Coincidence Momentum Imaging(CMI) is a powerful imaging technique that can determine the full momentum vectors of all particles released from a single parent molecule in coincidence and thus provide detailed informati...Coincidence Momentum Imaging(CMI) is a powerful imaging technique that can determine the full momentum vectors of all particles released from a single parent molecule in coincidence and thus provide detailed information on transient molecular structures.So far,the CMI technique has been extensively employed for investigating a variety of molecular reaction dynamics induced,e.g.,by particle collisions,intense laser fields and synchrotron radiation.In this article,we first introduce the principle of the CMI technique,which is followed by several typical experimental designs of the CMI systems realizing the coincidence momentum detections.We then present representative examples of studying molecular reaction dynamics using the CMI technique.展开更多
Hexanuclear ruthenium cluster compound Ru<sub>6</sub>C （CO）<sub>17</sub> has interesting activity in the gase-phase. The ion-molecular reaction of Ru<sub>6</sub>C （CO）<sub>...Hexanuclear ruthenium cluster compound Ru<sub>6</sub>C （CO）<sub>17</sub> has interesting activity in the gase-phase. The ion-molecular reaction of Ru<sub>6</sub>C （CO）<sub>17</sub> with triphcnylphosphine was investigated by EI-MS. The experimental results showed that Ru<sub>6</sub>C （CO）<sub>17</sub> could undergo the ligand substitution by PPh<sub>2</sub> or PPh<sub>3</sub> to initially yield monosubstituted product [Ru<sub>6</sub>C（CO）<sub>16</sub>PPh<sub>2</sub>]<sup>+</sup> or [Ru<sub>6</sub>C （CO）<sub>16</sub>PPh<sub>3</sub>]<sup>+</sup>.展开更多
This work presents a new science called atomic and molecular reaction statics (AMRS). There are four parts for AMRS, i.e. the group theoretical derivation of mo- lecular electronic states, the principle of microscopic...This work presents a new science called atomic and molecular reaction statics (AMRS). There are four parts for AMRS, i.e. the group theoretical derivation of mo- lecular electronic states, the principle of microscopic reversibility, the principle of microscopic transitivity and the optimum energy process rule. AMRS has been developed for about twenty years.展开更多
The effect of coatings(Y_2O_3, Zr O_2 and Al_2O_3) on the interfacial reaction of Ti Al alloys was studied with molecular dynamics. The binding energy of coatings and the diffusion process of oxygen in the melt were s...The effect of coatings(Y_2O_3, Zr O_2 and Al_2O_3) on the interfacial reaction of Ti Al alloys was studied with molecular dynamics. The binding energy of coatings and the diffusion process of oxygen in the melt were simulated, and then the simulation results were compared with the experimental results. The simulation results indicate that for each of the three simulated coatings, inordinate interfacial reactions have occurred between the coating and the melt. The binding energy results show that Y_2O_3 has the best stability and is the most difficult to break down. Zr O_2 has the greatest decomposition energy and is the easiest to break down in the melt. Besides, the molecular dynamics indicate that the diffusion coefficient of the oxygen atom in Al_2O_3 is larger than that in the other two coatings, indicating that oxygen diffusion in Al_2O_3 is the fastest at a given temperature. The experimental results show that the oxygen concentration of the melt with Al_2O_3 coating is the highest, and the oxygen diffusion is of similar magnitude to the simulation values, from which the conclusion can be obtained that the oxygen concentration is significantly influenced by the coating materials.展开更多
The microscopic moleeular theory for electron transfer in a model solvent ishahr developed. The nonlinear response of the solvent molecules is be computedquanitatively in a new way. Adopting computer simulation daa an...The microscopic moleeular theory for electron transfer in a model solvent ishahr developed. The nonlinear response of the solvent molecules is be computedquanitatively in a new way. Adopting computer simulation daa and choosingappropriate reaction coordinae, a reasonable free energy dinram is constructed and thercorganhaion energy for the product state is calculated.展开更多
