The corrosion of waste canisters in the deep geological disposal facilities(GDFs)for high-level radioactive waste(HLRW)can generate gas,which escapes from the engineered barrier system through the interfaces between t...The corrosion of waste canisters in the deep geological disposal facilities(GDFs)for high-level radioactive waste(HLRW)can generate gas,which escapes from the engineered barrier system through the interfaces between the bentonite buffer blocks and the host rock and those between the bentonite blocks.In this study,a series of water infiltration and gas breakthrough experiments were conducted on granite and on granite-bentonite specimens with smooth and grooved interfaces.On this basis,this study presents new insights and a quantitative assessment of the impact of the interface between clay and host rock on gas transport.As the results show,the water permeability values from water infiltration tests on granite and granite-bentonite samples(10−19-10−20m^(2))are found to be slightly higher than that of bentonite.The gas permeability of the mock-up samples with smooth interfaces is one order of magnitude larger than that of the mock-up with grooved interfaces.The gas results of breakthrough pressures for the granite and the granite-bentonite mock-up samples are significantly lower than that of bentonite.The results highlight the potential existence of preferential gas migration channels between the rock and bentonite buffer that require further considerations in safety assessment.展开更多
Based on the microscopic phase-field model, ordered domain interfaces formed between D022 （Ni3V） phases along [001] direction in Ni75AlxV25-x alloys were simulated, and the effects of atomic structure on the migrati...Based on the microscopic phase-field model, ordered domain interfaces formed between D022 （Ni3V） phases along [001] direction in Ni75AlxV25-x alloys were simulated, and the effects of atomic structure on the migration characteristic and solute segregation of interfaces were studied. It is found that the migration ability is related to the atomic structure of interfaces, and three kinds of interfaces can migrate except the interface （001）//（002） which has the characteristic of L12 （Ni3Al） structure. V atoms jump to the nearest neighbor site and substitute for Ni, and vice versa. Because of the site selectivity behaviors of jumping atoms, the number of jumping atoms during the migration is the least and the jumping distance of atoms is the shortest among all possible modes, and the atomic structures of interfaces are unchanged before and after the migration. The preferences and degree of segregation or depletion of alloy elements are also related to the atomic structure of interface.展开更多
An Fe-0.2C-1.5Si-1.67Mn steel was subjected to quenching and partitioning （Q＆P） process, and the interface migration between martensite and austenite at an elevated partitioning temperature was observed. The interf...An Fe-0.2C-1.5Si-1.67Mn steel was subjected to quenching and partitioning （Q＆P） process, and the interface migration between martensite and austenite at an elevated partitioning temperature was observed. The interface migration is excluded in constrained paraequilibrium （CPE） model. Based on ＂endpoint＂ predicted by CPE model the thermodynamic condition of interface migration is analyzed, that is, the difference in the chemical potential of iron in both ferrite （martenisite） and austenite produces the driving force of the iron atoms to migrate from one phase to the other phase. In addition, the interface migration can change the austenite fraction; as a result, the austenite fraction at partitioning temperature may be higher than that at quenching temperature through the interface migration, but this phenomenon cannot be explained by CPE model.展开更多
Friction stir lap joints of LY12 aluminum alloy plates with a thickness of 3 mm were fabricated using several tools with different pin profiles. The effects of tool pin profile on the interface migration of friction s...Friction stir lap joints of LY12 aluminum alloy plates with a thickness of 3 mm were fabricated using several tools with different pin profiles. The effects of tool pin profile on the interface migration of friction stir lap joints were investigated with the comparison of weld morphologies. The results show that the screw thread of the pin plays an important role in the migration of weld interface in the thickness direction. The interface between the sheets will move upwards to the top of the plate when the pin with left hand thread was used. Conversely, the interface will move downwards to the tip of the pin when the pin with right hand thread was used： As for a stir pin with smooth surface was used, the upward or downward migration of the weld interface was largely reduced, but the extension of weld interface to the weld center line from the retreating side becomes more serious. By analyzing the force on the pin according to the sucking-extruding theory for the weld formation, the obtained results have been well explained.展开更多
Based on the microscopic phase-field model, the structure and migration characteristic of ordered domain interfaces formed between DO22 and L12 phase are investigated, and the atomistic mechanism of phase transformati...Based on the microscopic phase-field model, the structure and migration characteristic of ordered domain interfaces formed between DO22 and L12 phase are investigated, and the atomistic mechanism of phase transformation from L12 （Ni3Al） to DO22 （Ni3V） in Ni75AlxV25-x alloys are explored, using the simulated microstructure evolution pictures and the occupation probability evolution of alloy elements at the interface. The results show that five kinds of heterointerfaces are formed between DO22 and L12 phase and four of them can migrate during the phase transformation from L12 to DO22 except the interface （002）D//（001）L. The structure of interface （100）D//（200）L and interface （100）D//（200）L·^1/2[001] remain the same before and after migration, while the interface （002）D//（002）L is formed after the migration of interface （002）D//（002）L·^1/2[100] and vice versa. These two kinds of interface appear alternatively. The jump and substitute of atoms selects the optimization way to induce the migration of interface during the phase transformation, and the number of atoms needing to jump during the migration is the least among all of the possible atom jump modes.展开更多
