BACKGROUND Anaesthetic care during upper gastrointestinal(GI)endoscopy has the unique challenge of maintaining ventilation and oxygenation via a shared upper airway.Supplemental oxygen is recommended by international ...BACKGROUND Anaesthetic care during upper gastrointestinal(GI)endoscopy has the unique challenge of maintaining ventilation and oxygenation via a shared upper airway.Supplemental oxygen is recommended by international society guidelines,however,the optimal route or rate of oxygen delivery is not known.Various oxygen delivery devices have been investigated to improve oxygenation during upper GI endoscopy,however,these are limited by commercial availability,costs and in some cases,the expertise required for insertion.Anecdotally at our centre,higher flows of supplemental oxygen can safely be delivered via an oxygenating mouthguard routinely used during upper GI endoscopic procedures.AIM To assess the incidence of hypoxaemia(SpO2<90%)in patients undergoing upper GI endoscopy receiving supplemental oxygen using an oxygenating mouthguard at 20 L/min flow compared to standard nasal cannula(SNC)at 2 L/min flow.METHODS A single centre,prospective,randomised clinical trial at two sites of an Australian tertiary hospital between October 2020 and September 2021 was conducted.Patients undergoing elective upper gastrointestinal endoscopy under deep sedation were randomised to receive supplemental oxygen via high-flow via oxygenating mouthguard(HFMG)at 20 L/min flow or SNC at 2 L/min flow.The primary outcome was the incidence of hypoxaemia of any duration measured by pulse oximetry.Intraprocedural-related,procedural-related,and sedation-related adverse events and patient-reported outcomes were also recorded.RESULTS Three hundred patients were randomised.Eight patients were excluded after randomisation.292 patients were included in the intention-to-treat analysis.The incidence of hypoxaemia was significantly reduced in those allocated HFMG.Six patients(4.4%)allocated to HFMG experienced an episode of hypoxaemia,compared to thirty-four(22.1%)patients allocated to SNC(P value<0.001).No significant difference was observed in the rates of adverse events or patient-reported outcome measures.CONCLUSION The use of HFMG offers a novel approach to reducing the incidence of hypoxaemia during short upper gastrointestinal endoscopic procedures in low-risk patients undergoing deep sedation.展开更多
Diabetic peripheral neuropathy is a common complication of diabetes mellitus.Elucidating the pathophysiological metabolic mechanism impels the generation of ideal therapies.However,existing limited treatments for diab...Diabetic peripheral neuropathy is a common complication of diabetes mellitus.Elucidating the pathophysiological metabolic mechanism impels the generation of ideal therapies.However,existing limited treatments for diabetic peripheral neuropathy expose the urgent need for cell metabolism research.Given the lack of comprehensive understanding of energy metabolism changes and related signaling pathways in diabetic peripheral neuropathy,it is essential to explore energy changes and metabolic changes in diabetic peripheral neuropathy to develop suitable treatment methods.This review summarizes the pathophysiological mechanism of diabetic peripheral neuropathy from the perspective of cellular metabolism and the specific interventions for different metabolic pathways to develop effective treatment methods.Various metabolic mechanisms(e.g.,polyol,hexosamine,protein kinase C pathway)are associated with diabetic peripheral neuropathy,and researchers are looking for more effective treatments through these pathways.展开更多
The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct ...The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct activity-stability trade-off model is full of significance but challenging.Herein,a single atom Zn stabilized RuO_(2)with enriched oxygen vacancies(SA Zn-RuO_(2))is developed as a promising alternative to iridium oxide for acidic oxygen evolution reaction(OER).Compared with commercial RuO_(2),the enhanced Ru–O bond strength of SA Zn-RuO_(2)by forming Zn-O-Ru local structure motif is favorable to stabilize surface Ru,while the electrons transferred from Zn single atoms to adjacent Ru atoms protects the Ru active sites from overoxidation.Simultaneously,the optimized surrounding electronic structure of Ru sites in SA ZnRuO_(2)decreases the adsorption energies of OER intermediates to reduce the reaction barrier.As a result,the representative SA Zn-RuO_(2)exhibits a low overpotential of 210 mV to achieve 10 mA cm^(-2)and a greatly enhanced durability than commercial RuO_(2).This work provides a promising dual-engineering strategy by coupling single atom doping and vacancy for the tradeoff of high activity and catalytic stability toward acidic OER.展开更多
The amount of oxygen blown into the converter is one of the key parameters for the control of the converter blowing process,which directly affects the tap-to-tap time of converter. In this study, a hybrid model based ...The amount of oxygen blown into the converter is one of the key parameters for the control of the converter blowing process,which directly affects the tap-to-tap time of converter. In this study, a hybrid model based on oxygen balance mechanism (OBM) and deep neural network (DNN) was established for predicting oxygen blowing time in converter. A three-step method was utilized in the hybrid model. First, the oxygen consumption volume was predicted by the OBM model and DNN model, respectively. Second, a more accurate oxygen consumption volume was obtained by integrating the OBM model and DNN model. Finally, the converter oxygen blowing time was calculated according to the oxygen consumption volume and the oxygen supply intensity of each heat. The proposed hybrid model was verified using the actual data collected from an integrated steel plant in China, and compared with multiple linear regression model, OBM model, and neural network model including extreme learning machine, back propagation neural network, and DNN. The test results indicate that the hybrid model with a network structure of 3 hidden layer layers, 32-16-8 neurons per hidden layer, and 0.1 learning rate has the best prediction accuracy and stronger generalization ability compared with other models. The predicted hit ratio of oxygen consumption volume within the error±300 m^(3)is 96.67%;determination coefficient (R^(2)) and root mean square error (RMSE) are0.6984 and 150.03 m^(3), respectively. The oxygen blow time prediction hit ratio within the error±0.6 min is 89.50%;R2and RMSE are0.9486 and 0.3592 min, respectively. As a result, the proposed model can effectively predict the oxygen consumption volume and oxygen blowing time in the converter.展开更多
Direct seawater electrolysis for hydrogen production has been regarded as a viable route to utilize surplus renewable energy and address the climate crisis.However,the harsh electrochemical environment of seawater,par...Direct seawater electrolysis for hydrogen production has been regarded as a viable route to utilize surplus renewable energy and address the climate crisis.However,the harsh electrochemical environment of seawater,particularly the presence of aggressive Cl^(-),has been proven to be prone to parasitic chloride ion oxidation and corrosion reactions,thus restricting seawater electrolyzer lifetime.Herein,hierarchical structure(Ni,Fe)O(OH)@NiCoS nanorod arrays(NAs)catalysts with heterointerfaces and localized oxygen vacancies were synthesized at nickel foam substrates via the combination of hydrothermal and annealing methods to boost seawater dissociation.The hiera rchical nanostructure of NiCoS NAs enhanced electrode charge transfer rate and active surface area to accelerate oxygen evolution reaction(OER)and generated sulfate gradient layers to repulsive aggressive Cl^(-).The fabricated heterostructure and vacancies of(Ni,Fe)O(OH)tuned catalyst electronic structure into an electrophilic state to enhance the binding affinity of hydroxyl intermediates and facilitate the structural transformation into amorphousγ-NiFeOOH for promoting OER.Furthermore,through operando electrochemistry techniques,we found that theγ-NiFeOOH possessing an unsaturated coordination environment and lattice-oxygen-participated OER mechanism can minimize electrode Cl^(-)corrosion enabled by stabilizing the adsorption of OH*intermediates,making it one of the best OER catalysts in the seawater medium reported to date.Consequently,these catalysts can deliver current densities of 100 and 500 mA cm-2for boosting OER at minimal overpotentials of 245and 316 mV,respectively,and thus prevent chloride ion oxidation simultaneously.Impressively,a highly stable anion exchange membrane(AEM)seawater electrolyzer based on the non-noble metal heterostructure electrodes reached a record low degradation rate under 100μV h-1at constant industrial current densities of 400 and 600 mA cm-2over 300 h,which exhibits a promising future for the nonprecious and stable AEMWE in the direct seawater electrolysis industry.展开更多
