The oxidative dehydrogenation(ODH) of propane on monomeric VO3 supported by CeO2(111)(VO3/CeO 2(111)) is studied by periodic density functional theory calculations. Detailed energetic, structural, and electron...The oxidative dehydrogenation(ODH) of propane on monomeric VO3 supported by CeO2(111)(VO3/CeO 2(111)) is studied by periodic density functional theory calculations. Detailed energetic, structural, and electronic properties of these reactions are determined. The calculated activation energies of the breaking of the first and second C–H bonds of propane on the VO3/CeO2(111) catalyst are compared, and it is found that both the unique structural and electronic effects of the VO3/CeO2(111) catalyst contribute to the relatively easy rupture of the first C–H bond of the propane molecule during the ODH reaction. In particular, the so-called new empty localized states that are mainly constituted of O2 porbitals of the ceria-supported VO3 species are determined to be crucial for assisting the cleavage of the first C–H bond of the propane molecule. Following this they become occupied and the remaining C–H bonds become increasingly difficult to break owing to the increasing repulsion between the localized 4 felectrons at the Cecations, resulting in the adsorption of more H and other moieties. This work illustrates that CeO2-supported monomeric vanadium oxides can exhibit unique activity and selectivity for the catalytic ODH of alkanes to alkenes.展开更多
Evaluating the effect of metal surface density on catalytic performance is critical for designing high-activity metal-based catalysts.In this study,a series of ceria(CeCO_(2))-supported Ru catalysts(Ru/CeCO_(2))were p...Evaluating the effect of metal surface density on catalytic performance is critical for designing high-activity metal-based catalysts.In this study,a series of ceria(CeCO_(2))-supported Ru catalysts(Ru/CeCO_(2))were prepared to analyze the effect of Ru surface density on the catalytic performance of Ru/CeCO_(2) for ammonia synthesis.For the Ru/CeCO_(2) catalysts with Ru surface densities lower than 0.68 Ru nm^(-2),the Ru layers were in close contact with CeCO_(2),and electrons were transferred directly from the CeCO_(2) defect sites to the Ru species.In such cases,the adsorption of hydrogen species on the Ru sites in the vicinity of 0 atoms was high,leading to a high ammonia synthesis activity and strong hydrogen poisoning.In contrast,the preferential aggregation of Ru species into large particles on top of the Ru overlayer resulted in the coexistence of Ru clusters and particles,for catalysts with a Ru surface density higher than 1.4 Ru nm^(-2),for which Ru particles were isolated from the direct electronic influence of CeCO_(2).Consequently,the Ru-Ceth interactions were weak,and hydrogen poisoning can be significantly alleviated.Overall,electron transfer and hydrogen adsorption synergistically affected the synthesis of ammonia over Ru/CeCO_(2) catalysts,and catalyst samples with a Ru surface density lower than 0.31 Ru nm^(-2) or exactly 2.1 Ru nm^(-2) exhibited high catalytic activity for ammonia synthesis.展开更多
The optimization of high density and concentrated-weight freights loading requires an even distribution of the freight's weight and unconcentrated loading on the floor of the car.Based on the characteristics of co...The optimization of high density and concentrated-weight freights loading requires an even distribution of the freight's weight and unconcentrated loading on the floor of the car.Based on the characteristics of concentrated-weight category freights,an improvement method is put forward to build freight towers and a greedy-construction algorithm is utilized based on heuristic information for the initial layout.Then a feasibility analysis is performed to judge if the balanced and unconcentrated loading constrains are reached.Through introducing optimization or adjustment methods,an overall optimal solution can be obtained.Experiments are conducted using data generated from real cases showing the effectiveness of our approach: volume utility ratio of 90.4% and load capacity utility ratio of 86.7% which is comparably even to the packing of the general freights.展开更多
