Hydrogen catalyzed adsorption of alkenes on the diamond (001) surface

Jun-Hyung Cho, Leonard Kleinman

Research output: Contribution to journalArticle

16 Citations (Scopus)

Abstract

We present first-principles density-functional calculations for the [2+2] cycloaddition reaction of ethylene on the (001) surface of diamond. For comparison we also study the same reaction of ethylene on the Si(001) surface as well as that of two ethylene molecules. Similar to the latter case, a concerted reaction on top of the C dimer is symmetry forbidden due to the symmetric dimer configuration of C(001). However, in both cases the symmetry-forbidden reaction can be avoided by allowing a rotation of the C—C bond of ethylene. This asymmetric reaction path yields an energy barrier of 2.29 and 0.90 eV for the cases of two ethylene molecules and C2H4/C(001), respectively. In contrast, the reaction of ethylene on Si(001) takes place via an intermediate state, caused by the asymmetric Si dimer structure. The reaction energy barrier of C2H4 on C(001) is too high to attain direct adsorption. Here we propose that the [2+2] reaction path is catalyzed by a few hydrogen impurities.

Original languageEnglish
JournalPhysical Review B - Condensed Matter and Materials Physics
Volume68
Issue number19
DOIs
StatePublished - 2003 Nov 15

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Diamond
Alkenes
alkenes
Olefins
Hydrogen
Diamonds
Ethylene
diamonds
Adsorption
adsorption
ethylene
hydrogen
Dimers
Energy barriers
dimers
Molecules
Cycloaddition
Density functional theory
cycloaddition
symmetry

Cite this

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title = "Hydrogen catalyzed adsorption of alkenes on the diamond (001) surface",
abstract = "We present first-principles density-functional calculations for the [2+2] cycloaddition reaction of ethylene on the (001) surface of diamond. For comparison we also study the same reaction of ethylene on the Si(001) surface as well as that of two ethylene molecules. Similar to the latter case, a concerted reaction on top of the C dimer is symmetry forbidden due to the symmetric dimer configuration of C(001). However, in both cases the symmetry-forbidden reaction can be avoided by allowing a rotation of the C—C bond of ethylene. This asymmetric reaction path yields an energy barrier of 2.29 and 0.90 eV for the cases of two ethylene molecules and C2H4/C(001), respectively. In contrast, the reaction of ethylene on Si(001) takes place via an intermediate state, caused by the asymmetric Si dimer structure. The reaction energy barrier of C2H4 on C(001) is too high to attain direct adsorption. Here we propose that the [2+2] reaction path is catalyzed by a few hydrogen impurities.",
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Hydrogen catalyzed adsorption of alkenes on the diamond (001) surface. / Cho, Jun-Hyung; Kleinman, Leonard.

In: Physical Review B - Condensed Matter and Materials Physics, Vol. 68, No. 19, 15.11.2003.

Research output: Contribution to journalArticle

TY - JOUR

T1 - Hydrogen catalyzed adsorption of alkenes on the diamond (001) surface

AU - Cho, Jun-Hyung

AU - Kleinman, Leonard

PY - 2003/11/15

Y1 - 2003/11/15

N2 - We present first-principles density-functional calculations for the [2+2] cycloaddition reaction of ethylene on the (001) surface of diamond. For comparison we also study the same reaction of ethylene on the Si(001) surface as well as that of two ethylene molecules. Similar to the latter case, a concerted reaction on top of the C dimer is symmetry forbidden due to the symmetric dimer configuration of C(001). However, in both cases the symmetry-forbidden reaction can be avoided by allowing a rotation of the C—C bond of ethylene. This asymmetric reaction path yields an energy barrier of 2.29 and 0.90 eV for the cases of two ethylene molecules and C2H4/C(001), respectively. In contrast, the reaction of ethylene on Si(001) takes place via an intermediate state, caused by the asymmetric Si dimer structure. The reaction energy barrier of C2H4 on C(001) is too high to attain direct adsorption. Here we propose that the [2+2] reaction path is catalyzed by a few hydrogen impurities.

AB - We present first-principles density-functional calculations for the [2+2] cycloaddition reaction of ethylene on the (001) surface of diamond. For comparison we also study the same reaction of ethylene on the Si(001) surface as well as that of two ethylene molecules. Similar to the latter case, a concerted reaction on top of the C dimer is symmetry forbidden due to the symmetric dimer configuration of C(001). However, in both cases the symmetry-forbidden reaction can be avoided by allowing a rotation of the C—C bond of ethylene. This asymmetric reaction path yields an energy barrier of 2.29 and 0.90 eV for the cases of two ethylene molecules and C2H4/C(001), respectively. In contrast, the reaction of ethylene on Si(001) takes place via an intermediate state, caused by the asymmetric Si dimer structure. The reaction energy barrier of C2H4 on C(001) is too high to attain direct adsorption. Here we propose that the [2+2] reaction path is catalyzed by a few hydrogen impurities.

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DO - 10.1103/PhysRevB.68.195413

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