The interaction between metal and support is critical in oxygen catalysis as it governs the charge transfer between these two entities,influences the electronic structures of the supported metal,affects the adsorption...The interaction between metal and support is critical in oxygen catalysis as it governs the charge transfer between these two entities,influences the electronic structures of the supported metal,affects the adsorption energies of reaction intermediates,and ultimately impacts the catalytic performance.In this study,we discovered a unique charge transfer reversal phenomenon in a metal/carbon nanohybrid system.Specifically,electrons were transferred from the metal-based species to N-doped carbon,while the carbon support reciprocally donated electrons to the metal domain upon the introduction of nickel.This led to the exceptional electrocatalytic performances of the resulting Ni-Fe/Mo_(2)C@nitrogen-doped carbon catalyst,with a half-wave potential of 0.91 V towards oxygen reduction reaction(ORR)and a low overpotential of 290 m V at 10 mA cm^(-2)towards oxygen evolution reaction(OER)under alkaline conditions.Additionally,the Fe-Ni/Mo_(2)C@carbon heterojunction catalyst demonstrated high specific capacity(794 mA h g_(Zn)~(-1))and excellent cycling stability(200 h)in a Zn-air battery.Theoretical calculations revealed that Mo_(2)C effectively inhibited charge transfer from Fe to the support,while secondary doping of Ni induced a charge transfer reversal,resulting in electron accumulation in the Fe-Ni alloy region.This local electronic structure modulation significantly reduced energy barriers in the oxygen catalysis process,enhancing the catalytic efficiency of both ORR and OER.Consequently,our findings underscore the potential of manipulating charge transfer reversal between the metal and support as a promising strategy for developing highly-active and durable bi-functional oxygen electrodes.展开更多
Industry decarbonization requires the development of highly efficient and flexible technologies relying on renewable energy resources,especially biomass and solar/wind electricity.In the case of pure oxygen production...Industry decarbonization requires the development of highly efficient and flexible technologies relying on renewable energy resources,especially biomass and solar/wind electricity.In the case of pure oxygen production,oxygen transport membranes(OTMs)appear as an alternative technology for the cryogenic distillation of air,the industrially-established process of producing oxygen.Moreover,OTMs could provide oxygen from different sources(air,water,CO_(2),etc.),and they are more flexible in adapting to current processes,producing oxygen at 700^(-1)000℃.Furthermore,OTMs can be integrated into catalytic membrane reactors,providing new pathways for different processes.The first part of this study was focused on electrification on a traditional OTM material(Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3-δ)),imposing different electric currents/voltages along a capillary membrane.Thanks to the emerging Joule effect,the membrane-surface temperature and the associated O_(2) permeation flux could be adjusted.Here,the OTM is electrically and locally heated and reaches 900℃on the surface,whereas the surrounding of the membrane was maintained at 650℃.The O_(2)permeation flux reached for the electrified membranes was~3.7 NmL min^(-1)cm^(-2),corresponding to the flux obtained with an OTM non-electrified at 900℃.The influence of depositing a porous Ce_(0.8)Tb_(0.2)O_(2-δ) catalytic/protective layer on the outer membrane surface revealed that lower surface temperatures(830℃)were detected at the same imposed electric power.Finally,the electrification concept was demonstrated in a catalytic membrane reactor(CMR)where the oxidative dehydrogenation of ethane(ODHE)was carried out.ODHE reaction is very sensitive to temperature,and here,we demonstrate an improvement of the ethylene yield by reaching moderate temperatures in the reaction chamber while the O_(2) injection into the reaction can be easily fine-tuned.展开更多
Improving the reversibility of anionic redox and inhibiting irreversible oxygen evolution are the main challenges in the application of high reversible capacity Li-rich Mn-based cathode materials.A facile synchronous ...Improving the reversibility of anionic redox and inhibiting irreversible oxygen evolution are the main challenges in the application of high reversible capacity Li-rich Mn-based cathode materials.A facile synchronous lithiation strategy combining the advantages of yttrium doping and LiYO_(2) surface coating is proposed.Yttrium doping effectively suppresses the oxygen evolution during the delithiation process by increasing the energy barrier of oxygen evolution reaction through strong Y–O bond energy.LiYO_(2) nanocoating has the function of structural constraint and protection,that protecting the lattice oxygen exposed to the surface,thus avoiding irreversible oxidation.As an Li^(+) conductor,LiYO_(2) nano-coating can provide a fast Li^(+) transfer channel,which enables the sample to have excellent rate performance.The synergistic effect of Y doping and nano-LiYO_(2) coating integration suppresses the oxygen release from the surface,accelerates the diffusion of Li^(+)from electrolyte to electrode and decreases the interfacial side reactions,enabling the lithium ion batteries to obtain good electrochemical performance.The lithium-ion full cell employing the Y-1 sample(cathode)and commercial graphite(anode)exhibit an excellent specific energy density of 442.9 Wh kg^(-1) at a current density of 0.1C,with very stable safety performance,which can be used in a wide temperature range(60 to-15℃)stable operation.This result illustrates a new integration strategy for advanced cathode materials to achieve high specific energy density.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
Smart wearable devices are regarded to be the next prevailing technology product after smartphones and smart homes,and thus there has recently been rapid development in flexible electronic energy storage devices.Among...Smart wearable devices are regarded to be the next prevailing technology product after smartphones and smart homes,and thus there has recently been rapid development in flexible electronic energy storage devices.Among them,flexible solid-state zinc-air batteries have received widespread attention because of their high energy density,good safety,and stability.Efficient bifunctional oxygen electrocatalysts are the primary consideration in the development of flexible solid-state zinc-air batteries,and self-supported air cathodes are strong candidates because of their advantages including simplified fabrication process,reduced interfacial resistance,accelerated electron transfer,and good flexibility.This review outlines the research progress in the design and construction of nanoarray bifunctional oxygen electrocatalysts.Starting from the configuration and basic principles of zinc-air batteries and the strategies for the design of bifunctional oxygen electrocatalysts,a detailed discussion of self-supported air cathodes on carbon and metal substrates and their uses in flexible zinc-air batteries will follow.Finally,the challenges and opportunities in the development of flexible zinc-air batteries will be discussed.展开更多