The sluggish Li^(+)migration kinetics and unstable electrode/electrolyte interface severely hinder the commercial application of high-performance lithium metal batteries(LMBs).Herein,an artificial protective layer is ...The sluggish Li^(+)migration kinetics and unstable electrode/electrolyte interface severely hinder the commercial application of high-performance lithium metal batteries(LMBs).Herein,an artificial protective layer is constructed using zwitterionic covalent organic framework(Z-COF)simultaneously containing sulfonate and ethidium groups,aiming to facilitate rapid,uniform Li^(+)transport and stabilize anode interface.The sulfonate groups with high lithiophilicity provide abundant hopping sites for fast Li^(+)diffusion.The ethidium cations immobilize TFSI-and solvent molecules by ion-dipole interactions,which accelerate the dissociation of LiTFSI and Li^(+)desolvation.Moreover,the monodispersed zwitterionic units coupling with ordered micropore structures in Z-COF create exclusive Li^(+)migration channels,modulate homogeneous space charge distribution,kinetically facilitating uniform Li^(+)deposition.Experiments and theoretical calculations indicate that C-F and S-N bonds of TFSI-exhibit enhanced cleavage susceptibility driven by electrostatic attraction,realizing a LiF/Li_(3)N-rich electrolyte/electrode interface.The designed Z-COF protection layer enables Li|Li symmetrical cells stable cycling over 6300 h at 2 mA cm^(-2)/2 mAh cm^(-2).The Z-COF@Li|LiFePO_(4)(LFP)full cells deliver high-capacity retention of 85.2%after 1000 cycles at 8 C.The assembled Z-COF@Li|LFP pouch cells demonstrate a lifespan of more than 240 cycles.This work provides fresh insights into the practical application of zwitterionic COF in next-generation LMBs.展开更多
Faceted interphase boundaries(IPBs)are commonly observed in lath-shaped precipitates in alloys consisting of simple face-centred cubic(fcc),body centred-cubic(bcc)or hexagonal closed packed(hcp)phases,which normally c...Faceted interphase boundaries(IPBs)are commonly observed in lath-shaped precipitates in alloys consisting of simple face-centred cubic(fcc),body centred-cubic(bcc)or hexagonal closed packed(hcp)phases,which normally contain one or two sets of parallel dislocations.The influence of these dislocations on interface migration and possible accompanying long-range strain field remain unclear.To elucidate this,we carried out atomistic simulations to investigate the dislocation-mediated migration processes of IPBs in a pure-iron system.Our results show that the migration of these IPBs is accompanied with the slip of interfacial dislocations,even in high-index slip planes,with two migration modes were observed:the first mode is the uniform migration mode that occurs only when all of the dislocations slip in a common slip plane.A shear-coupled interface migration was observed for this mode.The other interfaces propagate in the stick-slip migration mode that occurs when the dislocations glide on different slip planes,involving dislocation reaction or tangling.A quantitative relationship was established to link the atomic displacements with the dislocation structure,slip plane,and interface normal.The macroscopic shear deformation due to the effect of overall atomic displacement shows a good agreement with the results obtained based on the phenomenological theory of martensite crystallography.Our findings have general implications for the understanding of phase transformations and the surface relief effect at the atomic scale.展开更多
Seasonal frozen soil accounts for about 53.50%of the land area in China.Frozen soil is a complex multiphase system where ice,water,soil,and air coexist.The distribution and migration of salts in frozen soil during soi...Seasonal frozen soil accounts for about 53.50%of the land area in China.Frozen soil is a complex multiphase system where ice,water,soil,and air coexist.The distribution and migration of salts in frozen soil during soil freezing are notably different from those in unfrozen soil areas.However,little knowledge is available about the process and mechanisms of salt migration in frozen soil.This study explores the mechanisms of salt migration at the ice-liquid interface during the freezing of pore fluids through batch experiments.The results are as follows.The solute concentrations of liquid and solid phases at the ice-liquid interface(C*_(L),C*_(S))gradually increased at the initial stage of freezing and remained approximately constant at the middle stage.As the ice-liquid interface advanced toward the system boundary,the diffusion of the liquid phase was blocked but the ice phase continued rejecting salts.As a result,C*_(L)and C*_(S)rapidly increased at the final stage of freezing.The distribution characteristics of solutes in ice and the liquid phases before C*_(L)and C*_(S)became steady were mainly affected by the freezing temperature,initial concentrations,and particle-size distribution of media(quartz sand and kaolin).In detail,the lower the freezing temperature and the better the particle-size distribution of media,the higher the solute proportion in the ice phase at the initial stage of freezing.Meanwhile,the increase in concentration first promoted but then inhibited the increase of solutes in the ice phase.These results have insights and scientific significance for the tackling of climate change,the environmental protection of groundwater and soil,and infrastructure protection such as roads,among other things.展开更多
