Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Her...Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Herein,with crystal and atomic structures of the self-assembled PDI revealed from the X-ray diffraction pattern,the electronic structure is theoretically illustrated by the first-principles density functional theory calculations,suggesting the suitable band structure and the direct electronic transition for efficient photocatalytic oxygen evolution over PDI.It is confirmed that the carbonyl O atoms on the conjugation structure serve as the active sites for oxygen evolution reaction by the crystal orbital Hamiltonian group analysis.The calculations of reaction free energy changes indicate that the oxygen evolution reaction should follow the reaction pathway of H_(2)O→^(*)OH→^(*)O→^(*)OOH→^(*)O_(2)with an overpotential of 0.81 V.Through an in-depth theoretical computational analysis in the atomic and electronic structures,the origin of photocatalytic oxygen evolution activity for PDI is well illustrated,which would help the rational design and modification of polymeric photocatalysts for efficient oxygen evolution.展开更多
Electrocatalytic reduction of carbon dioxide(CO_(2))to carbon monoxide(CO)is an effective strategy to achieve carbon neutrality.High selective and low-cost catalysts for the electrocatalytic reduction of CO_(2)have re...Electrocatalytic reduction of carbon dioxide(CO_(2))to carbon monoxide(CO)is an effective strategy to achieve carbon neutrality.High selective and low-cost catalysts for the electrocatalytic reduction of CO_(2)have received increasing attention.In contrast to the conventional tube furnace method,the high-temperature shock(HTS)method enables ultra-fast thermal processing,superior atomic efficiency,and a streamlined synthesis protocol,offering a simplified method for the preparation of high-performance single-atom catalysts(SACs).The reports have shown that nickel-based SACs can be synthesized quickly and conveniently using the HTS method,making their application in CO_(2)reduction reactions(CO_(2)RR)a viable and promising avenue for further exploration.In this study,the effect of heating temperature,metal loading and different nitrogen(N)sources on the catalyst morphology,coordination environment and electrocatalytic performance were investigated.Under optimal conditions,0.05Ni-DCD-C-1050 showed excellent performance in reducing CO_(2)to CO,with CO selectivity close to 100%(−0.7 to−1.0 V vs RHE)and current density as high as 130 mA/cm^(2)(−1.1 V vs RHE)in a flow cell under alkaline environment.展开更多
Effects of ultrasonic bonding parameters on atomic diffusion, microstructure at the Al-Au interface, and shear strength of Al-Au ultrasonic bonding were investigated by the combining experiments and finite element (FE...Effects of ultrasonic bonding parameters on atomic diffusion, microstructure at the Al-Au interface, and shear strength of Al-Au ultrasonic bonding were investigated by the combining experiments and finite element (FE) simulation. The quantitative model of atomic diffusion, which is related to the ultrasonic bonding parameters, time and distance, is established to calculate the atomic diffusion of the Al-Au interface. The maximum relative error between the calculated and experimental fraction of Al atom is 7.35%, indicating high prediction accuracy of this model. During the process of ultrasonic bonding, Au8Al3 is the main intermetallic compound (IMC) at the Al-Au interface. With larger bonding forces, higher ultrasonic powers and longer bonding time, it is more difficult to remove the oxide particles from the Al-Au interface, which hinders the atomic diffusion. Therefore, the complicated stress state and the existence of oxide particles both promotes the formation of holes. The shear strength of Al-Au ultrasonic bonding increases with increasing bonding force, ultrasonic power and bonding time. However, combined with the presence of holes at especial parameters, the optimal ultrasonic bonding parameter is confirmed to be a bonding force of 23 gf, ultrasonic power of 75 mW and bonding time of 21 ms.展开更多