Herein,the co-pyrolysis reaction characteristics of corn straw(CS)and bituminous coal in the presence of ilmenite oxygen carriers(OCs)are investigated via thermogravimetry coupled with mass spectrometry.The results re...Herein,the co-pyrolysis reaction characteristics of corn straw(CS)and bituminous coal in the presence of ilmenite oxygen carriers(OCs)are investigated via thermogravimetry coupled with mass spectrometry.The results reveal that the participation of OCs weakens the devolatilization intensity of co-pyrolysis.When the CS blending ratio is<50%,the mixed fuel exhibits positive synergistic effects.The fitting results according to the Coats-Redfern integral method show that the solidesolid interaction between OCs and coke changes the reaction kinetics,enhancing the co-pyrolysis reactivity at the high-temperature zone(750e950C).The synergistic effect is most prominent at a 30%CS blending ratio,with copyrolysis activation energy in the range of 26.35-40.57 kJ·mol^(-1).展开更多
Dissolved oxygen(DO)usually refers to the amount of oxygen dissolved in water.In the environment,medicine,and fermentation industries,the DO level needs to be accurate and capable of online monitoring to guide the pre...Dissolved oxygen(DO)usually refers to the amount of oxygen dissolved in water.In the environment,medicine,and fermentation industries,the DO level needs to be accurate and capable of online monitoring to guide the precise control of water quality,clinical treatment,and microbial metabolism.Compared with other analytical methods,the electrochemical strategy is superior in its fast response,low cost,high sensitivity,and portable device.However,an electrochemical DO sensor faces a trade-off between sensitivity and long-term stability,which strongly limits its practical applications.To solve this problem,various advanced nanomaterials have been proposed to promote detection performance owing to their excellent electrocatalysis,conductivity,and chemical stability.Therefore,in this review,we focus on the recent progress of advanced nanomaterial-based electrochemical DO sensors.Through the comparison of the working principles on the main analysis techniques toward DO,the advantages of the electrochemical method are discussed.Emphasis is placed on recently developed nanomaterials that exhibit special characteristics,including nanostructures and preparation routes,to benefit DO determination.Specifically,we also introduce some interesting research on the configuration design of the electrode and device,which is rarely introduced.Then,the different requirements of the electrochemical DO sensors in different application fields are included to provide brief guidance on the selection of appropriate nanomaterials.Finally,the main challenges are evaluated to propose future development prospects and detection strategies for nanomaterial-based electrochemical sensors.展开更多
The mineralogical and geochemical characteristics of the K-rich granites from the Armoor granitic rocks in the northeastern portion of the Eastern Dharwar Craton(EDC) are presented.In order to understand its physicoch...The mineralogical and geochemical characteristics of the K-rich granites from the Armoor granitic rocks in the northeastern portion of the Eastern Dharwar Craton(EDC) are presented.In order to understand its physicochemical conditions,the petrogenesis of the granitoid was explained from biotite chemistry and geochemical systematics.Studies of mineral chemistry expose that compositionally,K-feldspar and plagioclase in Armoor granite rocks range from An0,Ab_(3-5.9),Or_(94-96.9) and An_(5-29,-Ab71.9-94.9),Or_(0-1.5),respectively.The mineral chemistry of biotite crystals exhibits composition that varies from primary to re-equilibrated primary biotites.Although biotites from the Armoor granites generally exhibit an I-type trend,with calc-alkaline parental magma in a subduction setting.Biotite chemistry of granites displays magnetite(oxidized)series nature,which has oxygen fugacity(fO_(2))=-15.1 to-16.7(log_(10) bar),under high oxidizing conditions.Temperature and pressure estimates for the crystallization of Armoor granites based on biotite composition are T=612-716 ℃ and 1.0-0.4 kbar,respectively.Geochemically,these rocks are metaluminous to slightly peraluminous and magnesian,with calc-alkaline potassiumrich granite.On the chondrite normalized REE diagram,the granites have positive europium anomalies;rich Sr/Y,(Dy/Yb)_(N) ratios and reduced Mg#,Rb/Sr,Rb,Sr indicate that the melting of earlier rocks,crystal accumulation and residual garnet source formed at high pressures.The examined granites show that they are produced from the melting of crustal sources.Thus,the extensive analyses of the described Armoor granite suggest that they were produced by crust sources and developed under oxidizing conditions in subduction setting.展开更多
Achieving composition tunability and structure editability of nanoalloys with high level strain may be an efficient strategy to remarkably boost catalytic performance toward oxygen evolution reaction(OER)in acidic wat...Achieving composition tunability and structure editability of nanoalloys with high level strain may be an efficient strategy to remarkably boost catalytic performance toward oxygen evolution reaction(OER)in acidic water oxidation.Herein,lotus root-like RuIr alloys with native micro-strain were constructed by an epitaxial growth of Ru-richened hcp-(0001)branches on Ir-richened fcc-(111)seeds using a polyol thermal synthesis strategy.The resultant Ru_(60)Ir_(40) alloy shows an OER overpotential of 197 mV at 10 mA cm^(-2) and a Tafel slope of 46.59 mV dec^(-1),showing no obvious activity decay for 80 h continuous chronopotentiometry test in 0.5 M H_(2)SO_(4).The related characterizations including X-ray absorption fine structure(XAFS)spectroscopy and density functional theory(DFT)calculations show that that the remarkably improved activity of the lotus root-like alloy can be attributed to the(0001)facet-triggered strain,which can efficiently optimize the electronic band structure of the active metal and the weakening of the chemisorption of oxygen-containing substances to boost OER electrocatalysis.Therefore,this work provides a new strategy to designing a class of advanced electrocatalysts with high strain using diverse nanostructures as building materials for carbon-free clean energy conversion systems.展开更多
Melt treatment is well known to have an important influence on the properties of metallic glasses(MGs).However,for the MGs quenched from different melt temperatures with a quartz tube,the underlying physical origin re...Melt treatment is well known to have an important influence on the properties of metallic glasses(MGs).However,for the MGs quenched from different melt temperatures with a quartz tube,the underlying physical origin responsible for the variation of properties remains poorly understood.In the present work,we systematically studied the influence of melt treatment on the thermal properties of a Zr50Cu36Al14 glass-forming alloy and unveiled the microscopic origins.Specifically,we quenched the melt at different temperatures ranging from 1.1Tl to 1.5Tl(Tl is the liquidus temperature)to obtain melt-spun MG ribbons and investigated the variation of thermal properties of the MGs upon heating.We found that glass transition temperature,Tg,increases by as much as 36 K,and the supercooled liquid region disappears in the curve of differential scanning calorimetry when the melt is quenched at a high temperature up to 1.5Tl.The careful chemical analyses indicate that the change in glass transition behavior originates from the incorporation of oxygen and silicon in the molten alloys.The incorporated oxygen and silicon can both enhance the interactions between atoms,which renders the cooperative rearrangements of atoms difficult,and thus enhances the kinetic stability of the MGs.展开更多
