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首页> 外文期刊>The journal of physical chemistry, A. Molecules, spectroscopy, kinetics, environment, & general theory >Binding Energies of 0_2and CO to Small Gold, Silver, and Binary Silver—Gold ClusterAnions from Temperature Dependent Reaction Kinetics Measurements
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Binding Energies of 0_2and CO to Small Gold, Silver, and Binary Silver—Gold ClusterAnions from Temperature Dependent Reaction Kinetics Measurements

机译：通过温度依赖性反应动力学测量，0_2和CO与小金，银和二元银-金簇阴离子的结合能

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摘要

A detailed analysis of experimentally obtained temperature-dependent gas-phase kinetic data for the oxygenand carbon monoxide adsorption on small anionic gold (Au_n~-,n = 1-3),silver (Ag_n~-,5),and binarysilver-gold (Ag_nAu_m,~-,n+m =2, 3) clusters is presented. The Lindemann energy transfer model inconjunction with statistical unimolecular reaction rate theory is employed to determine the bond dissociationenergies E_0of the observed metal cluster complexes with 0_2and CO. The accuracy limits of obtainedbinding energies are evaluated by applying different transition-state models. The assumptions involved in thedata evaluation procedure as well as possible sources of error are discussed. The thus-derived binding energiesof 0_2to pure silver and binary silver-gold cluster anions are generally in excellent agreement with previouslyreported theoretical values. In marked contrast, the binding energies of 0_2and CO to Au_2~- and 3~-determinedvia temperature-dependent reaction kinetics are consistently lower than the theoretically predicted values.
机译：对通过实验获得的随温度变化的气相动力学数据的详细分析，该动力学数据涉及氧气和一氧化碳吸附在小型阴离子金（Au_n〜-，n = 1-3），银（Ag_n〜-，5）和二元银金（ Ag_nAu_m，〜-，n + m = 2，表示3）簇。采用林德曼能量转移模型与统计单分子反应速率理论相结合，确定观察到的金属团簇与0_2和CO的键解离能E_0。通过应用不同的过渡态模型，评价了所获得的结合能的准确度极限。讨论了数据评估程序中涉及的假设以及可能的错误源。如此得出的0_2与纯银和二元银-金团簇阴离子的结合能通常与先前报道的理论值高度吻合。与之形成鲜明对比的是，通过温度依赖性反应动力学确定的0_2和CO与Au_2〜-和3〜的结合能始终低于理论预测值。

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