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Use of molecular beams for kinetic measurements of chemical reactions on solid surfaces
Surface Science Reports ( IF 9.8 ) Pub Date : 2017-03-15 , DOI: 10.1016/j.surfrep.2017.02.002
Francisco Zaera

In this review we survey the contributions that molecular beam experiments have provided to our understanding of the dynamics and kinetics of chemical interactions of gas molecules with solid surfaces. First, we describe the experimental details of the different instrumental setups and approaches available for the study of these systems under the ultrahigh vacuum conditions and with the model planar surfaces often used in modern surface-science experiments. Next, a discussion is provided of the most important fundamental aspects of the dynamics of chemical adsorption that have been elucidated with the help of molecular beam experiments, which include the development of potential energy surfaces, the determination of the different channels for energy exchange between the incoming molecules and the surface, the identification of adsorption precursor states, the understanding of dissociative chemisorption, the determination of the contributions of corrugation, steps, and other structural details of the surface to the adsorption process, the effect to molecular steering, the identification of avenues for assisting adsorption, and the molecular details associated with the kinetics of the uptake of adsorbates as a function of coverage. We follow with a summary of the work directed at the determination of kinetic parameters and mechanistic details of surface reactions associated with catalysis, mostly those promoted by late transition metals. This discussion we initiate with an overview of what has been learned about simple bimolecular reactions such as the oxidation of CO and H2 with O2 and the reaction of CO with NO, and continue with the review of the studies of more complex systems such as the oxidation of alcohols, the conversion of organic acids, the hydrogenation and isomerization of olefins, and the oxidative activation of alkanes under conditions of short contact times. 6 Reactions on supported nanoparticles: Materials gap, 7 Low-probability reactions: Pressure gap of this review deal with the advances made in the use of molecular beams with more realistic models for catalysis, using surfaces comprised of metal nanoparticles dispersed on the oxide surfaces used as catalyst support and high-flux beams to approach the pressures used in catalysis. The next section deals with the study of systems associated with fields other than catalysis, mainly with the etching and oxidation of semiconductor surfaces and with the chemistry used to grow thin solid films by chemical means (chemical vapor deposition, CVD, or atomic layer deposition, ALD). We end with a personal assessment of the past accomplishments, present state, and future promise of the use of molecular beams for the study of the kinetics of surface reactions relevant to practical applications.



中文翻译:

分子束在固体表面化学反应动力学测量中的应用

在这篇综述中,我们调查了分子束实验对了解气体分子与固体表面化学相互作用的动力学和动力学的贡献。首先,我们描述了在超高真空条件下以及现代表面科学实验中经常使用的模型平面表面下,可用于研究这些系统的不同仪器设置和方法的实验细节。接下来,将讨论分子吸附实验已阐明的化学吸附动力学的最重要的基本方面,其中包括势能面的开发,确定分子之间的能量交换的不同途径。传入的分子和表面,识别吸附前体状态,理解解离化学吸附,确定波纹,台阶和表面其他结构细节对吸附过程的贡献,对分子转向的影响,确定辅助吸附的途径以及与吸收物吸收动力学相关的分子细节随覆盖率的变化而变化。我们对旨在确定与催化有关的表面反应的动力学参数和机理细节的工作进行了总结,这些反应主要是由后期过渡金属促进的。在此讨论中,我们首先概述了有关简单的双分子反应(例如CO和H的氧化)的知识 确定波纹,台阶和表面其他结构细节对吸附过程的贡献,对分子操纵的影响,确定辅助吸附的途径以及与被吸附物吸收动力学有关的分子细节覆盖功能。我们对旨在确定与催化有关的表面反应的动力学参数和机理细节的工作进行了总结,这些反应主要是由后期过渡金属促进的。在此讨论中,我们首先概述了有关简单的双分子反应(例如CO和H的氧化)的知识 确定波纹,台阶和表面其他结构细节对吸附过程的贡献,对分子操纵的影响,确定辅助吸附的途径以及与被吸附物吸收动力学有关的分子细节覆盖功能。我们对旨在确定与催化有关的表面反应的动力学参数和机理细节的工作进行了总结,这些反应主要是由后期过渡金属促进的。在此讨论中,我们首先概述了有关简单的双分子反应(例如CO和H的氧化)的知识 确定辅助吸附途径的分子,以及与被吸附物吸收动力学相关的分子细节(作为覆盖率的函数)。我们对旨在确定与催化有关的表面反应的动力学参数和机理细节的工作进行了总结,这些反应主要是由后期过渡金属促进的。在此讨论中,我们首先概述了有关简单的双分子反应(例如CO和H的氧化)的知识 确定辅助吸附途径的分子,以及与被吸附物吸收动力学相关的分子细节(作为覆盖率的函数)。我们对旨在确定与催化有关的表面反应的动力学参数和机理细节的工作进行了总结,这些反应主要是由后期过渡金属促进的。在此讨论中,我们首先概述了有关简单的双分子反应(例如CO和H的氧化)的知识2与O 2以及CO与NO的反应,并继续审查更复杂系统的研究,例如醇的氧化,有机酸的转化,烯烃的加氢和异构化以及在短时间条件下烷烃的氧化活化联系时间。6负载型纳米颗粒上的反应:材料缺口,7低概率反应:这篇综述的压力缺口涉及分子束的使用进展,该模型采用更现实的催化模型,使用的金属纳米颗粒表面分散在所用的氧化物表面上用作催化剂载体和高通量梁以接近催化中使用的压力。下一部分将研究与催化以外的领域相关的系统,主要用于半导体表面的蚀刻和氧化,以及用于通过化学手段(化学气相沉积,CVD或原子层沉积,ALD)生长固体薄膜的化学方法。最后,我们对分子束用于研究与实际应用相关的表面反应动力学的过去成就,当前状态和未来前景进行了个人评估。

更新日期:2017-03-15
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