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
The movement mode of the atomizer is a very important parameter during spray deposition process,which has direct influence on the size and surface texture of the billets. To resolve the problem of manufacturing large ...The movement mode of the atomizer is a very important parameter during spray deposition process,which has direct influence on the size and surface texture of the billets. To resolve the problem of manufacturing large size billets,a method of spray deposition by the atomizer with off-center swing was put forward. The atomizer was driven by the alternating current servomotor to swing within 7° at varying speed. The influence of the atomizer parameters,such as translation of the atomizer,swing angle of the atomizer,substrate falling speed and spraying pressure,on the spray deposition was studied. The optimized parameters of the spray deposition process were obtained. The results show that the large size billets with uniform surface quality can be made through adjusting swing frequency and angle of the atomizer,offset distance of the atomizer and inclined angle of the substrate; the valid spray area will decrease and the dimension of top surface will reduce when pressure is less than 0.4 MPa within certain spray distance; meantime,the moving time and cooling time of the droplets are extended,which will lead to loose structure and bad densification. When the pressure,the swing angle and the eccentric offset of the atomization equal 0.5 MPa,7° and 60 mm,respectively,large size billets with fine texture and diameter of 500 mm can be produced.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(G1999064900) supported by the National Key Fundamental Research and Development Program of China
文摘The movement mode of the atomizer is a very important parameter during spray deposition process,which has direct influence on the size and surface texture of the billets. To resolve the problem of manufacturing large size billets,a method of spray deposition by the atomizer with off-center swing was put forward. The atomizer was driven by the alternating current servomotor to swing within 7° at varying speed. The influence of the atomizer parameters,such as translation of the atomizer,swing angle of the atomizer,substrate falling speed and spraying pressure,on the spray deposition was studied. The optimized parameters of the spray deposition process were obtained. The results show that the large size billets with uniform surface quality can be made through adjusting swing frequency and angle of the atomizer,offset distance of the atomizer and inclined angle of the substrate; the valid spray area will decrease and the dimension of top surface will reduce when pressure is less than 0.4 MPa within certain spray distance; meantime,the moving time and cooling time of the droplets are extended,which will lead to loose structure and bad densification. When the pressure,the swing angle and the eccentric offset of the atomization equal 0.5 MPa,7° and 60 mm,respectively,large size billets with fine texture and diameter of 500 mm can be produced.
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。
