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
The production of renewable fuels through water splitting via photocatalytic hydrogen production holds significant promise.Nonetheless,the sluggish kinetics of hydrogen evolution and the inadequate water adsorption on...The production of renewable fuels through water splitting via photocatalytic hydrogen production holds significant promise.Nonetheless,the sluggish kinetics of hydrogen evolution and the inadequate water adsorption on photocatalysts present notable challenges.In this study,we have devised a straightforward hydrothermal method to synthesize Bi_(2)O_(3)(BO)derived from metal‐organic frameworks(MOFs),loaded with flower-like ZnIn_(2)S_(4)(ZIS).This approach substantially enhances water adsorption and surface catalytic reactions,resulting in a remarkable enhancement of photocatalytic activity.By employing triethanolamine(TEOA)as a sacrificial agent,the hydrogen evolution rate achieved with 15%(mass fraction)ZIS loading on BO reached an impressive value of 1610μmol∙h^(−1)∙g^(−1),marking a 6.34-fold increase compared to that observed for bare BO.Furthermore,through density functional theory(DFT)and ab initio molecular dynamics(AIMD)calculations,we have identified the reactions occurring at the ZIS/BO S-scheme heterojunction interface,including the identification of active sites for water adsorption and catalytic reactions.This study provides valuable insights into the development of high-performance composite photocatalytic materials with tailored electronic properties and wettability.展开更多
By combination of the transient Raman spectroscopic measurement and the density functional theoretical calculations,the structural evolution and stability of TATB under shock compression was investigated.Due to the im...By combination of the transient Raman spectroscopic measurement and the density functional theoretical calculations,the structural evolution and stability of TATB under shock compression was investigated.Due to the improvement in synchronization control between two-stage light gas gun and the transient Raman spectra acquisition,as well as the sample preparation,the Raman peak of the N-O mode of TATB was firstly observed under shock pressure up to 13.6 GPa,noticeably higher than the upper limit of 8.5 GPa reported in available literatures.By taking into account of the continuous shift of the main peak and other observed Raman peaks,we did not distinguish any structural transition or any new species.Moreover,both the present Raman spectra and the time-resolved radiation of TATB during shock loading showed that TATB exhibits higher chemical stability than previous declaration.To reveal the detailed structural response and evolution of TATB under compression,the density functional theoretical calculations were conducted,and it was found that the pressure make N-O bond lengths shorter,nitro bond angles larger,and intermolecular and intra-molecular hydrogen bond interactions enhanced.The observed red shift of Raman peak was ascribed to the abnormal enhancement of H-bound effect on the scissor vibration mode of the nitro group.展开更多
Cubic boron nitride(CBN) micro powders and mixture of CBN micro powders with Al or Ti powders were fast heated at 1 300,1 400,1 450,1 500℃,and then kept for 5 min under spark plasma sintering (SPS).The obtained powde...Cubic boron nitride(CBN) micro powders and mixture of CBN micro powders with Al or Ti powders were fast heated at 1 300,1 400,1 450,1 500℃,and then kept for 5 min under spark plasma sintering (SPS).The obtained powders were analyzed with XRD.The results show that,simple CBN kept cubic structure after heated at 1 300℃;when the temperature rose to 1 400℃,some CBN was transformed into hexagonal structured boron nitride(hBN).As for CBN micro powders mixed with aluminum or titanium micro powders,the onset transforming temperature of CBN to hBN get raised.This results indicated that the structural transformation of boron nitride begun from the surface of CBN crystal particle,different coexist elements affect the surface situation of CBN particles.As the stabilities of CBN crystal particle surface improved,the onset structural transform temperature of CBN was also increased.展开更多
