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Structure and Reactivity of Intermediates. N-Overlayer On Pd(100), Rh(100) and Pt-Rh(110) and Its Reaction With H2

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Rh(100), Pt(100), and Pt-Rh(100) surfaces are inert for the dissociative adsorption of N2, but they are active for the catalytic reaction of NO with H2 During the reaction on Rh(100) and Pt-Rh(100) surfaces, N atoms are accumulated by making a c(2x2)-N overlayer, but no accumulation of N atoms occurs on Pt(100) surface. The fact that N atoms on the PtRh(100) surface gives the c(2x2) structure indicates that the N atoms have equal affinity to Pt and Rh on the alloy surface. When the c(2x2)-N surface was exposed to H2 of 10-7 to 10-8 Torr, a prominent loss peak being assignable to NHx appeared at 3200 - 3240 cm-1 at around 400 K The in-situ HREELS study proved that NH are prominent species which are formed during the hydrogenation of the c(2x2)-N, that is, a quasi-equilibrium of N + 1/2 H2 NH is established. When a clean Pt-Rh(100) (Pt/Rh = 1/3) alloy surface is exposed to NO at about 440 K, the LEED pattern changes sequentially as (1x1)→ c (2x2) → c (2x2) + p (3x1)→ p (3x1), where the c (2x2) pattern appears instantaneously on the alloy surface of any Pt/Rh ratio but the p(3xl) pattern accompanies a certain characteristic interval times being responsible to the segregation of Rh. The p(3x1) surface reflects the formation of an intermediate of Rh-O complex overlayer and it reacts rapidly with H2.

Affiliations: 1: The Institute for Solid State Physics University of Tokyo 7-22-1 Roppongi, Minato-ku, Tokyo 106, JAPAN


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