Niobium pentoxide(Nb_(2)O_(5))is deemed one of the promising anode materials for lithium-ion batteries(LIBs)for its outstanding intrinsic fast Li-(de)intercalation kinetics.The specific capacity,however,is still limit...Niobium pentoxide(Nb_(2)O_(5))is deemed one of the promising anode materials for lithium-ion batteries(LIBs)for its outstanding intrinsic fast Li-(de)intercalation kinetics.The specific capacity,however,is still limited,because the(de)intercalation of excessive Li-ions brings the undesired stress to damage Nb_(2)O_(5) crystals.To increase the capacity of Nb_(2)O_(5) and alleviate the lattice distortion caused by stress,numerous homogeneous H-and M-phases junction interfaces were proposed to produce coercive stress within theNb_(2)O_(5)crystals.Such interfaces bring about rich oxygen vacancies with structural shrinkage tendency,which pre-generate coercive stress to resist the expansion stress caused by excessive Li-ions intercalation.Therefore,the synthesized Nb_(2)O_(5) achieves the highest lithium storage capacity of 315 mA h g−1 to date,and exhibits high-rate performance(118 mA h g^(-1) at 20 C)as well as excellent cycling stability(138 mA h g^(-1) at 10 C after 600 cycles).展开更多
Exploring effective iridium(Ir)-based electrocatalysts with stable iridium centers is highly desirable for oxygen evolution reaction(OER).Herein,we regulated the incorporation manner of Ir in Co_(3)O_(4)support to sta...Exploring effective iridium(Ir)-based electrocatalysts with stable iridium centers is highly desirable for oxygen evolution reaction(OER).Herein,we regulated the incorporation manner of Ir in Co_(3)O_(4)support to stabilize the Ir sites for effective OER.When anchored on the surface of Co_(3)O_(4)in the form of Ir(OH)_6 species,the created Ir-OH-Co interface leads to a limited stability and poor acidic OER due to Ir leaching.When doped into Co_(3)O_(4)lattice,the analyses of X-ray absorption spectroscopy,in-situ Raman,and OER measurements show that the partially replacement of Co in Co_(3)O_(4)by Ir atoms inclines to cause strong electronic effect and activate lattice oxygen in the presence of Ir-O-Co interface,and simultaneously master the reconstruction effect to mitigate Ir dissolution,realizing the improved OER activity and stability in alkaline and acidic environments.As a result,Ir_(lat)@Co_(3)O_(4)with Ir loading of 3.67 wt%requires 294±4 mV/285±3 mV and 326±2 mV to deliver 10 mA cm^(-2)in alkaline(0.1 M KOH/1.0 M KOH)and acidic(0.5 M H_(2)SO_(4))solution,respectively,with good stability.展开更多
Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy ...Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.展开更多
The practical engineering applications of powder metallurgy (PM) Ti alloys produced through cold compaction and pressure-less sintering are impeded by poor sintering densification, embrittlement caused by excessive O ...The practical engineering applications of powder metallurgy (PM) Ti alloys produced through cold compaction and pressure-less sintering are impeded by poor sintering densification, embrittlement caused by excessive O impurities, and severe sintering deforma-tion resulting from the use of heterogeneous powder mixtures. This review presents a summary of our previous work on addressing the above challenges. Initially, we proposed a novel strategy using reaction-induced liquid phases to enhance sintering densification. Near- complete density (relative density exceeding 99%) was achieved by applying the above strategy and newly developed sintering aids. By focusing on the O-induced embrittlement issue, we determined the onset dissolution temperature of oxide films in the Ti matrix. On the basis of this finding, we established a design criterion for effective O scavengers that require reaction with oxide films before their dissol-ution. Consequently, a ductile PM Ti alloy was successfully obtained by introducing 0.3wt% NdB6 as the O scavenger. Lastly, a powder- coating strategy was adopted to address the sintering deformation issue. The ultrafine size and shell-like distribution characteristics of coating particles ensured rapid dissolution and homogeneity in the Ti matrix, thereby facilitating linear shrinkage during sintering. As a result, geometrically complex Ti alloy parts with high dimensional accuracy were fabricated by using the coated powder. Our fundament-al findings and related technical achievements enabled the development of an integrated production technology for the high-performance and accurate shaping of low-cost PM Ti alloys. Additionally, the primary engineering applications and progress in the industrialization practice of our developed technology are introduced in this review.展开更多
A rice cyclase gene,OsCYL4b,identified as an alternative splice variant of the cyclase gene OsCYL4a,is involved in the regulation of drought stress and oxidative response.Compared with OsCYL4a,OsCYL4b lacks the second...A rice cyclase gene,OsCYL4b,identified as an alternative splice variant of the cyclase gene OsCYL4a,is involved in the regulation of drought stress and oxidative response.Compared with OsCYL4a,OsCYL4b lacks the second exon,which is located in the conserved motif 3,and may be a functionally important site.Our results suggested that OsCYL4b was responsive to multiple abiotic stresses,and was localized to both the cytoplasm and plasma membrane.The overexpression of OsCYL4b resulted in significantly enhanced drought and osmotic stress tolerance,reduced water loss,and increased abscisic acid(ABA)content compared with the wild type(WT).展开更多
文摘BACKGROUND Anaesthetic care during upper gastrointestinal(GI)endoscopy has the unique challenge of maintaining ventilation and oxygenation via a shared upper airway.Supplemental oxygen is recommended by international society guidelines,however,the optimal route or rate of oxygen delivery is not known.Various oxygen delivery devices have been investigated to improve oxygenation during upper GI endoscopy,however,these are limited by commercial availability,costs and in some cases,the expertise required for insertion.Anecdotally at our centre,higher flows of supplemental oxygen can safely be delivered via an oxygenating mouthguard routinely used during upper GI endoscopic procedures.AIM To assess the incidence of hypoxaemia(SpO2<90%)in patients undergoing upper GI endoscopy receiving supplemental oxygen using an oxygenating mouthguard at 20 L/min flow compared to standard nasal cannula(SNC)at 2 L/min flow.METHODS A single centre,prospective,randomised clinical trial at two sites of an Australian tertiary hospital between October 2020 and September 2021 was conducted.Patients undergoing elective upper gastrointestinal endoscopy under deep sedation were randomised to receive supplemental oxygen via high-flow via oxygenating mouthguard(HFMG)at 20 L/min flow or SNC at 2 L/min flow.The primary outcome was the incidence of hypoxaemia of any duration measured by pulse oximetry.Intraprocedural-related,procedural-related,and sedation-related adverse events and patient-reported outcomes were also recorded.RESULTS Three hundred patients were randomised.Eight patients were excluded after randomisation.292 patients were included in the intention-to-treat analysis.The incidence of hypoxaemia was significantly reduced in those allocated HFMG.Six patients(4.4%)allocated to HFMG experienced an episode of hypoxaemia,compared to thirty-four(22.1%)patients allocated to SNC(P value<0.001).No significant difference was observed in the rates of adverse events or patient-reported outcome measures.CONCLUSION The use of HFMG offers a novel approach to reducing the incidence of hypoxaemia during short upper gastrointestinal endoscopic procedures in low-risk patients undergoing deep sedation.
