Angle-resolved desorption and removal of surface nitrogen in deNOx

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.