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Angle-resolved desorption and removal of surface nitrogen in deNOx
Authors:Tatsuo Matsushima  Anton Kokalj
Institution:1. Catalysis Research Center, Hokkaido University, Sapporo 001-0021, Japan;2. Department of Physical and Organic Chemistry, Jo?ef Stefan Institute, Jamova 39, 1000 Ljubljana, Slovenia
Abstract:This paper reports on recent progress on angle-resolved desorption leading to structure-sensitive desorption dynamics. The sensitivity is exemplified in NO and N2O reduction on Pd and Rh surfaces. The energy partitioning in the repulsive desorption of hyper-thermal products into their rotational and translational modes is an indispensable concept to examine the structure of a reaction site from desorbing molecules because it connects the structure of a transition state with each energy of desorbed products. The extent of the energy partitioning will be derived from the desorption-angle dependences of both the rotational and translational energies at each vibrational state. Such energy analysis has never been completed for any thermal reactive desorption. A new type of measurement is thus proposed. Additionally, we discuss the inadequate use of the detailed balance principle in desorption dynamics, which has prevented desorption dynamics from being sensitive to surface structures.
Keywords:Spatial distribution  Transition state  Energy partitioning  NO reduction  Corresponding author  
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