基金supported by the Projects of the National Key R&D Program of China,Nos.2021YFC2400803(to YO),2021YFC2400801(to YQ)the National Natural Science Foundation of China,Nos.82002290(to YQ),82072452(to YO),82272475(to YO)+5 种基金the Young Elite Scientist Sponsorship Program by Cast,No.YESS20200153(to YQ)the Sino-German Mobility Programme,No.M-0699(to YQ)the Excellent Youth Cultivation Program of Shanghai Sixth People’s Hospital,No.ynyq202201(to YQ)the Shanghai Sailing Program,No.20YF1436000(to YQ)the Medical Engineering Co-Project of University of Shanghai for Science and Technology,10-22-310-520(to YO)a grant from Shanghai Municipal Health Commission,No.202040399(to YO).
文摘Diabetic peripheral neuropathy is a common complication of diabetes mellitus.Elucidating the pathophysiological metabolic mechanism impels the generation of ideal therapies.However,existing limited treatments for diabetic peripheral neuropathy expose the urgent need for cell metabolism research.Given the lack of comprehensive understanding of energy metabolism changes and related signaling pathways in diabetic peripheral neuropathy,it is essential to explore energy changes and metabolic changes in diabetic peripheral neuropathy to develop suitable treatment methods.This review summarizes the pathophysiological mechanism of diabetic peripheral neuropathy from the perspective of cellular metabolism and the specific interventions for different metabolic pathways to develop effective treatment methods.Various metabolic mechanisms(e.g.,polyol,hexosamine,protein kinase C pathway)are associated with diabetic peripheral neuropathy,and researchers are looking for more effective treatments through these pathways.
基金supported by the Taishan Scholar Program of Shandong Province,China (tsqn202211162)the National Natural Science Foundation of China (22102079)the Natural Science Foundation of Shandong Province of China (ZR2021YQ10,ZR2022QB163)。
文摘The poor stability of RuO_(2)electrocatalysts has been the primary obstacles for their practical application in polymer electrolyte membrane electrolyzers.To dramatically enhance the durability of RuO_(2)to construct activity-stability trade-off model is full of significance but challenging.Herein,a single atom Zn stabilized RuO_(2)with enriched oxygen vacancies(SA Zn-RuO_(2))is developed as a promising alternative to iridium oxide for acidic oxygen evolution reaction(OER).Compared with commercial RuO_(2),the enhanced Ru–O bond strength of SA Zn-RuO_(2)by forming Zn-O-Ru local structure motif is favorable to stabilize surface Ru,while the electrons transferred from Zn single atoms to adjacent Ru atoms protects the Ru active sites from overoxidation.Simultaneously,the optimized surrounding electronic structure of Ru sites in SA ZnRuO_(2)decreases the adsorption energies of OER intermediates to reduce the reaction barrier.As a result,the representative SA Zn-RuO_(2)exhibits a low overpotential of 210 mV to achieve 10 mA cm^(-2)and a greatly enhanced durability than commercial RuO_(2).This work provides a promising dual-engineering strategy by coupling single atom doping and vacancy for the tradeoff of high activity and catalytic stability toward acidic OER.
基金financially supported by the National Natural Science Foundation of China (Nos.51974023 and52374321)the funding of State Key Laboratory of Advanced Metallurgy,University of Science and Technology Beijing,China (No.41620007)。
文摘The amount of oxygen blown into the converter is one of the key parameters for the control of the converter blowing process,which directly affects the tap-to-tap time of converter. In this study, a hybrid model based on oxygen balance mechanism (OBM) and deep neural network (DNN) was established for predicting oxygen blowing time in converter. A three-step method was utilized in the hybrid model. First, the oxygen consumption volume was predicted by the OBM model and DNN model, respectively. Second, a more accurate oxygen consumption volume was obtained by integrating the OBM model and DNN model. Finally, the converter oxygen blowing time was calculated according to the oxygen consumption volume and the oxygen supply intensity of each heat. The proposed hybrid model was verified using the actual data collected from an integrated steel plant in China, and compared with multiple linear regression model, OBM model, and neural network model including extreme learning machine, back propagation neural network, and DNN. The test results indicate that the hybrid model with a network structure of 3 hidden layer layers, 32-16-8 neurons per hidden layer, and 0.1 learning rate has the best prediction accuracy and stronger generalization ability compared with other models. The predicted hit ratio of oxygen consumption volume within the error±300 m^(3)is 96.67%;determination coefficient (R^(2)) and root mean square error (RMSE) are0.6984 and 150.03 m^(3), respectively. The oxygen blow time prediction hit ratio within the error±0.6 min is 89.50%;R2and RMSE are0.9486 and 0.3592 min, respectively. As a result, the proposed model can effectively predict the oxygen consumption volume and oxygen blowing time in the converter.
基金supported by the National Key Research and Development Program of China(2022YFB4002100)the Key Program of the National Natural Science Foundation of China(22090032,22090030)。
文摘Direct seawater electrolysis for hydrogen production has been regarded as a viable route to utilize surplus renewable energy and address the climate crisis.However,the harsh electrochemical environment of seawater,particularly the presence of aggressive Cl^(-),has been proven to be prone to parasitic chloride ion oxidation and corrosion reactions,thus restricting seawater electrolyzer lifetime.Herein,hierarchical structure(Ni,Fe)O(OH)@NiCoS nanorod arrays(NAs)catalysts with heterointerfaces and localized oxygen vacancies were synthesized at nickel foam substrates via the combination of hydrothermal and annealing methods to boost seawater dissociation.The hiera rchical nanostructure of NiCoS NAs enhanced electrode charge transfer rate and active surface area to accelerate oxygen evolution reaction(OER)and generated sulfate gradient layers to repulsive aggressive Cl^(-).The fabricated heterostructure and vacancies of(Ni,Fe)O(OH)tuned catalyst electronic structure into an electrophilic state to enhance the binding affinity of hydroxyl intermediates and facilitate the structural transformation into amorphousγ-NiFeOOH for promoting OER.Furthermore,through operando electrochemistry techniques,we found that theγ-NiFeOOH possessing an unsaturated coordination environment and lattice-oxygen-participated OER mechanism can minimize electrode Cl^(-)corrosion enabled by stabilizing the adsorption of OH*intermediates,making it one of the best OER catalysts in the seawater medium reported to date.Consequently,these catalysts can deliver current densities of 100 and 500 mA cm-2for boosting OER at minimal overpotentials of 245and 316 mV,respectively,and thus prevent chloride ion oxidation simultaneously.Impressively,a highly stable anion exchange membrane(AEM)seawater electrolyzer based on the non-noble metal heterostructure electrodes reached a record low degradation rate under 100μV h-1at constant industrial current densities of 400 and 600 mA cm-2over 300 h,which exhibits a promising future for the nonprecious and stable AEMWE in the direct seawater electrolysis industry.