This paper presents an application of a metapopulation model structured in classes for the study of population evolution of a network of schools.The global dynamics are considered in two parts,the local,where the evol...This paper presents an application of a metapopulation model structured in classes for the study of population evolution of a network of schools.The global dynamics are considered in two parts,the local,where the evolution for each grade in a cycle is accounted,and the metapopulation or the movement of students between schools.Simulation of the model is presented.展开更多
Prior to the collision and accretion of the Kohistan arc terrane during the late Cretaceous and the Indian plate after the early Eocene, the southern margin of Asia along the Hindu Kush, Karakoram and Lhasa block terr...Prior to the collision and accretion of the Kohistan arc terrane during the late Cretaceous and the Indian plate after the early Eocene, the southern margin of Asia along the Hindu Kush, Karakoram and Lhasa block terranes was an active Andean\|type continental margin. In south Tibet this margin was dominated by the calc\|alkaline Ladakh—Gangdese granite batholith, associated andesitic volcanic rocks and continental red\|beds. In contrast, the southern Karakoram exposes deep crustal metamorphic rocks and crustal melt leucogranites. New U\|Pb age dating from the Hunza valley and Baltoro glacier region has revealed four spatially and temporally distinct metamorphic episodes. M1 sillimanite grade metamorphism in Hunza was a late Cretaceous event, probably caused by the accretion of the Kohistan arc to Asia. M2 was the major kyanite and sillimanite grade event during late Eocene—Oligocene crustal thickening and shortening, following India\|Asia collision. Numerous melting events resulted in the formation of crustal melt granites throughout the last 50Ma with multiple generations of dykes and very large scale crustal melting along the Baltoro monzogranite\|leucogranite ba tholith during the late Oligocene—early Miocene. M3 metamorphism was a high\| T , low\| p contact thermal metamorphism around the Baltoro granite. In Hunza, younger staurolite grade metamorphism has been dated by U\|Pb monazites at 16Ma, with the Sumayar leucogranite intruded at 9 5Ma cross\|cutting the metamorphic isograds. In the Baltoro region the youngest metamorphism, M4, is the sillimanite grade Dassu gneiss core complex dated by U\|Pb on monazites as late Miocene—Pliocene (5 4±0 25)Ma with Precambrian protolith zircon cores (1855±11)Ma. Numerous gem\|bearing pegmatite dykes cross\|cut these rocks and are thought to have been intruded within the last 2～3Ma. Structural mapping, combined with U\|Pb geochronology shows that major metamorphic events can be both long\|lasting (up to 20Ma) and very restrictive, both in time and space.展开更多
Qaidam basin is located at northeast Qinghai—Xizang (Tibet) plateau, and surrounded by east Kunlun, south Qilian and Altun mountain systems. The purpose of this paper is to study the Cenozoic basin evolutionary stage...Qaidam basin is located at northeast Qinghai—Xizang (Tibet) plateau, and surrounded by east Kunlun, south Qilian and Altun mountain systems. The purpose of this paper is to study the Cenozoic basin evolutionary stages, structural styles of the Qaidam, and the denudation in adjacent mountain systems through seismic profile interpretation and complemented by field observation. The Qaidam basin has experienced two tectonic stages of Paleogene—early Miocene (65～12Ma) and late Miocene—present (12～0Ma). The former is characterized by differential uplift of the mountains and subsidence of the basin, and the latter by intense compression, wrench, thrusting and folding. The compressional structural styles are mainly distributed in the Circle Hero—Range Depression of southwest Qaidam, such as Nanyishan, Youquanzi, Younan, Youshashan anticline belts and thrust faults. The wrench structural styles of the northern Qaidam include en echelon uplifts (fault—block outcrops) such as Seshitengshan, Luliangshan, Xitieshan and Eimnikshan, which are mainly composed of pre\|Sinian and Paleozoic rocks; en echelon anticlines such as Lenghu—Nanbaxian belts; and en echelon depressions such as Kunteyi, Senan and Yibei depressions, which are mainly composed of Mesozoic and Cenozoic rocks.展开更多
