Temporal analysis of products (TAP) reactor study of the dynamics of CO2 interaction with a Ru/γ-Al2O3 supported catalyst II: Interaction strength, formation of intermediates and oxygen exchange
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Abstract
Continuing a comprehensive study of the reduction of CO over supported Ru catalysts, we explored the interaction of CO with Ru/γ-AlO by TAP reactor measurements, focusing on dynamic aspects in adsorption/desorption, reaction and oxygen exchange processes. Pulse shape analysis in H/CO multipulse sequences provides information on the interaction of reactant/product species with the catalyst. The measurements provide information on the dynamic build-up of reaction intermediates and more stable adspecies during pulsing, and its relation to CH formation. Facile oxygen exchange between CO and catalyst, followed by isotope labeling experiments, is quantitatively reconciled in a simple model, relating the ratio between different CO isotopologues to the O:O ratio in the total exchangeable oxygen on the surface and in the CO pulse. The results provide detailed insight into various aspects of the interaction between CO and Ru/AlO catalysts important for a mechanistic understanding of various catalytic reactions involving CO.
在继续对支撑型 Ru 催化剂还原 CO 的综合研究的同时，我们通过 TAP 反应器测量探究了 CO 与 Ru/γ-AlO 的相互作用，重点关注吸附/解吸、反应和氧交换过程的动态方面。H/CO 多脉冲序列中的脉冲形状分析提供了反应物/产物物种与催化剂相互作用的信息。测量结果提供了脉冲过程中反应中间产物和更稳定吸附物种的动态积累及其与 CH 形成之间关系的信息。一氧化碳与催化剂之间的便捷氧交换，以及随后的同位素标记实验，都可以通过一个简单的模型进行定量调节，该模型将不同一氧化碳同位素之间的比率与表面和一氧化碳脉冲中总可交换氧的 O:O 比率联系起来。研究结果详细揭示了 CO 与 Ru/AlO 催化剂之间相互作用的各个方面，对于从机理上理解涉及 CO 的各种催化反应非常重要。
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