The poor reversibility of Zn anodes induced by dendrite growth,surface passivation,and corrosion,severely hinders the practical applicability of Zn metal batteries.To address these issues,a plasmaassisted aerogel(PAG)...The poor reversibility of Zn anodes induced by dendrite growth,surface passivation,and corrosion,severely hinders the practical applicability of Zn metal batteries.To address these issues,a plasmaassisted aerogel(PAG)interface engineering was proposed as efficient ion transport modulator that can simultaneously regulate uniform Zn^(2+)flux and desolvation behavior during battery operation.The PAG with ordered mesopores acted as an ion sieve to homogenize Zn deposition and accelerate Zn^(2+)flux,which is favorable for corrosion resistance and dendrite suppression.Importantly,the plasma-assisted aerogel with abundant hydrophilic groups can facilitate the desolvation kinetics of Zn^(2+)due to the multiple hydrogen-bonding interaction with the activated water molecules,thus accelerating the Zn^(2+)migration kinetics.Consequently,the Zn/Zn cell assembled with PAG-modified separator demonstrates stable plating and stripping behavior(over 1400 h at 1 mA cm^(-2))and high Coulombic efficiency(99.8%at1 mA cm^(-2)after 1100 cycles),and the Zn‖MnO_(2)full cell shows excellent long-term cycling stability and maintains a high capacity of 154.9 mA h g^(-1)after 1000 cycles at 1 A g^(-1).This study provides a feasible approach for the large-scale fabrication of aerogel functionalized separators to realize ultra-stable Zn metal batteries.展开更多
Ordered domain interfaces formed between DO22 (Ni3V) phases along [100] direction during the precipitation process of Ni75AlxV25-x alloys were simulated by using the microscopic phase-field model. The atomic structure...Ordered domain interfaces formed between DO22 (Ni3V) phases along [100] direction during the precipitation process of Ni75AlxV25-x alloys were simulated by using the microscopic phase-field model. The atomic structure, migration process, and compositions of interfaces were investigated. It is found that there are four kinds of stable ordered domain interfaces formed between DO22 phases along [100] direction and all of them can migrate. During the migration of interfaces, the jump of atoms shows site selectivity behaviors and each stable interface forms a distinctive transition interface. The atom jump selects the optimist way to induce the migration of interface, and the atomic structures of interfaces retain the same before and after the migration. The alloy elements have different preferences of segregation or depletion at different interfaces. At all the four kinds of interfaces, Ni and Al segregate but V depletes. The degrees of segregation and depletion are also different at different interfaces.展开更多
Wide-bandgap(>1.7 eV)perovskites suffer from severe light-induced phase segregation due to high bromine content,causing irreversible damage to devices stability.However,the strategies of suppressing photoinduced ph...Wide-bandgap(>1.7 eV)perovskites suffer from severe light-induced phase segregation due to high bromine content,causing irreversible damage to devices stability.However,the strategies of suppressing photoinduced phase segregation and related mechanisms have not been fully disclosed.Here,we report a new passivation agent 4-aminotetrahydrothiopyran hydrochloride(4-ATpHCl)with multifunctional groups for the interface treatment of a 1.77-eV wide-bandgap perovskite film.4-ATpH^(+)impeded halogen ion migration by anchoring on the perovskite surface,leading to the inhibition of phase segregation and thus the passivation of defects,which is ascribed to the interaction of 4-ATpH^(+)with perovskite and the formation of low-dimensional perovskites.Finally,the champion device achieved an efficiency of 19.32%with an open-circuit voltage(V_(OC))of 1.314 V and a fill factor of 83.32%.Moreover,4-ATpHCl modified device exhibited significant improved stability as compared with control one.The target device maintained 80%of its initial efficiency after 519 h of maximum power output(MPP)tracking under 1 sun illumination,however,the control device showed a rapid decrease in efficiency after 267 h.Finally,an efficiency of 27.38%of the champion 4-terminal all-perovskite tandem solar cell was achieved by mechanically stacking this wide-bandgap top subcell with a 1.25-eV low-bandgap perovskite bottom subcell.展开更多
Layered lithium-rich manganese-based oxide(LRMO)has the limitation of inevitable evolution of lattice oxygen release and layered structure transformation.Herein,a multilayer reconstruction strategy is applied to LRMO ...Layered lithium-rich manganese-based oxide(LRMO)has the limitation of inevitable evolution of lattice oxygen release and layered structure transformation.Herein,a multilayer reconstruction strategy is applied to LRMO via facile pyrolysis of potassium Prussian blue.The multilayer interface is visually observed using an atomic-resolution scanning transmission electron microscope and a high-resolution transmission electron microscope.Combined with the electrochemical characterization,the redox of lattice oxygen is suppressed during the initial charging.In situ X-ray diffraction and the high-resolution transmission electron microscope demonstrate that the suppressed evolution of lattice oxygen eliminates the variation in the unit cell parameters during initial(de)lithiation,which further prevents lattice distortion during long cycling.As a result,the initial Coulombic efficiency of the modified LRMO is up to 87.31%,and the rate capacity and long-term cycle stability also improved considerably.In this work,a facile surface reconstruction strategy is used to suppress vigorous anionic redox,which is expected to stimulate material design in high-performance lithium ion batteries.展开更多
Formamidinium(FA)-based perovskite solar cells(PSCs)have emerged as one of the most promising candidates for next-generation photovoltaics due to their exceptional power conversion efficiency(PCE).However,their commer...Formamidinium(FA)-based perovskite solar cells(PSCs)have emerged as one of the most promising candidates for next-generation photovoltaics due to their exceptional power conversion efficiency(PCE).However,their commercial deployment is hindered by poor stability,particularly under strict environmental stresses like high temperature,with interface degradation and ion migration being key challenges.In this work,we introduce metal–organic framework(MOF)materials composed of assembled Zr clusters and functional amino/sulfhydryl groups at the SnO_(2)/perovskite interface within the n–i–p structure to address these issues.The incorporation of MOFs—specifically their robust framework with confined spatial structure and functional groups—plays a pivotal role in hindering oxygen migration from SnO_(2)to perovskite,leading to enhanced thermal stability of both perovskite films and PSCs.Furthermore,the anchoring of MOF on SnO_(2)and perovskite is essential for passivating interface defects,promoting perovskite crystallization,and reducing carrier recombination,all of which contribute to enhanced charge transport.As a result,the MOF-modified devices achieve a champion PCE of 25.22%,with the MOF-modified devices retaining 100%of their initial PCE after 2000 h of thermal aging at 85°C in N_(2).This study highlights the structural integrity and functionality of MOFs for achieving high-performance and long-term stable PSCs.展开更多
