Precise control of the local environment and electronic state of the guest is an important method of controlling catalytic activity and reaction pathways.In this paper,guest Pd NPs were introduced into a series of hos...Precise control of the local environment and electronic state of the guest is an important method of controlling catalytic activity and reaction pathways.In this paper,guest Pd NPs were introduced into a series of host UiO-67 MOFs with different functional ligands and metal nodes,the microenvironment and local electronic structure of Pd is modulated by introducing bipyridine groups and changing metal nodes(Ce6O6 or Zr6O6).The bipyridine groups not only promoted the dispersion Pd NPs,but also facilitated electron transfer between Pd and UiO-67 MOFs through the formation of Pd-N bridges.Compared with Zr6 clusters,the tunability and orbital hybridisation of the 4f electronic structure in the Ce6 clusters modulate the electronic structure of Pd through the construction of the Ce-O-Pd interfaces.The optimal catalyst Pd/UiO-67(Ce)-bpy presented excellent low-temperature activity towards dicyclopentadiene hydrogenation with a conversion of>99%and a selectivity of>99%(50℃,10 bar).The results show that the synergy of Ce-O-Pd and Pd-N promotes the formation of active Pdδ+,which not only enhances the adsorption of H2 and electron-rich C=C bonds,but also contributes to the reduction of proton migration distance and improves proton utilization efficiency.These results provide valuable insights for investigating the regulatory role of the host MOFs,the nature of host-guest interactions,and their correlation with catalytic performance.展开更多
Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is chall...Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is challenging because of the inefficient mass transfer of the catalyst and the presence of the hydrogen evolution reaction(HER).In this study,dendritic Cu/Cu_(2)O with abundant Cu^(0)/Cu^(+)interfaces and numerous dendritic curves was synthesized in a CO_(2)atmosphere,resulting in the high selectivity and current density of the C_(2)products.Dendritic Cu/Cu_(2)O achieved a C_(2)Faradaic efficiency of 69.8%and a C_(2)partial current density of 129.5 mA cm^(-2)in an H-cell.Finite element simulations showed that a dendritic structure with a high curvature generates a strong electric field,leading to a localized CO_(2)concentration.Additionally,DRT analysis showed that a dendritic struc-ture with a high curvature actively adsorbed the surrounding high concentration of CO_(2),enhancing the mass transfer rate and achieving a high current density.During the experiment,the impact of the electronic structure on the performance of the catalyst was investigated by varying the atomic ratio of Cu^(0)/Cu^(+)on the catalyst surface,which resulted in improved ethylene selectivity.Under the optimal atomic ratio of Cu^(0)/Cu^(+),the charge transfer resistance was minimized,and the desorption rate of the intermediates was low,favoring C_(2)generation.Density functional theory calculations indicated that the Cu^(0)/Cu^(+)interfaces exhibited a lower Gibbs free energy for the rate-determining step,enhancing C_(2)H4 formation.The Cu/Cu_(2)O catalyst also exhibited a low Cu d-band center,which enhanced the adsorption stability of*CO on the surface and facilitated C_(2)formation.This observa-tion explained the higher yield of C_(2)products at the Cu^(0)/Cu^(+)interface than that of H_(2)under rapid mass transfer.The results of the net present value model showed that the H-cell holds promising industrial prospects,contingent upon it being a catalyst with both high selectivity and high current density.This approach of integrating the structure and composition provides new insights for ad-vancing the CO_(2)RR towards high-current C_(2)products.展开更多
Calcium carbonate was synthesized in a CaCl2/NaCO3 mixed solution by using ethylenediaminetetraacetic acid (EDTA) as an additive. The thermodynamics and kinetics analyses indicate that although the driving force of ...Calcium carbonate was synthesized in a CaCl2/NaCO3 mixed solution by using ethylenediaminetetraacetic acid (EDTA) as an additive. The thermodynamics and kinetics analyses indicate that although the driving force of amorphous calcium carbonate (ACC) precipitation is always less than that of calcite and vaterite precipitation, the nucleation rate of ACC is greater than that of calcite and vaterite at the initial stage of the precipitation reaction. With the increasing incubation time, vaterite and calcite particles nucleate heterogeneously by using the as-formed particles as active sites. Scanning electron microscopy images indicate that the transformation mechanism of ACC and vaterite to calcite is the dissolution-recrystallisation reaction. The presence of EDTA not only improves the stabilities of ACC and vaterite, but also leads to forming enlongated, connected rhombohedral calcite crystals after incubation 7 days in solutions. The ACC and vaterite are stabler in air than in solutions at room temperature, although the dissolution-recrystallisation reaction occurs on the surface.展开更多