基金financially supported by the Outstanding Youth Scientific Research Project for Colleges and Universities of Anhui Province of China (2022AH020054)the Anhui Provincial Natural Science Foundation (2208085Y06)+2 种基金the National Natural Science Foundation of China (Nos.21975001 and U2002213)the Support Program of Excellent Young Talents in Anhui Provincial Colleges and Universities (gxyq ZD2022034)the Double Tops Joint Fund of the Yunnan Science and Technology Bureau and Yunnan University (2019FY003025)。
文摘The interaction between metal and support is critical in oxygen catalysis as it governs the charge transfer between these two entities,influences the electronic structures of the supported metal,affects the adsorption energies of reaction intermediates,and ultimately impacts the catalytic performance.In this study,we discovered a unique charge transfer reversal phenomenon in a metal/carbon nanohybrid system.Specifically,electrons were transferred from the metal-based species to N-doped carbon,while the carbon support reciprocally donated electrons to the metal domain upon the introduction of nickel.This led to the exceptional electrocatalytic performances of the resulting Ni-Fe/Mo_(2)C@nitrogen-doped carbon catalyst,with a half-wave potential of 0.91 V towards oxygen reduction reaction(ORR)and a low overpotential of 290 m V at 10 mA cm^(-2)towards oxygen evolution reaction(OER)under alkaline conditions.Additionally,the Fe-Ni/Mo_(2)C@carbon heterojunction catalyst demonstrated high specific capacity(794 mA h g_(Zn)~(-1))and excellent cycling stability(200 h)in a Zn-air battery.Theoretical calculations revealed that Mo_(2)C effectively inhibited charge transfer from Fe to the support,while secondary doping of Ni induced a charge transfer reversal,resulting in electron accumulation in the Fe-Ni alloy region.This local electronic structure modulation significantly reduced energy barriers in the oxygen catalysis process,enhancing the catalytic efficiency of both ORR and OER.Consequently,our findings underscore the potential of manipulating charge transfer reversal between the metal and support as a promising strategy for developing highly-active and durable bi-functional oxygen electrodes.
基金Financial support by the Spanish Ministry of Science(PID2022139663OB-I00 and CEX2021-001230-S grant funded by MCIN/AE I/10.13039/501100011033)with funding from Next Generation EU(PRTR-C17.I1)within the Planes Complementarios con CCAA(Area of Green Hydrogen and Energy)+2 种基金carried out in the CSIC Interdisciplinary Thematic Platform(PTI+)Transición Energética Sostenible+(PTI-TRANSENER+)the Universitat Politècnica de València(UPV)the support of the Servicio de Microscopía Elcectronica of the UPV。
文摘Industry decarbonization requires the development of highly efficient and flexible technologies relying on renewable energy resources,especially biomass and solar/wind electricity.In the case of pure oxygen production,oxygen transport membranes(OTMs)appear as an alternative technology for the cryogenic distillation of air,the industrially-established process of producing oxygen.Moreover,OTMs could provide oxygen from different sources(air,water,CO_(2),etc.),and they are more flexible in adapting to current processes,producing oxygen at 700^(-1)000℃.Furthermore,OTMs can be integrated into catalytic membrane reactors,providing new pathways for different processes.The first part of this study was focused on electrification on a traditional OTM material(Ba_(0.5)Sr_(0.5)Co_(0.8)Fe_(0.2)O_(3-δ)),imposing different electric currents/voltages along a capillary membrane.Thanks to the emerging Joule effect,the membrane-surface temperature and the associated O_(2) permeation flux could be adjusted.Here,the OTM is electrically and locally heated and reaches 900℃on the surface,whereas the surrounding of the membrane was maintained at 650℃.The O_(2)permeation flux reached for the electrified membranes was~3.7 NmL min^(-1)cm^(-2),corresponding to the flux obtained with an OTM non-electrified at 900℃.The influence of depositing a porous Ce_(0.8)Tb_(0.2)O_(2-δ) catalytic/protective layer on the outer membrane surface revealed that lower surface temperatures(830℃)were detected at the same imposed electric power.Finally,the electrification concept was demonstrated in a catalytic membrane reactor(CMR)where the oxidative dehydrogenation of ethane(ODHE)was carried out.ODHE reaction is very sensitive to temperature,and here,we demonstrate an improvement of the ethylene yield by reaching moderate temperatures in the reaction chamber while the O_(2) injection into the reaction can be easily fine-tuned.
基金This work was supported by the Fundamental Research Funds for the Central Universities(DUT20LAB123 and DUT20LAB307)the Natural Science Foundation of Jiangsu Province(BK20191167).
文摘Improving the reversibility of anionic redox and inhibiting irreversible oxygen evolution are the main challenges in the application of high reversible capacity Li-rich Mn-based cathode materials.A facile synchronous lithiation strategy combining the advantages of yttrium doping and LiYO_(2) surface coating is proposed.Yttrium doping effectively suppresses the oxygen evolution during the delithiation process by increasing the energy barrier of oxygen evolution reaction through strong Y–O bond energy.LiYO_(2) nanocoating has the function of structural constraint and protection,that protecting the lattice oxygen exposed to the surface,thus avoiding irreversible oxidation.As an Li^(+) conductor,LiYO_(2) nano-coating can provide a fast Li^(+) transfer channel,which enables the sample to have excellent rate performance.The synergistic effect of Y doping and nano-LiYO_(2) coating integration suppresses the oxygen release from the surface,accelerates the diffusion of Li^(+)from electrolyte to electrode and decreases the interfacial side reactions,enabling the lithium ion batteries to obtain good electrochemical performance.The lithium-ion full cell employing the Y-1 sample(cathode)and commercial graphite(anode)exhibit an excellent specific energy density of 442.9 Wh kg^(-1) at a current density of 0.1C,with very stable safety performance,which can be used in a wide temperature range(60 to-15℃)stable operation.This result illustrates a new integration strategy for advanced cathode materials to achieve high specific energy density.
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supported by the National Natural Science Foundation of China(22072107,21872105)the Natural Science Foundation of Shanghai(23ZR1464800)+1 种基金the Fundamental Research Funds for the Central Universitiesthe Science&Technology Commission of Shanghai Municipality(19DZ2271500)。
文摘Smart wearable devices are regarded to be the next prevailing technology product after smartphones and smart homes,and thus there has recently been rapid development in flexible electronic energy storage devices.Among them,flexible solid-state zinc-air batteries have received widespread attention because of their high energy density,good safety,and stability.Efficient bifunctional oxygen electrocatalysts are the primary consideration in the development of flexible solid-state zinc-air batteries,and self-supported air cathodes are strong candidates because of their advantages including simplified fabrication process,reduced interfacial resistance,accelerated electron transfer,and good flexibility.This review outlines the research progress in the design and construction of nanoarray bifunctional oxygen electrocatalysts.Starting from the configuration and basic principles of zinc-air batteries and the strategies for the design of bifunctional oxygen electrocatalysts,a detailed discussion of self-supported air cathodes on carbon and metal substrates and their uses in flexible zinc-air batteries will follow.Finally,the challenges and opportunities in the development of flexible zinc-air batteries will be discussed.