The exploration of stable and highly efficient alkaline hydrogen evolution reaction(HER)electrocatalysts is imperative for alkaline water splitting.Herein,Se-doped NiCoP with hierarchical nanoarray structures directly...The exploration of stable and highly efficient alkaline hydrogen evolution reaction(HER)electrocatalysts is imperative for alkaline water splitting.Herein,Se-doped NiCoP with hierarchical nanoarray structures directly grown on carbon cloth(Se-NiCoP/CC)was prepared by hydrothermal reaction and phosphorization/selenization process.The experimental results reveal that Se doping could increase the electrochemical active sites and alter the electronic structure of NiCoP.The optimized Se-NiCoP/CC electrode exhibits outstanding HER activity in alkaline electrolyte,which only needs a low overpotential of 79 mV at the current density of 10 mA/cm^(2).When serving as anode and cathode electrode simultaneously,the Se-NiCoP/CC electrodes achieve current density of 50 mA/cm^(2) at a low voltage of only 1.62 V.This work provides a feasible way to rationally design high active HER electrocatalysts.展开更多
Resistance genes enable plants to fight against plant pathogens. Plant resistance genes （R gene） are organized complexly in genome. Some resistance gene sequence data enable an insight into R gene structure and gene...Resistance genes enable plants to fight against plant pathogens. Plant resistance genes （R gene） are organized complexly in genome. Some resistance gene sequence data enable an insight into R gene structure and gene evolution. Some sites like Leucine-Rich Repeat （LRR） are of specific interest since homologous recombination can happen. Crossing over, transposon insertion and excision and mutation can produce new specificity. Three models explaining R gene evolution were discussed. More information needed for dissection of R gene evolution though some step can be inferred from genetic and sequence analysis.展开更多
Gossypium hirsutum,the most widely planted cotton species,its evolution has long been an unsolved puzzle because of its hybrid origin from D-genome and A-genome species.To better understand the genetic component of co...Gossypium hirsutum,the most widely planted cotton species,its evolution has long been an unsolved puzzle because of its hybrid origin from D-genome and A-genome species.To better understand the genetic component of cotton,Huang et al.recently sequenced and assembled the first A1-genome G.herbaceum,and updated the A2-genome G.arboreum and(AD)1-genome G.hirsutum.On the basis of the three reference genomes,they resolved existing controversial concepts and provided novel evolutionary insights surrounding the A-genome.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.
文摘The production of renewable fuels through water splitting via photocatalytic hydrogen production holds significant promise.Nonetheless,the sluggish kinetics of hydrogen evolution and the inadequate water adsorption on photocatalysts present notable challenges.In this study,we have devised a straightforward hydrothermal method to synthesize Bi_(2)O_(3)(BO)derived from metal‐organic frameworks(MOFs),loaded with flower-like ZnIn_(2)S_(4)(ZIS).This approach substantially enhances water adsorption and surface catalytic reactions,resulting in a remarkable enhancement of photocatalytic activity.By employing triethanolamine(TEOA)as a sacrificial agent,the hydrogen evolution rate achieved with 15%(mass fraction)ZIS loading on BO reached an impressive value of 1610μmol∙h^(−1)∙g^(−1),marking a 6.34-fold increase compared to that observed for bare BO.Furthermore,through density functional theory(DFT)and ab initio molecular dynamics(AIMD)calculations,we have identified the reactions occurring at the ZIS/BO S-scheme heterojunction interface,including the identification of active sites for water adsorption and catalytic reactions.This study provides valuable insights into the development of high-performance composite photocatalytic materials with tailored electronic properties and wettability.
