Metal-ceramic composites combine the excellent properties of metals and ceramics,which have high strength,stability,and corrosion re-sistance.Al_(2)O_(3)/FeCo composites have been proven to be useful in ap-plications ...Metal-ceramic composites combine the excellent properties of metals and ceramics,which have high strength,stability,and corrosion re-sistance.Al_(2)O_(3)/FeCo composites have been proven to be useful in ap-plications such as catalysts,mi-crowave absorption materials,and enhanced permeability dielectric.The understanding of the mechani-cal properties and dynamics at the atomic scale of the Al_(2)O_(3)/FeCo in-terface can promote the design and exploitment of metal-ceramic composites.In this work,we have obtained Young’s modulus and diffusion coefficient of the Al_(2)O_(3)/FeCo interface using molecular dynamics simulation,elucidated the structural characteristics of the Al_(2)O_(3)/FeCo interface at the atomic scale,and investigated the impact of atomic magnetism and the exter-nal magnetic field on the interface.Simulated results show that Young’s modulus of the Al_(2)O_(3)/FeCo interface is significantly improved compared with pure Al_(2)O_(3)and FeCo alloy at room and high temperatures.When the atomic magnetism and the external magnetic field are applied,Young’s modulus of the Al_(2)O_(3)/FeCo interface further increases to 612 GPa at 300 K and 602 GPa at 500 K.Moreover,the average density,diffusion coefficient,and radial distri-bution function are found to be modified substantially.This study will shed light on the atom-istic investigations of the metal-ceramic composites.展开更多
The difficulty in fabricating a multifaceted composite heterojunction system based on Cd_(x) Zn_(1-x) S limits the enhancement of photocatalytic performance.In the present scrutiny,novel ZnO/Cd_(x) Zn_(1-x) S/CdS com-...The difficulty in fabricating a multifaceted composite heterojunction system based on Cd_(x) Zn_(1-x) S limits the enhancement of photocatalytic performance.In the present scrutiny,novel ZnO/Cd_(x) Zn_(1-x) S/CdS com-posite heterojunctions are successfully prepared by the alkaline dissolution etching method.The internal electric field at the interface of I-type and Z-scheme heterojunction improved the effective charge sepa-ration.The ZC 8 sample exhibits excellent photocatalytic performance and the H2 production efficiency is 15.67 mmol g^(−1) h^(−1) with good stability up to 82.9%in 24-hour cycles.The performance of CH_(4) and CO capacity in the CO_(2) RR process is 3.47μmol g^(−1) h^(−1) and 23.5μmol g^(−1) h^(−1),respectively.The photogener-ated accelerated charge transport is then examined in detail by in situ X-ray photoelectron spectroscopy(ISXPS)and density functional theory(DFT)calculations.This work presents a new idea for the synthe-sis of Cd_(x) Zn_(1-x) S solid-solution-based materials and provides a solid reference for the detailed mechanism regarding the electric field at the heterojunction interface.展开更多
Use of metallic Li anode raises serious concerns on the safety and operational performance of Li-S batteries due to uncontrolled hazard of Li dendrite formation, which is difficultly eliminated as long as the metallic...Use of metallic Li anode raises serious concerns on the safety and operational performance of Li-S batteries due to uncontrolled hazard of Li dendrite formation, which is difficultly eliminated as long as the metallic Li exists in the cells. Pairing lithium sulfide (Li2S) cathode with currently available metallic Lifree high-capacity anodes offers an alternative solution to this challenge. However, the performance of Li2S cathode is primarily restricted by high activation barrier upon initial charge, low active mass utilization and sluggish redox kinetics. Herein, a MXene-induced multifunctional collaborative interface is proposed to afford superb activity towards redox solid-liquid/liquid-liquid phase transformation, strong chemisorption, high conductivity and fast ionic/charge transport in high Li2S loading cathode. Applying collaborative interface effectively reduces initial voltage barrier of Li2S activation and regulates the kinetic behavior of redox polysulfide conversion. Therefore, stable operation of additive-free Li2S cathode with high areal capacities at high Li2S loading up to 9 mg cm^-2 can be achieved with less sacrifice of high capacity and rate capability in Li-S batteries. Rechargeable metallic Li-free batteries are successfully constructed by pairing this high-performance Li2S cathode with high-capacity metal oxide anodes, which delivers superior energy density to current Li-ion batteries.展开更多
Catechol adsorbed on TiO_(2)is one of the simplest models to explore the relevant properties of dye-sensitized solar cells.However,the effects of water and defects on the electronic levels and the excitonic properties...Catechol adsorbed on TiO_(2)is one of the simplest models to explore the relevant properties of dye-sensitized solar cells.However,the effects of water and defects on the electronic levels and the excitonic properties of the catechol/TiO_(2)interface have been rarely explored.Here,we investigate four catechol/TiO_(2)interfaces aiming to study the influence of coverage,water,and defects on the electronic levels and the excitonic properties of the catechol/TiO_(2)interface through the first-principles many-body Green’s function theory.We find that the adsorption of catechol on the rutile(110)surface increases the energies of both the TiO_(2)valence band maximum and conduction band minimum by approximately 0.7 eV.The increasing coverage and the presence of water can reduce the optical absorption of charge-transfer excitons with maximum oscillator strength.Regarding the reduced hydroxylated TiO_(2)substrate,the conduction band minimum decreases greatly,resulting in a sub-bandgap of 2.51 eV.The exciton distributions in the four investigated interfaces can spread across several unit cells,especially for the hydroxylated TiO2substrate.Although the hydroxylated TiO_(2)substrate leads to a lower open-circuit voltage,it may increase the separation between photogenerated electrons and holes and may therefore be beneficial for improving the photovoltaic efficiency by controlling its concentration.Our results may provide guidance for the design of highly efficient solar cells in future.展开更多