Consider the inverse problem of time-harmonic acoustic scattering by an unbounded locally rough interface with bounded obstacles embedded in the lower half-space.An extended reverse time migration(RTM)is proposed to s...Consider the inverse problem of time-harmonic acoustic scattering by an unbounded locally rough interface with bounded obstacles embedded in the lower half-space.An extended reverse time migration(RTM)is proposed to simultaneously reconstruct the locally rough interface and embedded obstacles.By constructing a modified Helmholtz-Kirchhoff identity associated with a planar interface and a mixed reciprocity relation,we propose two new imaging functionals with using both the near-field and far-field measurements.It is shown that the imaging functionals always peak on the local perturbation of the interface and the embedded obstacle.Thus,the two imaging functional can be used to reconstruct the location and shape of the rough surface and the embedded obstacle.Numerical examples are presented to demonstrate the effectiveness of the method.展开更多
Halide perovskites have emerged as promising materials for X-ray detection with exceptional properties and reasonable costs.Among them,heterostructures between 3D perovskites and low-dimensional perovskites attract in...Halide perovskites have emerged as promising materials for X-ray detection with exceptional properties and reasonable costs.Among them,heterostructures between 3D perovskites and low-dimensional perovskites attract intensive studies of their advantages due to low-level ion migration and decent stability.However,there is still a lack of methods to precisely construct heterostructures and a fundamental understanding of their structure-dependent optoelectronic properties.Herein,a gas-phase method was developed to grow 2D perovskites directly on 3D perovskites with nanoscale accuracy.In addition,the larger steric hindrance of organic layers of 2D perovskites was proved to enable slower ion migration,which resulted in reduced trap states and better stability.Based on MAPbBr_(3)single crystals with the(PA)_(2)PbBr_(4)capping layer,the X-ray detector achieved a sensitivity of 22,245μC Gy_(air)^(−1)cm^(−2),a response speed of 240μs,and a dark current drift of 1.17.10^(–4)nA cm^(−1)s^(−1)V^(−1),which were among the highest reported for state-of-the-art perovskite-based X-ray detectors.This study presents a precise synthesis method to construct perovskite-based heterostructures.It also brings an in-depth understanding of the relationship between lattice structures and properties,which are beneficial for advancing high-performance and cost-effective X-ray detectors.展开更多
The efficient utilization of visible light catalysts for organic reactions necessitates not only the effective separation of photogenerated electrons and holes to participate in the reaction,but also their ability to ...The efficient utilization of visible light catalysts for organic reactions necessitates not only the effective separation of photogenerated electrons and holes to participate in the reaction,but also their ability to form key intermediates with reactant molecules.The present study successfully synthesized a crusiform-like mesoporous structure of nitrogen-doped carbon-coated Cu_(2)O/Cu(Cu_(2)O/Cu/N-C)with a Cu_(2)O/dual electron acceptor interface using etched HKUST-1 as the precursor.A series of theoretical and experimental studies have demonstrated that the Cu_(2)O/Cu/N-C interface in the photocatalytic homo-coupling of terminal alkynes not only effectively enhances the separation of photogenerated electron−hole pairs,but also facilitates the formation of the key intermediate[Cu_(2)O/Cu/N-C]-phenylacetylide and promotes the rearrangement of its internal charges.As a result,the homo-coupling reaction can be effectively facilitated.The primary reason for the functional role of Cu_(2)O/Cu/N-C interface lies in the downward bending of energy band from Cu_(2)O to N-doped C layers,induced by the different work functions of Cu_(2)O,Cu and N-doped C layers.Consequently,Cu_(2)O/Cu/N-C photocatalysts demonstrate exceptional photocatalytic activity in the homo-coupling reaction of terminal alkynes under blue-light irradiation and air atmosphere.The present study presents a novel research methodology for the development of highly efficient visible light catalysts to facilitate organic reactions in future applications.展开更多
基金The Royal Society,UK,Grant/Award Number:IEC\NSFC\211366Fundamental Research Funds for the Central Universities(China University of Mining and Technology),Grant/Award Number:2023ZDPY11National Natural Science Foundation of China,Grant/Award Numbers:51809263,52174133。
文摘The corrosion of waste canisters in the deep geological disposal facilities(GDFs)for high-level radioactive waste(HLRW)can generate gas,which escapes from the engineered barrier system through the interfaces between the bentonite buffer blocks and the host rock and those between the bentonite blocks.In this study,a series of water infiltration and gas breakthrough experiments were conducted on granite and on granite-bentonite specimens with smooth and grooved interfaces.On this basis,this study presents new insights and a quantitative assessment of the impact of the interface between clay and host rock on gas transport.As the results show,the water permeability values from water infiltration tests on granite and granite-bentonite samples(10−19-10−20m^(2))are found to be slightly higher than that of bentonite.The gas permeability of the mock-up samples with smooth interfaces is one order of magnitude larger than that of the mock-up with grooved interfaces.The gas results of breakthrough pressures for the granite and the granite-bentonite mock-up samples are significantly lower than that of bentonite.The results highlight the potential existence of preferential gas migration channels between the rock and bentonite buffer that require further considerations in safety assessment.
