ELSEVIER Surface Science 360 (1996) 255 260
surface science
The coadsorption of hydrogen and potassium on Ir(111)
M. Schick, J. Lauterbach, W.H. Weinberg *
Department of Chemical Engineering, University of California at Santa Barbara, Santa Barbara, CA 93106, USA
Received 28 December 1995; accepted for publication 4 March 1996
Abstract
The adsorption of gas-phase atomic hydrogen on potassium-precovered Ir(111) surfaces was investigated. Even very low coverages
of potassium adatoms strongly inhibit the dissociative adsorption of molecular hydrogen. However,using gas-phase atomic hydrogen
allows us to overcome the activation barrier for dissociative hydrogen adsorption. In addition, abstraction of hydrogen adatoms by
impinging atomic hydrogen occurs. The probabilities and cross-sections for both reactions and the maximum number of hydrogen
adsorption sites are derived and compared to data obtained on other surfaces. Furthermore, a kinetic isotope effectin the desorption
of hydrogen and deuterium was observed. Implications of these results with respect to the potassium hydrogen interaction
are discussed.
Keywords: Adsorption kinetics; Alkali metals; Atom-solid reactions; Deuterium; Hydrogen; Iridium; Solid-gas interfaces; Thermal
desorption spectroscopy
1. Introduction
In recent years, the coadsorption of potassium
with various gases has been studied on a wide
variety of transition metal surfaces. Our work was
motivated by the promoter properties of potassium
in many catalytic reactions, in particular in
Fischer~Tropsch synthesis and ammonia synthesis
[1,2]. Many investigations have focused on the
CO/K and N2/K coadsorption systems on trans-
ition metals I-3-5]. However, only in relatively few
cases has the influence of potassium on the dissoci-
ative adsorption kinetics of hydrogen, the other
reactant in Fischer-Tropsch and ammonia synthe-
sis, been characterized [6-13].
In general, the influence of potassium adatoms
* Corresponding author. Fax: + 1 805 8934731; e-mail:
chari@engineering.ucsb.edu.
on the dissociative adsorption of hydrogen is char-
acterized by a large decrease in the adsorption
probability. This behavior can be explained by an
increased electron density in the metal due to
electron donation from the electropositive potas-
sium adatoms. This causes a large work-function
decrease, enhancing the Pauli repulsion between
the lo bonding level of the impinging H 2 molecules
and the metal surface [7]. In addition, hydrogen
generally desorbs at higher temperatures in the
presence of potassium as compared to the clean
surface, i.e. adsorbed hydrogen is stabilized by the
presence of potassium on the surface.
In this work, the potassium-precovered Ir(111)
surface was exposed to gas-phase atomic hydrogen
and deuterium in order to overcome the potas-
sium induced activation barrier for dissociative
hydrogen adsorption [ 11 ]. This approach permits
not only study of the hydrogen-potassium inter-
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