In order to enhance the atomization efficiency of atomizer, a new type of wind-spray dust controller combining the rotary-atomization and colliding broken of droplets was designed by the method of opening the water ci...In order to enhance the atomization efficiency of atomizer, a new type of wind-spray dust controller combining the rotary-atomization and colliding broken of droplets was designed by the method of opening the water circulation within the blades. The experiment test for dust controller was conducted by adjusting the following parameters: rotating speed, diversion hole-exit diameter, and colliding tooth angle. Results show that the atomization efficiency increases firstly then decreases with them. And the optimal parameters are obtained with rotating speed 1500-2200 r/min, diversion hole-exit diameter 2-2.5 mm and colliding tooth angle 30°-40°, and under these conditions the corresponding atomization efficiency tops to 95%. Then, the atomization situation under the optimal parameters is held from the aspect of simulation internal flow field and the results of droplet size(30-80 μm) are got, which indicates that the conclusion on the optimized parameters of dust controller is reasonable. The collecting efficiencies of different dust concentrations are determined, ranging from 85% to 98.4%, which shows that the designed dust controller can obtain a good atomizing effect and achieve well dustfall efficiency for the wetting dust control of coal mine.展开更多
The almost completely dense copper was prepared by ultrafine copper powder prepared with both methods of electrolysis and novel water-gas atomization through cold isostatic pressing(CIP)and sintering under atmospheric...The almost completely dense copper was prepared by ultrafine copper powder prepared with both methods of electrolysis and novel water-gas atomization through cold isostatic pressing(CIP)and sintering under atmospheric hydrogen.Fine copper powder possesses the higher sintering driving force,thereby promoting shrinkage and densification during the sintering process.The grain size of sintered samples by electrolytic copper powder is smaller than that prepared by the atomized copper powder,and the twin crystals are particularly prone to forming in the former sintered microstructure due to the raw powder with low oxygen content and high residual stress originating from the CIP process.The relative density of samples by electrolytic and atomized powder at 1000℃ sintering temperature achieves 99.3%and 97.4%,respectively,significantly higher than that of the powder metallurgy copper parts reported in the literature.Correspondingly,the ultimate tensile strength and yield strength of samples by both kinds of copper powder are approximately similar,while the elongation of the sintered sample by the electrolytic powder(60%)is apparently higher than the atomized powder(44%).The superior performance of samples fabricated by electrolytic powder is inferred from the full density and low oxygen level for there is no cuprous oxide in the grain boundaries.展开更多
Hypereutectic Al-40 wt.%Si alloys were fabricated by the combination of gas atomization and spark plasma sintering(SPS) technology. The effects of holding time(15-60 min) on phase composition, microstructure, density,...Hypereutectic Al-40 wt.%Si alloys were fabricated by the combination of gas atomization and spark plasma sintering(SPS) technology. The effects of holding time(15-60 min) on phase composition, microstructure, density,mechanical properties of Al-Si alloys were investigated by XRD, SEM, a hydrostatic balance, an automatic micro hardness tester and a universal tensile testing machine. The results showed that homogenous distribution of ultrafine primary Si and high density of alloys can be obtained at holding time of 30 min. Compared with primary Si(3.7 μm)fabricated by gas atomization, the average size increased from 5.17 to 7.72 μm with the increase of holding time during SPS process. Overall, the relative density, maximum tensile strength and Vickers hardness of 94.9%, 205 MPa and HV;196.86 were achieved at holding time of 30 min, respectively. In addition, all the diffraction peaks were corresponded to α-Al or β-Si and no other phase can be detected. Finally, the densification process of SPS was also discussed.展开更多
In the present study,electrostatic atomization(EA)behavior of several test liquids having much higher viscosities(1 400 mPa·s)than have previously been studied was investigated by spraying at a series of applied ...In the present study,electrostatic atomization(EA)behavior of several test liquids having much higher viscosities(1 400 mPa·s)than have previously been studied was investigated by spraying at a series of applied voltages and flow rates.The results showed that to obtain stable cone-jet mode spraying and hence gain better monodispersity of droplets,electrical conductivity,viscosity and surface tension of the liquid are important controlling factors.The stable cone-jet mode could be easily established for liquids having shear viscosities in the range from 80 to 1 400 mPa·s and surface tensions below 65 mN·m-1.In contrast,methylcellulose aqueous solutions with shear viscosities ranging from 10 to 540 mPa·s and moderate surface tensions(50~56 mN·m-1)generated more complicated spraying modes.However,fine TiO2 powder(a few micrometers in size)could be prepared using the EA method from its precursor solutions.展开更多