基金Projects (50941020, 10902086, 50875217, 20903075) supported by the National Natural Science Foundation of ChinaProjects (SJ08-ZT05, SJ08-B14) supported by the Natural Science Foundation of Shaanxi Province, ChinaProject (CX200905) supported by the Doctorate Foundation of Northwestern Polytechnical University, China
文摘Based on the microscopic phase-field model, ordered domain interfaces formed between D022 （Ni3V） phases along [001] direction in Ni75AlxV25-x alloys were simulated, and the effects of atomic structure on the migration characteristic and solute segregation of interfaces were studied. It is found that the migration ability is related to the atomic structure of interfaces, and three kinds of interfaces can migrate except the interface （001）//（002） which has the characteristic of L12 （Ni3Al） structure. V atoms jump to the nearest neighbor site and substitute for Ni, and vice versa. Because of the site selectivity behaviors of jumping atoms, the number of jumping atoms during the migration is the least and the jumping distance of atoms is the shortest among all possible modes, and the atomic structures of interfaces are unchanged before and after the migration. The preferences and degree of segregation or depletion of alloy elements are also related to the atomic structure of interface.
文摘An Fe-0.2C-1.5Si-1.67Mn steel was subjected to quenching and partitioning （Q＆P） process, and the interface migration between martensite and austenite at an elevated partitioning temperature was observed. The interface migration is excluded in constrained paraequilibrium （CPE） model. Based on ＂endpoint＂ predicted by CPE model the thermodynamic condition of interface migration is analyzed, that is, the difference in the chemical potential of iron in both ferrite （martenisite） and austenite produces the driving force of the iron atoms to migrate from one phase to the other phase. In addition, the interface migration can change the austenite fraction; as a result, the austenite fraction at partitioning temperature may be higher than that at quenching temperature through the interface migration, but this phenomenon cannot be explained by CPE model.
基金This work was sponsored by the National Natural Science Foundation of China （50875119 ） , the Aerospace Science Foundation of China （20081156009） and the Natural Science Foundation of Jiangxi Province, China （0450090）.
文摘Friction stir lap joints of LY12 aluminum alloy plates with a thickness of 3 mm were fabricated using several tools with different pin profiles. The effects of tool pin profile on the interface migration of friction stir lap joints were investigated with the comparison of weld morphologies. The results show that the screw thread of the pin plays an important role in the migration of weld interface in the thickness direction. The interface between the sheets will move upwards to the top of the plate when the pin with left hand thread was used. Conversely, the interface will move downwards to the tip of the pin when the pin with right hand thread was used： As for a stir pin with smooth surface was used, the upward or downward migration of the weld interface was largely reduced, but the extension of weld interface to the weld center line from the retreating side becomes more serious. By analyzing the force on the pin according to the sucking-extruding theory for the weld formation, the obtained results have been well explained.
基金Funded by the National Natural Science Foundation of China (Nos.50941020, 10902086, 50875217, and 20903075)Natural Science Foundation of Shaanxi Province (Nos. SJ08-ZT05 and SJ08-B14)Doctorate Foundation of Northwest Polytechnical University (No. CX200905)
文摘Based on the microscopic phase-field model, the structure and migration characteristic of ordered domain interfaces formed between DO22 and L12 phase are investigated, and the atomistic mechanism of phase transformation from L12 （Ni3Al） to DO22 （Ni3V） in Ni75AlxV25-x alloys are explored, using the simulated microstructure evolution pictures and the occupation probability evolution of alloy elements at the interface. The results show that five kinds of heterointerfaces are formed between DO22 and L12 phase and four of them can migrate during the phase transformation from L12 to DO22 except the interface （002）D//（001）L. The structure of interface （100）D//（200）L and interface （100）D//（200）L·^1/2[001] remain the same before and after migration, while the interface （002）D//（002）L is formed after the migration of interface （002）D//（002）L·^1/2[100] and vice versa. These two kinds of interface appear alternatively. The jump and substitute of atoms selects the optimization way to induce the migration of interface during the phase transformation, and the number of atoms needing to jump during the migration is the least among all of the possible atom jump modes.
基金supported by the National Natural Science Foundation of China(52472093,52176185)the Department of Science and Technology of Hubei Province of China(2022CFA069,2022BAA086).
文摘The sluggish Li^(+)migration kinetics and unstable electrode/electrolyte interface severely hinder the commercial application of high-performance lithium metal batteries(LMBs).Herein,an artificial protective layer is constructed using zwitterionic covalent organic framework(Z-COF)simultaneously containing sulfonate and ethidium groups,aiming to facilitate rapid,uniform Li^(+)transport and stabilize anode interface.The sulfonate groups with high lithiophilicity provide abundant hopping sites for fast Li^(+)diffusion.The ethidium cations immobilize TFSI-and solvent molecules by ion-dipole interactions,which accelerate the dissociation of LiTFSI and Li^(+)desolvation.Moreover,the monodispersed zwitterionic units coupling with ordered micropore structures in Z-COF create exclusive Li^(+)migration channels,modulate homogeneous space charge distribution,kinetically facilitating uniform Li^(+)deposition.Experiments and theoretical calculations indicate that C-F and S-N bonds of TFSI-exhibit enhanced cleavage susceptibility driven by electrostatic attraction,realizing a LiF/Li_(3)N-rich electrolyte/electrode interface.The designed Z-COF protection layer enables Li|Li symmetrical cells stable cycling over 6300 h at 2 mA cm^(-2)/2 mAh cm^(-2).The Z-COF@Li|LiFePO_(4)(LFP)full cells deliver high-capacity retention of 85.2%after 1000 cycles at 8 C.The assembled Z-COF@Li|LFP pouch cells demonstrate a lifespan of more than 240 cycles.This work provides fresh insights into the practical application of zwitterionic COF in next-generation LMBs.
