The aerobic,selective oxidation of hydrocarbons via C-H bond activation is still a challenge.This work shows the achievement of the room temperature visible light driven photocatalytic activation of benzylic C-H bonds...The aerobic,selective oxidation of hydrocarbons via C-H bond activation is still a challenge.This work shows the achievement of the room temperature visible light driven photocatalytic activation of benzylic C-H bonds with N-hydroxysuccinimide over BiOBr_(x)I_(1-x)(0≤x≤1)solid solutions,whose valance bands were engineered through varying the ratio of bromide to iodide.The optimal BiOBr0.85I0.15 catalyst exhibited over 98%conversion ratio of ethylbenzene,which was about 3.9 and 8.9 times that of pure BiOBr and BiOI,respectively.The excellent photocatalytic activity of BiOBr0.85I0.15 solid solution can be ascribed to the orbital hybridization of the valence band containing both Br 4p and I 5p orbitals,which could promote photo-induced charge carrier separation and improve the generation of singlet oxygen.This work shed some light on the rational design of photocatalysts for targeted organic transformation.展开更多
I_(1)stacking faults(SFs)in Mg alloys are regarded as the nucleation sites of<c+a>dislocations that are critical for these alloys to achieve high ductility.Previously it was proposed that the formation of I_(1)S...I_(1)stacking faults(SFs)in Mg alloys are regarded as the nucleation sites of<c+a>dislocations that are critical for these alloys to achieve high ductility.Previously it was proposed that the formation of I_(1)SFs requires the accumulations of a large number of vacancies,which are difficult to achieve at low temperatures.In this study,molecular dynamics(MD)and molecular statics(MS)simulations based on empirical interatomic potentials were applied to investigate the deformation defect evolutions from the symmetric tilt grain boundaries(GBs)in Mg and Mg-Y alloys under external loading along<c>-axis.The results show the planar faults(PFs)on Pyramidal I planes first appear due to the nucleation and glide of(1/2 c+p)partial dislocations from GBs,where p=1/3(1010).These partial dislocations with pyramidal PFs interact with other defects,including pyramidal PFs themselves,GBs,and ppartial dislocations,generating a large amount of I_(1)SFs.Detailed analyses show the nucleation and growth of I_(1)SFs are achieved by atomic shuffle events and deformation defect reactions without the requirements of vacancy diffusion.Our simulations also suggest the Y clusters at GBs can reduce the critical stress for the formation of pyramidal PFs and I_(1)SFs,which provide a possible reason for the experimental observations that Y promotes the<c+a>dislocation activities.展开更多
Lead-free inorganic copper-silver-bismuth-halide materials have attracted more and more attention due to their environmental friendliness,high element abundance,and low cost.Here,we developed a strategy of one-step ga...Lead-free inorganic copper-silver-bismuth-halide materials have attracted more and more attention due to their environmental friendliness,high element abundance,and low cost.Here,we developed a strategy of one-step gas-solid-phase diffusioninduced reaction to fabricate a series of bandgap-tunable Cu_(a)Agm_(1)Bim_(2)I_(n)/CuI bilayer films due to the atomic diffusion effect for the first time.By designing and regulating the sputtered Cu/Ag/Bi metal film thickness,the bandgap of Cu_(a)Agm_(1)Bim_(2)I_(n)/CuI could be reduced from 2.06 to 1.78 eV.Solar cells with the structure of FTO/TiO_(2)/Cu_(a)Agm_(1)Bim_(2)I_(n)/CuI/carbon were constructed,yielding a champion power conversion efficiency of 2.76%,which is the highest reported for this class of materials owing to the bandgap reduction and the peculiar bilayer structure.The current work provides a practical path for developing the next generation of efficient,stable,and environmentally friendly photovoltaic materials.展开更多
Single-atomic-layer-height disconnections that connect with I1stacking faults are produced on{1011}twin boundaries in pure magnesium through transmutation of basalmixed dislocations across the twin boundaries,and thei...Single-atomic-layer-height disconnections that connect with I1stacking faults are produced on{1011}twin boundaries in pure magnesium through transmutation of basalmixed dislocations across the twin boundaries,and their stabilities are examined using molecular dynamics simulations.The stable configuration for a single-atomic-layer-height disconnection is a pyramidal-basal(PyB)disconnection connecting an I1fault associated with a stacking sequence change of ABACA,or a basal-pyramidal(BPy)disconnection connecting an I_(1)fault associated with a stacking sequence change of BABCB.A stable single-atomic-layer-height disconnection can transform to a less stable single-atomiclayer-height disconnection when its step orientation changes solely.A stable single-atomic-layer-height disconnection can also transform to another stable single-atomic-layer-height disconnection,when the step orientation of the disconnection and the type of the I_(1)fault that connects with the disconnection change synchronously,and this process is accompanied with the emission of a Shockley partial dislocation from the twin boundary.展开更多
基金supported by the National Natural Science Foundation of China(No.21671176)Post-doctoral Foundation of Henan。
文摘The aerobic,selective oxidation of hydrocarbons via C-H bond activation is still a challenge.This work shows the achievement of the room temperature visible light driven photocatalytic activation of benzylic C-H bonds with N-hydroxysuccinimide over BiOBr_(x)I_(1-x)(0≤x≤1)solid solutions,whose valance bands were engineered through varying the ratio of bromide to iodide.The optimal BiOBr0.85I0.15 catalyst exhibited over 98%conversion ratio of ethylbenzene,which was about 3.9 and 8.9 times that of pure BiOBr and BiOI,respectively.The excellent photocatalytic activity of BiOBr0.85I0.15 solid solution can be ascribed to the orbital hybridization of the valence band containing both Br 4p and I 5p orbitals,which could promote photo-induced charge carrier separation and improve the generation of singlet oxygen.This work shed some light on the rational design of photocatalysts for targeted organic transformation.