Formic acid oxidation reaction(FAOR),as the anodic reaction in direct formic acid fuel cells,has attracted much attention but increasing the mass activity and stability of catalysts still face a bottleneck to meet the...Formic acid oxidation reaction(FAOR),as the anodic reaction in direct formic acid fuel cells,has attracted much attention but increasing the mass activity and stability of catalysts still face a bottleneck to meet the requirements of practical applications.In the past decades,researchers developed many strategies to fix these issues by improving the structure of catalysts and the newly raised single atom catalysts(SACs)show the high mass activity and stability in FAOR.This review first summarized the reaction mechanism involved in FAOR.The mass activity as well as stability of catalysts reported in the past five years have been outlined.Moreover,the synthetic strategies to improve the catalytic performance of catalysts are also reviewed in this work.Finally,we proposed the research directions to guide the rational design of new FAOR catalysts in the future.展开更多
应用Realizable k-ε湍流模型和VOF(Volume of Fraction)两相流模型对某压力旋流喷嘴进行数值研究,分析了旋流室锥角、旋流孔角度及喷嘴入口压力变化对雾化锥角、雾化粒径及分布、液滴速度分布等参数的影响。结果表明:雾化锥角受旋流室...应用Realizable k-ε湍流模型和VOF(Volume of Fraction)两相流模型对某压力旋流喷嘴进行数值研究,分析了旋流室锥角、旋流孔角度及喷嘴入口压力变化对雾化锥角、雾化粒径及分布、液滴速度分布等参数的影响。结果表明:雾化锥角受旋流室锥角的影响幅度随压力增大而减小,雾化粒径及分布受旋流室锥角影响不明显,当旋流室锥角为90°时雾化范围广且雾化稳定性好;雾化锥角随旋流孔角度增大先增后减,当角度为45°时雾化锥角最大,平均粒径及其分布更佳;当喷嘴入口压力逐渐增大时,雾化锥角与雾化粒径均逐渐减小,液滴速度区间逐渐缩小,当入口压力达到0.4 MPa时,Sauter粒径及液滴粒径分布趋于稳定,液滴速度分布最为集中。展开更多
基金supported by National Natural Science Foundation of China(No.523B2070,No.52225606).
文摘Polymeric perylene diimide(PDI)has been evidenced as a good candidate for photocatalytic water oxidation,yet the origin of the photocatalytic oxygen evolution activity remains unclear and needs further exploration.Herein,with crystal and atomic structures of the self-assembled PDI revealed from the X-ray diffraction pattern,the electronic structure is theoretically illustrated by the first-principles density functional theory calculations,suggesting the suitable band structure and the direct electronic transition for efficient photocatalytic oxygen evolution over PDI.It is confirmed that the carbonyl O atoms on the conjugation structure serve as the active sites for oxygen evolution reaction by the crystal orbital Hamiltonian group analysis.The calculations of reaction free energy changes indicate that the oxygen evolution reaction should follow the reaction pathway of H_(2)O→^(*)OH→^(*)O→^(*)OOH→^(*)O_(2)with an overpotential of 0.81 V.Through an in-depth theoretical computational analysis in the atomic and electronic structures,the origin of photocatalytic oxygen evolution activity for PDI is well illustrated,which would help the rational design and modification of polymeric photocatalysts for efficient oxygen evolution.
基金supported by the National Key R&D Program of China(2024YFB4106400)National Natural Science Foundation of China(22209200,52302331)。
文摘Electrocatalytic reduction of carbon dioxide(CO_(2))to carbon monoxide(CO)is an effective strategy to achieve carbon neutrality.High selective and low-cost catalysts for the electrocatalytic reduction of CO_(2)have received increasing attention.In contrast to the conventional tube furnace method,the high-temperature shock(HTS)method enables ultra-fast thermal processing,superior atomic efficiency,and a streamlined synthesis protocol,offering a simplified method for the preparation of high-performance single-atom catalysts(SACs).The reports have shown that nickel-based SACs can be synthesized quickly and conveniently using the HTS method,making their application in CO_(2)reduction reactions(CO_(2)RR)a viable and promising avenue for further exploration.In this study,the effect of heating temperature,metal loading and different nitrogen(N)sources on the catalyst morphology,coordination environment and electrocatalytic performance were investigated.Under optimal conditions,0.05Ni-DCD-C-1050 showed excellent performance in reducing CO_(2)to CO,with CO selectivity close to 100%(−0.7 to−1.0 V vs RHE)and current density as high as 130 mA/cm^(2)(−1.1 V vs RHE)in a flow cell under alkaline environment.
