High-quality steel production requires superior-performance refractories.To meet the requirements of quality enhancement and efficiency improvement in the steelmaking industry,the application of the novel microporous ...High-quality steel production requires superior-performance refractories.To meet the requirements of quality enhancement and efficiency improvement in the steelmaking industry,the application of the novel microporous magnesia with high strength,remarkable slag resistance,and excellent thermal insulation is promoted.The interface reaction between H13 steel and novel microporous magnesia castable was investigated by using the crucible method,to elucidate the molten steel purification mechanism.The interface microstructure was observed by scanning electron microscopy,and the composition,size,and amount of inclusions were statistically analyzed.A thermal calculation was conducted to gain a deeper understanding of the modification process of inclusions.Fused magnesia castables were used as the blank control.The results show that the average number density and size of inclusions were reduced by 5.99 mm^(−2) and 0.28μm respectively after the same reaction time because the micropores enhanced the inclusion adsorption.The size of inclusions caused by erosion decreased.Also,more[Mg]dissolved into molten steel over 60 min reaction time and resulted in a 0.49 wt.%increase in inclusion Mg content,which modified the inclusion by decreasing their melting point.Therefore,applying novel microporous magnesia was beneficial for purifying H13 steel.展开更多
The nitrate reduction via electrochemical catalysis offers an environmentally friendly method for sustainable ammonia production and wastewater remediation.However,conventional Co-based catalysts suffer from a major l...The nitrate reduction via electrochemical catalysis offers an environmentally friendly method for sustainable ammonia production and wastewater remediation.However,conventional Co-based catalysts suffer from a major limitation:their nitrate(NO_(3)^(-))adsorption capacity remains weak.This drawback severely restricts their catalytic efficiency.To overcome this limitation,we synthesized a triphasic interface material(Cu/Co/CoO@C)via rapid joule heating and elucidated its performance-enhancing mechanisms.The exceptional catalytic performance originates from the phase interface-induced multiscale structural regulation.At the microscopic scale,electronic structure modulation through interfacial charge redistribution between Cu and Co/CoO significantly reduces intermediate adsorption energies.Co 3d and O 2p orbitals coupling generates a localized polarized electric field,enhancing NO_(3)^(-)activation.At the macroscopic scale,defect-rich structures improve mass transfer and expose abundant active sites.With the Cu/Co/CoO@C,the yield of NH_(3) is achieved to 2.03 mmol h^(-1)cm^(-2)(-0.4 V vs.RHE,Faradaic efficiency(FE)98.4%).The assembled Zn-NO_(3)^(-)battery delivered a maximum power density of 52.09 mW cm^(-2)and a NH_(3) production rate of 297.5μmol h^(-1)cm^(-2)(FE 95.4%).Based on these results,this work offers new insights into multiphase interface design.展开更多
Additive manufacturing(AM)methods have garnered considerable attention owing to their flexibility in fabricating complex parts with desirable mechanical properties.However,the poor surface quality of the resulting met...Additive manufacturing(AM)methods have garnered considerable attention owing to their flexibility in fabricating complex parts with desirable mechanical properties.However,the poor surface quality of the resulting metal parts remains a severe challenge for the applications.Here,a novel dual-additive synergy strategy is presented,which simultaneously enhances material removal efficiency and regulates electrode surface reactions during electrochemical polishing(ECP)of AM AlSi10Mg.Theoretical studies and experimental characterizations confirm that NaF promotes selective dissolution at the peaks,while glucose acts as a stabilizer for the surface valleys.This approach effectively facilitates the selective removal of surface protrusions,achieving a smoother and more uniform surface finish,resulting in a surface roughness reduction of approximately 86%,compared to a 63%reduction without additives.This study not only provides a new approach for optimizing surface quality of AM AlSi10Mg but also offers new insights into electrolyte design and the stabilization of metal anodes.展开更多
Ta/NiFe film is deposited on Si substrate precoated with SiO_2 by magnetron sputtering.SiO_2/Ta interface and Ta_5Si_3 standard sample are investigated by using X-ray photoelectron spectroscopy (XPS) and peak decompos...Ta/NiFe film is deposited on Si substrate precoated with SiO_2 by magnetron sputtering.SiO_2/Ta interface and Ta_5Si_3 standard sample are investigated by using X-ray photoelectron spectroscopy (XPS) and peak decomposition technique.The results show that there is a thermodynamically favorable reaction at the SiO_2/Ta interface:37Ta+15SiO_2=5Ta_5Si_3+6Ta_2O_5.The more stable products Ta_5Si_3 and Ta_2O_5 may be beneficial to stop the diffusion of Cu into SiO_2.展开更多
Ta/NiO/NiFe/Ta multilayers were prepared by rf reactive and dc magnetron sputtering. The exchange coupling field (Hex) between NiO and NiFe reached 120O e. The composition and chemical states at the interface region o...Ta/NiO/NiFe/Ta multilayers were prepared by rf reactive and dc magnetron sputtering. The exchange coupling field (Hex) between NiO and NiFe reached 120O e. The composition and chemical states at the interface region of NiO/NiFe were studied using the X-ray photoelectron spectroscopy (XPS) and peak decomposition technique. The results show that there are two thermodynamically favorable reactions at NiO/NiFe interface: NiO+Fe=Ni+FeO and 3NiO+2Fe=3Ni+Fe2O3. The thickness of the chemical reaction as estimated by angle-resolved XPS was about 1-1.5 nm. These interface reaction products are magnetic defects, and we believe that the Hex and the coercivity (Hc) of NiO/NiFe are affected by these defects. Moreover, the results also show that there is an intermixing layer at the Ta/NiO (and NiO/Ta) interface due to a thermodynamically favorable reaction: 2Ta+5NiO+Ta2O5. This interface reaction has an effect on the exchange coupling as well. The thickness of the intermixing layer as estimated by XPS depth-profiles was about 8-10 nm.展开更多
