Plasmon-generated hot electrons show great potential for driving chemical reactions.The utilization efficiency of hot electrons is highly dependent on the interaction of the electronic states at the interfaces between...Plasmon-generated hot electrons show great potential for driving chemical reactions.The utilization efficiency of hot electrons is highly dependent on the interaction of the electronic states at the interfaces between plasmonic nanoparticles and other materials/molecules.Strong interaction can produce new hybridized electron states,which permit direct hot-electron transfer,a more efficient transfer mechanism.However,Au usually has very weak interaction with most molecules because of its inertness,which makes direct hot-electron transfer impossible.Herein,the improvement of the hot-electron transfer efficiency from Au to N_(2)is demonstrated by introducing a Ru bridging layer.Both the N_(2)fixation rate and Faradic efficiency(FE)are enhanced by the excitation of plasmons.The enhancement of the N_(2)fixation rate is found to arise from plasmon-generated hot electrons.Theoretical calculations show that the strong interaction of the Ru electronic states with the N_(2)molecular orbitals produces new hybridized electronic states,and the Ru d electrons also strongly couple with the Au sp electrons.Such a bridging role of Ru makes direct hot-electron transfer from Au to N_(2)possible,improving the FE of nitrogen fixation.Our findings demonstrate a new approach to increasing the utilization efficiency of plasmonic hot electrons for chemical reactions and will be helpful to the design of plasmonic catalysts in the future.展开更多
Aerogels have become a hot topic of research due to their extremely low density and special interconnected structure as well as their enzyme-like activity.The development of new multifunctional nano-enzyme aerogels wi...Aerogels have become a hot topic of research due to their extremely low density and special interconnected structure as well as their enzyme-like activity.The development of new multifunctional nano-enzyme aerogels with high activity and good stability is still a considerable challenge.In this paper,AuRu aerogels with peroxidase and oxidase activities were synthesized using a simple one-step method and successfully used to construct colorimetric sensors for the detection of Fe^(2+)and glucose based on their enzyme-like activities.Furthermore,we are fortunate to find that AuRu aerogels have good photothermal properties.This suggests that AuRu aerogels can be used not only for in vitro testing but also for promising applications such as disease treatment.展开更多
基金This work was supported by Fundamental Research Funds for Central Universities(No.GK202201003)Funded Projects for the Academic Leaders and Academic Backbones of Shaanxi Normal University(No.18QNGG008)Shaanxi Sanqin Scholars Innovation Team,and Free Exploring Research Project for PhD Students of Shaanxi Normal University(No.2020TS106).
文摘Plasmon-generated hot electrons show great potential for driving chemical reactions.The utilization efficiency of hot electrons is highly dependent on the interaction of the electronic states at the interfaces between plasmonic nanoparticles and other materials/molecules.Strong interaction can produce new hybridized electron states,which permit direct hot-electron transfer,a more efficient transfer mechanism.However,Au usually has very weak interaction with most molecules because of its inertness,which makes direct hot-electron transfer impossible.Herein,the improvement of the hot-electron transfer efficiency from Au to N_(2)is demonstrated by introducing a Ru bridging layer.Both the N_(2)fixation rate and Faradic efficiency(FE)are enhanced by the excitation of plasmons.The enhancement of the N_(2)fixation rate is found to arise from plasmon-generated hot electrons.Theoretical calculations show that the strong interaction of the Ru electronic states with the N_(2)molecular orbitals produces new hybridized electronic states,and the Ru d electrons also strongly couple with the Au sp electrons.Such a bridging role of Ru makes direct hot-electron transfer from Au to N_(2)possible,improving the FE of nitrogen fixation.Our findings demonstrate a new approach to increasing the utilization efficiency of plasmonic hot electrons for chemical reactions and will be helpful to the design of plasmonic catalysts in the future.
基金the financial support from Sichuan Province Science and Technology Support Program(No.2020YFN0029)the One-Thousand-Talents Scheme in Sichuan Province,Scientific Start-up Research Fund of Chengdu University of Information Technology(No.KYTZ201714).
文摘Aerogels have become a hot topic of research due to their extremely low density and special interconnected structure as well as their enzyme-like activity.The development of new multifunctional nano-enzyme aerogels with high activity and good stability is still a considerable challenge.In this paper,AuRu aerogels with peroxidase and oxidase activities were synthesized using a simple one-step method and successfully used to construct colorimetric sensors for the detection of Fe^(2+)and glucose based on their enzyme-like activities.Furthermore,we are fortunate to find that AuRu aerogels have good photothermal properties.This suggests that AuRu aerogels can be used not only for in vitro testing but also for promising applications such as disease treatment.