基金Project(2022YFB3707201) supported by the National Key R&D Program of ChinaProject(U2341254) supported by the Ye Qisun Science Foundation of National Natural Science Foundation of China+1 种基金Projects(0604022GH0202143,0604022SH0201143) supported by the NPU Aoxiang Distinguished Young Scholars,ChinaProject supported by the Funding of Young Top-notch Talent of the National Ten Thousand Talent Program,China。
文摘Effects of ultrasonic bonding parameters on atomic diffusion, microstructure at the Al-Au interface, and shear strength of Al-Au ultrasonic bonding were investigated by the combining experiments and finite element (FE) simulation. The quantitative model of atomic diffusion, which is related to the ultrasonic bonding parameters, time and distance, is established to calculate the atomic diffusion of the Al-Au interface. The maximum relative error between the calculated and experimental fraction of Al atom is 7.35%, indicating high prediction accuracy of this model. During the process of ultrasonic bonding, Au8Al3 is the main intermetallic compound (IMC) at the Al-Au interface. With larger bonding forces, higher ultrasonic powers and longer bonding time, it is more difficult to remove the oxide particles from the Al-Au interface, which hinders the atomic diffusion. Therefore, the complicated stress state and the existence of oxide particles both promotes the formation of holes. The shear strength of Al-Au ultrasonic bonding increases with increasing bonding force, ultrasonic power and bonding time. However, combined with the presence of holes at especial parameters, the optimal ultrasonic bonding parameter is confirmed to be a bonding force of 23 gf, ultrasonic power of 75 mW and bonding time of 21 ms.
基金Project(U1261107)supported by the Joint Funds of the National Natural Science Foundation of China
文摘In order to enhance the atomization efficiency of atomizer, a new type of wind-spray dust controller combining the rotary-atomization and colliding broken of droplets was designed by the method of opening the water circulation within the blades. The experiment test for dust controller was conducted by adjusting the following parameters: rotating speed, diversion hole-exit diameter, and colliding tooth angle. Results show that the atomization efficiency increases firstly then decreases with them. And the optimal parameters are obtained with rotating speed 1500-2200 r/min, diversion hole-exit diameter 2-2.5 mm and colliding tooth angle 30°-40°, and under these conditions the corresponding atomization efficiency tops to 95%. Then, the atomization situation under the optimal parameters is held from the aspect of simulation internal flow field and the results of droplet size(30-80 μm) are got, which indicates that the conclusion on the optimized parameters of dust controller is reasonable. The collecting efficiencies of different dust concentrations are determined, ranging from 85% to 98.4%, which shows that the designed dust controller can obtain a good atomizing effect and achieve well dustfall efficiency for the wetting dust control of coal mine.
基金Project(92066205)supported by the National Natural Science Foundation of ChinaProject(2019-Z10)supported by the State Key Lab for Advanced Metals and Materials of ChinaProject(FRF-MP-20-52)supported by the Fundamental Research Funds for the Central Universities,China。
文摘The almost completely dense copper was prepared by ultrafine copper powder prepared with both methods of electrolysis and novel water-gas atomization through cold isostatic pressing(CIP)and sintering under atmospheric hydrogen.Fine copper powder possesses the higher sintering driving force,thereby promoting shrinkage and densification during the sintering process.The grain size of sintered samples by electrolytic copper powder is smaller than that prepared by the atomized copper powder,and the twin crystals are particularly prone to forming in the former sintered microstructure due to the raw powder with low oxygen content and high residual stress originating from the CIP process.The relative density of samples by electrolytic and atomized powder at 1000℃ sintering temperature achieves 99.3%and 97.4%,respectively,significantly higher than that of the powder metallurgy copper parts reported in the literature.Correspondingly,the ultimate tensile strength and yield strength of samples by both kinds of copper powder are approximately similar,while the elongation of the sintered sample by the electrolytic powder(60%)is apparently higher than the atomized powder(44%).The superior performance of samples fabricated by electrolytic powder is inferred from the full density and low oxygen level for there is no cuprous oxide in the grain boundaries.