Electrocatalytic CO_(2) reduction reaction(CO_(2) RR) can store and transform the intermittent renewable energy in the form of chemical energy for industrial production of chemicals and fuels,which can dramatically re...Electrocatalytic CO_(2) reduction reaction(CO_(2) RR) can store and transform the intermittent renewable energy in the form of chemical energy for industrial production of chemicals and fuels,which can dramatically reduce CO_(2) emission and contribute to carbon-neutral cycle. E cient electrocatalytic reduction of chemically inert CO_(2) is challenging from thermodynamic and kinetic points of view. Therefore,low-cost,highly e cient,and readily available electrocatalysts have been the focus for promoting the conversion of CO_(2). Very recently,interface engineering has been considered as a highly e ective strategy to modulate the electrocatalytic performance through electronic and/or structural modulation,regulations of electron/proton/mass/intermediates,and the control of local reactant concentration,thereby achieving desirable reaction pathway,inhibiting competing hydrogen generation,breaking binding-energy scaling relations of intermediates,and promoting CO_(2) mass transfer. In this review,we aim to provide a comprehensive overview of current developments in interface engineering for CO_(2) RR from both a theoretical and experimental stand-point,involving interfaces between metal and metal,metal and metal oxide,metal and nonmetal,metal oxide and metal oxide,organic molecules and inorganic materials,electrode and electrolyte,molecular catalysts and electrode,etc. Finally,the opportunities and challenges of interface engineering for CO_(2) RR are proposed.展开更多
The formation mechanism of calcium vanadate and manganese vanadate and the difference between calcium and manganese in the reaction with vanadium are basic issues in the calcification roasting and manganese roasting p...The formation mechanism of calcium vanadate and manganese vanadate and the difference between calcium and manganese in the reaction with vanadium are basic issues in the calcification roasting and manganese roasting process with vanadium slag.In this work,CaO–V_(2)O_(5) and MnO_(2)–V_(2)O_(5) diffusion couples were prepared and roasted for different time periods to illustrate and compare the diffusion reaction mechanisms.Then,the changes in the diffusion product and diffusion coefficient were investigated and calculated based on scanning electron microscopy (SEM) with energy dispersive X-ray spectroscopy (EDS) analysis.Results show that with the extension of the roasting time,the diffusion reaction gradually proceeds among the CaO–V_(2)O_(5) and MnO_(2)–V_(2)O_(5) diffusion couples.The regional boundaries of calcium and vanadium are easily identifiable for the CaO–V_(2)O_(5) diffusion couple.Meanwhile,for the MnO_(2)–V_(2)O_(5) diffusion couple,MnO_(2) gradually decomposes to form Mn_(2)O_(3),and vanadium diffuses into the interior of Mn_(2)O_(3).Only a part of vanadium combines with manganese to form the diffusion production layer.CaV_(2)O_(6) and MnV_(2)O_(6) are the interfacial reaction products of the CaO–V_(2)O_(5) and MnO_(2)–V_(2)O_(5) diffusion couples,respectively,whose thicknesses are 39.85 and 32.13μm when roasted for 16 h.After 16 h,both diffusion couples reach the reaction equilibrium due to the limitation of diffusion.The diffusion coefficient of the CaO–V_(2)O_(5) diffusion couple is higher than that of the MnO_(2)–V_(2)O_(5) diffusion couple for the same roasting time,and the diffusion reaction between vanadium and calcium is easier than that between vanadium and manganese.展开更多
The influence of active elements C and Hf on the interface reactions and wettability between a Ni3Albased superalloy and the ceramic mould material was studied by using a sessile drop experiment, The microstructure of...The influence of active elements C and Hf on the interface reactions and wettability between a Ni3Albased superalloy and the ceramic mould material was studied by using a sessile drop experiment, The microstructure of the alloy interface was investigated by scanning electron microscopy analysis and the phase identification was performed by X-ray diffraction analysis, The results show that interface reactions occur as C and Hf contents reach a critical value, The critical values for C and Hf to cause interface reactions are 0,12 wt% and 1,17 wt%, respectively, The reaction products contain HfO2 and 9Al2OH,Cr2O3, Adsorptions of Hf and interface reactions improve the wettability obviously,展开更多
Interface chemical modulation strategies are considered as promising method to prepare electrocatalysts for the urea oxidation reaction(UOR).However,conventional interface catalysts are generally limited by the inhere...Interface chemical modulation strategies are considered as promising method to prepare electrocatalysts for the urea oxidation reaction(UOR).However,conventional interface catalysts are generally limited by the inherent activity and incompatibility of the individual components themselves,and the irregular charge distribution and slow charge transfer ability between interfaces severely limit the activity of UOR.Therefore,we optimized and designed a Ni_(2)P/CoP interface with modulated surface charge distribution and directed charge transfer to promote UOR activity.Density functional theorycalculations first predict a regular charge transfer from CoP to Ni_(2)P,which creates a built-in electric field between Ni_(2)P and CoP interface.Optimization of the adsorption/desorption process of UOR/HER reaction intermediates leads to the improvement of catalytic activity.Electrochemical impedance spectroscopy and ex situ X-ray photoelectron spectroscopy characterization confirm the unique mechanism of facilitated reaction at the Ni_(2)P/CoP interface.Electrochemical tests further validated the prediction with excellent UOR/HER activities of 1.28 V and 19.7 mV vs.RHE,at 10 mA cm^(-2),respectively.Furthermore,Ni_(2)P/CoP achieves industrial-grade current densities(500 mA cm^(−2))at 1.75 V and 1.87 V in the overall urea electrolyzer(UOR||HER)and overall human urine electrolyzer(HUOR||HER),respectively,and demonstrates considerable durability.展开更多