基金support by the Key Research and Development Program of Ningxia Province of China(2018BCE01002)funded by the Joint Funds of the National Natural Science Foundation of China(U20A20124)the Natural Science Foundation Project of Ningxia(2022AAC01001).
文摘Herein,the co-pyrolysis reaction characteristics of corn straw(CS)and bituminous coal in the presence of ilmenite oxygen carriers(OCs)are investigated via thermogravimetry coupled with mass spectrometry.The results reveal that the participation of OCs weakens the devolatilization intensity of co-pyrolysis.When the CS blending ratio is<50%,the mixed fuel exhibits positive synergistic effects.The fitting results according to the Coats-Redfern integral method show that the solidesolid interaction between OCs and coke changes the reaction kinetics,enhancing the co-pyrolysis reactivity at the high-temperature zone(750e950C).The synergistic effect is most prominent at a 30%CS blending ratio,with copyrolysis activation energy in the range of 26.35-40.57 kJ·mol^(-1).
基金supported by the National Key Research and Development Program of China(2021YFC2103300)the National Natural Science Foundation of China(22078148)the Natural Science Foundation of Jiangsu Province(BK20220002).
文摘Dissolved oxygen(DO)usually refers to the amount of oxygen dissolved in water.In the environment,medicine,and fermentation industries,the DO level needs to be accurate and capable of online monitoring to guide the precise control of water quality,clinical treatment,and microbial metabolism.Compared with other analytical methods,the electrochemical strategy is superior in its fast response,low cost,high sensitivity,and portable device.However,an electrochemical DO sensor faces a trade-off between sensitivity and long-term stability,which strongly limits its practical applications.To solve this problem,various advanced nanomaterials have been proposed to promote detection performance owing to their excellent electrocatalysis,conductivity,and chemical stability.Therefore,in this review,we focus on the recent progress of advanced nanomaterial-based electrochemical DO sensors.Through the comparison of the working principles on the main analysis techniques toward DO,the advantages of the electrochemical method are discussed.Emphasis is placed on recently developed nanomaterials that exhibit special characteristics,including nanostructures and preparation routes,to benefit DO determination.Specifically,we also introduce some interesting research on the configuration design of the electrode and device,which is rarely introduced.Then,the different requirements of the electrochemical DO sensors in different application fields are included to provide brief guidance on the selection of appropriate nanomaterials.Finally,the main challenges are evaluated to propose future development prospects and detection strategies for nanomaterial-based electrochemical sensors.
文摘The mineralogical and geochemical characteristics of the K-rich granites from the Armoor granitic rocks in the northeastern portion of the Eastern Dharwar Craton(EDC) are presented.In order to understand its physicochemical conditions,the petrogenesis of the granitoid was explained from biotite chemistry and geochemical systematics.Studies of mineral chemistry expose that compositionally,K-feldspar and plagioclase in Armoor granite rocks range from An0,Ab_(3-5.9),Or_(94-96.9) and An_(5-29,-Ab71.9-94.9),Or_(0-1.5),respectively.The mineral chemistry of biotite crystals exhibits composition that varies from primary to re-equilibrated primary biotites.Although biotites from the Armoor granites generally exhibit an I-type trend,with calc-alkaline parental magma in a subduction setting.Biotite chemistry of granites displays magnetite(oxidized)series nature,which has oxygen fugacity(fO_(2))=-15.1 to-16.7(log_(10) bar),under high oxidizing conditions.Temperature and pressure estimates for the crystallization of Armoor granites based on biotite composition are T=612-716 ℃ and 1.0-0.4 kbar,respectively.Geochemically,these rocks are metaluminous to slightly peraluminous and magnesian,with calc-alkaline potassiumrich granite.On the chondrite normalized REE diagram,the granites have positive europium anomalies;rich Sr/Y,(Dy/Yb)_(N) ratios and reduced Mg#,Rb/Sr,Rb,Sr indicate that the melting of earlier rocks,crystal accumulation and residual garnet source formed at high pressures.The examined granites show that they are produced from the melting of crustal sources.Thus,the extensive analyses of the described Armoor granite suggest that they were produced by crust sources and developed under oxidizing conditions in subduction setting.
基金supported by the National Natural Science Funds of China(Grant number 22278016)Science and technology planning project of Yunnan Precious Metals Laboratory(Grant number YPML-2023050204)。
文摘Achieving composition tunability and structure editability of nanoalloys with high level strain may be an efficient strategy to remarkably boost catalytic performance toward oxygen evolution reaction(OER)in acidic water oxidation.Herein,lotus root-like RuIr alloys with native micro-strain were constructed by an epitaxial growth of Ru-richened hcp-(0001)branches on Ir-richened fcc-(111)seeds using a polyol thermal synthesis strategy.The resultant Ru_(60)Ir_(40) alloy shows an OER overpotential of 197 mV at 10 mA cm^(-2) and a Tafel slope of 46.59 mV dec^(-1),showing no obvious activity decay for 80 h continuous chronopotentiometry test in 0.5 M H_(2)SO_(4).The related characterizations including X-ray absorption fine structure(XAFS)spectroscopy and density functional theory(DFT)calculations show that that the remarkably improved activity of the lotus root-like alloy can be attributed to the(0001)facet-triggered strain,which can efficiently optimize the electronic band structure of the active metal and the weakening of the chemisorption of oxygen-containing substances to boost OER electrocatalysis.Therefore,this work provides a new strategy to designing a class of advanced electrocatalysts with high strain using diverse nanostructures as building materials for carbon-free clean energy conversion systems.
基金The work was financially supported by the National Key Research and Development Program of China(Grant Nos.2018YFA0703600,2021YFA0716302,and 2021YFA0718703)the National Natural Science Foundation of China(Grant Nos.51825104 and 52192602)China Postdoctoral Science Foundation(Grant No.2022T150691).
文摘Melt treatment is well known to have an important influence on the properties of metallic glasses(MGs).However,for the MGs quenched from different melt temperatures with a quartz tube,the underlying physical origin responsible for the variation of properties remains poorly understood.In the present work,we systematically studied the influence of melt treatment on the thermal properties of a Zr50Cu36Al14 glass-forming alloy and unveiled the microscopic origins.Specifically,we quenched the melt at different temperatures ranging from 1.1Tl to 1.5Tl(Tl is the liquidus temperature)to obtain melt-spun MG ribbons and investigated the variation of thermal properties of the MGs upon heating.We found that glass transition temperature,Tg,increases by as much as 36 K,and the supercooled liquid region disappears in the curve of differential scanning calorimetry when the melt is quenched at a high temperature up to 1.5Tl.The careful chemical analyses indicate that the change in glass transition behavior originates from the incorporation of oxygen and silicon in the molten alloys.The incorporated oxygen and silicon can both enhance the interactions between atoms,which renders the cooperative rearrangements of atoms difficult,and thus enhances the kinetic stability of the MGs.