基金supported by the National Natural Science Foundation of China(Grant Nos.12072299,11902276)the Natural Science Foundation of Sichuan Province(Grant No.2022NSFSC1802)+1 种基金the Basic Research Project of Southwest Jiaotong University(Grant No.2682023ZTPY009)the National Key Laboratory for Shock Wave and Detonation Physics of China(Grant No.JCKYS2019212007)。
文摘By combination of the transient Raman spectroscopic measurement and the density functional theoretical calculations,the structural evolution and stability of TATB under shock compression was investigated.Due to the improvement in synchronization control between two-stage light gas gun and the transient Raman spectra acquisition,as well as the sample preparation,the Raman peak of the N-O mode of TATB was firstly observed under shock pressure up to 13.6 GPa,noticeably higher than the upper limit of 8.5 GPa reported in available literatures.By taking into account of the continuous shift of the main peak and other observed Raman peaks,we did not distinguish any structural transition or any new species.Moreover,both the present Raman spectra and the time-resolved radiation of TATB during shock loading showed that TATB exhibits higher chemical stability than previous declaration.To reveal the detailed structural response and evolution of TATB under compression,the density functional theoretical calculations were conducted,and it was found that the pressure make N-O bond lengths shorter,nitro bond angles larger,and intermolecular and intra-molecular hydrogen bond interactions enhanced.The observed red shift of Raman peak was ascribed to the abnormal enhancement of H-bound effect on the scissor vibration mode of the nitro group.
基金support provided by Natural Science Foundation of Hebei Province(No.E 2006000226)
文摘Cubic boron nitride(CBN) micro powders and mixture of CBN micro powders with Al or Ti powders were fast heated at 1 300,1 400,1 450,1 500℃,and then kept for 5 min under spark plasma sintering (SPS).The obtained powders were analyzed with XRD.The results show that,simple CBN kept cubic structure after heated at 1 300℃;when the temperature rose to 1 400℃,some CBN was transformed into hexagonal structured boron nitride(hBN).As for CBN micro powders mixed with aluminum or titanium micro powders,the onset transforming temperature of CBN to hBN get raised.This results indicated that the structural transformation of boron nitride begun from the surface of CBN crystal particle,different coexist elements affect the surface situation of CBN particles.As the stabilities of CBN crystal particle surface improved,the onset structural transform temperature of CBN was also increased.
文摘This paper presents an application of a metapopulation model structured in classes for the study of population evolution of a network of schools.The global dynamics are considered in two parts,the local,where the evolution for each grade in a cycle is accounted,and the metapopulation or the movement of students between schools.Simulation of the model is presented.
文摘Prior to the collision and accretion of the Kohistan arc terrane during the late Cretaceous and the Indian plate after the early Eocene, the southern margin of Asia along the Hindu Kush, Karakoram and Lhasa block terranes was an active Andean\|type continental margin. In south Tibet this margin was dominated by the calc\|alkaline Ladakh—Gangdese granite batholith, associated andesitic volcanic rocks and continental red\|beds. In contrast, the southern Karakoram exposes deep crustal metamorphic rocks and crustal melt leucogranites. New U\|Pb age dating from the Hunza valley and Baltoro glacier region has revealed four spatially and temporally distinct metamorphic episodes. M1 sillimanite grade metamorphism in Hunza was a late Cretaceous event, probably caused by the accretion of the Kohistan arc to Asia. M2 was the major kyanite and sillimanite grade event during late Eocene—Oligocene crustal thickening and shortening, following India\|Asia collision. Numerous melting events resulted in the formation of crustal melt granites throughout the last 50Ma with multiple generations of dykes and very large scale crustal melting along the Baltoro monzogranite\|leucogranite ba tholith during the late Oligocene—early Miocene. M3 metamorphism was a high\| T , low\| p contact thermal metamorphism around the Baltoro granite. In Hunza, younger staurolite grade metamorphism has been dated by U\|Pb monazites at 16Ma, with the Sumayar leucogranite intruded at 9 5Ma cross\|cutting the metamorphic isograds. In the Baltoro region the youngest metamorphism, M4, is the sillimanite grade Dassu gneiss core complex dated by U\|Pb on monazites as late Miocene—Pliocene (5 4±0 25)Ma with Precambrian protolith zircon cores (1855±11)Ma. Numerous gem\|bearing pegmatite dykes cross\|cut these rocks and are thought to have been intruded within the last 2～3Ma. Structural mapping, combined with U\|Pb geochronology shows that major metamorphic events can be both long\|lasting (up to 20Ma) and very restrictive, both in time and space.
