for Gas Turbine Project(No.P2021-A-IV-001-002)Science and Technology on Advanced High Temperature Structural Materials Laboratory(No.6142903210306)Xiaomi Young Scholars Program.
文摘Co-Ni-based superalloys are known for their capability to function at elevated temperatures and superior hot corrosion and thermal fatigue resistance.Therefore,these alloys show potential as crucial high-temperature structural materials for aeroengine and gas turbine hot-end components.Our previous work elucidated the influence of Ti and Ta on the high-temperature mechanical properties of alloys.However,the intricate interaction among elements considerably affects the oxidation resistance of alloys.In this paper,Co-35Ni-10Al-2W-5Cr-2Mo-1Nb-xTi-(5−x)Ta alloys(x=1,2,3,4)with varying Ti and Ta contents were designed and compounded,and their oxidation resistance was investigated at the temperature range from 800 to 1000℃.After oxidation at three test conditions,namely,800℃for 200 h,900℃for 200 h,and 1000℃for 50 h,the main structure of the oxide layer of the alloy consisted of spinel,Cr_(2)O_(3),and Al_(2)O_(3)from outside to inside.Oxides consisting of Ta,W,and Mo formed below the Cr_(2)O_(3)layer.The interaction of Ti and Ta imparted the highest oxidation resistance to 3Ti2Ta alloy.Conversely,an excessive amount of Ti or Ta resulted in an adverse effect on the oxidation resistance of the alloys.This study reports the volatilization of W and Mo oxides during the oxidation process of Co-Ni-based cast superalloys with a high Al content for the first time and explains the formation mechanism of holes in the oxide layer.The results provide a basis for gaining insights into the effects of the interaction of alloying elements on the oxidation resistance of the alloys they form.
文摘Currently,there is a lack of effective medicines capable of halting or reve rsing the progression of neurodegenerative disorde rs,including amyotrophic lateral sclerosis,Parkinson s disease,multiple sclerosis,or Alzheimer s disease.Given the unmet medical need,it is necessary to reevaluate the existing para digms of how to to rget these diseases.When considering neurodegenerative diseases from a systemic neurometabolic perspective,it becomes possible to explain the shared pathological features.This innovative approach presented in this paper draws upon exte nsive research conducted by the authors and researchers worldwide.In this review,we highlight the importance of metabolic mitochondrial dysfunction in the context of neurodegenerative diseases.We provide an overview of the risk factors associated with developing neurodegenerative disorders,including genetic,epigenetic,and environmental fa ctors.Additionally,we examine pathological mechanisms implicated in these diseases such as oxidative stress,accumulation of misfolded proteins,inflammation,demyelination,death of neurons,insulin resistance,dysbiosis,and neurotransmitter disturbances.Finally,we outline a proposal for the restoration of mitochondrial metabolism,a crucial aspect that may hold the key to facilitating curative therapeutic interventions for neurodegenerative disorders in forthcoming advancements.
基金funded by the National Key Research and Development Program of China (2018YFE0104200)National Natural Science Foundation of China (51875310, 52175274, 82172065)Tsinghua Precision Medicine Foundation
文摘Laser powder bed fusion(L-PBF)has been employed to additively manufacture WE43 magnesium(Mg)alloy biodegradable implants,but WE43 L-PBF samples exhibit excessively rapid corrosion.In this work,dense WE43 L-PBF samples were built with the relativity density reaching 99.9%.High temperature oxidation was performed on the L-PBF samples in circulating air via various heating temperatures and holding durations.The oxidation and diffusion at the elevated temperature generated a gradient structure composed of an oxide layer at the surface,a transition layer in the middle and the matrix.The oxide layer consisted of rare earth(RE)oxides,and became dense and thick with increasing the holding duration.The matrix was composed ofα-Mg,RE oxides and Mg_(24)RE_(5) precipitates.The precipitates almost disappeared in the transition layer.Enhanced passivation effect was observed in the samples treated by a suitable high temperature oxidation.The original L-PBF samples lost 40%weight after 3-day immersion in Hank’s solution,and broke into fragments after 7-day immersion.The casted and solution treated samples lost roughly half of the weight after 28-day immersion.The high temperature oxidation samples,which were heated at 525℃ for 8 h,kept the structural integrity,and lost only 6.88%weight after 28-day immersion.The substantially improved corrosion resistance was contributed to the gradient structure at the surface.On one hand,the outmost dense layer of RE oxides isolated the corrosive medium;on the other hand,the transition layer considerably inhibited the corrosion owing to the lack of precipitates.Overall,high temperature oxidation provides an efficient,economic and safe approach to inhibit the corrosion of WE43 L-PBF samples,and has promising prospects for future clinical applications.
