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Kinetic and geometric isotope effects originating from different adsorption potential energy surfaces: Cyclohexane on Rh(111)
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10.1063/1.4725714
/content/aip/journal/jcp/136/21/10.1063/1.4725714
http://aip.metastore.ingenta.com/content/aip/journal/jcp/136/21/10.1063/1.4725714
View: Figures

Figures

Image of FIG. 1.
FIG. 1.

IRAS spectra of (a) C6H12 and (b) C6D12 as a function of heating temperature. Cyclohexane exposure is 5 shots (θ = 0.3). After heating to the indicated temperatures, the spectra were recorded at 20 K.

Image of FIG. 2.
FIG. 2.

C 1s photoelectron spectra (hν = 410 eV) of adsorbed cyclohexane at saturation coverage (dots), and residual species after heating to 240 K (solid lines).

Image of FIG. 3.
FIG. 3.

(a) TPD spectra of cyclohexane on the clean Rh(111) surface as a function of exposure. The heating rate is 1.4 K/s. (b) Fractional amounts of desorption (filled circles) and dehydrogenation (open circles) of C6H12 during TPD measurements as a function of exposure. (c) Arrhenius plots of C6H12 (red open circles) and C6D12 (black filled circles) TPD spectra in (a) at submonolayer coverages. Desorption onset and 5% threshold increments are indicated by arrows. (d) Desorption energies as a function of cyclohexane exposure obtained by TTPD analysis.

Image of FIG. 4.
FIG. 4.

(a) TPD spectra of cyclohexane on the hydrogen-saturated Rh(111) surface. The cyclohexane exposure is 5 shots, and the heating rate is 1.3 K/s. (b) Arrhenius plots of the C6H12 (red open circles) and C6D12 (black filled circles) TPD spectra. Desorption onset and 5% threshold increments are indicated by arrows.

Image of FIG. 5.
FIG. 5.

C6H12 (open circles) and C6D12 (filled circles) coverages as a function of exposure in PES measurements. The coverage was estimated from the area intensity of the C 1s spectra using an Al Kα source. The experimental results are fitted by uptake curves assuming the Kisliuk precursor-mediated adsorption model.

Image of FIG. 6.
FIG. 6.

(a) A secondary electron cutoff region in UPS spectra of C6H12 (open circles) and C6D12 (filled circles) adsorbed on the clean and hydrogen-saturated Rh(111) surfaces at 90 K. In the spectra on the clean surface, cyclohexane coverages are also indicated, which are estimated from the uptake curves in Fig. 5. The measurements on the hydrogen-saturated Rh(111) surface were performed at the saturation cyclohexane coverage (0.174 molecules per one surface Rh atom). (b) Work function changes of the clean Rh(111) surface as a function of cyclohexane coverage; C6H12 (open circles) and C6D12 (filled circles).

Image of FIG. 7.
FIG. 7.

LEED patterns of (a) and (b) submonolayer superstructures (exposure of 5 shots), and (c) and (d) dense layers (20 shots) of cyclohexane adsorbed on the clean Rh(111) surface together with the intermolecular distance (dm) and domain angle (α) with respect to the substrate unit cell. The reciprocal lattices of hexagonal cyclohexane unit cells are indicated by solid lines. (e) and (f) LEED patterns of the cyclohexane layers (exposure of 5 shots) on the hydrogen-saturated Rh(111) surface. The sample temperature was 90 K, and the incident electron energy was 75 eV.

Image of FIG. 8.
FIG. 8.

(a) A summary of the observed isotope effects in cyclohexane adsorption on the clean Rh(111) surface: adsorption energy (Ead), work function change (Δϕ), adsorption distance (rad), and intermolecular distance (dm). These indicated values are estimated from the results at θ = 0.3. (b) Schematic adsorption potentials for C6H12 and C6D12 at a submonolayer coverage on the clean Rh(111) surface.

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/content/aip/journal/jcp/136/21/10.1063/1.4725714
2012-06-07
2014-04-18
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752b84549af89a08dbdd7fdb8b9568b5 journal.articlezxybnytfddd
Scitation: Kinetic and geometric isotope effects originating from different adsorption potential energy surfaces: Cyclohexane on Rh(111)
http://aip.metastore.ingenta.com/content/aip/journal/jcp/136/21/10.1063/1.4725714
10.1063/1.4725714
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