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首页> 外文期刊>Chemistry: A European journal >A Single-Molecule-Level Mechanistic Study of Pd-Catalyzed and Cu-Catalyzed Homocoupling of Aryl Bromide on an Au(111) Surface
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A Single-Molecule-Level Mechanistic Study of Pd-Catalyzed and Cu-Catalyzed Homocoupling of Aryl Bromide on an Au(111) Surface

机译：Au（111）表面上Pd催化和Cu催化芳基溴的均偶联的单分子级机理研究

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On-surface Pd- and Cu-catalyzed C-C coupling reactions between phenyl bromide functionalized porphyrin derivatives on an Au(111) surface have been investigated under ultra-high vacuum conditions by using scanning tunneling microscopy and kinetic Monte Carlo simulations. We monitored the isothermal reaction kinetics by allowing the reaction to proceed at different temperatures. We discovered that the reactions catalyzed by Pd or Cu can be described as a two-phase process that involves an initial activation followed by C-C bond formation. However, the distinctive reaction kinetics and the C-C bond-formation yield associated with the two catalysts account for the different reaction mechanisms: the initial activation phase is the ratelimiting step for the Cu-catalyzed reaction at all temperatures tested, whereas the later phase of C-C formation is the rate-limiting step for the Pd-catalyzed reaction at high temperature. Analysis of rate constants of the Pd-catalyzed reactions allowed us to determine its activation energy as (0.41±0.03) eV.
机译：通过使用扫描隧道显微镜和动力学蒙特卡洛模拟研究了在超高真空条件下对苯基溴官能化卟啉衍生物在Au（111）表面上的表面Pd和Cu催化的C-C偶联反应。我们通过允许反应在不同温度下进行来监控等温反应动力学。我们发现，由Pd或Cu催化的反应可以描述为一个两阶段过程，该过程涉及初始活化，然后形成C-C键。然而，与两种催化剂相关的独特的反应动力学和CC键形成产率解释了不同的反应机理：初始活化阶段是在所有测试温度下Cu催化反应的速率限制步骤，而CC的后期阶段形成是高温下Pd催化反应的限速步骤。 Pd催化反应速率常数的分析使我们能够确定其活化能为（0.41±0.03）eV。

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