The design of efficient and cost‐effective bifunctional catalysts, which are capable of driving both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), is of paramount importance for advancing...The design of efficient and cost‐effective bifunctional catalysts, which are capable of driving both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), is of paramount importance for advancing overall water splitting. Here, we developed an innovative heterogeneous interface engineering strategy to boost the electrocatalytic performance of overall water splitting. This approach involves the synergistic integration of ultra‐fine CoMoP nanocrystals coupled with three‐ dimensional (3D) porous C3N4/N‐doped carbon (NC) architectures, constructing a distinctive CoMoP/C3N4/NC heterogeneous interface. The CoMoP/C3N4/NC exhibits distinguished overall water splitting performance. To drive the overall water splitting current of 10 mA cm−2, the CoMoP/C3N4/NC||CoMoP/C3N4/NC electrolysis cell only needs an ultralow cell voltage of 1.496 V. The electronic properties and localized coordination environments characterizations, and density functional theory (DFT) calculations elucidate that the improved catalytic activities of CoMoP/C3N4/NC are primarily attributed to the synergistic interfacial coupling between CoMoP/C3N4/NC heterogeneous interface. A novel multi‐site synergistic catalytic mechanism was revealed by the DFT calculations, in which the optimum H* adsorption site on CoMoP/C3N4/NC for HER is on the cobalt atoms in CoMoP with the ultralow Gibbs free energy of hydrogen bonding (ΔGH*) of 0.018 eV, while for the OER, the optimum intermediates adsorption site of the CoMoP/C3N4/NC is on the carbon atoms in C3N4/NC. Besides, the intricately engineered 3D hierarchical porous framework of the CoMoP/C3N4/NC can facilitate the ion and electron transport and improve mass transfer, which gives rise to enhanced water splitting performance.展开更多
Insertion of species A into species B forms a product P through two kinetic processes, namely, （1） the chemical reaction between A and B that occurs at the B-P interface, and （2） the diffusion of species A in prod...Insertion of species A into species B forms a product P through two kinetic processes, namely, （1） the chemical reaction between A and B that occurs at the B-P interface, and （2） the diffusion of species A in product P. These two processes are symbiotic in that the chemical reaction provides the driving force for the diffusion, while the diffusion sustains the chemical reaction by providing sufficient reactant to the reactive interface. In this paper, a math- ematical framework is developed for the coupled reaction- diffusion processes. The resulting system of boundary and initial value problem is solved analytically for the case of interface-reaction controlled diffusion, i.e., the rate of diffu- sion is much faster than the rate of chemical reaction at the interface so that the final kinetics are limited by the interface chemical reaction. Asymptotic expressions are given for the velocity of the reactive interface and the concentration of diffusing species under two different boundary conditions.展开更多
The microstructure together with the formation and growth ofreaction phases in the interfacial diffusion zone of the explosive cladding TA2/A3 has been investigated by means of OM, SEM, AES and XRD techniques. When th...The microstructure together with the formation and growth ofreaction phases in the interfacial diffusion zone of the explosive cladding TA2/A3 has been investigated by means of OM, SEM, AES and XRD techniques. When the specimen annealed at temperature under the βTi→αTi transformation, i. e. below 1173 K, only TiC forms along TA2 side of interface and hinders the interdiffusion of Fe and Ti atoms, thus Fe2Ti or FeTi is unable to occur. While heated up to the transformation temperature of βTi, e. g, over 1223 K, the parabolic growth of intermetallic compounds of Fe2Ti and FeTi with layer structure may form intergranularly and the formation of βTi or βTi+αTi structure at the Fe enriched side of TA2 and the martensitic transformation products at the Fedepleted side are observed owing to the diffusion of Fe. Furthermore, the growth of βTi transformation layer is revealed to follow the parabolic rule.展开更多
Designing a durable lithium metal anode for solid state batteries requires a controllable and uniform deposition of lithium, and the metal lithium layer should maintain a good interface contact with solid state electr...Designing a durable lithium metal anode for solid state batteries requires a controllable and uniform deposition of lithium, and the metal lithium layer should maintain a good interface contact with solid state electrolyte during cycles. In this work, we construct a robust functional interface layer on the modified LiB electrode which considerably improves the electrochemical stability of lithium metal electrode in solid state batteries. It is found that the functional interface layer consisting of polydioxolane, polyiodide ion and Li TFSI effectively restrains the growth of lithium dendrites through the redox shuttle reaction of I-/I3-and maintains a good contact between lithium anode and solid electrolyte during cycles. Benefit from these two advantages, the modified Li-B anode exhibits a remarkable cyclic performance in comparison with those of the bare Li-B anode.展开更多
Interface reaction of SiC w/6061Al aluminium matrix composite subjected to laser welding was studied. It is pointed out that the main reason for bad weldability of the material is concerned with the interface reaction...Interface reaction of SiC w/6061Al aluminium matrix composite subjected to laser welding was studied. It is pointed out that the main reason for bad weldability of the material is concerned with the interface reaction during the welding. Effects of welding parameters on interface reaction were also investigated. The results show that the interface bonding state can be improved by laser beam, and the main welding parameter affecting the strength of weld is laser output power. The smaller the output power, the lower the extent of interface reaction and the better the mechanical properties.展开更多