In this study, a work-of-fracture method using a three-point bend beam （3PBB） specimen, which is commonly used to determine the fracture energy of concrete, was adapted to evaluate the mode-I fracture and durability...In this study, a work-of-fracture method using a three-point bend beam （3PBB） specimen, which is commonly used to determine the fracture energy of concrete, was adapted to evaluate the mode-I fracture and durability of fiber-reinforced polymer （FRP） composite-concrete bonded interfaces. Interface fracture properties were evaluated with established data reduction procedures. The proposed test method is primarily for use in evaluating the effects of freeze-thaw （F-T） and wet-dry （W-D） cycles that are the accelerated aging protocols on the mode-I fracture of carbon FRP-concrete bonded interfaces. The results of the mode-I fracture tests of F-T and W-D cycle-conditioned specimens show that both the critical load and fracture energy decrease as the number of cycles increases, and their degradation pattern has a nearly linear relationship with the number of cycles. However, compared with the effect of the F-T cycles, the critical load and fracture energy degrade at a slower rate with W-D cycles, which suggests that F-T cyclic conditioning causes more deterioration of carbon fiber-reinforced polymer （CFRP）-concrete bonded interface. After 50 and 100 conditioning cycles, scaling of concrete was observed in all the specimens subjected to F-T cycles, but not in those subjected to W-D cycles. The examination of interface fracture surfaces along the bonded interfaces with varying numbers of F-T and W-D conditioning cycles shows that （1） cohesive failure of CFRP composites is not observed in all fractured surfaces; （2） for the control specimens that have not been exposed to any conditioning cycles, the majority of interface failure is a result of cohesive fracture of concrete （peeling of concrete from the concrete substrate）, which means that the cracks mostly propagate within the concrete; and （3） as the number of F-T or W-D conditioning cycles increases, adhesive failure along the interface begins to emerge and gradually increases. It is thus concluded that the fracture properties （i.e., the critical load and fracture energy） of the bonded interface are controlled primarily by the concrete cohesive fracture before conditioning and by the adhesive interface fracture after many cycles of F-T or W-D conditioning. As demonstrated in this study, a test method using 3PBB specimens combined with a fictitious crack model and experimental conditioning protocols for durability can be used as an effective qualification method to test new hybrid material interface bonds and to evaluate durability-related effects on the interfaces.展开更多
Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)has attracted considerable attention as a non-toxic and earthabundant solar cell material.During selenization of CZTSSe film at high temperature,the reaction between CZTSSe and Mo...Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)has attracted considerable attention as a non-toxic and earthabundant solar cell material.During selenization of CZTSSe film at high temperature,the reaction between CZTSSe and Mo is one of the main reasons that result in unfavorable absorber and interface quality,which leads to large open circuit voltage deficit(VOC-def)and low fill factor(FF).Herein,a WO_(3)intermediate layer introduced at the back interface can effectually inhibit the unfavorable interface reaction between absorber and back electrode in the preliminary selenization progress;thus high-quality crystals are obtained.Through this back interface engineering,the traditional problems of phase segregation,voids in the absorber and over thick Mo(S,Se)_(2)at the back interface can be well solved,which greatly lessens the recombination in the bulk and at the interface.The increased minority carrier diffusion length,decreased barrier height at back interface contact and reduced deep acceptor defects give rise to systematic improvement in VOCand FF,finally a 12.66%conversion efficiency for CZTSSe solar cell has been achieved.This work provides a simple way to fabricate highly efficient solar cells and promotes a deeper understanding of the function of intermediate layer at back interface in kesterite-based solar cells.展开更多
Focusing on the low open circuit voltage(V_(OC))and fill factor(FF)in flexible Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells,indium(In)ions are introduced into the CZTSSe absorbers near Mo foils to modify the back interface...Focusing on the low open circuit voltage(V_(OC))and fill factor(FF)in flexible Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells,indium(In)ions are introduced into the CZTSSe absorbers near Mo foils to modify the back interface and passivate deep level defects in CZTSSe bulk concurrently for improving the performance of flexible device.The results show that In doping effectively inhibits the formation of secondary phase(Cu(S,Se)_(2))and VSndefects.Further studies demonstrate that the barrier height at the back interface is decreased and the deep level defects(Cu_(Sn)defects)in CZTSSe bulk are passivated.Moreover,the carrier concentration is increased and the V_(OC) deficit(V_(OC,def))is decreased significantly due to In doping.Finally,the flexible CZTSSe solar cell with 10.01%power conversion efficiency(PCE)has been obtained.The synergistic strategy of interface modification and bulk defects passivation through In incorporation provides a new thought for the fabrication of efficient flexible kesterite-based solar cells.展开更多
Heterojunction photocatalysts have shown considerable activities for organic pollutants degradation.However,the faint connection interface and inferior charge shift efficiency critically block the property of heteroju...Heterojunction photocatalysts have shown considerable activities for organic pollutants degradation.However,the faint connection interface and inferior charge shift efficiency critically block the property of heterojunction photocatalysis.Herein,Bi_(2)O_(2)S/NiFe_(2)O_(4) nanosheets heterojunction with ultrastrong inter-face interaction and high internal electric field are designed by an in-situ growth method.Tentative and theoretical consequences prove that the interfacial interaction and internal electric field not only act as the electron flow bridge but also decrease the electrons shift energy obstacle,thus speeding up electrons transfer and achieving effective spatial electron-hole separation.Therefore,a large amount of·O_(2)^(-)and holes as active species were generated.Remarkably,Bi_(2)O_(2) S/NiFe_(2)O_(4) establishes a considerably boosted photocatalytic performance for tetracycline degradation(0.032 min^(-1)),which is about 14.2-fold and 7.8-fold of the pristine BOS and NFO,respectively.This work provides a promising motivation for modulating charge transfer by interface control and internal electric field to boost photocatalytic performance.展开更多
