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Title: Novel insight into the hydrogen absorption mechanism at the Pd(110) surface

The microscopic mechanism of low-temperature (80 K < T < 160 K) hydrogen (H) ingress into the H{sub 2} (<2.66 × 10{sup −3} Pa) exposed Pd(110) surface is explored by H depth profiling with {sup 15}N nuclear reaction analysis (NRA) and thermal desorption spectroscopy (TDS) with isotope (H, D) labeled surface hydrogen. NRA and TDS reveal two types of absorbed hydrogen states of distinctly different depth distributions. Between 80 K and ∼145 K a near-surface hydride phase evolving as the TDS α{sub 1} feature at 160 K forms, which initially extends only several nanometers into depth. On the other hand, a bulk-absorbed hydrogen state develops between 80 K and ∼160 K which gives rise to a characteristic α{sub 3} TDS feature above 190 K. These two absorbed states are populated at spatially separated surface entrance channels. The near-surface hydride is populated through rapid penetration at minority sites (presumably defects) while the bulk-absorbed state forms at regular terraces with much lower probability per site. In both cases, absorption of gas phase hydrogen transfers pre-adsorbed hydrogen atoms below the surface and replaces them at the chemisorption sites by post-dosed hydrogen in a process that requires much less activation energy (<100 meV) thanmore » monatomic diffusion of chemisorbed H atoms into subsurface sites. This small energy barrier suggests that the rate-determining step of the absorption process is either H{sub 2} dissociation on the H-saturated Pd surface or a concerted penetration mechanism, where excess H atoms weakly bound to energetically less favorable adsorption sites stabilize themselves in the chemisorption wells while pre-chemisorbed H atoms simultaneously transit into the subsurface. The peculiarity of absorption at regular Pd(110) terraces in comparison to Pd(111) and Pd(100) is discussed.« less
Authors:
; ;  [1]
  1. Institute of Industrial Science, University of Tokyo, 4-6-1 Komaba, Meguro-ku, Tokyo 153-8505 (Japan)
Publication Date:
OSTI Identifier:
22253329
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 140; Journal Issue: 13; Other Information: (c) 2014 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ABSORPTION; ACTIVATION ENERGY; ADSORPTION; CHEMISORPTION; DESORPTION; DISSOCIATION; DOSES; HYDRIDES; HYDROGEN; HYDROGEN TRANSFER; NUCLEAR REACTION ANALYSIS; PALLADIUM 100; PALLADIUM 110; PALLADIUM 111; SPATIAL DISTRIBUTION; SPECTROSCOPY; SURFACES