The ceramic filter in continuous casting tundish can effectively improve the cleanliness of high-performance steel by regulating tundish flow field to promote the removal of inclusions and adsorbing or blocking fine i...The ceramic filter in continuous casting tundish can effectively improve the cleanliness of high-performance steel by regulating tundish flow field to promote the removal of inclusions and adsorbing or blocking fine inclusions in the molten steel into the mold.The interaction between microporous magnesia refractories used as tundish filter and molten interstitial-free(IF)steel at 1873 K was investigated to reveal the formation mechanism of their interface layer and its effect on steel cleanliness by laboratory research and thermodynamic calculations.The results show that the magnesium–aluminum spinel layer at the interface between the molten IF steel and the microporous magnesia refractories is formed mainly by the reaction of MgO in the refractory with the[Al]and[O]in the molten steel,significantly reducing the total O content,the size and amount of inclusions of the molten steel.In addition,the interparticle phases of microporous magnesia refractories at high temperature can adsorb Al_(2)O_(3) and TiO_(2) inclusions in the molten steel into interparticle channels of the refractories to form high melting point spinel,impeding the further penetration of the molten steel.As a result,the consecutive interface layer of high melting point spinel between microporous magnesia refractories and molten steel can improve the cleanliness of the molten steel by adsorbing inclusions in the molten steel and avoid the direct dissolution of refractories of the tundish ceramic filter immersed in the molten steel,increasing their service life.展开更多
Acetylacetone(AcAc)is a typical class ofβ-diketones with broad industrial applications due to the property of the keto-enol isomers,but its isomerization and chemical reactions at the air-droplet interface are still ...Acetylacetone(AcAc)is a typical class ofβ-diketones with broad industrial applications due to the property of the keto-enol isomers,but its isomerization and chemical reactions at the air-droplet interface are still unclear.Hence,using combined molecular dynamics and quantum chemistry methods,the heterogeneous chemistry of AcAc at the air-droplet interface was investigated,including the attraction of AcAc isomers by the droplets,the distribution of isomers at the air-droplet interface,and the hydration reactions of isomers at the air-droplet interface.The results reveal that the preferential orientation of two AcAc isomers(keto-and enol-AcAc)to accumulate and accommodate at the acidic air-droplet interface.The isomerization of two AcAc isomers at the acidic air-droplet interface is more favorable than that at the neutral air-droplet interface because the“water bridge”structure is destroyed by H_(3)O^(+),especially for the isomerization from keto-Ac Ac to enol-AcAc.At the acidic air-droplet interface,the carbonyl or hydroxyl O-atoms of two AcAc isomers display an energetical preference to hydration.Keto-diol is the dominant products to accumulate at the air-droplet interface,and excessive keto-diol can enter the droplet interior to engage in the oligomerization.The photooxidation reaction of AcAc will increase the acidity of the air-droplet interface,which indirectly facilitate the uptake and formation of more keto-diol.Our results provide an insight into the heterogeneous chemistry ofβ-diketones and their influence on the environment.展开更多
Based on the diffusion channel,the influence of Si content on the microstructure evolution of iron-based hot-dip Al-χSi coating was analyzed(χ=0,1.5 wt%,3.0 wt% and 7.0 wt%).The results show that the introduction of...Based on the diffusion channel,the influence of Si content on the microstructure evolution of iron-based hot-dip Al-χSi coating was analyzed(χ=0,1.5 wt%,3.0 wt% and 7.0 wt%).The results show that the introduction of Si makes the reaction interface change from the lingual-tooth interface of hot-dip Al to the flat interface of hot-dip Al-Si.It also reduces the thickness of the alloy layer in the coating,especially the Fe_(2)Al_(5) layer.When the Si content is 1.5 wt%or 3.0 wt%,the diffusion channel crosses the conjugate line of the two-phase region(FeAl_(3)+liquid phase)into the FeAl_(3) single-phase region,and then moves to the region with higher Si content.Next,the diffusion channel cuts off the conjugate line of FeAl_(3)phase,τ_(1)/τ_(9) phase,and Fe_(2)Al_(5)phase,which promotes the form ofτ_(1)/τ_(9) phase.The formedτ_(1)/τ_(9) phase inhibits the diffusion between Fe and Al atoms.When the Si content is 7.0 wt%,the diffusion channel passes through the two-phase region(liquid phase+τ_(5))and enters theτ_(5) single-phase region.The form ofτ_(5) single-phase region has a strong inhibitory effect on the interatomic diffusion of Fe and Al,thereby reducing the thickness of the coating,especially the Fe_(2)Al_(5)layer.展开更多
A reaction interface between the aluminum and K_2ZrF_6 during molten salt reaction process was frozen by quenching the mold in water, and the interface structure was analyzed to determine the formation process of Al_3...A reaction interface between the aluminum and K_2ZrF_6 during molten salt reaction process was frozen by quenching the mold in water, and the interface structure was analyzed to determine the formation process of Al_3Zr. Results show that a clear conical interface existed between the K_2ZrF_6 and aluminum. A zirconium accumulation layer with the thickness of about 2–3 lm was formed at the aluminum side of the interface. Many initially formed Al_3Zr particles（with the size of 0.4–16 lm） distributed in this layer, most of which located at the interface. The morphology of Al_3Zr particles is closely related with their size. For the size of 0.4–1 lm, the Al_3Zr appeared as globular and ellipsoid shapes. When it grew to the size of 1–2 and 2–16 lm, it exhibited the rule cube shape, and rule cuboids shape, respectively.展开更多
Mg batteries have high energy density,economic safety,and environmental friendliness.They show great potential as an ideal energy storage technology.This review summarizes the limitations of Mg batteries and explores ...Mg batteries have high energy density,economic safety,and environmental friendliness.They show great potential as an ideal energy storage technology.This review summarizes the limitations of Mg batteries and explores the complex reactions at the Mg anode/electrolyte interface.It focuses on critical issues such as the dissolution of Mg anodes,the evolution of hydrogen gas,the formation of a passivation layer that hinders Mg^(2+)migration,and dendrite growth.To address these interface problems,the review discusses strategies to improve interface reactions.These include the structural design of Mg anodes,suitable substitute materials for the anode,and artificial solid electrolyte interphase films.Finally,it outlines the future research directions for the ideal Mg anode interfaces.The goal is to develop more efficient interface design schemes and optimization strategies to advance Mg battery technology further.展开更多
基金support of this study by the National Natural Science Foundation of China(Grant Nos.U22A20173 and U21A2058).
