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Abstract
The role of the byproduct N2O has long been unknown in the NO reduction on the best metal catalysts regardless of many mechanistic studies. This paper clarifies how N2O works as an intermediate that emits N2 in the main pathway of deNOx processes. The off-normal emission of N2 from the decomposition of intermediate N2O(a) has been separately studied in a steady-state NO + CO + D2 reaction on stepped Pd(211) as well as NO + CO and NO + D2 reactions by means of angle-resolved product desorption. In these reactions, the N2 emission commonly takes place through either N2O(a) → N2(g) + O(a) or N(a) + N(a) → N2(g). With increasing surface temperature, a channel change from the former to the latter occurs slowly in the NO + CO reaction, whereas it proceeds quickly in the NO + D2 and NO + CO + D2 reactions around a kinetic transition. With increasing D2 pressure in the NO + CO + D2 system, the N2 emission via N2O(a) decomposition increases or remains constant below the kinetic transition, whereas CO2 formation is...
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