The morphology and formation mechanism of the substructure of martensite in TC21 alloy was investigated by XRD and TEM. The results showed that the martensitic transformation from β to α" occurs upon quenching afte...The morphology and formation mechanism of the substructure of martensite in TC21 alloy was investigated by XRD and TEM. The results showed that the martensitic transformation from β to α" occurs upon quenching after solution treatment between 960-1000 ℃. The antiphase boundary (APB)-like structure was observed clearly in the α" martensite plates. The APB-like contrasts exist along the (001) and (020) planes of α" martensite. This APB-like structure of α" martensite was identified as a kind of stacking fault with an APB-like morphology induced by martensitic transformation and not by order/disorder transition. During martensitic transformation, martensitic domains nucleate and grow, eventually encounter each other, resulting in the formation of the APBdike contrast.展开更多
The influences of sodium silicate on manganese electrodeposition in sulfate solution were investigated. Manganese electrodeposition experiments indicate that a certain amount of sodium silicate can improve cathode cur...The influences of sodium silicate on manganese electrodeposition in sulfate solution were investigated. Manganese electrodeposition experiments indicate that a certain amount of sodium silicate can improve cathode current efficiency and initial pH 7.0?8.0 is the optimized pH for high cathode current efficiency. The analyses of scanning electron microscopy (SEM) and X-ray diffraction (XRD) indicate the compact morphology and nanocrystalline structure of electrodeposits. X-ray photoelectron spectrometry (XPS) analysis shows that the elements of Mn, Si and O exist in the deposit. The solution chemistry calculations of sulfate electrolyte and sodium silicate solution indicate that species of Mn2+, MnSO4, Mn(SO4)2?2 , Mn2+, MnSiO3, Mn(NH3)2+, SiO32?and HSiO3? are the main active species during the process of manganese electrodeposition. The reaction trend between Mn2+ and Si-containing ions is confirmed by the thermodynamic analysis. In addition, polarization curve tests confirm that sodium silicate can increase the overpotential of hydrogen evolution reaction, and then indirectly improve the cathode current efficiency.展开更多
In CSEM exploration, the receivers are generally located about three to five times the skin depth from the transmitter. In this paper, we study the effect of a conductor between the transmitter and the survey area on ...In CSEM exploration, the receivers are generally located about three to five times the skin depth from the transmitter. In this paper, we study the effect of a conductor between the transmitter and the survey area on the target conductor response using forward modeling and inversion. The 2D forward finite element calculations show that the conductor mainly affects the response at middle and low frequencies. The lower the resistivity and the larger the conductor, the larger the effect and the effect increases with decreasing frequency. The inversion results indicate that the calculated position of the target body can move towards the source, leading to an incorrect interpretation without considering the conductor. In order to reduce the effect of a conductor between the source and the survey area, CSEM acquisition should be conducted in three dimensions using multiple sources and 3D inversion should be used during interpretation.展开更多
