A kinetic analysis methodology to elucidate the roles of metal, support and solvent for the hydrogenation of 4-phenyl-2-butanone over Pt/TiO2
A kinetic analysis methodology to elucidate the roles of metal, support and solvent for the hydrogenation of 4-phenyl-2-butanone over Pt/TiO2
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DOI：
10.1016/j.jcat.2015.06.007
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发表时间：
2015-10-01
影响因子：
7.3
通讯作者：
Stitt, E. H.
中科院分区：
文献类型：
--
作者：
Wilkinson, S. K.;McManus, I.;Stitt, E. H.
4-苯基-2-丁酮在 Pt/TiO2 催化剂上氢化的速率和更重要的选择性（酮与芳环）已被证明随溶剂的不同而变化。在这项研究中，已经开发了这种多相反应的基本动力学模型，结合了统计分析方法，以加强机械上合理的动力学模型的基础。确定2位点模型是最合适的，描述芳香族氢化（假设在铂位点上）和酮氢化（假设在铂-二氧化钛界面处）。溶剂的选择对酮氢化速率常数影响不大，但由于溶剂-催化剂相互作用而强烈影响芳烃氢化。反应选择性还与拟合的产物吸附常数参数相关。所示的动力学分析方法证明了溶剂在影响反应物吸附和反应选择性方面的作用。 (C) 2015 年作者。由爱思唯尔公司出版
The rate and, more importantly, selectivity (ketone vs aromatic ring) of the hydrogenation of 4-phenyl-2-butanone over a Pt/TiO2 catalyst have been shown to vary with solvent. In this study, a fundamental kinetic model for this multi-phase reaction has been developed incorporating statistical analysis methods to strengthen the foundations of mechanistically sound kinetic models.A 2-site model was determined to be most appropriate, describing aromatic hydrogenation (postulated to be over a platinum site) and ketone hydrogenation (postulated to be at the platinum-titania interface). Solvent choice has little impact on the ketone hydrogenation rate constant but strongly impacts aromatic hydrogenation due to solvent-catalyst interaction. Reaction selectivity is also correlated to a fitted product adsorption constant parameter. The kinetic analysis method shown has demonstrated the role of solvents in influencing reactant adsorption and reaction selectivity. (C) 2015 The Authors. Published by Elsevier Inc.