AVS 66th International Symposium & Exhibition
    Surface Science Division Tuesday Sessions
       Session SS-TuP

Paper SS-TuP13
The Two-faced Role of Steps in the Isotopic Scrambling of Hydrogen on Pt

Tuesday, October 22, 2019, 6:30 pm, Room Union Station B

Session: Surface Science Poster Session
Presenter: Richard van Lent, Leiden University, Netherlands
Authors: R. van Lent, Leiden University, Netherlands
L.B.F. Juurlink, Leiden University, Netherlands
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The simplest heterogeneously catalyzed reaction possible is isotopic scrambling of hydrogen:

H2 + D2 --> 2 HD

On Pt, this reaction occurs by dissociative adsorption of H2 and D2, mixing of H and D atoms on the surface, and recombination to form the three isotopologues, H2, D­2, and HD. Full isotopic scrambling would lead to a product ratio of 1:1:2.

Step edges are well-known to enhance dissociative adsorption, especially at low impact energies. However, it is unknown whether subsequent diffusion and desorption only occur along the steps or involves diffusion onto terraces. We study this by combining supersonic molecular beam techniques with a curved Pt single crystal surface with straight A and B type step edges, c-Pt(111)[1-10]310. At a high surface temperature, we probe HD formation, spatially resolved, along the curved surface by impinging a 50:50 mixture of low energy H2 and D2. HD formation tracks the trend in dissociation: higher step densities yield higher HD formation. However, relatively, HD formation does not increase as rapidly as the dissociation probability. We explain why the (111) terraces are more selective toward HD formation and show that anisotropic diffusion affects isotopic scrambling.