Reactive brazing of TiAl-based intermetallics and Ni-based alloy with Ti foil as interlayer was investigated. The interfacial microstructure and shear strength of the joints were studied. According to the experimental...Reactive brazing of TiAl-based intermetallics and Ni-based alloy with Ti foil as interlayer was investigated. The interfacial microstructure and shear strength of the joints were studied. According to the experimental observations, the molten interlayer reacts vigorously with base metals, forming several continuous reaction layers. The typical interfacial microstructure of the joint can be expressed as GH99/(Ni,Cr)ss(γ)/TiNi(β2)+TiNi2Al(τ4)+Ti2Ni(δ)/δ+Ti3Al(α2)+Al3NiTi2(τ3)/α2+τ3/TiAl. The maximum shear strength is 258 MPa for the specimen brazed at 1000°C for 10 min. Higher brazing temperature or longer brazing time causes coarsening of the phases in the brazing seam and formation of brittle intermetallic layer, which greatly depresses the shear strength of the joints.展开更多
Understanding the continental margin of the Northeastern South China Sea is critical to the study of deep structures, tectonic evolution, and dynamics of the region. One set of important data for this endeavor is the ...Understanding the continental margin of the Northeastern South China Sea is critical to the study of deep structures, tectonic evolution, and dynamics of the region. One set of important data for this endeavor is the total-field magnetic data. Given the challenges associated with the magnetic data at low latitudes and with remanent magnetism in this area, we combine the equivalent-source technique and magnetic amplitude inversion to recover 3D subsurface magnetic structures. The inversion results show that this area is characterized by a north-south block division and east-west zonation. Magnetic regions strike in EW, NE and NW direction and are consistent with major tectonic trends in the region. The highly magnetic zone recovered from inversion in the continental margin differs visibly from that of the magnetically quiet zones to the south. The magnetic anomaly zone strikes in NE direction, covering an area of about 500 km × 60 km, and extending downward to a depth of 25 km or more. In combination with other geophysical data, we suggest that this strongly magnetic zone was produced by deep underplating of magma associated with plate subduction in Mesozoic period. The magnetically quiet zone in the south is an EW trending unit underlain by broad and gentle magnetic layers of lower crust. Its magnetic structure bears a clear resemblance to oceanic crust, assumed to be related to the presence of ancient oceanic crust there.展开更多
In this paper, a new method of time reversal for defect diagnosis of concealed structure has been proposed based on the detecting technique of structure acoustic wave and the theory of time reversal. The time reversal...In this paper, a new method of time reversal for defect diagnosis of concealed structure has been proposed based on the detecting technique of structure acoustic wave and the theory of time reversal. The time reversal recurrence formula for detecting the acoustic wave speed constitution of concealed structures with bilevel asynchronous test has been established. The wave speed constitution can be reconstructed in 2 D graticule form by means of this method. The result of model test shows the method is valid.展开更多
The fluidity of fresh cemented tailings backfill(CTB) slurry depends on its rheological properties. Hence, it is crucial to understand the rheology of fresh CTB slurry, which is related to the cement hydration progr...The fluidity of fresh cemented tailings backfill(CTB) slurry depends on its rheological properties. Hence, it is crucial to understand the rheology of fresh CTB slurry, which is related to the cement hydration progress and temperature evolution within CTB mixtures. For this reason, a numerical model was developed to predict the evolution of the rheological properties of fresh CTB slurry under the coupled effect of cement hydration and temperature. Experiments were conducted to investigate the rheological behaviours of the fresh CTB slurry. By comparing the simulated results with the experimental ones, the availability of this developed model was validated. Thereafter, the model was used to demonstrate the coupled effect of cement hydration and temperature on the evolution of fresh CTB slurry's rheological properties, under various conditions(initial CTB temperature, cement to tailings ratio, and water to cement ratio). The obtained results are helpful to better understanding the rheology of CTB slurry.展开更多