Comparison in electron transfer(ET) processes from decamethyferrocene(DMFe) in nitrobenzene(NB) to ferric ion in aqueous phase was investigated for the first time by the scanning electrochemical microscopy(SECM).As co...Comparison in electron transfer(ET) processes from decamethyferrocene(DMFe) in nitrobenzene(NB) to ferric ion in aqueous phase was investigated for the first time by the scanning electrochemical microscopy(SECM).As compared with the system of Fe(CN)_6^(3-)-DMFe,the ET rate obtained from Fe^(3+)-DMFe was lower in spite of larger driving force,which may arise from the effect of reorganization energy.Otherwise,the effect of common ion on rate constants was also probed and results suggested additional complexit...展开更多
The scanning electron microscope (SEM) results of bone interface of titanium-coated 317L plate screw are reported in this article. 317L plate screw had a rough surface composed of sprayed pure titanium which formed a ...The scanning electron microscope (SEM) results of bone interface of titanium-coated 317L plate screw are reported in this article. 317L plate screw had a rough surface composed of sprayed pure titanium which formed a bone/metal interface in biointegration after implanted into the mandible of dog. Though a bone/metal interface in osseointegration was also formed on the surface of uncoated 317L plate screw after implantation, a smal1 space was seen between the bone and surface of the screw, indicating that the tissue compatibility of titanium-coated 317L plate screw may be better than that of the non-coated screw.展开更多
A transient three-dimensional coupling model based on the compressible volume of fluid （VOF） method was developed to simulate the transport of volatile pollutants at the air-water interface. VOF is a numerical techn...A transient three-dimensional coupling model based on the compressible volume of fluid （VOF） method was developed to simulate the transport of volatile pollutants at the air-water interface. VOF is a numerical technique for locating and tracking the free surface of water flow. The relationships between Henry＇s constant, thermodynamics parameters, and the enlarged topological index were proposed for nonstandard conditions. A series of experiments and numerical simulations were performed to study the transport of benzene and carbinol. The simulation results agreed with the experimental results. Temperature had no effect on mass transfer of pollutants with low transfer free energy and high Henry＇s constant. The temporal and spatial distribution of pollutants with high transfer free energy and low Henry＇s constant was affected by temperature. The total enthalpy and total transfer free energy increased significantly with temperature, with significant fluctuations at low temperatures. The total enthalpy and total transfer free energy increased steadily without fluctuation at high temperatures.展开更多
Very recently,experimental evidence showed that the hydrogen is retained in dithiol-terminated single-molecule junction under the widely adopted preparation conditions,which is in contrast to the accepted view[Nat.Che...Very recently,experimental evidence showed that the hydrogen is retained in dithiol-terminated single-molecule junction under the widely adopted preparation conditions,which is in contrast to the accepted view[Nat.Chem.11351(2019)].However,the hydrogen is generally assumed to be lost in the previous physical models of single-molecule junctions.Whether the retention of the hydrogen at the gold-sulfur interface exerts a significant effect on the theoretical prediction of spin transport properties is an open question.Therefore,here in this paper we carry out a comparative study of spin transport in M-tetraphenylporphyrin-based(M=V,Cr,Mn,Fe,and Co;M-TPP)single-molecule junction through Au-SR and Au-S(H)R bondings.The results show that the hydrogen at the gold-sulfur interface may dramatically affect the spin-filtering efficiency of M-TPP-based single-molecule junction,depending on the type of transition metal ions embedded into porphyrin ring.Moreover,we find that for the Co-TPP-based molecular junction,the hydrogen at the gold-sulfur interface has no obvious effect on transmission at the Fermi level,but it has a significant effect on the spin-dependent transmission dip induced by the quantum interference on the occupied side.Thus the fate of hydrogen should be concerned in the physical model according to the actual preparation condition,which is important for our fundamental understanding of spin transport in the single-molecule junctions.Our work also provides guidance in how to experimentally identify the nature of gold-sulfur interface in the single-molecule junction with spin-polarized transport.展开更多
We developed the high-gravity coupled liquid-liquid interface reaction technique on the basis of the rotating packed bed(RPB)reactor for the continuous and ultrafast synthesis of silver sulfide(Ag2S)quantum dots(QDs)w...We developed the high-gravity coupled liquid-liquid interface reaction technique on the basis of the rotating packed bed(RPB)reactor for the continuous and ultrafast synthesis of silver sulfide(Ag2S)quantum dots(QDs)with near-infrared(NIR)luminescence.The formation of Ag2S QDs occurs at the interface of microdroplets,and the average size of Ag2S QDs was 4.5 nm with a narrow size distribution.Ag2S QDs can disperse well in various organic solvents and exhibit NIR luminescence with a peak wavelength at 1270 nm under 980-nm laser excitation.The mechanism of the process intensification was revealed by both the computational fluid dynamics simulation and fluorescence imaging,and the mechanism is attributed to the small and uniform droplet formation in the RPB reactor.This study provides a novel approach for the continuous and ultrafast synthesis of NIR Ag2S QDs for potential scale-up.展开更多
