Characterization of ammonia adsorption on ruthenium sulfide: Identification of amino species by inelastic neutron scattering

The interaction of ammonia with the surface of a model ruthenium sulfide catalyst has been investigated using conventional adsorption measurements, temperature programmed desorption and inelastic neutron scattering. This work has provided evidence that the amount and also the nature of adsorbed species vary with the sulfur to metal ratio of the solid. On the unreduced sample, ammonia interacts weakly with the solid and ammonium ions are not observed, On the partially desulfurized catalyst, the chemisorption of ammonia is dissociative. The NH2 fragment is bonded to a coordinatively unsaturated ruthenium ion formed upon reduction of the solid while the proton is trapped by a sulfur anion leading to the formation of SH groups. It was previously shown that hydrogen adsorption also involves unsaturated sites, Adsorption of ND, on a hydrogen-covered surface provokes a desorption of HD indicating that a competition of adsorption occurs between hydrogen and ammonia. This result explains why ammonia generally acts as a poison for hydrogenation, hydrodenitrogenation, and hydrodesulfurization reactions. (C) 1995 Academic Press, Inc.