A reverse bias silicon p-n junction based on light emitting diode is designed in standard 0.6μm industrial CMOS technology.The mechanism of the light emitting of this device is discussed.The device is simulated by th...A reverse bias silicon p-n junction based on light emitting diode is designed in standard 0.6μm industrial CMOS technology.The mechanism of the light emitting of this device is discussed.The device is simulated by the commercial software.I-V characteristic under forward or reverse bias is simulated utilizing the commercial software.The results between simulation and experiment data are compared.The results show that it is a promising device and may find applications in light linking.展开更多
In this paper, we consider a reaction diffusion system with Hamitonian structure, we first prove the existence of an invariant region for system and the continuity of the semigroup, then establish the absorbing sets ...In this paper, we consider a reaction diffusion system with Hamitonian structure, we first prove the existence of an invariant region for system and the continuity of the semigroup, then establish the absorbing sets and global attractor.展开更多
文摘Precise control of the local environment and electronic state of the guest is an important method of controlling catalytic activity and reaction pathways.In this paper,guest Pd NPs were introduced into a series of host UiO-67 MOFs with different functional ligands and metal nodes,the microenvironment and local electronic structure of Pd is modulated by introducing bipyridine groups and changing metal nodes(Ce6O6 or Zr6O6).The bipyridine groups not only promoted the dispersion Pd NPs,but also facilitated electron transfer between Pd and UiO-67 MOFs through the formation of Pd-N bridges.Compared with Zr6 clusters,the tunability and orbital hybridisation of the 4f electronic structure in the Ce6 clusters modulate the electronic structure of Pd through the construction of the Ce-O-Pd interfaces.The optimal catalyst Pd/UiO-67(Ce)-bpy presented excellent low-temperature activity towards dicyclopentadiene hydrogenation with a conversion of>99%and a selectivity of>99%(50℃,10 bar).The results show that the synergy of Ce-O-Pd and Pd-N promotes the formation of active Pdδ+,which not only enhances the adsorption of H2 and electron-rich C=C bonds,but also contributes to the reduction of proton migration distance and improves proton utilization efficiency.These results provide valuable insights for investigating the regulatory role of the host MOFs,the nature of host-guest interactions,and their correlation with catalytic performance.
文摘Electrocatalytic reduction of CO_(2)(CO_(2)RR)to multicarbon products is an efficient approach for ad-dressing the energy crisis and achieving carbon neutrality.In H-cells,achieving high-current C_(2)products is challenging because of the inefficient mass transfer of the catalyst and the presence of the hydrogen evolution reaction(HER).In this study,dendritic Cu/Cu_(2)O with abundant Cu^(0)/Cu^(+)interfaces and numerous dendritic curves was synthesized in a CO_(2)atmosphere,resulting in the high selectivity and current density of the C_(2)products.Dendritic Cu/Cu_(2)O achieved a C_(2)Faradaic efficiency of 69.8%and a C_(2)partial current density of 129.5 mA cm^(-2)in an H-cell.Finite element simulations showed that a dendritic structure with a high curvature generates a strong electric field,leading to a localized CO_(2)concentration.Additionally,DRT analysis showed that a dendritic struc-ture with a high curvature actively adsorbed the surrounding high concentration of CO_(2),enhancing the mass transfer rate and achieving a high current density.During the experiment,the impact of the electronic structure on the performance of the catalyst was investigated by varying the atomic ratio of Cu^(0)/Cu^(+)on the catalyst surface,which resulted in improved ethylene selectivity.Under the optimal atomic ratio of Cu^(0)/Cu^(+),the charge transfer resistance was minimized,and the desorption rate of the intermediates was low,favoring C_(2)generation.Density functional theory calculations indicated that the Cu^(0)/Cu^(+)interfaces exhibited a lower Gibbs free energy for the rate-determining step,enhancing C_(2)H4 formation.The Cu/Cu_(2)O catalyst also exhibited a low Cu d-band center,which enhanced the adsorption stability of*CO on the surface and facilitated C_(2)formation.This observa-tion explained the higher yield of C_(2)products at the Cu^(0)/Cu^(+)interface than that of H_(2)under rapid mass transfer.The results of the net present value model showed that the H-cell holds promising industrial prospects,contingent upon it being a catalyst with both high selectivity and high current density.This approach of integrating the structure and composition provides new insights for ad-vancing the CO_(2)RR towards high-current C_(2)products.