基金financially supported by the National Natural Science Foundation of China (Nos.51471097 and 51671111)the National Key Research and Development Program of China (No. 2016YFB0701304)
文摘Faceted interphase boundaries(IPBs)are commonly observed in lath-shaped precipitates in alloys consisting of simple face-centred cubic(fcc),body centred-cubic(bcc)or hexagonal closed packed(hcp)phases,which normally contain one or two sets of parallel dislocations.The influence of these dislocations on interface migration and possible accompanying long-range strain field remain unclear.To elucidate this,we carried out atomistic simulations to investigate the dislocation-mediated migration processes of IPBs in a pure-iron system.Our results show that the migration of these IPBs is accompanied with the slip of interfacial dislocations,even in high-index slip planes,with two migration modes were observed:the first mode is the uniform migration mode that occurs only when all of the dislocations slip in a common slip plane.A shear-coupled interface migration was observed for this mode.The other interfaces propagate in the stick-slip migration mode that occurs when the dislocations glide on different slip planes,involving dislocation reaction or tangling.A quantitative relationship was established to link the atomic displacements with the dislocation structure,slip plane,and interface normal.The macroscopic shear deformation due to the effect of overall atomic displacement shows a good agreement with the results obtained based on the phenomenological theory of martensite crystallography.Our findings have general implications for the understanding of phase transformations and the surface relief effect at the atomic scale.
基金This research was financially supported by the National Natural Science Foundation of China(41572225)project of China Geological Survey(DD20189662,DD20211256).
文摘Seasonal frozen soil accounts for about 53.50%of the land area in China.Frozen soil is a complex multiphase system where ice,water,soil,and air coexist.The distribution and migration of salts in frozen soil during soil freezing are notably different from those in unfrozen soil areas.However,little knowledge is available about the process and mechanisms of salt migration in frozen soil.This study explores the mechanisms of salt migration at the ice-liquid interface during the freezing of pore fluids through batch experiments.The results are as follows.The solute concentrations of liquid and solid phases at the ice-liquid interface(C*_(L),C*_(S))gradually increased at the initial stage of freezing and remained approximately constant at the middle stage.As the ice-liquid interface advanced toward the system boundary,the diffusion of the liquid phase was blocked but the ice phase continued rejecting salts.As a result,C*_(L)and C*_(S)rapidly increased at the final stage of freezing.The distribution characteristics of solutes in ice and the liquid phases before C*_(L)and C*_(S)became steady were mainly affected by the freezing temperature,initial concentrations,and particle-size distribution of media(quartz sand and kaolin).In detail,the lower the freezing temperature and the better the particle-size distribution of media,the higher the solute proportion in the ice phase at the initial stage of freezing.Meanwhile,the increase in concentration first promoted but then inhibited the increase of solutes in the ice phase.These results have insights and scientific significance for the tackling of climate change,the environmental protection of groundwater and soil,and infrastructure protection such as roads,among other things.
基金financially supported by the National Natural Science Foundation of China(NSFC)(52203261)Natural Science Foundation of Jiangsu Province(BK20210474)the project of research on the industrial application of"controllable synthesis of nanocarbon-based polymer composites and their application in new energy”(N0.CJGJZD20210408092400002).
文摘The poor reversibility of Zn anodes induced by dendrite growth,surface passivation,and corrosion,severely hinders the practical applicability of Zn metal batteries.To address these issues,a plasmaassisted aerogel(PAG)interface engineering was proposed as efficient ion transport modulator that can simultaneously regulate uniform Zn^(2+)flux and desolvation behavior during battery operation.The PAG with ordered mesopores acted as an ion sieve to homogenize Zn deposition and accelerate Zn^(2+)flux,which is favorable for corrosion resistance and dendrite suppression.Importantly,the plasma-assisted aerogel with abundant hydrophilic groups can facilitate the desolvation kinetics of Zn^(2+)due to the multiple hydrogen-bonding interaction with the activated water molecules,thus accelerating the Zn^(2+)migration kinetics.Consequently,the Zn/Zn cell assembled with PAG-modified separator demonstrates stable plating and stripping behavior(over 1400 h at 1 mA cm^(-2))and high Coulombic efficiency(99.8%at1 mA cm^(-2)after 1100 cycles),and the Zn‖MnO_(2)full cell shows excellent long-term cycling stability and maintains a high capacity of 154.9 mA h g^(-1)after 1000 cycles at 1 A g^(-1).This study provides a feasible approach for the large-scale fabrication of aerogel functionalized separators to realize ultra-stable Zn metal batteries.