Sluggish kinetics of lithium/sulfur(Li/S)conversion chemistry and the ion channels formation in the cathode is still a bottleneck for developing future Li/S batteries with high-rate,long-cycling and high-energy.Here,a...Sluggish kinetics of lithium/sulfur(Li/S)conversion chemistry and the ion channels formation in the cathode is still a bottleneck for developing future Li/S batteries with high-rate,long-cycling and high-energy.Here,a rational cathode structure design of an oxygen(O)and nitrogen(N)tailoring carbon fiber aerogel(OCNF)as a host material integrated with platinum(Pt)electrocatalysis interface is employed to regulate Li/S conversion chemistry and ion channel.The Pt nanoparticles were uniformly sprayed onto the S surface to construct the electrocatalysis interface(Pt/S/OCNF)for generating ion channels to promote the effective penetration of electrolyte into the cathode.This Pt/S/OCNF gives the cathode a high sulfur utilization of 77.5%,an excellent rate capacity of 813.2 m Ah/g(2 C),and an outstanding long-cycling performance with a capacitance retention of 82.6%and a decay of 0.086%per cycle after 200 cycles at 0.5 C.Density functional theory(DFT)calculations reveal that the Pt electrocatalysis interface makes the cathode a high density of state(DOS)at Fermi level to facilitate the electrical conductivity,charge transfer kinetics and electrocatalysis to accelerate the lithium polysulfides(LiPSs)electrochemical conversion.Furthermore,the unique chemisorption structure and adsorption ability of Li2Sn(n=1,2,4,6,8)and S8on OCNF are attributed to the bridging effects of interfacial Pt and the bonding of N-Li.The Pt electrocatalysis interface combined with the unique 3D hierarchical porous structure and abundant functional active sites at OCNF guarantee strong adsorption confinement,fast Li/S electrocatalytic conversion and unblocked ion channels for electrolyte permeation in cathode.展开更多
Rechargeable magnesium-ion(Mg-ion)batteries have attracted wide attention for energy storage.However,magnesium anode is still limited by the irreversible Mg plating/stripping procedure.Herein,a well-designed binary Bi...Rechargeable magnesium-ion(Mg-ion)batteries have attracted wide attention for energy storage.However,magnesium anode is still limited by the irreversible Mg plating/stripping procedure.Herein,a well-designed binary Bi_(2)O_(3)-Bi_(2)S_(3)(BO-BS)heterostructure is fulfilled by virtue of the cooperative interface and energy band engineering targeted fast Mg-ion storage.The built-in electronic field resulting from the asymmetrical electron distribution at the interface of electron-rich S center at Bi_(2)S_(3) side and electron-poor O center at Bi_(2)O_(3) side effectively accelerates the electrochemical reaction kinetics in the Mg-ion battery system.Moreover,the as-designed heterogenous interface also benefits to maintaining the electrode integrity.With these advantages,the BO-BS electrode displays a remarkable capacity of 150.36 mAh g^(−1) at 0.67 A g^(-1) and a superior cycling stability.This investigation would offer novel insights into the rational design of functional heterogenous electrode materials targeted the fast reaction kinetics for energy storage systems.展开更多
The austenite medium Mn steel modified with controlled additions of Ca, Y, Si were directionally solidified using the vertical Bridgman method to study the effects of Ca（Y）-Si modifier on the solid-liquid （S-L） in...The austenite medium Mn steel modified with controlled additions of Ca, Y, Si were directionally solidified using the vertical Bridgman method to study the effects of Ca（Y）-Si modifier on the solid-liquid （S-L） interface morphology and solute segregation. The interface morphology and the C and Mn segregation of the steel directionally solidified at 6.9 μtrn/s were investigated with an image analysis and a scanning electron microscope equipped with energy dispersive X-ray analysis. The 0.5wt% Ca-Si modified steel is solidified with a planar S-L interface. The interface of the 1.0wt% Ca-Si modified steel is similar to that of the 0.5wt% Ca-Si modified steel, but with larger nodes. The 1.5wt% Ca-Si modified steel displays a cellular growth parttern. The S-L interface morphology of the 0.5wt% Ca-Si＋1.0wt% Y-Si modified Mn steel appears as dendritic interface, and primary austenite dendrites reveal developed lateral branching at the quenched liquid. In the meantime, the independent austenite colonies are formed ahead of the S-L interface. A mechanism involving constitutional supercooling explains the S-L interface evolution. It depends mainly on the difference in the contents of Ca, Y, and Si ahead of the S-L interface. The segregation of C and Mn ahead of the S-L interface enhanced by the modifiers is observed.展开更多
Characteristics of Mode I crack near the interface of elasticity matched but plasticity and strength mismatched materials differ from those of the crack in a homogenous body. Interface body of different strength influ...Characteristics of Mode I crack near the interface of elasticity matched but plasticity and strength mismatched materials differ from those of the crack in a homogenous body. Interface body of different strength influences the plastic or cohesive zone at the crack tip in parent body. The mathematical model for load line opening of the crack near the interface in linear elastic regime involves singular integrals. The paper presents explicit solution of these integrals with the help of Cauchy’s principal value theorem. Cases of thin and thick welds between the materials are investigated. Solutions of the integrals are well substantiated. Final results are provided in a consolidated form.展开更多
基金supported by the National Natural Science Foundation of China(Nos.22173057,52130204,12074241,11929401,12311530675)Science and Technology Commission of Shanghai Municipality(Nos.21JC1402700,22XD1400900,20501130600,21JC1402600)High-Performance Computing Center,Shanghai Technical Service Center of Science and Engineering Computing,Shanghai University。
文摘Metal-ceramic composites combine the excellent properties of metals and ceramics,which have high strength,stability,and corrosion re-sistance.Al_(2)O_(3)/FeCo composites have been proven to be useful in ap-plications such as catalysts,mi-crowave absorption materials,and enhanced permeability dielectric.The understanding of the mechani-cal properties and dynamics at the atomic scale of the Al_(2)O_(3)/FeCo in-terface can promote the design and exploitment of metal-ceramic composites.In this work,we have obtained Young’s modulus and diffusion coefficient of the Al_(2)O_(3)/FeCo interface using molecular dynamics simulation,elucidated the structural characteristics of the Al_(2)O_(3)/FeCo interface at the atomic scale,and investigated the impact of atomic magnetism and the exter-nal magnetic field on the interface.Simulated results show that Young’s modulus of the Al_(2)O_(3)/FeCo interface is significantly improved compared with pure Al_(2)O_(3)and FeCo alloy at room and high temperatures.When the atomic magnetism and the external magnetic field are applied,Young’s modulus of the Al_(2)O_(3)/FeCo interface further increases to 612 GPa at 300 K and 602 GPa at 500 K.Moreover,the average density,diffusion coefficient,and radial distri-bution function are found to be modified substantially.This study will shed light on the atom-istic investigations of the metal-ceramic composites.