文摘Calcium carbonate was synthesized in a CaCl2/NaCO3 mixed solution by using ethylenediaminetetraacetic acid (EDTA) as an additive. The thermodynamics and kinetics analyses indicate that although the driving force of amorphous calcium carbonate (ACC) precipitation is always less than that of calcite and vaterite precipitation, the nucleation rate of ACC is greater than that of calcite and vaterite at the initial stage of the precipitation reaction. With the increasing incubation time, vaterite and calcite particles nucleate heterogeneously by using the as-formed particles as active sites. Scanning electron microscopy images indicate that the transformation mechanism of ACC and vaterite to calcite is the dissolution-recrystallisation reaction. The presence of EDTA not only improves the stabilities of ACC and vaterite, but also leads to forming enlongated, connected rhombohedral calcite crystals after incubation 7 days in solutions. The ACC and vaterite are stabler in air than in solutions at room temperature, although the dissolution-recrystallisation reaction occurs on the surface.
基金Project (2011AA030101) supported by the High-tech Research and Development Program of China
文摘The morphology and formation mechanism of the substructure of martensite in TC21 alloy was investigated by XRD and TEM. The results showed that the martensitic transformation from β to α" occurs upon quenching after solution treatment between 960-1000 ℃. The antiphase boundary (APB)-like structure was observed clearly in the α" martensite plates. The APB-like contrasts exist along the (001) and (020) planes of α" martensite. This APB-like structure of α" martensite was identified as a kind of stacking fault with an APB-like morphology induced by martensitic transformation and not by order/disorder transition. During martensitic transformation, martensitic domains nucleate and grow, eventually encounter each other, resulting in the formation of the APBdike contrast.
基金Project(2015BAB17B01)supported by the National Science and Technology Support Program of ChinaProject(21376273)supported by the National Natural Science Foundation of China
文摘The influences of sodium silicate on manganese electrodeposition in sulfate solution were investigated. Manganese electrodeposition experiments indicate that a certain amount of sodium silicate can improve cathode current efficiency and initial pH 7.0?8.0 is the optimized pH for high cathode current efficiency. The analyses of scanning electron microscopy (SEM) and X-ray diffraction (XRD) indicate the compact morphology and nanocrystalline structure of electrodeposits. X-ray photoelectron spectrometry (XPS) analysis shows that the elements of Mn, Si and O exist in the deposit. The solution chemistry calculations of sulfate electrolyte and sodium silicate solution indicate that species of Mn2+, MnSO4, Mn(SO4)2?2 , Mn2+, MnSiO3, Mn(NH3)2+, SiO32?and HSiO3? are the main active species during the process of manganese electrodeposition. The reaction trend between Mn2+ and Si-containing ions is confirmed by the thermodynamic analysis. In addition, polarization curve tests confirm that sodium silicate can increase the overpotential of hydrogen evolution reaction, and then indirectly improve the cathode current efficiency.
基金supported by the Project kzcx2-yw-113,kzcx2-yw-121 and kzcx1-yw-15-4,CAS
文摘In CSEM exploration, the receivers are generally located about three to five times the skin depth from the transmitter. In this paper, we study the effect of a conductor between the transmitter and the survey area on the target conductor response using forward modeling and inversion. The 2D forward finite element calculations show that the conductor mainly affects the response at middle and low frequencies. The lower the resistivity and the larger the conductor, the larger the effect and the effect increases with decreasing frequency. The inversion results indicate that the calculated position of the target body can move towards the source, leading to an incorrect interpretation without considering the conductor. In order to reduce the effect of a conductor between the source and the survey area, CSEM acquisition should be conducted in three dimensions using multiple sources and 3D inversion should be used during interpretation.
