The intrinsic dynamics of two interacting electric polarized nanorods is theoretically investigated. The relative motion between them caused by electric dipole-dipole interaction is derived based on the generalized La...The intrinsic dynamics of two interacting electric polarized nanorods is theoretically investigated. The relative motion between them caused by electric dipole-dipole interaction is derived based on the generalized Lagrangian formulation. The results show that the relative translation and rotation are nonlinear and closely dependent on the initial configuration of the two nanorods. Furthermore, the general conditions of the initial configuration, which determine the two nanorods to repel or attract each other at the initial time, are obtained. The two-dimensional relative motion of the two nanorods shows that the antiparallel and head-to-tail ordering stable self-assembly are respectively formed in two planar initial configurations. For different three-dimensional initial configurations, the interesting dynamic relative attraction, repulsion, and oscillation with rotation are respectively realized. Finally, the theoretical schemes which realize the relaxing, direct head-to-tail ordering, and direct antiparallel ordering stable self-assembly are presented according to the different modes of the motion of the nanoparticles. Some of our results agree well with the results of experiments and simulations.展开更多
Plasmonic hot electrons have long been regarded as a promising energy source for inducing chemical transformations.However,because of the mismatch between the electron cloud of reactant molecules and the hot-electron ...Plasmonic hot electrons have long been regarded as a promising energy source for inducing chemical transformations.However,because of the mismatch between the electron cloud of reactant molecules and the hot-electron gas of metal nanoparticles(NPs),the highly localized and short-lived hot electrons are dif-ficult to utilize in bulk synthesis when the reactant molecules do not have a strong affinity for the metal surface.Here,we propose the concept of polarized nanocatalysts to mimic chemical polarity at the nanometer scale.Under plasmonic photorecycling conditions,the rationally designed asymmetric Ag-TiO_(2) hybrid NPs enable six-electron reduction of molecules in bulk solution.This hot-electron-driven reaction does not require a conventional hydrogen or hydride reducing agent.As a proof-of-concept,one-pot photocatalytic syntheses of amides,such as paracetamol,using nitro reactants were performed.This provides a new opportunity to enable challenging multielectron transformations in organic chemistry.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.11174222)the National Basic Research Program of China(Grant No.2011CB922203)
文摘The intrinsic dynamics of two interacting electric polarized nanorods is theoretically investigated. The relative motion between them caused by electric dipole-dipole interaction is derived based on the generalized Lagrangian formulation. The results show that the relative translation and rotation are nonlinear and closely dependent on the initial configuration of the two nanorods. Furthermore, the general conditions of the initial configuration, which determine the two nanorods to repel or attract each other at the initial time, are obtained. The two-dimensional relative motion of the two nanorods shows that the antiparallel and head-to-tail ordering stable self-assembly are respectively formed in two planar initial configurations. For different three-dimensional initial configurations, the interesting dynamic relative attraction, repulsion, and oscillation with rotation are respectively realized. Finally, the theoretical schemes which realize the relaxing, direct head-to-tail ordering, and direct antiparallel ordering stable self-assembly are presented according to the different modes of the motion of the nanoparticles. Some of our results agree well with the results of experiments and simulations.
基金financial support from the National Key R&D Program of China(grant no.2021YFB4000600)the National Natural Science Foundation of China(grant no.22022406)+2 种基金the Natural Science Foundation of Tianjin(grant nos.20JCJQJC00110 and 20JCYBJC00590)the 111 project(grant no.B12015)the Haihe Laboratory of Sustainable Chemical Transformations.
文摘Plasmonic hot electrons have long been regarded as a promising energy source for inducing chemical transformations.However,because of the mismatch between the electron cloud of reactant molecules and the hot-electron gas of metal nanoparticles(NPs),the highly localized and short-lived hot electrons are dif-ficult to utilize in bulk synthesis when the reactant molecules do not have a strong affinity for the metal surface.Here,we propose the concept of polarized nanocatalysts to mimic chemical polarity at the nanometer scale.Under plasmonic photorecycling conditions,the rationally designed asymmetric Ag-TiO_(2) hybrid NPs enable six-electron reduction of molecules in bulk solution.This hot-electron-driven reaction does not require a conventional hydrogen or hydride reducing agent.As a proof-of-concept,one-pot photocatalytic syntheses of amides,such as paracetamol,using nitro reactants were performed.This provides a new opportunity to enable challenging multielectron transformations in organic chemistry.