基金supported by the National Natural Science Foundation of China(Nos.51673199,51972301,51677176)the Youth Innovation Promotion Association of CAS(2015148,Y201940)+2 种基金the Youth Innovation Foundation of DICP(ZZBS201615,ZZBS201708)the Dalian Outstanding Young Scientific Talent(2018RJ03)the National Key Research and Development Project(2019YFA0705600)。
文摘Niobium pentoxide(Nb_(2)O_(5))is deemed one of the promising anode materials for lithium-ion batteries(LIBs)for its outstanding intrinsic fast Li-(de)intercalation kinetics.The specific capacity,however,is still limited,because the(de)intercalation of excessive Li-ions brings the undesired stress to damage Nb_(2)O_(5) crystals.To increase the capacity of Nb_(2)O_(5) and alleviate the lattice distortion caused by stress,numerous homogeneous H-and M-phases junction interfaces were proposed to produce coercive stress within theNb_(2)O_(5)crystals.Such interfaces bring about rich oxygen vacancies with structural shrinkage tendency,which pre-generate coercive stress to resist the expansion stress caused by excessive Li-ions intercalation.Therefore,the synthesized Nb_(2)O_(5) achieves the highest lithium storage capacity of 315 mA h g−1 to date,and exhibits high-rate performance(118 mA h g^(-1) at 20 C)as well as excellent cycling stability(138 mA h g^(-1) at 10 C after 600 cycles).
基金supported by the National Natural Science Foundation of China(52150410409).
文摘Exploring effective iridium(Ir)-based electrocatalysts with stable iridium centers is highly desirable for oxygen evolution reaction(OER).Herein,we regulated the incorporation manner of Ir in Co_(3)O_(4)support to stabilize the Ir sites for effective OER.When anchored on the surface of Co_(3)O_(4)in the form of Ir(OH)_6 species,the created Ir-OH-Co interface leads to a limited stability and poor acidic OER due to Ir leaching.When doped into Co_(3)O_(4)lattice,the analyses of X-ray absorption spectroscopy,in-situ Raman,and OER measurements show that the partially replacement of Co in Co_(3)O_(4)by Ir atoms inclines to cause strong electronic effect and activate lattice oxygen in the presence of Ir-O-Co interface,and simultaneously master the reconstruction effect to mitigate Ir dissolution,realizing the improved OER activity and stability in alkaline and acidic environments.As a result,Ir_(lat)@Co_(3)O_(4)with Ir loading of 3.67 wt%requires 294±4 mV/285±3 mV and 326±2 mV to deliver 10 mA cm^(-2)in alkaline(0.1 M KOH/1.0 M KOH)and acidic(0.5 M H_(2)SO_(4))solution,respectively,with good stability.
基金supported by the National Natural Science Foundation of China(52363028,21965005)the Natural Science Foundation of Guangxi Province(2021GXNSFAA076001)the Guangxi Technology Base and Talent Subject(GUIKE AD18126001,GUIKE AD20297039)。
文摘Tackling the problem of poor conductivity and catalytic stability of pristine metal-organic frameworks(MOFs) is crucial to improve their oxygen evolution reaction(OER) performance.Herein,we introduce a novel strategy of dysprosium(Dy) doping,using the unique 4f orbitals of this rare earth element to enhance electrocatalytic activity of MOFs.Our method involves constructing Dy-doped Ni-MOF(Dy@Ni-MOF) nanoneedles on carbon cloth via a Dy-induced valence electronic perturbation approach.Experiments and density functional theory(DFT) calculations reveal that Dy doping can effectively modify the electronic structure of the Ni active centers and foster a strong electronic interaction between Ni and Dy.The resulting benefits include a reduced work function and a closer proximity of the d-band center to the Fermi level,which is conducive to improving electrical conductivity and promoting the adsorption of oxygen-containing intermediates.Furthermore,the Dy@Ni-MOF achieves superhydrophilicity,ensuring effective electrolyte contact and thus accelerating reaction kinetics,Ex-situ and in-situ analysis results manifest Dy_(2)O_(3)/NiOOH as the actual active species.Therefore,Dy@Ni-MOF shows impressive OER performance,significantly surpassing Ni-MOF.Besides,the overall water splitting device with Dy@NiMOF as an anode delivers a low cell voltage of 1.51 V at 10 mA cm^(-2) and demonstrates long-term stability for 100 h,positioning it as a promising substitute for precious metal catalysts.
基金supported by the National Natural Science Foundation of China (Nos.52074254 and 52174349)the CAS Project for Young Scientists in Basic Research,China (No.YSBR-025)+3 种基金the Shandong Provincial Science and Technology Innovation Project,China (No.2019JZZY010363)the Key Projects of International Cooperation,China (No.122111KYSB20200034)the Project of Key Laboratory of Science and Technology on Particle Materials,China (No.CXJJ-22S043)Chinese Academy of Sciences.This work was also financially supported by the Selection of Best Candidates to Undertake Key Research Projects,China (No.211110230200).
文摘The practical engineering applications of powder metallurgy (PM) Ti alloys produced through cold compaction and pressure-less sintering are impeded by poor sintering densification, embrittlement caused by excessive O impurities, and severe sintering deforma-tion resulting from the use of heterogeneous powder mixtures. This review presents a summary of our previous work on addressing the above challenges. Initially, we proposed a novel strategy using reaction-induced liquid phases to enhance sintering densification. Near- complete density (relative density exceeding 99%) was achieved by applying the above strategy and newly developed sintering aids. By focusing on the O-induced embrittlement issue, we determined the onset dissolution temperature of oxide films in the Ti matrix. On the basis of this finding, we established a design criterion for effective O scavengers that require reaction with oxide films before their dissol-ution. Consequently, a ductile PM Ti alloy was successfully obtained by introducing 0.3wt% NdB6 as the O scavenger. Lastly, a powder- coating strategy was adopted to address the sintering deformation issue. The ultrafine size and shell-like distribution characteristics of coating particles ensured rapid dissolution and homogeneity in the Ti matrix, thereby facilitating linear shrinkage during sintering. As a result, geometrically complex Ti alloy parts with high dimensional accuracy were fabricated by using the coated powder. Our fundament-al findings and related technical achievements enabled the development of an integrated production technology for the high-performance and accurate shaping of low-cost PM Ti alloys. Additionally, the primary engineering applications and progress in the industrialization practice of our developed technology are introduced in this review.
基金supported by the Fundamental Research Funds for the Central Universities,South-Central Minzu University,China(Grant No.CZY23002)Hubei Province Natural Science Foundation of China(Grant No.2019CFB804).
文摘A rice cyclase gene,OsCYL4b,identified as an alternative splice variant of the cyclase gene OsCYL4a,is involved in the regulation of drought stress and oxidative response.Compared with OsCYL4a,OsCYL4b lacks the second exon,which is located in the conserved motif 3,and may be a functionally important site.Our results suggested that OsCYL4b was responsive to multiple abiotic stresses,and was localized to both the cytoplasm and plasma membrane.The overexpression of OsCYL4b resulted in significantly enhanced drought and osmotic stress tolerance,reduced water loss,and increased abscisic acid(ABA)content compared with the wild type(WT).