文摘High-quality steel production requires superior-performance refractories.To meet the requirements of quality enhancement and efficiency improvement in the steelmaking industry,the application of the novel microporous magnesia with high strength,remarkable slag resistance,and excellent thermal insulation is promoted.The interface reaction between H13 steel and novel microporous magnesia castable was investigated by using the crucible method,to elucidate the molten steel purification mechanism.The interface microstructure was observed by scanning electron microscopy,and the composition,size,and amount of inclusions were statistically analyzed.A thermal calculation was conducted to gain a deeper understanding of the modification process of inclusions.Fused magnesia castables were used as the blank control.The results show that the average number density and size of inclusions were reduced by 5.99 mm^(−2) and 0.28μm respectively after the same reaction time because the micropores enhanced the inclusion adsorption.The size of inclusions caused by erosion decreased.Also,more[Mg]dissolved into molten steel over 60 min reaction time and resulted in a 0.49 wt.%increase in inclusion Mg content,which modified the inclusion by decreasing their melting point.Therefore,applying novel microporous magnesia was beneficial for purifying H13 steel.
基金financial support provided by the National Natural Science Foundation of Yunnan Province(202301AS070040,202301AU070209)the Major Science and Technology Projects of Yunnan Province(202302AB080019-3)+3 种基金the Scientific Research Fund Project of Yunnan Provincial Department of Education(2023J0033)the Laboratory of Solid-State Ions for Green Energy of Yunnan Universitythe Analysis and Measurements Center of Yunnan University for the sample testing servicethe Electron Microscope Center of Yunnan University for the support of this work。
文摘The nitrate reduction via electrochemical catalysis offers an environmentally friendly method for sustainable ammonia production and wastewater remediation.However,conventional Co-based catalysts suffer from a major limitation:their nitrate(NO_(3)^(-))adsorption capacity remains weak.This drawback severely restricts their catalytic efficiency.To overcome this limitation,we synthesized a triphasic interface material(Cu/Co/CoO@C)via rapid joule heating and elucidated its performance-enhancing mechanisms.The exceptional catalytic performance originates from the phase interface-induced multiscale structural regulation.At the microscopic scale,electronic structure modulation through interfacial charge redistribution between Cu and Co/CoO significantly reduces intermediate adsorption energies.Co 3d and O 2p orbitals coupling generates a localized polarized electric field,enhancing NO_(3)^(-)activation.At the macroscopic scale,defect-rich structures improve mass transfer and expose abundant active sites.With the Cu/Co/CoO@C,the yield of NH_(3) is achieved to 2.03 mmol h^(-1)cm^(-2)(-0.4 V vs.RHE,Faradaic efficiency(FE)98.4%).The assembled Zn-NO_(3)^(-)battery delivered a maximum power density of 52.09 mW cm^(-2)and a NH_(3) production rate of 297.5μmol h^(-1)cm^(-2)(FE 95.4%).Based on these results,this work offers new insights into multiphase interface design.
基金financially supported by the National Natural Science Foundation of China(Nos.52175444,51905506,21871065 and 22071038)the Sichuan Science and Technology Program(No.2021JDJQ0014).
文摘Additive manufacturing(AM)methods have garnered considerable attention owing to their flexibility in fabricating complex parts with desirable mechanical properties.However,the poor surface quality of the resulting metal parts remains a severe challenge for the applications.Here,a novel dual-additive synergy strategy is presented,which simultaneously enhances material removal efficiency and regulates electrode surface reactions during electrochemical polishing(ECP)of AM AlSi10Mg.Theoretical studies and experimental characterizations confirm that NaF promotes selective dissolution at the peaks,while glucose acts as a stabilizer for the surface valleys.This approach effectively facilitates the selective removal of surface protrusions,achieving a smoother and more uniform surface finish,resulting in a surface roughness reduction of approximately 86%,compared to a 63%reduction without additives.This study not only provides a new approach for optimizing surface quality of AM AlSi10Mg but also offers new insights into electrolyte design and the stabilization of metal anodes.
文摘Ta/NiFe film is deposited on Si substrate precoated with SiO_2 by magnetron sputtering.SiO_2/Ta interface and Ta_5Si_3 standard sample are investigated by using X-ray photoelectron spectroscopy (XPS) and peak decomposition technique.The results show that there is a thermodynamically favorable reaction at the SiO_2/Ta interface:37Ta+15SiO_2=5Ta_5Si_3+6Ta_2O_5.The more stable products Ta_5Si_3 and Ta_2O_5 may be beneficial to stop the diffusion of Cu into SiO_2.
基金supported by the National Natural Science Foundation of China and Beijing under grant No.19890310 and 2012011,respectively
文摘Ta/NiO/NiFe/Ta multilayers were prepared by rf reactive and dc magnetron sputtering. The exchange coupling field (Hex) between NiO and NiFe reached 120O e. The composition and chemical states at the interface region of NiO/NiFe were studied using the X-ray photoelectron spectroscopy (XPS) and peak decomposition technique. The results show that there are two thermodynamically favorable reactions at NiO/NiFe interface: NiO+Fe=Ni+FeO and 3NiO+2Fe=3Ni+Fe2O3. The thickness of the chemical reaction as estimated by angle-resolved XPS was about 1-1.5 nm. These interface reaction products are magnetic defects, and we believe that the Hex and the coercivity (Hc) of NiO/NiFe are affected by these defects. Moreover, the results also show that there is an intermixing layer at the Ta/NiO (and NiO/Ta) interface due to a thermodynamically favorable reaction: 2Ta+5NiO+Ta2O5. This interface reaction has an effect on the exchange coupling as well. The thickness of the intermixing layer as estimated by XPS depth-profiles was about 8-10 nm.