基金Projects(50671084, 50875217) supported by the National Natural Science Foundation of ChinaProjects(2003E106, SJ08-ZT05) supported by the Natural Science Foundation of Shaanxi Province, ChinaProject(20070420218) supported by China Postdoctoral Science Foundation
文摘Ordered domain interfaces formed between DO22 (Ni3V) phases along [100] direction during the precipitation process of Ni75AlxV25-x alloys were simulated by using the microscopic phase-field model. The atomic structure, migration process, and compositions of interfaces were investigated. It is found that there are four kinds of stable ordered domain interfaces formed between DO22 phases along [100] direction and all of them can migrate. During the migration of interfaces, the jump of atoms shows site selectivity behaviors and each stable interface forms a distinctive transition interface. The atom jump selects the optimist way to induce the migration of interface, and the atomic structures of interfaces retain the same before and after the migration. The alloy elements have different preferences of segregation or depletion at different interfaces. At all the four kinds of interfaces, Ni and Al segregate but V depletes. The degrees of segregation and depletion are also different at different interfaces.
基金financially supported by the National Key R&D Program of China (2022YFB4200304)the National Natural Science Foundation of China (52303347)+3 种基金the Fundamental Research Funds for the Central Universities (YJ2021157)the Engineering Featured Team Fund of Sichuan University (2020SCUNG102)open foundation of Guangxi Key Laboratory of Processing for Non-Ferrous Metals and Featured Materials, Guangxi University (2022GXYSOF05)the support from the National Natural Science Foundation of China (E30853YM19)
文摘Wide-bandgap(>1.7 eV)perovskites suffer from severe light-induced phase segregation due to high bromine content,causing irreversible damage to devices stability.However,the strategies of suppressing photoinduced phase segregation and related mechanisms have not been fully disclosed.Here,we report a new passivation agent 4-aminotetrahydrothiopyran hydrochloride(4-ATpHCl)with multifunctional groups for the interface treatment of a 1.77-eV wide-bandgap perovskite film.4-ATpH^(+)impeded halogen ion migration by anchoring on the perovskite surface,leading to the inhibition of phase segregation and thus the passivation of defects,which is ascribed to the interaction of 4-ATpH^(+)with perovskite and the formation of low-dimensional perovskites.Finally,the champion device achieved an efficiency of 19.32%with an open-circuit voltage(V_(OC))of 1.314 V and a fill factor of 83.32%.Moreover,4-ATpHCl modified device exhibited significant improved stability as compared with control one.The target device maintained 80%of its initial efficiency after 519 h of maximum power output(MPP)tracking under 1 sun illumination,however,the control device showed a rapid decrease in efficiency after 267 h.Finally,an efficiency of 27.38%of the champion 4-terminal all-perovskite tandem solar cell was achieved by mechanically stacking this wide-bandgap top subcell with a 1.25-eV low-bandgap perovskite bottom subcell.
基金This work was financially supported by the High‐level Talents'Discipline Construction Fund of Shandong University(31370089963078)the Shandong Provincial Science and Technology Major Project(2018JM RH0211 and 2017CXGC1010)+3 种基金the Research Funds of Shandong University(10000089395121)the Natural Science Foundation of Shandong Province(ZR2019MEM052 and ZR2017MEM002)The National Natural Science Foundation of China(grant no.52002287)the Start‐up Funding of Wenzhou University are acknowledged.
文摘Layered lithium-rich manganese-based oxide(LRMO)has the limitation of inevitable evolution of lattice oxygen release and layered structure transformation.Herein,a multilayer reconstruction strategy is applied to LRMO via facile pyrolysis of potassium Prussian blue.The multilayer interface is visually observed using an atomic-resolution scanning transmission electron microscope and a high-resolution transmission electron microscope.Combined with the electrochemical characterization,the redox of lattice oxygen is suppressed during the initial charging.In situ X-ray diffraction and the high-resolution transmission electron microscope demonstrate that the suppressed evolution of lattice oxygen eliminates the variation in the unit cell parameters during initial(de)lithiation,which further prevents lattice distortion during long cycling.As a result,the initial Coulombic efficiency of the modified LRMO is up to 87.31%,and the rate capacity and long-term cycle stability also improved considerably.In this work,a facile surface reconstruction strategy is used to suppress vigorous anionic redox,which is expected to stimulate material design in high-performance lithium ion batteries.
基金support from the National Natural Science Foundation of China(Nos.62105293,91963212,52303257,52321006,22479131)the National Key Research and Development Program of China(No.2018YFA0208501)+6 种基金the Beijing National Laboratory for Molecular Sciences(No.BNLMSCXXM-202005)Graduate Education Reform Project of Henan Province(No.2023SJGLX136Y)the Outstanding Young Talent Research Fund of Zhengzhou University,Opening Project of State Key Laboratory of Advanced Technology for Float Glass(No.2022KF04)Program for Science&Technology Innovation Talents in Universities of Henan Province(No.25HASTIT005)Training Plan for Young Backbone Teachers of Zhengzhou University(No.2023ZDGGJS017)the Joint Research Project of Puyang Shengtong Juyuan New Materials Co.,Ltd.(No.20230128A)Outstanding Young Talents Innovation Team Support Plan of Zhengzhou University.