Lithium-sulfur(Li-S) batteries have attracted considerable attention due to their high energy density(2600 Wh kg-1). However, its commercialization is hindered seriously by the low loading and utilization rate of sulf...Lithium-sulfur(Li-S) batteries have attracted considerable attention due to their high energy density(2600 Wh kg-1). However, its commercialization is hindered seriously by the low loading and utilization rate of sulfur cathodes. Herein, we designed the cellulose-based graphene carbon composite aerogel(CCA) self-standing electrode to enhance the performance of Li-S batteries. The CCA contributes to the mass loading and utilization efficiency of sulfur, because of its unique physical structure: low density(0.018 g cm-3), large specific surface area(657.85 m2 g-1), high porosity(96%), and remarkable electrolyte adsorption(42.25 times). Compared to Al(about 49%), the CCA displayed excellent sulfur use efficiency(86%) and could reach to high area capacity of 8.60 mAh cm-2 with 9.11 mgS loading. Meanwhile,the CCA exhibits the excellent potential for pulse sensing applications due to its flexibility and superior sensitivity to electrical response signals.展开更多
The aim of this paper is to describe and analyse the behaviour of heart rate variability(HRV)during constant-load,high-intensity exercise using a time frequency analysis(Wavelet Transform).Eleven elite cyclists took p...The aim of this paper is to describe and analyse the behaviour of heart rate variability(HRV)during constant-load,high-intensity exercise using a time frequency analysis(Wavelet Transform).Eleven elite cyclists took part in the study(age:18.6±3.0 years;VO_(2max):4.88±0.61 litres·min^(-1)).Initially,all subjects performed an incremental cycloergometer test to determine load power in a constant load-test(379.55±36.02 W;89.0%).HRV declined dramatically from the start of testing(p<0.05).The behaviour of power spectral density within the LF band mirrored that of total energy,recording a significant decrease from the outset LF peaks fell rapidly thereafter,remaining stable until the end of the test.HF-VHF fell sharply in the first 20 to 30 seconds.The relative weighting(%) of HF-VHF was inverted with the onset of fatigue,[1.6%at the start,7.1(p<0.05) at the end of the first phase,and 43.1%(p<0.05) at the end of the test].HF-VHF_(peak) displayed three phases:a moderate initial increase,followed by a slight fall,thereafter increasing to the end of the test.The LF/HF-VHF ratio increased at the start,later falling progressively until the end of the first phase and remaining around minimal values until the end of the test.展开更多
基金supported by the National Natural Science Foundation of China(21421004,21573067,91545103)Program of Shanghai Academic Research Leader(17XD1401400)~~
文摘The oxidative dehydrogenation(ODH) of propane on monomeric VO3 supported by CeO2(111)(VO3/CeO 2(111)) is studied by periodic density functional theory calculations. Detailed energetic, structural, and electronic properties of these reactions are determined. The calculated activation energies of the breaking of the first and second C–H bonds of propane on the VO3/CeO2(111) catalyst are compared, and it is found that both the unique structural and electronic effects of the VO3/CeO2(111) catalyst contribute to the relatively easy rupture of the first C–H bond of the propane molecule during the ODH reaction. In particular, the so-called new empty localized states that are mainly constituted of O2 porbitals of the ceria-supported VO3 species are determined to be crucial for assisting the cleavage of the first C–H bond of the propane molecule. Following this they become occupied and the remaining C–H bonds become increasingly difficult to break owing to the increasing repulsion between the localized 4 felectrons at the Cecations, resulting in the adsorption of more H and other moieties. This work illustrates that CeO2-supported monomeric vanadium oxides can exhibit unique activity and selectivity for the catalytic ODH of alkanes to alkenes.