基金supported by the U.S.Department of Energy,Office of Basic Energy Sciences,Division of Materials Sciences and Engineering under Award DE-SC0008637 as part of the Center for PRedictive Integrated Structural Materials Science(PRISMS Center)at University of Michigan。
文摘I_(1)stacking faults(SFs)in Mg alloys are regarded as the nucleation sites of<c+a>dislocations that are critical for these alloys to achieve high ductility.Previously it was proposed that the formation of I_(1)SFs requires the accumulations of a large number of vacancies,which are difficult to achieve at low temperatures.In this study,molecular dynamics(MD)and molecular statics(MS)simulations based on empirical interatomic potentials were applied to investigate the deformation defect evolutions from the symmetric tilt grain boundaries(GBs)in Mg and Mg-Y alloys under external loading along<c>-axis.The results show the planar faults(PFs)on Pyramidal I planes first appear due to the nucleation and glide of(1/2 c+p)partial dislocations from GBs,where p=1/3(1010).These partial dislocations with pyramidal PFs interact with other defects,including pyramidal PFs themselves,GBs,and ppartial dislocations,generating a large amount of I_(1)SFs.Detailed analyses show the nucleation and growth of I_(1)SFs are achieved by atomic shuffle events and deformation defect reactions without the requirements of vacancy diffusion.Our simulations also suggest the Y clusters at GBs can reduce the critical stress for the formation of pyramidal PFs and I_(1)SFs,which provide a possible reason for the experimental observations that Y promotes the<c+a>dislocation activities.
基金supported by National Natural Science Foundation of China(Grant No.52072327,62074052,61874159)Zhongyuan Thousand Talents(Zhongyuan Scholars)Program of Henan Province(202101510004)+6 种基金Higher Education and Teaching Reformation Project(2014SJGLX064)Academic Degrees&Graduate Education Reform Project of Henan Province(2021SJGLX060Y)Key research and development projects of Universities in Henan Province(20A140026)the Scientific Research Innovation Team of Xuchang University(2022CXTD008)Science and Technology Project of Henan Province(222102230009).L.Ding thanks the National Key Research and Development Program of China(2022YFB3803300)the open research fund of Songshan Lake Materials Laboratory(2021SLABFK02)the National Natural Science Foundation of China(21961160720).
文摘Lead-free inorganic copper-silver-bismuth-halide materials have attracted more and more attention due to their environmental friendliness,high element abundance,and low cost.Here,we developed a strategy of one-step gas-solid-phase diffusioninduced reaction to fabricate a series of bandgap-tunable Cu_(a)Agm_(1)Bim_(2)I_(n)/CuI bilayer films due to the atomic diffusion effect for the first time.By designing and regulating the sputtered Cu/Ag/Bi metal film thickness,the bandgap of Cu_(a)Agm_(1)Bim_(2)I_(n)/CuI could be reduced from 2.06 to 1.78 eV.Solar cells with the structure of FTO/TiO_(2)/Cu_(a)Agm_(1)Bim_(2)I_(n)/CuI/carbon were constructed,yielding a champion power conversion efficiency of 2.76%,which is the highest reported for this class of materials owing to the bandgap reduction and the peculiar bilayer structure.The current work provides a practical path for developing the next generation of efficient,stable,and environmentally friendly photovoltaic materials.
文摘Single-atomic-layer-height disconnections that connect with I1stacking faults are produced on{1011}twin boundaries in pure magnesium through transmutation of basalmixed dislocations across the twin boundaries,and their stabilities are examined using molecular dynamics simulations.The stable configuration for a single-atomic-layer-height disconnection is a pyramidal-basal(PyB)disconnection connecting an I1fault associated with a stacking sequence change of ABACA,or a basal-pyramidal(BPy)disconnection connecting an I_(1)fault associated with a stacking sequence change of BABCB.A stable single-atomic-layer-height disconnection can transform to a less stable single-atomiclayer-height disconnection when its step orientation changes solely.A stable single-atomic-layer-height disconnection can also transform to another stable single-atomic-layer-height disconnection,when the step orientation of the disconnection and the type of the I_(1)fault that connects with the disconnection change synchronously,and this process is accompanied with the emission of a Shockley partial dislocation from the twin boundary.