基金financially supported by the National Key Re-search and Development Program of China[No.2022YFF1202500,2022YFF1202502]the National Natural Science Foundation of China[62071459]+1 种基金the Subject arrangement Foundation of Shen-zhen[No.JCYJ20180507182057026]the International Science and Technology Cooperation Project of Bingtuan[No.2022BC008]。
文摘The difficulty in fabricating a multifaceted composite heterojunction system based on Cd_(x) Zn_(1-x) S limits the enhancement of photocatalytic performance.In the present scrutiny,novel ZnO/Cd_(x) Zn_(1-x) S/CdS com-posite heterojunctions are successfully prepared by the alkaline dissolution etching method.The internal electric field at the interface of I-type and Z-scheme heterojunction improved the effective charge sepa-ration.The ZC 8 sample exhibits excellent photocatalytic performance and the H2 production efficiency is 15.67 mmol g^(−1) h^(−1) with good stability up to 82.9%in 24-hour cycles.The performance of CH_(4) and CO capacity in the CO_(2) RR process is 3.47μmol g^(−1) h^(−1) and 23.5μmol g^(−1) h^(−1),respectively.The photogener-ated accelerated charge transport is then examined in detail by in situ X-ray photoelectron spectroscopy(ISXPS)and density functional theory(DFT)calculations.This work presents a new idea for the synthe-sis of Cd_(x) Zn_(1-x) S solid-solution-based materials and provides a solid reference for the detailed mechanism regarding the electric field at the heterojunction interface.
基金supported by the National Natural Science Foundation of China (NSFC, No. 51522203, 51772040)Fok Ying Tung Education Foundation (No. 151047)+2 种基金the Recruitment Program of Global Youth ExpertsXinghai Scholarship of Dalian University of Technologythe Fundamental Research Funds for the Central Universities (No. DUT18LAB19)
文摘Use of metallic Li anode raises serious concerns on the safety and operational performance of Li-S batteries due to uncontrolled hazard of Li dendrite formation, which is difficultly eliminated as long as the metallic Li exists in the cells. Pairing lithium sulfide (Li2S) cathode with currently available metallic Lifree high-capacity anodes offers an alternative solution to this challenge. However, the performance of Li2S cathode is primarily restricted by high activation barrier upon initial charge, low active mass utilization and sluggish redox kinetics. Herein, a MXene-induced multifunctional collaborative interface is proposed to afford superb activity towards redox solid-liquid/liquid-liquid phase transformation, strong chemisorption, high conductivity and fast ionic/charge transport in high Li2S loading cathode. Applying collaborative interface effectively reduces initial voltage barrier of Li2S activation and regulates the kinetic behavior of redox polysulfide conversion. Therefore, stable operation of additive-free Li2S cathode with high areal capacities at high Li2S loading up to 9 mg cm^-2 can be achieved with less sacrifice of high capacity and rate capability in Li-S batteries. Rechargeable metallic Li-free batteries are successfully constructed by pairing this high-performance Li2S cathode with high-capacity metal oxide anodes, which delivers superior energy density to current Li-ion batteries.
基金supported by the Scientific and Technological Innovation Programs of Higher Education Institutions in Shanxi(No.2020L0609 and No.2020L0556)the Doctoral research funds of Jinzhong University(jzxybsjjxm2019005)the Basic Research Program in Shanxi Province under the Grant No.20210302124345。
文摘Catechol adsorbed on TiO_(2)is one of the simplest models to explore the relevant properties of dye-sensitized solar cells.However,the effects of water and defects on the electronic levels and the excitonic properties of the catechol/TiO_(2)interface have been rarely explored.Here,we investigate four catechol/TiO_(2)interfaces aiming to study the influence of coverage,water,and defects on the electronic levels and the excitonic properties of the catechol/TiO_(2)interface through the first-principles many-body Green’s function theory.We find that the adsorption of catechol on the rutile(110)surface increases the energies of both the TiO_(2)valence band maximum and conduction band minimum by approximately 0.7 eV.The increasing coverage and the presence of water can reduce the optical absorption of charge-transfer excitons with maximum oscillator strength.Regarding the reduced hydroxylated TiO_(2)substrate,the conduction band minimum decreases greatly,resulting in a sub-bandgap of 2.51 eV.The exciton distributions in the four investigated interfaces can spread across several unit cells,especially for the hydroxylated TiO2substrate.Although the hydroxylated TiO_(2)substrate leads to a lower open-circuit voltage,it may increase the separation between photogenerated electrons and holes and may therefore be beneficial for improving the photovoltaic efficiency by controlling its concentration.Our results may provide guidance for the design of highly efficient solar cells in future.