基金supported by the National Natural Science Foundation of China (22071172)the Ministry of Science and Technology of China (2016YFB0401100,2017YFA0204503,and 2018YFA0703200)Shandong Provincial Natural Science Foundation (No. ZR2019BB025)。
文摘Electrocatalytic CO_(2) reduction reaction(CO_(2) RR) can store and transform the intermittent renewable energy in the form of chemical energy for industrial production of chemicals and fuels,which can dramatically reduce CO_(2) emission and contribute to carbon-neutral cycle. E cient electrocatalytic reduction of chemically inert CO_(2) is challenging from thermodynamic and kinetic points of view. Therefore,low-cost,highly e cient,and readily available electrocatalysts have been the focus for promoting the conversion of CO_(2). Very recently,interface engineering has been considered as a highly e ective strategy to modulate the electrocatalytic performance through electronic and/or structural modulation,regulations of electron/proton/mass/intermediates,and the control of local reactant concentration,thereby achieving desirable reaction pathway,inhibiting competing hydrogen generation,breaking binding-energy scaling relations of intermediates,and promoting CO_(2) mass transfer. In this review,we aim to provide a comprehensive overview of current developments in interface engineering for CO_(2) RR from both a theoretical and experimental stand-point,involving interfaces between metal and metal,metal and metal oxide,metal and nonmetal,metal oxide and metal oxide,organic molecules and inorganic materials,electrode and electrolyte,molecular catalysts and electrode,etc. Finally,the opportunities and challenges of interface engineering for CO_(2) RR are proposed.
基金supported by the National Natural Science Foundation of China(Nos.52174277 and 51874077)the Fundamental Funds for the Central Universities,China(No.N2225032)+1 种基金the China Postdoctoral Science Foundation(No.2022M720683)the Postdoctoral Fund of Northeastern University,China。
文摘The formation mechanism of calcium vanadate and manganese vanadate and the difference between calcium and manganese in the reaction with vanadium are basic issues in the calcification roasting and manganese roasting process with vanadium slag.In this work,CaO–V_(2)O_(5) and MnO_(2)–V_(2)O_(5) diffusion couples were prepared and roasted for different time periods to illustrate and compare the diffusion reaction mechanisms.Then,the changes in the diffusion product and diffusion coefficient were investigated and calculated based on scanning electron microscopy (SEM) with energy dispersive X-ray spectroscopy (EDS) analysis.Results show that with the extension of the roasting time,the diffusion reaction gradually proceeds among the CaO–V_(2)O_(5) and MnO_(2)–V_(2)O_(5) diffusion couples.The regional boundaries of calcium and vanadium are easily identifiable for the CaO–V_(2)O_(5) diffusion couple.Meanwhile,for the MnO_(2)–V_(2)O_(5) diffusion couple,MnO_(2) gradually decomposes to form Mn_(2)O_(3),and vanadium diffuses into the interior of Mn_(2)O_(3).Only a part of vanadium combines with manganese to form the diffusion production layer.CaV_(2)O_(6) and MnV_(2)O_(6) are the interfacial reaction products of the CaO–V_(2)O_(5) and MnO_(2)–V_(2)O_(5) diffusion couples,respectively,whose thicknesses are 39.85 and 32.13μm when roasted for 16 h.After 16 h,both diffusion couples reach the reaction equilibrium due to the limitation of diffusion.The diffusion coefficient of the CaO–V_(2)O_(5) diffusion couple is higher than that of the MnO_(2)–V_(2)O_(5) diffusion couple for the same roasting time,and the diffusion reaction between vanadium and calcium is easier than that between vanadium and manganese.
基金financial support from the National Natural Science Foundation of China (Grant Nos. U1037601 and 51271186)
文摘The influence of active elements C and Hf on the interface reactions and wettability between a Ni3Albased superalloy and the ceramic mould material was studied by using a sessile drop experiment, The microstructure of the alloy interface was investigated by scanning electron microscopy analysis and the phase identification was performed by X-ray diffraction analysis, The results show that interface reactions occur as C and Hf contents reach a critical value, The critical values for C and Hf to cause interface reactions are 0,12 wt% and 1,17 wt%, respectively, The reaction products contain HfO2 and 9Al2OH,Cr2O3, Adsorptions of Hf and interface reactions improve the wettability obviously,
文摘Interface chemical modulation strategies are considered as promising method to prepare electrocatalysts for the urea oxidation reaction(UOR).However,conventional interface catalysts are generally limited by the inherent activity and incompatibility of the individual components themselves,and the irregular charge distribution and slow charge transfer ability between interfaces severely limit the activity of UOR.Therefore,we optimized and designed a Ni_(2)P/CoP interface with modulated surface charge distribution and directed charge transfer to promote UOR activity.Density functional theorycalculations first predict a regular charge transfer from CoP to Ni_(2)P,which creates a built-in electric field between Ni_(2)P and CoP interface.Optimization of the adsorption/desorption process of UOR/HER reaction intermediates leads to the improvement of catalytic activity.Electrochemical impedance spectroscopy and ex situ X-ray photoelectron spectroscopy characterization confirm the unique mechanism of facilitated reaction at the Ni_(2)P/CoP interface.Electrochemical tests further validated the prediction with excellent UOR/HER activities of 1.28 V and 19.7 mV vs.RHE,at 10 mA cm^(-2),respectively.Furthermore,Ni_(2)P/CoP achieves industrial-grade current densities(500 mA cm^(−2))at 1.75 V and 1.87 V in the overall urea electrolyzer(UOR||HER)and overall human urine electrolyzer(HUOR||HER),respectively,and demonstrates considerable durability.
基金supported by the National Natural Science Foundation of China(Grant No.12375303)the Natural Science Foundation of Guangdong Province(Grants No.2024A1515030034 and 2023A1515140156).