文摘Formamidinium(FA)-based perovskite solar cells(PSCs)have emerged as one of the most promising candidates for next-generation photovoltaics due to their exceptional power conversion efficiency(PCE).However,their commercial deployment is hindered by poor stability,particularly under strict environmental stresses like high temperature,with interface degradation and ion migration being key challenges.In this work,we introduce metal–organic framework(MOF)materials composed of assembled Zr clusters and functional amino/sulfhydryl groups at the SnO_(2)/perovskite interface within the n–i–p structure to address these issues.The incorporation of MOFs—specifically their robust framework with confined spatial structure and functional groups—plays a pivotal role in hindering oxygen migration from SnO_(2)to perovskite,leading to enhanced thermal stability of both perovskite films and PSCs.Furthermore,the anchoring of MOF on SnO_(2)and perovskite is essential for passivating interface defects,promoting perovskite crystallization,and reducing carrier recombination,all of which contribute to enhanced charge transport.As a result,the MOF-modified devices achieve a champion PCE of 25.22%,with the MOF-modified devices retaining 100%of their initial PCE after 2000 h of thermal aging at 85°C in N_(2).This study highlights the structural integrity and functionality of MOFs for achieving high-performance and long-term stable PSCs.
基金supported by the NNSF of China grants No.12171057,12122114Education Department of Hunan Province No.21B0299.
文摘Consider the inverse problem of time-harmonic acoustic scattering by an unbounded locally rough interface with bounded obstacles embedded in the lower half-space.An extended reverse time migration(RTM)is proposed to simultaneously reconstruct the locally rough interface and embedded obstacles.By constructing a modified Helmholtz-Kirchhoff identity associated with a planar interface and a mixed reciprocity relation,we propose two new imaging functionals with using both the near-field and far-field measurements.It is shown that the imaging functionals always peak on the local perturbation of the interface and the embedded obstacle.Thus,the two imaging functional can be used to reconstruct the location and shape of the rough surface and the embedded obstacle.Numerical examples are presented to demonstrate the effectiveness of the method.
基金support from National Key Research and Development Program of China(2024YFE0217100)the National Natural Science Foundation of China(21905006,22261160370,and 62105075)+7 种基金the Guangdong Provincial Science and Technology Plan(2021A0505110003)the Natural Science Foundation of Hunan Province,China(2023JJ50132)Guangxi Department of Science and Technology(2020GXNSFBA159049 and AD19110030)the Shenzhen Science and Technology Program(SGDX20230116093205009,JCYJ20220818100211025 and 2022378670)the Natural Science Foundation of Top Talent of SZTU(GDRC202343)financial support of Innovation and Technology Fund(#GHP/245/22SZ)The University Grant Council of the University of Hong Kong(grant No.2302101786)General Research Fund(grant Nos.17200823 and 17310624)from the Research Grants Council.
文摘Halide perovskites have emerged as promising materials for X-ray detection with exceptional properties and reasonable costs.Among them,heterostructures between 3D perovskites and low-dimensional perovskites attract intensive studies of their advantages due to low-level ion migration and decent stability.However,there is still a lack of methods to precisely construct heterostructures and a fundamental understanding of their structure-dependent optoelectronic properties.Herein,a gas-phase method was developed to grow 2D perovskites directly on 3D perovskites with nanoscale accuracy.In addition,the larger steric hindrance of organic layers of 2D perovskites was proved to enable slower ion migration,which resulted in reduced trap states and better stability.Based on MAPbBr_(3)single crystals with the(PA)_(2)PbBr_(4)capping layer,the X-ray detector achieved a sensitivity of 22,245μC Gy_(air)^(−1)cm^(−2),a response speed of 240μs,and a dark current drift of 1.17.10^(–4)nA cm^(−1)s^(−1)V^(−1),which were among the highest reported for state-of-the-art perovskite-based X-ray detectors.This study presents a precise synthesis method to construct perovskite-based heterostructures.It also brings an in-depth understanding of the relationship between lattice structures and properties,which are beneficial for advancing high-performance and cost-effective X-ray detectors.
基金supported by the Xuzhou Key Research and Development Program(Social Development)(No.KC23298)the National Natural Science Foundation of China(No.22271122)+1 种基金the Natural Science Foundation of Jiangsu Province(No.BK20211549)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX23_2903).
文摘The efficient utilization of visible light catalysts for organic reactions necessitates not only the effective separation of photogenerated electrons and holes to participate in the reaction,but also their ability to form key intermediates with reactant molecules.The present study successfully synthesized a crusiform-like mesoporous structure of nitrogen-doped carbon-coated Cu_(2)O/Cu(Cu_(2)O/Cu/N-C)with a Cu_(2)O/dual electron acceptor interface using etched HKUST-1 as the precursor.A series of theoretical and experimental studies have demonstrated that the Cu_(2)O/Cu/N-C interface in the photocatalytic homo-coupling of terminal alkynes not only effectively enhances the separation of photogenerated electron−hole pairs,but also facilitates the formation of the key intermediate[Cu_(2)O/Cu/N-C]-phenylacetylide and promotes the rearrangement of its internal charges.As a result,the homo-coupling reaction can be effectively facilitated.The primary reason for the functional role of Cu_(2)O/Cu/N-C interface lies in the downward bending of energy band from Cu_(2)O to N-doped C layers,induced by the different work functions of Cu_(2)O,Cu and N-doped C layers.Consequently,Cu_(2)O/Cu/N-C photocatalysts demonstrate exceptional photocatalytic activity in the homo-coupling reaction of terminal alkynes under blue-light irradiation and air atmosphere.The present study presents a novel research methodology for the development of highly efficient visible light catalysts to facilitate organic reactions in future applications.