文摘Evaluating the effect of metal surface density on catalytic performance is critical for designing high-activity metal-based catalysts.In this study,a series of ceria(CeCO_(2))-supported Ru catalysts(Ru/CeCO_(2))were prepared to analyze the effect of Ru surface density on the catalytic performance of Ru/CeCO_(2) for ammonia synthesis.For the Ru/CeCO_(2) catalysts with Ru surface densities lower than 0.68 Ru nm^(-2),the Ru layers were in close contact with CeCO_(2),and electrons were transferred directly from the CeCO_(2) defect sites to the Ru species.In such cases,the adsorption of hydrogen species on the Ru sites in the vicinity of 0 atoms was high,leading to a high ammonia synthesis activity and strong hydrogen poisoning.In contrast,the preferential aggregation of Ru species into large particles on top of the Ru overlayer resulted in the coexistence of Ru clusters and particles,for catalysts with a Ru surface density higher than 1.4 Ru nm^(-2),for which Ru particles were isolated from the direct electronic influence of CeCO_(2).Consequently,the Ru-Ceth interactions were weak,and hydrogen poisoning can be significantly alleviated.Overall,electron transfer and hydrogen adsorption synergistically affected the synthesis of ammonia over Ru/CeCO_(2) catalysts,and catalyst samples with a Ru surface density lower than 0.31 Ru nm^(-2) or exactly 2.1 Ru nm^(-2) exhibited high catalytic activity for ammonia synthesis.
基金Project(71371193)supported by the National Natural Science Foundation of ChinaProjects(2005K1001,2007K1005)supported by Guangzhou-Shenzhen Railway Company Limited,China
文摘The optimization of high density and concentrated-weight freights loading requires an even distribution of the freight's weight and unconcentrated loading on the floor of the car.Based on the characteristics of concentrated-weight category freights,an improvement method is put forward to build freight towers and a greedy-construction algorithm is utilized based on heuristic information for the initial layout.Then a feasibility analysis is performed to judge if the balanced and unconcentrated loading constrains are reached.Through introducing optimization or adjustment methods,an overall optimal solution can be obtained.Experiments are conducted using data generated from real cases showing the effectiveness of our approach: volume utility ratio of 90.4% and load capacity utility ratio of 86.7% which is comparably even to the packing of the general freights.
基金This work was financially supported by the National Natural Science Foundation of China(51773165,51973171)Innovation Capability Support Program of Shaanxi(2018PT-28,2019PT-05).
文摘Lithium-sulfur(Li-S) batteries have attracted considerable attention due to their high energy density(2600 Wh kg-1). However, its commercialization is hindered seriously by the low loading and utilization rate of sulfur cathodes. Herein, we designed the cellulose-based graphene carbon composite aerogel(CCA) self-standing electrode to enhance the performance of Li-S batteries. The CCA contributes to the mass loading and utilization efficiency of sulfur, because of its unique physical structure: low density(0.018 g cm-3), large specific surface area(657.85 m2 g-1), high porosity(96%), and remarkable electrolyte adsorption(42.25 times). Compared to Al(about 49%), the CCA displayed excellent sulfur use efficiency(86%) and could reach to high area capacity of 8.60 mAh cm-2 with 9.11 mgS loading. Meanwhile,the CCA exhibits the excellent potential for pulse sensing applications due to its flexibility and superior sensitivity to electrical response signals.
文摘The aim of this paper is to describe and analyse the behaviour of heart rate variability(HRV)during constant-load,high-intensity exercise using a time frequency analysis(Wavelet Transform).Eleven elite cyclists took part in the study(age:18.6±3.0 years;VO_(2max):4.88±0.61 litres·min^(-1)).Initially,all subjects performed an incremental cycloergometer test to determine load power in a constant load-test(379.55±36.02 W;89.0%).HRV declined dramatically from the start of testing(p<0.05).The behaviour of power spectral density within the LF band mirrored that of total energy,recording a significant decrease from the outset LF peaks fell rapidly thereafter,remaining stable until the end of the test.HF-VHF fell sharply in the first 20 to 30 seconds.The relative weighting(%) of HF-VHF was inverted with the onset of fatigue,[1.6%at the start,7.1(p<0.05) at the end of the first phase,and 43.1%(p<0.05) at the end of the test].HF-VHF_(peak) displayed three phases:a moderate initial increase,followed by a slight fall,thereafter increasing to the end of the test.The LF/HF-VHF ratio increased at the start,later falling progressively until the end of the first phase and remaining around minimal values until the end of the test.