Small cluster and periodic surface models with low coverages of intermediates are frequently employed to investigate reaction mechanisms and identify active sites on nanoparticles(NPs)in density functional theory(DFT)...Small cluster and periodic surface models with low coverages of intermediates are frequently employed to investigate reaction mechanisms and identify active sites on nanoparticles(NPs)in density functional theory(DFT)studies.However,diverse active sites on NPs cannot be sufficiently represented by these simple models,hampering the in-depth insights into the catalytic behavior of NPs.This paper describes the crucial roles of both model and coverage effect on understanding the nature of active sites for CO_(2)reduction over Au and Pd NPs using DFT calculations.Terrace sites exhibit higher selectivity for CO than edge sites on Au NPs,which is opposite to the results on Au periodic surfaces.This contradiction reveals the computational model effect on clarifying active site properties.For Pd catalysts,the coverage effect is more significant.On bare Pd NPs and periodic surfaces,the selectivity for CO at edge sites is nearly identical to that at terrace sites,whereas edge sites display higher selectivity for CO than terrace sites in the case of high CO coverages.Through considering the more realistic models and the coverage effect,we successfully describe the size effect of Au and Pd NPs on CO selectivity.More importantly,this work reminds us of the necessity of reasonable models in DFT calculations.展开更多
Undercooling solidification under a magnetic field(UMF)is an effective way to tailor the microstructure and properties of Co-based alloys.In this study,by attributing to the UMF treatment,the strength−ductility trade-...Undercooling solidification under a magnetic field(UMF)is an effective way to tailor the microstructure and properties of Co-based alloys.In this study,by attributing to the UMF treatment,the strength−ductility trade-off dilemma in GH605 superalloy is successfully overcome.The UMF treatment can effectively refine the grains and increase the solid solubility,leading to the high yield strength.The main deformation mechanism in the as-forged alloy is dislocation slipping.By contrast,multiple deformation mechanisms,including stacking faults,twining,dislocation slipping,and their strong interactions are activated in the UMF-treated sample during compression deformation,which enhances the strength and ductility simultaneously.In addition,the precipitation of hard Laves phases along the grain boundaries can be obtained after UMF treatment,hindering crack propagation during compression deformation.展开更多
文摘Small cluster and periodic surface models with low coverages of intermediates are frequently employed to investigate reaction mechanisms and identify active sites on nanoparticles(NPs)in density functional theory(DFT)studies.However,diverse active sites on NPs cannot be sufficiently represented by these simple models,hampering the in-depth insights into the catalytic behavior of NPs.This paper describes the crucial roles of both model and coverage effect on understanding the nature of active sites for CO_(2)reduction over Au and Pd NPs using DFT calculations.Terrace sites exhibit higher selectivity for CO than edge sites on Au NPs,which is opposite to the results on Au periodic surfaces.This contradiction reveals the computational model effect on clarifying active site properties.For Pd catalysts,the coverage effect is more significant.On bare Pd NPs and periodic surfaces,the selectivity for CO at edge sites is nearly identical to that at terrace sites,whereas edge sites display higher selectivity for CO than terrace sites in the case of high CO coverages.Through considering the more realistic models and the coverage effect,we successfully describe the size effect of Au and Pd NPs on CO selectivity.More importantly,this work reminds us of the necessity of reasonable models in DFT calculations.
基金the fund of National Key Laboratory for Precision Hot Processing of Metals,China(No.6142909200104)State Key Laboratory of Solidification Processing(NPU),China(No.2022-TS-08)National Training Program of Innovation and Entrepreneurship for Undergraduates.We thank Dr.ZHENG from ZKKF(Beijing)Science&Technology Company for supporting the characterization of the materials.
文摘Undercooling solidification under a magnetic field(UMF)is an effective way to tailor the microstructure and properties of Co-based alloys.In this study,by attributing to the UMF treatment,the strength−ductility trade-off dilemma in GH605 superalloy is successfully overcome.The UMF treatment can effectively refine the grains and increase the solid solubility,leading to the high yield strength.The main deformation mechanism in the as-forged alloy is dislocation slipping.By contrast,multiple deformation mechanisms,including stacking faults,twining,dislocation slipping,and their strong interactions are activated in the UMF-treated sample during compression deformation,which enhances the strength and ductility simultaneously.In addition,the precipitation of hard Laves phases along the grain boundaries can be obtained after UMF treatment,hindering crack propagation during compression deformation.