基金Projects (50975062, 51105107, 51021002) supported by the National Natural Science Foundation of ChinaProjects (QC2011C044) supported by the Natural Science Foundation of Heilongjiang Province,China+1 种基金Project (20112302130005) supported by the Specialized Research Fund for the Doctoral Program of Higher Education,ChinaProject (CUGA4130902510) supported by the China Postdoctoral Science Foundation Funded
文摘Reactive brazing of TiAl-based intermetallics and Ni-based alloy with Ti foil as interlayer was investigated. The interfacial microstructure and shear strength of the joints were studied. According to the experimental observations, the molten interlayer reacts vigorously with base metals, forming several continuous reaction layers. The typical interfacial microstructure of the joint can be expressed as GH99/(Ni,Cr)ss(γ)/TiNi(β2)+TiNi2Al(τ4)+Ti2Ni(δ)/δ+Ti3Al(α2)+Al3NiTi2(τ3)/α2+τ3/TiAl. The maximum shear strength is 258 MPa for the specimen brazed at 1000°C for 10 min. Higher brazing temperature or longer brazing time causes coarsening of the phases in the brazing seam and formation of brittle intermetallic layer, which greatly depresses the shear strength of the joints.
基金supported by the Chinese Scholarship Foundation,the Gravity and Magnetics Research Consortium(GMRC)the National Natural Science Foundation of China(No.41074095)+1 种基金the National Special Project(No.201011039)the Open Project of the National Key Laboratory for Geological Processes and Mineral Resources(No.GPMR0942)
文摘Understanding the continental margin of the Northeastern South China Sea is critical to the study of deep structures, tectonic evolution, and dynamics of the region. One set of important data for this endeavor is the total-field magnetic data. Given the challenges associated with the magnetic data at low latitudes and with remanent magnetism in this area, we combine the equivalent-source technique and magnetic amplitude inversion to recover 3D subsurface magnetic structures. The inversion results show that this area is characterized by a north-south block division and east-west zonation. Magnetic regions strike in EW, NE and NW direction and are consistent with major tectonic trends in the region. The highly magnetic zone recovered from inversion in the continental margin differs visibly from that of the magnetically quiet zones to the south. The magnetic anomaly zone strikes in NE direction, covering an area of about 500 km × 60 km, and extending downward to a depth of 25 km or more. In combination with other geophysical data, we suggest that this strongly magnetic zone was produced by deep underplating of magma associated with plate subduction in Mesozoic period. The magnetically quiet zone in the south is an EW trending unit underlain by broad and gentle magnetic layers of lower crust. Its magnetic structure bears a clear resemblance to oceanic crust, assumed to be related to the presence of ancient oceanic crust there.
文摘In this paper, a new method of time reversal for defect diagnosis of concealed structure has been proposed based on the detecting technique of structure acoustic wave and the theory of time reversal. The time reversal recurrence formula for detecting the acoustic wave speed constitution of concealed structures with bilevel asynchronous test has been established. The wave speed constitution can be reconstructed in 2 D graticule form by means of this method. The result of model test shows the method is valid.
基金Project(SKLCRSM13KFB05)supported by State Key Laboratory of Coal Resources and Safe Mining,China University of Mining and Technology(Beijing)
文摘The fluidity of fresh cemented tailings backfill(CTB) slurry depends on its rheological properties. Hence, it is crucial to understand the rheology of fresh CTB slurry, which is related to the cement hydration progress and temperature evolution within CTB mixtures. For this reason, a numerical model was developed to predict the evolution of the rheological properties of fresh CTB slurry under the coupled effect of cement hydration and temperature. Experiments were conducted to investigate the rheological behaviours of the fresh CTB slurry. By comparing the simulated results with the experimental ones, the availability of this developed model was validated. Thereafter, the model was used to demonstrate the coupled effect of cement hydration and temperature on the evolution of fresh CTB slurry's rheological properties, under various conditions(initial CTB temperature, cement to tailings ratio, and water to cement ratio). The obtained results are helpful to better understanding the rheology of CTB slurry.
文摘A reverse bias silicon p-n junction based on light emitting diode is designed in standard 0.6μm industrial CMOS technology.The mechanism of the light emitting of this device is discussed.The device is simulated by the commercial software.I-V characteristic under forward or reverse bias is simulated utilizing the commercial software.The results between simulation and experiment data are compared.The results show that it is a promising device and may find applications in light linking.
文摘In this paper, we consider a reaction diffusion system with Hamitonian structure, we first prove the existence of an invariant region for system and the continuity of the semigroup, then establish the absorbing sets and global attractor.