基金Project(18JS060) supported by the Shaanxi Key Laboratory of Nano-materials and Technology,ChinaProject(2018JQ5087) supported by Natural Science Basic Research Plan of Shaanxi Province,China。
文摘Hypereutectic Al-40 wt.%Si alloys were fabricated by the combination of gas atomization and spark plasma sintering(SPS) technology. The effects of holding time(15-60 min) on phase composition, microstructure, density,mechanical properties of Al-Si alloys were investigated by XRD, SEM, a hydrostatic balance, an automatic micro hardness tester and a universal tensile testing machine. The results showed that homogenous distribution of ultrafine primary Si and high density of alloys can be obtained at holding time of 30 min. Compared with primary Si(3.7 μm)fabricated by gas atomization, the average size increased from 5.17 to 7.72 μm with the increase of holding time during SPS process. Overall, the relative density, maximum tensile strength and Vickers hardness of 94.9%, 205 MPa and HV;196.86 were achieved at holding time of 30 min, respectively. In addition, all the diffraction peaks were corresponded to α-Al or β-Si and no other phase can be detected. Finally, the densification process of SPS was also discussed.
文摘In the present study,electrostatic atomization(EA)behavior of several test liquids having much higher viscosities(1 400 mPa·s)than have previously been studied was investigated by spraying at a series of applied voltages and flow rates.The results showed that to obtain stable cone-jet mode spraying and hence gain better monodispersity of droplets,electrical conductivity,viscosity and surface tension of the liquid are important controlling factors.The stable cone-jet mode could be easily established for liquids having shear viscosities in the range from 80 to 1 400 mPa·s and surface tensions below 65 mN·m-1.In contrast,methylcellulose aqueous solutions with shear viscosities ranging from 10 to 540 mPa·s and moderate surface tensions(50~56 mN·m-1)generated more complicated spraying modes.However,fine TiO2 powder(a few micrometers in size)could be prepared using the EA method from its precursor solutions.
基金Project(22102218)supported by the National Natural Science Foundation of ChinaProject(2022RC1110)supported by the Science and Technology Innovation Program of Hunan Province,ChinaProject(2022QNRC001)supported by the Young Elite Scientists Sponsorship Program by CAST,China。
文摘Formic acid oxidation reaction(FAOR),as the anodic reaction in direct formic acid fuel cells,has attracted much attention but increasing the mass activity and stability of catalysts still face a bottleneck to meet the requirements of practical applications.In the past decades,researchers developed many strategies to fix these issues by improving the structure of catalysts and the newly raised single atom catalysts(SACs)show the high mass activity and stability in FAOR.This review first summarized the reaction mechanism involved in FAOR.The mass activity as well as stability of catalysts reported in the past five years have been outlined.Moreover,the synthetic strategies to improve the catalytic performance of catalysts are also reviewed in this work.Finally,we proposed the research directions to guide the rational design of new FAOR catalysts in the future.
文摘应用Realizable k-ε湍流模型和VOF(Volume of Fraction)两相流模型对某压力旋流喷嘴进行数值研究,分析了旋流室锥角、旋流孔角度及喷嘴入口压力变化对雾化锥角、雾化粒径及分布、液滴速度分布等参数的影响。结果表明:雾化锥角受旋流室锥角的影响幅度随压力增大而减小,雾化粒径及分布受旋流室锥角影响不明显,当旋流室锥角为90°时雾化范围广且雾化稳定性好;雾化锥角随旋流孔角度增大先增后减,当角度为45°时雾化锥角最大,平均粒径及其分布更佳;当喷嘴入口压力逐渐增大时,雾化锥角与雾化粒径均逐渐减小,液滴速度区间逐渐缩小,当入口压力达到0.4 MPa时,Sauter粒径及液滴粒径分布趋于稳定,液滴速度分布最为集中。