The vinylidene-bridged cluster μ_3-FcCHCFeCo_2(CO)_9 2 was prepared by the expansionreaction of ferrocenyl-acetylene dicobalt complex μ-FcCCHCo_2(CO)_6 1. Benzylideneacetone-tricarbonyliron [(BDA)Fe(CO)_3] was used ...The vinylidene-bridged cluster μ_3-FcCHCFeCo_2(CO)_9 2 was prepared by the expansionreaction of ferrocenyl-acetylene dicobalt complex μ-FcCCHCo_2(CO)_6 1. Benzylideneacetone-tricarbonyliron [(BDA)Fe(CO)_3] was used as the source of Fe(CO)_3. The molecular structure of thecluster 2 was detendned by x-ray structural analysis.展开更多
A Molecular Dynamics (MD) simulation with Tersoff empirical many-bodypotential has been employed to investigate the growth processes of diamond film with energeticspecies deposition. In the present study, we have stud...A Molecular Dynamics (MD) simulation with Tersoff empirical many-bodypotential has been employed to investigate the growth processes of diamond film with energeticspecies deposition. In the present study, we have studied the reaction probabilities of energeticspecies with energies of 0.1 e V to 10eV at the substrate temperature of 1100K. In the cases of thediamond growth on the surface with H passivation, the reaction probability of hydrocarbon speciesconsiderably increases when the species energy is higher than 2eV. This means that the diamond filmcan grow in the case of high incident species energy without the process of hydrogen abstraction,which is needed in the case of incident species with low energy. The reaction mechanism of energeticspecies on hydrogen passivated diamond surface is also discussed.展开更多
Ethane steam cracking process in an industrial reactor was investigated.An one-demsional(1D)steady-state model was developed firstly by using an improved molecular reaction scheme and was then simulated in Aspen Plus....Ethane steam cracking process in an industrial reactor was investigated.An one-demsional(1D)steady-state model was developed firstly by using an improved molecular reaction scheme and was then simulated in Aspen Plus.A comparison of model results with industrial data and previously reported results showed that the model can predict the process kinetics more accurately.In addition,the validated model was used to study the effects of different process variables,including coil outlet temperature(COT),steam-to-ethane ratio and residence time on ethane conversion,ethylene selectivity,products yields,and coking rate.Finally,steady-state optimization was conducted to the operation of industrial reactor.The COT and steam-to-ethane ratio were taken as decision variables to maximize the annual operational profit.展开更多
基金Sponsored by the National Natural Science Foundation of China(Grant Nos.61625501 and 61427816)Open Fund of the State Key Laboratory of High Field Laser Physics(SIOM)Fundamental Research Funds for the Central Universities
文摘Coincidence Momentum Imaging(CMI) is a powerful imaging technique that can determine the full momentum vectors of all particles released from a single parent molecule in coincidence and thus provide detailed information on transient molecular structures.So far,the CMI technique has been extensively employed for investigating a variety of molecular reaction dynamics induced,e.g.,by particle collisions,intense laser fields and synchrotron radiation.In this article,we first introduce the principle of the CMI technique,which is followed by several typical experimental designs of the CMI systems realizing the coincidence momentum detections.We then present representative examples of studying molecular reaction dynamics using the CMI technique.
基金This work was supported by Fujian Natural Science Found
文摘Hexanuclear ruthenium cluster compound Ru<sub>6</sub>C （CO）<sub>17</sub> has interesting activity in the gase-phase. The ion-molecular reaction of Ru<sub>6</sub>C （CO）<sub>17</sub> with triphcnylphosphine was investigated by EI-MS. The experimental results showed that Ru<sub>6</sub>C （CO）<sub>17</sub> could undergo the ligand substitution by PPh<sub>2</sub> or PPh<sub>3</sub> to initially yield monosubstituted product [Ru<sub>6</sub>C（CO）<sub>16</sub>PPh<sub>2</sub>]<sup>+</sup> or [Ru<sub>6</sub>C （CO）<sub>16</sub>PPh<sub>3</sub>]<sup>+</sup>.