基金partially supported by the National Science Foundation(Grant No.CMS-0002829)
文摘In this study, a work-of-fracture method using a three-point bend beam （3PBB） specimen, which is commonly used to determine the fracture energy of concrete, was adapted to evaluate the mode-I fracture and durability of fiber-reinforced polymer （FRP） composite-concrete bonded interfaces. Interface fracture properties were evaluated with established data reduction procedures. The proposed test method is primarily for use in evaluating the effects of freeze-thaw （F-T） and wet-dry （W-D） cycles that are the accelerated aging protocols on the mode-I fracture of carbon FRP-concrete bonded interfaces. The results of the mode-I fracture tests of F-T and W-D cycle-conditioned specimens show that both the critical load and fracture energy decrease as the number of cycles increases, and their degradation pattern has a nearly linear relationship with the number of cycles. However, compared with the effect of the F-T cycles, the critical load and fracture energy degrade at a slower rate with W-D cycles, which suggests that F-T cyclic conditioning causes more deterioration of carbon fiber-reinforced polymer （CFRP）-concrete bonded interface. After 50 and 100 conditioning cycles, scaling of concrete was observed in all the specimens subjected to F-T cycles, but not in those subjected to W-D cycles. The examination of interface fracture surfaces along the bonded interfaces with varying numbers of F-T and W-D conditioning cycles shows that （1） cohesive failure of CFRP composites is not observed in all fractured surfaces; （2） for the control specimens that have not been exposed to any conditioning cycles, the majority of interface failure is a result of cohesive fracture of concrete （peeling of concrete from the concrete substrate）, which means that the cracks mostly propagate within the concrete; and （3） as the number of F-T or W-D conditioning cycles increases, adhesive failure along the interface begins to emerge and gradually increases. It is thus concluded that the fracture properties （i.e., the critical load and fracture energy） of the bonded interface are controlled primarily by the concrete cohesive fracture before conditioning and by the adhesive interface fracture after many cycles of F-T or W-D conditioning. As demonstrated in this study, a test method using 3PBB specimens combined with a fictitious crack model and experimental conditioning protocols for durability can be used as an effective qualification method to test new hybrid material interface bonds and to evaluate durability-related effects on the interfaces.
基金supported by the National Key R&D Program of China(no.2018YFE0203400)the National Natural Science Foundation of China(no.62074102)+1 种基金the Guangdong Basic and Applied Basic Research Foundation(no.2022A1515010979)the Science and Technology plan project of Shenzhen(nos.JCYJ20190808120001755 and 20220808165025003)。
文摘Kesterite Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)has attracted considerable attention as a non-toxic and earthabundant solar cell material.During selenization of CZTSSe film at high temperature,the reaction between CZTSSe and Mo is one of the main reasons that result in unfavorable absorber and interface quality,which leads to large open circuit voltage deficit(VOC-def)and low fill factor(FF).Herein,a WO_(3)intermediate layer introduced at the back interface can effectually inhibit the unfavorable interface reaction between absorber and back electrode in the preliminary selenization progress;thus high-quality crystals are obtained.Through this back interface engineering,the traditional problems of phase segregation,voids in the absorber and over thick Mo(S,Se)_(2)at the back interface can be well solved,which greatly lessens the recombination in the bulk and at the interface.The increased minority carrier diffusion length,decreased barrier height at back interface contact and reduced deep acceptor defects give rise to systematic improvement in VOCand FF,finally a 12.66%conversion efficiency for CZTSSe solar cell has been achieved.This work provides a simple way to fabricate highly efficient solar cells and promotes a deeper understanding of the function of intermediate layer at back interface in kesterite-based solar cells.
基金supported by the National Natural Science Foundation of China(62074037)the Science and Technology Department of Fujian Province(2020I0006)the Fujian Science&Technology Innovation Laboratory for Optoelectronic Information of China(2021ZZ124)。
文摘Focusing on the low open circuit voltage(V_(OC))and fill factor(FF)in flexible Cu_(2)ZnSn(S,Se)_(4)(CZTSSe)solar cells,indium(In)ions are introduced into the CZTSSe absorbers near Mo foils to modify the back interface and passivate deep level defects in CZTSSe bulk concurrently for improving the performance of flexible device.The results show that In doping effectively inhibits the formation of secondary phase(Cu(S,Se)_(2))and VSndefects.Further studies demonstrate that the barrier height at the back interface is decreased and the deep level defects(Cu_(Sn)defects)in CZTSSe bulk are passivated.Moreover,the carrier concentration is increased and the V_(OC) deficit(V_(OC,def))is decreased significantly due to In doping.Finally,the flexible CZTSSe solar cell with 10.01%power conversion efficiency(PCE)has been obtained.The synergistic strategy of interface modification and bulk defects passivation through In incorporation provides a new thought for the fabrication of efficient flexible kesterite-based solar cells.
基金the financial support by the National Natural Science Foundation of China as general projects(Grant Nos.51779068,52070066,52211530084,42277059,and 22006029)Tianjin Commission of Science and Technology as key technologies R&D projects(No.21YFSNSN00250)+1 种基金Doctoral Inno-vation Project of Hebei Province(CXZZBS2023031)the Royal Society/International Exchanges 2021 Cost Share/NSFC(Grant No.IEC\NSFC\211142).
文摘Heterojunction photocatalysts have shown considerable activities for organic pollutants degradation.However,the faint connection interface and inferior charge shift efficiency critically block the property of heterojunction photocatalysis.Herein,Bi_(2)O_(2)S/NiFe_(2)O_(4) nanosheets heterojunction with ultrastrong inter-face interaction and high internal electric field are designed by an in-situ growth method.Tentative and theoretical consequences prove that the interfacial interaction and internal electric field not only act as the electron flow bridge but also decrease the electrons shift energy obstacle,thus speeding up electrons transfer and achieving effective spatial electron-hole separation.Therefore,a large amount of·O_(2)^(-)and holes as active species were generated.Remarkably,Bi_(2)O_(2) S/NiFe_(2)O_(4) establishes a considerably boosted photocatalytic performance for tetracycline degradation(0.032 min^(-1)),which is about 14.2-fold and 7.8-fold of the pristine BOS and NFO,respectively.This work provides a promising motivation for modulating charge transfer by interface control and internal electric field to boost photocatalytic performance.
