A unique nest-type catalyst has been designed with a nest of oxygen capture surrounding catalytic Pt centers, which shows much promoted performance, on the base of Pt/C catalyst, for oxygen reduction reaction(ORR). Th...A unique nest-type catalyst has been designed with a nest of oxygen capture surrounding catalytic Pt centers, which shows much promoted performance, on the base of Pt/C catalyst, for oxygen reduction reaction(ORR). The nest is constructed with nitrogen-doped carbon matrix(NCM), derived from the controlled carbonization of PANI precursor, to cover Pt/C catalyst. The unique structure of the catalyst(denoted as NCM■ Pt/C) has many merits. Firstly, it can capture oxygen both in air and in acidic electrolyte. Compared with naked Pt/C, it is found that, in air, the oxygen concentration within the porous nest of NCM surrounding Pt/C particles is ~13 times higher than atmospheric oxygen concentration and, in acidic electrolyte, the concentration of activated oxygen over the catalyst NCM■ Pt/C rise to~1.9 times. Secondly, the NCM nest offers a special electronic modulation on Pt centers toward modified ORR kinetics and then catalytic performances. With these merits, compared with Pt/C, the NCM■ Pt/C catalyst shows 3.2 times higher turnover frequency value and 2.9 times enhanced specific activity for ORR with half-wave potential at 0.894 V. After 50,000 sweeping cycles, the NCM■ Pt/C catalyst retains~66% mass activity and still has advantages over the fresh Pt/C catalyst. We envision that the nest-type catalyst provides a new idea for progress of practical Pt/C ORR catalyst.展开更多
In this paper,a DG(Discontinuous Galerkin)method which has been widely employed in CFD(Computational Fluid Dynamics)is used to solve the twodimensional time-domain Maxwell’s equations for complex geometries on unstru...In this paper,a DG(Discontinuous Galerkin)method which has been widely employed in CFD(Computational Fluid Dynamics)is used to solve the twodimensional time-domain Maxwell’s equations for complex geometries on unstructured mesh.The element interfaces on solid boundary are treated in both curved way and straight way.Numerical tests are performed for both benchmark problems and complex cases with varying orders on a series of grids,where the high-order convergence in accuracy can be observed.Both the curved and the straight solid boundary implementation can give accurate RCS(Radar Cross-Section)results with sufficiently small mesh size,but the curved solid boundary implementation can significantly improve the accuracy when using relatively large mesh size.More importantly,this CFD-based high-order DG method for the Maxwell’s equations is very suitable for complex geometries.展开更多
A new mechanism of catalyst has been demonstrated in this article. With the interaction between carbon nitride(CN) and encapsulated nickel, the CN in the catalyst has been endowed with new active sites for the adsorpt...A new mechanism of catalyst has been demonstrated in this article. With the interaction between carbon nitride(CN) and encapsulated nickel, the CN in the catalyst has been endowed with new active sites for the adsorption and activation of hydrogen while nickel itself is physically isolated from the contact with reactive molecules. For the selective hydrogenation of acetylene in large amount of ethylene, the catalyst shows excellent ethylene selectivity than the nickel catalyst itself, which is almost totally unselective. Meanwhile, the CN itself is inactive for the reaction. The results of characterization demonstrate that pyridinic nitrogen doped in the carbon matrix should be the active sites for hydrogen dissociative adsorption. The theoretical calculations further confirm the results and provide with the detail in the electron transfer between nickel and CN in the catalyst. The current results supply a new concept for design of high performance catalyst.展开更多
基金supported by the National Natural Science Foundation of China(91963206,21932004)the Ministry of Science and Technology of China(2017YFB0702800)the China Postdoctoral Science Foundation(2021M691512)。
文摘A unique nest-type catalyst has been designed with a nest of oxygen capture surrounding catalytic Pt centers, which shows much promoted performance, on the base of Pt/C catalyst, for oxygen reduction reaction(ORR). The nest is constructed with nitrogen-doped carbon matrix(NCM), derived from the controlled carbonization of PANI precursor, to cover Pt/C catalyst. The unique structure of the catalyst(denoted as NCM■ Pt/C) has many merits. Firstly, it can capture oxygen both in air and in acidic electrolyte. Compared with naked Pt/C, it is found that, in air, the oxygen concentration within the porous nest of NCM surrounding Pt/C particles is ~13 times higher than atmospheric oxygen concentration and, in acidic electrolyte, the concentration of activated oxygen over the catalyst NCM■ Pt/C rise to~1.9 times. Secondly, the NCM nest offers a special electronic modulation on Pt centers toward modified ORR kinetics and then catalytic performances. With these merits, compared with Pt/C, the NCM■ Pt/C catalyst shows 3.2 times higher turnover frequency value and 2.9 times enhanced specific activity for ORR with half-wave potential at 0.894 V. After 50,000 sweeping cycles, the NCM■ Pt/C catalyst retains~66% mass activity and still has advantages over the fresh Pt/C catalyst. We envision that the nest-type catalyst provides a new idea for progress of practical Pt/C ORR catalyst.
基金National Natural Science Foundation of China:No.11272152 and Aeronautical Science Foundation of China:No.20101552018.
文摘In this paper,a DG(Discontinuous Galerkin)method which has been widely employed in CFD(Computational Fluid Dynamics)is used to solve the twodimensional time-domain Maxwell’s equations for complex geometries on unstructured mesh.The element interfaces on solid boundary are treated in both curved way and straight way.Numerical tests are performed for both benchmark problems and complex cases with varying orders on a series of grids,where the high-order convergence in accuracy can be observed.Both the curved and the straight solid boundary implementation can give accurate RCS(Radar Cross-Section)results with sufficiently small mesh size,but the curved solid boundary implementation can significantly improve the accuracy when using relatively large mesh size.More importantly,this CFD-based high-order DG method for the Maxwell’s equations is very suitable for complex geometries.
文摘A new mechanism of catalyst has been demonstrated in this article. With the interaction between carbon nitride(CN) and encapsulated nickel, the CN in the catalyst has been endowed with new active sites for the adsorption and activation of hydrogen while nickel itself is physically isolated from the contact with reactive molecules. For the selective hydrogenation of acetylene in large amount of ethylene, the catalyst shows excellent ethylene selectivity than the nickel catalyst itself, which is almost totally unselective. Meanwhile, the CN itself is inactive for the reaction. The results of characterization demonstrate that pyridinic nitrogen doped in the carbon matrix should be the active sites for hydrogen dissociative adsorption. The theoretical calculations further confirm the results and provide with the detail in the electron transfer between nickel and CN in the catalyst. The current results supply a new concept for design of high performance catalyst.