文摘This work presents a new science called atomic and molecular reaction statics (AMRS). There are four parts for AMRS, i.e. the group theoretical derivation of mo- lecular electronic states, the principle of microscopic reversibility, the principle of microscopic transitivity and the optimum energy process rule. AMRS has been developed for about twenty years.
基金financially supported by the National Natural Science Foundation of China(No.51304198)the Natural Science Foundation of Jiangsu Province,China(Nos.2013106,20141134 and 2014028-08)
文摘The effect of coatings(Y_2O_3, Zr O_2 and Al_2O_3) on the interfacial reaction of Ti Al alloys was studied with molecular dynamics. The binding energy of coatings and the diffusion process of oxygen in the melt were simulated, and then the simulation results were compared with the experimental results. The simulation results indicate that for each of the three simulated coatings, inordinate interfacial reactions have occurred between the coating and the melt. The binding energy results show that Y_2O_3 has the best stability and is the most difficult to break down. Zr O_2 has the greatest decomposition energy and is the easiest to break down in the melt. Besides, the molecular dynamics indicate that the diffusion coefficient of the oxygen atom in Al_2O_3 is larger than that in the other two coatings, indicating that oxygen diffusion in Al_2O_3 is the fastest at a given temperature. The experimental results show that the oxygen concentration of the melt with Al_2O_3 coating is the highest, and the oxygen diffusion is of similar magnitude to the simulation values, from which the conclusion can be obtained that the oxygen concentration is significantly influenced by the coating materials.
文摘The microscopic moleeular theory for electron transfer in a model solvent ishahr developed. The nonlinear response of the solvent molecules is be computedquanitatively in a new way. Adopting computer simulation daa and choosingappropriate reaction coordinae, a reasonable free energy dinram is constructed and thercorganhaion energy for the product state is calculated.
文摘The vinylidene-bridged cluster μ_3-FcCHCFeCo_2(CO)_9 2 was prepared by the expansionreaction of ferrocenyl-acetylene dicobalt complex μ-FcCCHCo_2(CO)_6 1. Benzylideneacetone-tricarbonyliron [(BDA)Fe(CO)_3] was used as the source of Fe(CO)_3. The molecular structure of thecluster 2 was detendned by x-ray structural analysis.
基金This work is supported by the National Natural Science Foundation (Grant No. 10075009) Sino-France Advance Research Program (PRA)
文摘A Molecular Dynamics (MD) simulation with Tersoff empirical many-bodypotential has been employed to investigate the growth processes of diamond film with energeticspecies deposition. In the present study, we have studied the reaction probabilities of energeticspecies with energies of 0.1 e V to 10eV at the substrate temperature of 1100K. In the cases of thediamond growth on the surface with H passivation, the reaction probability of hydrocarbon speciesconsiderably increases when the species energy is higher than 2eV. This means that the diamond filmcan grow in the case of high incident species energy without the process of hydrogen abstraction,which is needed in the case of incident species with low energy. The reaction mechanism of energeticspecies on hydrogen passivated diamond surface is also discussed.
基金The financial support provided by the Project of National Natural Science Foundation of China(21822809&21978256)the Fundamental Research Funds for the Central Universitiesthe Foundation of State Key Laboratory of High-efficiency Utilization of Coal and Green Chemical Engineering(Grant No.2018-K23)are gratefully acknowledged.
文摘Ethane steam cracking process in an industrial reactor was investigated.An one-demsional(1D)steady-state model was developed firstly by using an improved molecular reaction scheme and was then simulated in Aspen Plus.A comparison of model results with industrial data and previously reported results showed that the model can predict the process kinetics more accurately.In addition,the validated model was used to study the effects of different process variables,including coil outlet temperature(COT),steam-to-ethane ratio and residence time on ethane conversion,ethylene selectivity,products yields,and coking rate.Finally,steady-state optimization was conducted to the operation of industrial reactor.The COT and steam-to-ethane ratio were taken as decision variables to maximize the annual operational profit.