基金supported by the National Natural Science Foundation of China(No.20875077,No.20775060 and No.20927004)the Natural Science Foundation of Gansu(No.0701RJZA109 and No.0803RJZA105)Key Projects of Scientific Research Base of Department of Education,Gansu Province(No.08zx-07).
文摘Comparison in electron transfer(ET) processes from decamethyferrocene(DMFe) in nitrobenzene(NB) to ferric ion in aqueous phase was investigated for the first time by the scanning electrochemical microscopy(SECM).As compared with the system of Fe(CN)_6^(3-)-DMFe,the ET rate obtained from Fe^(3+)-DMFe was lower in spite of larger driving force,which may arise from the effect of reorganization energy.Otherwise,the effect of common ion on rate constants was also probed and results suggested additional complexit...
文摘The scanning electron microscope (SEM) results of bone interface of titanium-coated 317L plate screw are reported in this article. 317L plate screw had a rough surface composed of sprayed pure titanium which formed a bone/metal interface in biointegration after implanted into the mandible of dog. Though a bone/metal interface in osseointegration was also formed on the surface of uncoated 317L plate screw after implantation, a smal1 space was seen between the bone and surface of the screw, indicating that the tissue compatibility of titanium-coated 317L plate screw may be better than that of the non-coated screw.
基金supported by the National Natural Science Foundation of China(Grant No.51109106)the Natural Science Foundation of Jiangsu Province(Grant No.BK20130946)the Qing Lan Project of Jiangsu Province
文摘A transient three-dimensional coupling model based on the compressible volume of fluid （VOF） method was developed to simulate the transport of volatile pollutants at the air-water interface. VOF is a numerical technique for locating and tracking the free surface of water flow. The relationships between Henry＇s constant, thermodynamics parameters, and the enlarged topological index were proposed for nonstandard conditions. A series of experiments and numerical simulations were performed to study the transport of benzene and carbinol. The simulation results agreed with the experimental results. Temperature had no effect on mass transfer of pollutants with low transfer free energy and high Henry＇s constant. The temporal and spatial distribution of pollutants with high transfer free energy and low Henry＇s constant was affected by temperature. The total enthalpy and total transfer free energy increased significantly with temperature, with significant fluctuations at low temperatures. The total enthalpy and total transfer free energy increased steadily without fluctuation at high temperatures.
基金the National Natural Science Foundation of China(Grant Nos.11674092,11804093,and 61764005)the Natural Science Foundation of Hunan Province,China(Grant No.2019JJ40006)+2 种基金the Scientific Research Fund of the Education Department of Hunan Province,China(Grant No.18B368)the Science and Technology Development Plan Project of Hengyang City,China(Grant No.2018KJ121)the Science and Technology Plan Project of Hunan Province,China(Grant No.2016TP1020).
文摘Very recently,experimental evidence showed that the hydrogen is retained in dithiol-terminated single-molecule junction under the widely adopted preparation conditions,which is in contrast to the accepted view[Nat.Chem.11351(2019)].However,the hydrogen is generally assumed to be lost in the previous physical models of single-molecule junctions.Whether the retention of the hydrogen at the gold-sulfur interface exerts a significant effect on the theoretical prediction of spin transport properties is an open question.Therefore,here in this paper we carry out a comparative study of spin transport in M-tetraphenylporphyrin-based(M=V,Cr,Mn,Fe,and Co;M-TPP)single-molecule junction through Au-SR and Au-S(H)R bondings.The results show that the hydrogen at the gold-sulfur interface may dramatically affect the spin-filtering efficiency of M-TPP-based single-molecule junction,depending on the type of transition metal ions embedded into porphyrin ring.Moreover,we find that for the Co-TPP-based molecular junction,the hydrogen at the gold-sulfur interface has no obvious effect on transmission at the Fermi level,but it has a significant effect on the spin-dependent transmission dip induced by the quantum interference on the occupied side.Thus the fate of hydrogen should be concerned in the physical model according to the actual preparation condition,which is important for our fundamental understanding of spin transport in the single-molecule junctions.Our work also provides guidance in how to experimentally identify the nature of gold-sulfur interface in the single-molecule junction with spin-polarized transport.
基金supported by the National Natural Science Foundation of China(No.21808009)the Beijing Natural Science Foundation(No.2182051).
文摘We developed the high-gravity coupled liquid-liquid interface reaction technique on the basis of the rotating packed bed(RPB)reactor for the continuous and ultrafast synthesis of silver sulfide(Ag2S)quantum dots(QDs)with near-infrared(NIR)luminescence.The formation of Ag2S QDs occurs at the interface of microdroplets,and the average size of Ag2S QDs was 4.5 nm with a narrow size distribution.Ag2S QDs can disperse well in various organic solvents and exhibit NIR luminescence with a peak wavelength at 1270 nm under 980-nm laser excitation.The mechanism of the process intensification was revealed by both the computational fluid dynamics simulation and fluorescence imaging,and the mechanism is attributed to the small and uniform droplet formation in the RPB reactor.This study provides a novel approach for the continuous and ultrafast synthesis of NIR Ag2S QDs for potential scale-up.