文摘Qaidam basin is located at northeast Qinghai—Xizang (Tibet) plateau, and surrounded by east Kunlun, south Qilian and Altun mountain systems. The purpose of this paper is to study the Cenozoic basin evolutionary stages, structural styles of the Qaidam, and the denudation in adjacent mountain systems through seismic profile interpretation and complemented by field observation. The Qaidam basin has experienced two tectonic stages of Paleogene—early Miocene (65～12Ma) and late Miocene—present (12～0Ma). The former is characterized by differential uplift of the mountains and subsidence of the basin, and the latter by intense compression, wrench, thrusting and folding. The compressional structural styles are mainly distributed in the Circle Hero—Range Depression of southwest Qaidam, such as Nanyishan, Youquanzi, Younan, Youshashan anticline belts and thrust faults. The wrench structural styles of the northern Qaidam include en echelon uplifts (fault—block outcrops) such as Seshitengshan, Luliangshan, Xitieshan and Eimnikshan, which are mainly composed of pre\|Sinian and Paleozoic rocks; en echelon anticlines such as Lenghu—Nanbaxian belts; and en echelon depressions such as Kunteyi, Senan and Yibei depressions, which are mainly composed of Mesozoic and Cenozoic rocks.
基金Projects(51772086,51872087,51971089)supported by the National Natural Science Foundation of ChinaProject(2018TP1037-202102)supported by Open Fund of Hunan Provincial Key Laboratory of Advanced Materials for New Energy Storage and Conversion,China+1 种基金Project supported by Student National SIT Innovation Program,ChinaProject(2020CB1007)supported by Hunan Joint International Laboratory of Advanced Materials and Technology for Clean Energy,China。
文摘The exploration of stable and highly efficient alkaline hydrogen evolution reaction(HER)electrocatalysts is imperative for alkaline water splitting.Herein,Se-doped NiCoP with hierarchical nanoarray structures directly grown on carbon cloth(Se-NiCoP/CC)was prepared by hydrothermal reaction and phosphorization/selenization process.The experimental results reveal that Se doping could increase the electrochemical active sites and alter the electronic structure of NiCoP.The optimized Se-NiCoP/CC electrode exhibits outstanding HER activity in alkaline electrolyte,which only needs a low overpotential of 79 mV at the current density of 10 mA/cm^(2).When serving as anode and cathode electrode simultaneously,the Se-NiCoP/CC electrodes achieve current density of 50 mA/cm^(2) at a low voltage of only 1.62 V.This work provides a feasible way to rationally design high active HER electrocatalysts.
文摘Resistance genes enable plants to fight against plant pathogens. Plant resistance genes （R gene） are organized complexly in genome. Some resistance gene sequence data enable an insight into R gene structure and gene evolution. Some sites like Leucine-Rich Repeat （LRR） are of specific interest since homologous recombination can happen. Crossing over, transposon insertion and excision and mutation can produce new specificity. Three models explaining R gene evolution were discussed. More information needed for dissection of R gene evolution though some step can be inferred from genetic and sequence analysis.
文摘Gossypium hirsutum,the most widely planted cotton species,its evolution has long been an unsolved puzzle because of its hybrid origin from D-genome and A-genome species.To better understand the genetic component of cotton,Huang et al.recently sequenced and assembled the first A1-genome G.herbaceum,and updated the A2-genome G.arboreum and(AD)1-genome G.hirsutum.On the basis of the three reference genomes,they resolved existing controversial concepts and provided novel evolutionary insights surrounding the A-genome.
