Methane dissociative adsorption on the Pt(111) surface over the 300-500 K temperature and 1-10 torr pressure ranges

作者：Marsh AL; Becraft KA; Somorjai GA^*

来源：Journal of Physical Chemistry B, 2005, 109(28): 13619-13622.

DOI：10.1021/jp051718+

The dissociative adsorption of methane on the Pt(111) surface has been investigated and characterized over the 1-10 Torr pressure and 300-500 K temperature ranges using sum frequency generation (SFG) vibrational spectroscopy and Auger electron spectroscopy (AES). At a reaction temperature of 300 K and a pressure of I Torr, C-H bond dissociation occurs in methane on the Pt(111) surface to produce adsorbed methyl (CH3) groups, carbon, and hydrogen. SFG results suggest that C-C coupling occurs at higher reaction temperatures and pressures. At 400 K, methyl groups react with adsorbed C to form ethylidyne (C2H3) which dehydrogenates at 500 K to form ethynyl (C2H) and methylidyne (CH) species, as shown by SFG. By 600 K, all of the ethylidyne has reacted to form the dissociation products ethynyl and methylidyne. Calculated C-H bond dissociation probabilities for methane, determined by carbon deposition measured by AES, are in the 10(-8) range and increase with increasing reaction temperature. A mechanism has been developed and is compared with conclusions from other experimental and theoretical studies using single crystals.

• 出版日期2005-7-21