基金support from the Free Exploration Project of Frontier Technology for Laoshan Laboratory(No.16-02)the National Natural Science Foundation of China(Nos.22072015 and 21927811)。
文摘Electrocatalytic hydrogen production from seawater holds enormous promise for clean energy generation.Nevertheless,the direct electrolysis of seawater encounters significant challenges due to poor anodic stability caused by detrimental chlorine chemistry.Herein,we present our recent discovery that the incorporation of Ce into Ni Fe layered double hydroxide nanosheet array on Ni foam(Ce-Ni Fe LDH/NF)emerges as a robust electrocatalyst for seawater oxidation.During the seawater oxidation process,CeO_(2)is generated,effectively repelling Cl^(-)and inhibiting the formation of Cl O-,resulting in a notable enhancement in the oxidation activity and stability of alkaline seawater.The prepared Ce-Ni Fe LDH/NF requires only overpotential of 390 m V to achieve the current density of 1 A cm^(-2),while maintaining long-term stability for 500 h,outperforming the performance of Ni Fe LDH/NF(430 m V,150 h)by a significant margin.This study highlights the effectiveness of a Ce-doping strategy in augmenting the activity and stability of materials based on Ni Fe LDH in seawater electrolysis for oxygen evolution.
基金supported by the Science and Technology Research Program of Chongqing Municipal Education Commission(KJQN202200550)the Natural Science Foundation Joint Fund for Innovation and Development of Chongqing Municipal Education Commission(CSTB2022NSCQ-LZX0077)+4 种基金the National Natural Science Foundation of China(No.52100065)the Science and Technology Research Program of Natural Science Foundation of Chongqing(cstc2021ycjh-bgzxm0037)the Science and Technology Research Program of Chongqing Municipal Education Commission(KJZD-M202200503)the Chongqing Innovation Research Group Project(No.CXQT21015)the Doctor Start/Talent Introduction Program of Chongqing Normal University(No.02060404/2020009000321)。
文摘Transition metal chalcogenides(TMCs)are recognized as pre-catalysts,and their(oxy)hydroxides derived from electrochemical reconstruction are the active species in the water oxidation.However,understanding the role of the residual chalcogen in the reconstructed layer is lacking in detail,and the corresponding catalytic mechanism remains controversial.Here,taking Cu_(1-x)Co_(x)S as a platform,we explore the regulating effect and existence form of the residual S doped into the reconstructive layer for oxygen evolution reaction(OER),where a dual-path OER mechanism is proposed.First-principles calculations and operando~(18)O isotopic labeling experiments jointly reveal that the residual S in the reconstructive layer of Cu_(1-x)Co_(x)S can wisely balance the adsorbate evolution mechanism(AEM)and lattice oxygen oxidation mechanism(LOM)by activating lattice oxygen and optimizing the adsorption/desorption behaviors at metal active sites,rather than change the reaction mechanism from AEM to LOM.Following such a dual-path OER mechanism,Cu_(0.4)Co_(0.6)S-derived Cu_(0.4)Co_(0.6)OSH not only overcomes the restriction of linear scaling relationship in AEM,but also avoids the structural collapse caused by lattice oxygen migration in LOM,so as to greatly reduce the OER potential and improved stability.
基金Science and Technology Innovation Program of Hunan Province,Grant/Award Numbers:2020GK2070,2021RC4006Innovation‐Driven Project of Central South University,Grant/Award Number:2020CX008+3 种基金China Scholarship Council(CSC)National Key R&D Program of China,Grant/Award Number:2022YFE0105900National Natural Science Foundation of China,Grant/Award Number:52276093National Research Foundation Singapore,Grant/Award Number:CREATE。
文摘The surface properties of oxidic supports and their interaction with the supported metals play critical roles in governing the catalytic activities of oxide‐supported metal catalysts.When metals are supported on reducible oxides,dynamic surface reconstruction phenomena,including strong metal–support interaction(SMSI)and oxygen vacancy formation,complicate the determination of the structural–functional relationship at the active sites.Here,we performed a systematic investigation of the dynamic behavior of Au nanocatalysts supported on flame‐synthesized TiO_(2),which takes predominantly a rutile phase,using CO oxidation above room temperature as a probe reaction.Our analysis conclusively elucidated a negative correlation between the catalytic activity of Au/TiO_(2) and the oxygen vacancy at the Au/TiO_(2) interface.Although the reversible formation and retracting of SMSI overlayers have been ubiquitously observed on Au/TiO_(2) samples,the catalytic consequence of SMSI remains inconclusive.Density functional theory suggests that the electron transfer from TiO_(2) to Au is correlated to the presence of the interfacial oxygen vacancies,retarding the catalytic activation of CO oxidation.
文摘Vegetable oils are a source of energy, essential fatty acids, antioxidants and fat-soluble vitamins useful for human health care and development. These oils also contribute to organoleptic quality of their products’ derivatives. However, their chemical and physical properties can be modified by the mode of their extraction, storage and distribution. These modifications might negatively affect the nutritional quality of the oils. The goals of this study were to: sample different vegetable oils for cosmetic or dietary use marketed in Cameroon, and verify purity and oxidation states of each kind of oil through determination of its acidity, iodine, peroxide, saponification, refractive indexes and the conformity of the labeling. The carotene content, the level of polar components and specific absorbance were also determined. As the result, six oils namely palm, palm kernel, coconut, black cumin, peanut and shea butter were collected. Apart from labeling, chemicals and physicals parameters analyzed were generally in accordance with the Cameroonian and Codex Alimentarius standard. This study suggests that vegetable oils sampled in the Cameroonian market may not expose consumers to lipid oxidation products generating pathological oxidative stress and inflammation. However, efforts in application of existing standard need to be done as far as labeling are concerned.