基金funding support from National Key R&D Program of China(No.2016YFB0100100)The National Natural Science Foundation of China(Nos.21961024,21961025,21433013,U1832218)+5 种基金Inner Mongolia Natural Science Foundation(No.2018JQ05)Supported by Incentive Funding from Nano Innovation Institute(NII)of Inner Mongolia University for Nationalities(IMUN)Inner Mongolia Autonomous Region Funding Project for Science&Technology Achievement Transformation(No.CGZH2018156)Inner Mongolia Autonomous Region Incentive Funding Guided Project for Science&Technology Innovation(2016)Inner Mongolia Autonomous Region Science&Technology Planning Project for Applied Technology Research and Development(No.2019GG261)Tongliao Funding Project for Application Technology Research&Development(2017)。
文摘Sluggish kinetics of lithium/sulfur(Li/S)conversion chemistry and the ion channels formation in the cathode is still a bottleneck for developing future Li/S batteries with high-rate,long-cycling and high-energy.Here,a rational cathode structure design of an oxygen(O)and nitrogen(N)tailoring carbon fiber aerogel(OCNF)as a host material integrated with platinum(Pt)electrocatalysis interface is employed to regulate Li/S conversion chemistry and ion channel.The Pt nanoparticles were uniformly sprayed onto the S surface to construct the electrocatalysis interface(Pt/S/OCNF)for generating ion channels to promote the effective penetration of electrolyte into the cathode.This Pt/S/OCNF gives the cathode a high sulfur utilization of 77.5%,an excellent rate capacity of 813.2 m Ah/g(2 C),and an outstanding long-cycling performance with a capacitance retention of 82.6%and a decay of 0.086%per cycle after 200 cycles at 0.5 C.Density functional theory(DFT)calculations reveal that the Pt electrocatalysis interface makes the cathode a high density of state(DOS)at Fermi level to facilitate the electrical conductivity,charge transfer kinetics and electrocatalysis to accelerate the lithium polysulfides(LiPSs)electrochemical conversion.Furthermore,the unique chemisorption structure and adsorption ability of Li2Sn(n=1,2,4,6,8)and S8on OCNF are attributed to the bridging effects of interfacial Pt and the bonding of N-Li.The Pt electrocatalysis interface combined with the unique 3D hierarchical porous structure and abundant functional active sites at OCNF guarantee strong adsorption confinement,fast Li/S electrocatalytic conversion and unblocked ion channels for electrolyte permeation in cathode.
基金supported by the National Natural Science Foundation of China(52172239)Project of State Key Laboratory of Environment-Friendly Energy Materials(SWUST,Grant Nos.22fksy23 and 18ZD320304)+3 种基金the Frontier Project of Chengdu Tianfu New Area Institute(SWUST,Grand No.2022ZY017)Chongqing Talents:Exceptional Young Talents Project(Grant No.CQYC201905041)Natural Science Foundation of Chongqing China(Grant No.cstc2021jcyj-jqX0031)Interdiscipline Team Project under auspices of“Light of West”Program in Chinese Academy of Sciences(Grant No.xbzg-zdsys-202106).
文摘Rechargeable magnesium-ion(Mg-ion)batteries have attracted wide attention for energy storage.However,magnesium anode is still limited by the irreversible Mg plating/stripping procedure.Herein,a well-designed binary Bi_(2)O_(3)-Bi_(2)S_(3)(BO-BS)heterostructure is fulfilled by virtue of the cooperative interface and energy band engineering targeted fast Mg-ion storage.The built-in electronic field resulting from the asymmetrical electron distribution at the interface of electron-rich S center at Bi_(2)S_(3) side and electron-poor O center at Bi_(2)O_(3) side effectively accelerates the electrochemical reaction kinetics in the Mg-ion battery system.Moreover,the as-designed heterogenous interface also benefits to maintaining the electrode integrity.With these advantages,the BO-BS electrode displays a remarkable capacity of 150.36 mAh g^(−1) at 0.67 A g^(-1) and a superior cycling stability.This investigation would offer novel insights into the rational design of functional heterogenous electrode materials targeted the fast reaction kinetics for energy storage systems.
基金This work is financially supported by the National Natural Science Foundation of China (No.50001008 and No. 50271042).
文摘The austenite medium Mn steel modified with controlled additions of Ca, Y, Si were directionally solidified using the vertical Bridgman method to study the effects of Ca（Y）-Si modifier on the solid-liquid （S-L） interface morphology and solute segregation. The interface morphology and the C and Mn segregation of the steel directionally solidified at 6.9 μtrn/s were investigated with an image analysis and a scanning electron microscope equipped with energy dispersive X-ray analysis. The 0.5wt% Ca-Si modified steel is solidified with a planar S-L interface. The interface of the 1.0wt% Ca-Si modified steel is similar to that of the 0.5wt% Ca-Si modified steel, but with larger nodes. The 1.5wt% Ca-Si modified steel displays a cellular growth parttern. The S-L interface morphology of the 0.5wt% Ca-Si＋1.0wt% Y-Si modified Mn steel appears as dendritic interface, and primary austenite dendrites reveal developed lateral branching at the quenched liquid. In the meantime, the independent austenite colonies are formed ahead of the S-L interface. A mechanism involving constitutional supercooling explains the S-L interface evolution. It depends mainly on the difference in the contents of Ca, Y, and Si ahead of the S-L interface. The segregation of C and Mn ahead of the S-L interface enhanced by the modifiers is observed.
文摘Characteristics of Mode I crack near the interface of elasticity matched but plasticity and strength mismatched materials differ from those of the crack in a homogenous body. Interface body of different strength influences the plastic or cohesive zone at the crack tip in parent body. The mathematical model for load line opening of the crack near the interface in linear elastic regime involves singular integrals. The paper presents explicit solution of these integrals with the help of Cauchy’s principal value theorem. Cases of thin and thick welds between the materials are investigated. Solutions of the integrals are well substantiated. Final results are provided in a consolidated form.
