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Highly efficient electrocatalytic nitrogen fixation enabled by the bridging effect of ru in plasmonic nanoparticles

Nano Research 2023年第1期16卷 360-370页

作者： Hang Yin Jinwu Hu Caihong Fang Yuyang Wang Lixia Ma Nan Zhang Shouren Zhang ruibin Jiang Jianfang Wang Shaanxi Key Laboratory for Advanced Energy Devices Shaanxi Engineering Lab for Advanced Energy TechnologySchool of Materials Science and EngineeringShaanxi Normal UniversityXi’an 710119China College of Chemistry and Materials Science The Key Laboratory of Functional Molecular SolidsMinistry of EducationAnhui Laboratory of Molecular-Based MaterialsCenter for Nano Science and TechnologyKey Laboratory of Electrochemical Clean Energy of Anhui Higher Education InstitutesAnhui Normal UniversityWuhu 241000China Henan Provincial Key Laboratory of Nanocomposites and Applications Institute of Nanostructured Functional MaterialsHuanghe Science and Technology CollegeZhengzhou 450006China Department of Physics The Chinese University of Hong KongHong Kong 999077China

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.

关键词： electrocatalytic nitrogen fixation au/ru electrocatalysts localized surface plasmon resonance electronic state hybridization hot electron

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