首页|In Situ Monitoring of Transmetallation in Electric Potential-Promoted Oxidative Coupling in a Sinqle-Molecule Junction
In Situ Monitoring of Transmetallation in Electric Potential-Promoted Oxidative Coupling in a Sinqle-Molecule Junction
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To monitor and investigate chemical reactions in real time and in situ is a long-standing,challenging goal in chemistry.Herein,an electric potential-promoted oxidative coupling reaction of organoboron com-pounds without the addition of base is reported,and the transmetallation process involved is moni-tored in real time and in situ with the scanning tunneling microscopy break single-molecule junc-tions(STMBJ)technique.We found that the electric potential applied determined the transmetallation.At low-bias voltage,the first-step transmetallation process occurred and afforded Au—C-bonded aryl gold intermediates.The electronic properties of organoboron compounds have a strong influence on the transmetallation process,and electron-rich com-pounds facilitate this transformation.At high-bias voltage,the second-step transmetallation process took place,and the corresponding intermediate(highly reactive diaryl metal complex)was detected with the assistance of Pd(OAc)2.Our work demonstrates the applications of STMBJ on in situ monitoring and catalyzing of chemical reactions and provides a new methodology to fabricate single-molecule devices.
Yunpeng Li、Chengxi Zhao、Rui Wang、Ajun Tang、Wenjing Hong、Dahui Qu、He Tian、Hongxiang Li
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Key Laboratory for Advanced Materials,Feringa Nobel Prize Scientist Joint Research Center,Frontiers Science Center for Materiobiology and Dynamic Chemistry,Institute of Fine Chemicals,School of Chemistry and Molecular Engineer-ing,East China University of Science and Technology,Shanghai 200237
Key Laboratory of Physical Chemistry of Solid Surfaces,College of Chemistry and Chemical Engineering,Xiamen University,Xiamen 361005
国家自然科学基金国家自然科学基金国家自然科学基金上海市科技计划重大项目Fundamental Research Funds for the Central Universities,the Programme of Introducing Talents of Discipline to UniversitiesProgram of Shanghai Academic/Technology Research Leader