文摘The design of efficient and cost‐effective bifunctional catalysts, which are capable of driving both the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), is of paramount importance for advancing overall water splitting. Here, we developed an innovative heterogeneous interface engineering strategy to boost the electrocatalytic performance of overall water splitting. This approach involves the synergistic integration of ultra‐fine CoMoP nanocrystals coupled with three‐ dimensional (3D) porous C3N4/N‐doped carbon (NC) architectures, constructing a distinctive CoMoP/C3N4/NC heterogeneous interface. The CoMoP/C3N4/NC exhibits distinguished overall water splitting performance. To drive the overall water splitting current of 10 mA cm−2, the CoMoP/C3N4/NC||CoMoP/C3N4/NC electrolysis cell only needs an ultralow cell voltage of 1.496 V. The electronic properties and localized coordination environments characterizations, and density functional theory (DFT) calculations elucidate that the improved catalytic activities of CoMoP/C3N4/NC are primarily attributed to the synergistic interfacial coupling between CoMoP/C3N4/NC heterogeneous interface. A novel multi‐site synergistic catalytic mechanism was revealed by the DFT calculations, in which the optimum H* adsorption site on CoMoP/C3N4/NC for HER is on the cobalt atoms in CoMoP with the ultralow Gibbs free energy of hydrogen bonding (ΔGH*) of 0.018 eV, while for the OER, the optimum intermediates adsorption site of the CoMoP/C3N4/NC is on the carbon atoms in C3N4/NC. Besides, the intricately engineered 3D hierarchical porous framework of the CoMoP/C3N4/NC can facilitate the ion and electron transport and improve mass transfer, which gives rise to enhanced water splitting performance.
基金supported in part by an ISEN Booster Award at Northwestern Universityin part by NSF(CMMI-1200075)
文摘Insertion of species A into species B forms a product P through two kinetic processes, namely, （1） the chemical reaction between A and B that occurs at the B-P interface, and （2） the diffusion of species A in product P. These two processes are symbiotic in that the chemical reaction provides the driving force for the diffusion, while the diffusion sustains the chemical reaction by providing sufficient reactant to the reactive interface. In this paper, a math- ematical framework is developed for the coupled reaction- diffusion processes. The resulting system of boundary and initial value problem is solved analytically for the case of interface-reaction controlled diffusion, i.e., the rate of diffu- sion is much faster than the rate of chemical reaction at the interface so that the final kinetics are limited by the interface chemical reaction. Asymptotic expressions are given for the velocity of the reactive interface and the concentration of diffusing species under two different boundary conditions.
基金the+6 种基金Non-ferrousMetal Industry Corperation of China
文摘The microstructure together with the formation and growth ofreaction phases in the interfacial diffusion zone of the explosive cladding TA2/A3 has been investigated by means of OM, SEM, AES and XRD techniques. When the specimen annealed at temperature under the βTi→αTi transformation, i. e. below 1173 K, only TiC forms along TA2 side of interface and hinders the interdiffusion of Fe and Ti atoms, thus Fe2Ti or FeTi is unable to occur. While heated up to the transformation temperature of βTi, e. g, over 1223 K, the parabolic growth of intermetallic compounds of Fe2Ti and FeTi with layer structure may form intergranularly and the formation of βTi or βTi+αTi structure at the Fe enriched side of TA2 and the martensitic transformation products at the Fedepleted side are observed owing to the diffusion of Fe. Furthermore, the growth of βTi transformation layer is revealed to follow the parabolic rule.
基金supported by the National Natural Science Foundation of China (NO. 21805113)the Fundamental Research Funds for the Central Universities (NO. 11618410 and NO. 11619103)the China Postdoctoral Science Foundation (NO. 2019M653271)。
文摘Designing a durable lithium metal anode for solid state batteries requires a controllable and uniform deposition of lithium, and the metal lithium layer should maintain a good interface contact with solid state electrolyte during cycles. In this work, we construct a robust functional interface layer on the modified LiB electrode which considerably improves the electrochemical stability of lithium metal electrode in solid state batteries. It is found that the functional interface layer consisting of polydioxolane, polyiodide ion and Li TFSI effectively restrains the growth of lithium dendrites through the redox shuttle reaction of I-/I3-and maintains a good contact between lithium anode and solid electrolyte during cycles. Benefit from these two advantages, the modified Li-B anode exhibits a remarkable cyclic performance in comparison with those of the bare Li-B anode.
文摘Interface reaction of SiC w/6061Al aluminium matrix composite subjected to laser welding was studied. It is pointed out that the main reason for bad weldability of the material is concerned with the interface reaction during the welding. Effects of welding parameters on interface reaction were also investigated. The results show that the interface bonding state can be improved by laser beam, and the main welding parameter affecting the strength of weld is laser output power. The smaller the output power, the lower the extent of interface reaction and the better the mechanical properties.
基金The authors are grateful to the National Natural Science Foundation of China(Nos.U1860205 and 52174323)Innovation Team Cultivation Funding Project of Wuhan University of Science and Technology(2018TDX08).
文摘The ceramic filter in continuous casting tundish can effectively improve the cleanliness of high-performance steel by regulating tundish flow field to promote the removal of inclusions and adsorbing or blocking fine inclusions in the molten steel into the mold.The interaction between microporous magnesia refractories used as tundish filter and molten interstitial-free(IF)steel at 1873 K was investigated to reveal the formation mechanism of their interface layer and its effect on steel cleanliness by laboratory research and thermodynamic calculations.The results show that the magnesium–aluminum spinel layer at the interface between the molten IF steel and the microporous magnesia refractories is formed mainly by the reaction of MgO in the refractory with the[Al]and[O]in the molten steel,significantly reducing the total O content,the size and amount of inclusions of the molten steel.In addition,the interparticle phases of microporous magnesia refractories at high temperature can adsorb Al_(2)O_(3) and TiO_(2) inclusions in the molten steel into interparticle channels of the refractories to form high melting point spinel,impeding the further penetration of the molten steel.As a result,the consecutive interface layer of high melting point spinel between microporous magnesia refractories and molten steel can improve the cleanliness of the molten steel by adsorbing inclusions in the molten steel and avoid the direct dissolution of refractories of the tundish ceramic filter immersed in the molten steel,increasing their service life.
基金supported by the Guangdong Basic and Applied Basic Research Foundation(No.2019B151502064)the National Natural Science Foundation of China(Nos.42077189,42020104001,and 42277081)+3 种基金the Local Innovative and Research Teams Project of Guangdong Pearl River Talents Program(No.2017BT01Z032)the Science and Technology Key Project of Guangdong ProvinceChina(No.2019B110206002)the Guangdong Provincial Key R&D Program(No.2022-GDUT-A0007)。
文摘Acetylacetone(AcAc)is a typical class ofβ-diketones with broad industrial applications due to the property of the keto-enol isomers,but its isomerization and chemical reactions at the air-droplet interface are still unclear.Hence,using combined molecular dynamics and quantum chemistry methods,the heterogeneous chemistry of AcAc at the air-droplet interface was investigated,including the attraction of AcAc isomers by the droplets,the distribution of isomers at the air-droplet interface,and the hydration reactions of isomers at the air-droplet interface.The results reveal that the preferential orientation of two AcAc isomers(keto-and enol-AcAc)to accumulate and accommodate at the acidic air-droplet interface.The isomerization of two AcAc isomers at the acidic air-droplet interface is more favorable than that at the neutral air-droplet interface because the“water bridge”structure is destroyed by H_(3)O^(+),especially for the isomerization from keto-Ac Ac to enol-AcAc.At the acidic air-droplet interface,the carbonyl or hydroxyl O-atoms of two AcAc isomers display an energetical preference to hydration.Keto-diol is the dominant products to accumulate at the air-droplet interface,and excessive keto-diol can enter the droplet interior to engage in the oligomerization.The photooxidation reaction of AcAc will increase the acidity of the air-droplet interface,which indirectly facilitate the uptake and formation of more keto-diol.Our results provide an insight into the heterogeneous chemistry ofβ-diketones and their influence on the environment.
基金Projects(51971039,51671037)supported by the National Natural Science Foundation of ChinaProject(19KJA530001)supported by the Natural Science Research Project of Higher Education of Jiangsu,ChinaProject(KYCX21_2868)supported by the Postgraduate Research&Practice Innovation Program of Jiangsu Province,China。
文摘Based on the diffusion channel,the influence of Si content on the microstructure evolution of iron-based hot-dip Al-χSi coating was analyzed(χ=0,1.5 wt%,3.0 wt% and 7.0 wt%).The results show that the introduction of Si makes the reaction interface change from the lingual-tooth interface of hot-dip Al to the flat interface of hot-dip Al-Si.It also reduces the thickness of the alloy layer in the coating,especially the Fe_(2)Al_(5) layer.When the Si content is 1.5 wt%or 3.0 wt%,the diffusion channel crosses the conjugate line of the two-phase region(FeAl_(3)+liquid phase)into the FeAl_(3) single-phase region,and then moves to the region with higher Si content.Next,the diffusion channel cuts off the conjugate line of FeAl_(3)phase,τ_(1)/τ_(9) phase,and Fe_(2)Al_(5)phase,which promotes the form ofτ_(1)/τ_(9) phase.The formedτ_(1)/τ_(9) phase inhibits the diffusion between Fe and Al atoms.When the Si content is 7.0 wt%,the diffusion channel passes through the two-phase region(liquid phase+τ_(5))and enters theτ_(5) single-phase region.The form ofτ_(5) single-phase region has a strong inhibitory effect on the interatomic diffusion of Fe and Al,thereby reducing the thickness of the coating,especially the Fe_(2)Al_(5)layer.
基金Supported by the National Natural Science Foundation of China(Nos.51204053,51374067&51674078)Central University Basic R&D Operating Expenses(Nos.N130409005,N130709001&N130209001)
文摘A reaction interface between the aluminum and K_2ZrF_6 during molten salt reaction process was frozen by quenching the mold in water, and the interface structure was analyzed to determine the formation process of Al_3Zr. Results show that a clear conical interface existed between the K_2ZrF_6 and aluminum. A zirconium accumulation layer with the thickness of about 2–3 lm was formed at the aluminum side of the interface. Many initially formed Al_3Zr particles（with the size of 0.4–16 lm） distributed in this layer, most of which located at the interface. The morphology of Al_3Zr particles is closely related with their size. For the size of 0.4–1 lm, the Al_3Zr appeared as globular and ellipsoid shapes. When it grew to the size of 1–2 and 2–16 lm, it exhibited the rule cube shape, and rule cuboids shape, respectively.
基金supported by National Natural Science Foundation of China(52371095)Innovation Research Group of Universities in Chongqing(CXQT21030)+2 种基金Chongqing Overseas Chinese Entrepreneurship and Innovation Support Program(cx2023117)Chongqing Natural Science Foundation(CSTB2022NSCQ-LZX0054,CSTB2024TIADCYKJCXX0001)Chongqing Youth Expert Studio。
文摘Mg batteries have high energy density,economic safety,and environmental friendliness.They show great potential as an ideal energy storage technology.This review summarizes the limitations of Mg batteries and explores the complex reactions at the Mg anode/electrolyte interface.It focuses on critical issues such as the dissolution of Mg anodes,the evolution of hydrogen gas,the formation of a passivation layer that hinders Mg^(2+)migration,and dendrite growth.To address these interface problems,the review discusses strategies to improve interface reactions.These include the structural design of Mg anodes,suitable substitute materials for the anode,and artificial solid electrolyte interphase films.Finally,it outlines the future research directions for the ideal Mg anode interfaces.The goal is to develop more efficient interface design schemes and optimization strategies to advance Mg battery technology further.
