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Activity of Pd(110) for methanol synthesis

Journal Article · · J. Catal.; (United States)
The synthesis of methanol from CO and H/sub 2/ has been studied over unsupported, single-crystal Pd(110) at pressures of 72.3-244 KPa, temperatures of 493-553 K, and a H/sub 2//CO ratio of 3.9, in a combined high-pressure reactor/UHV surface analysis chamber. At 244 KPa the reaction exhibited linear Arrhenius behavior with an activation energy of 18.4 +/- 1.9 kcal/mol, and a pre-exponential factor of 8 x 10/sup 4/ s/sup -1/. These values are in good agreement with values reported for supported Pd/SiO/sub 2/. At 553 K the reaction was roughly first order in total pressure (1.2 +/- 0.2) over the pressure range studied. Specific rates (turnover frequencies) observed in this study, extrapolated to pressures typical of most methanol synthesis work (1-1.5 MPa), are in good agreement with rates observed for Pd dispersed on noninteracting supports such as SiO/sub 2/, and some basic supports such as ZnO and MgO. These rates are higher than those observed over Pd supported on zeolite and acidic supports (e.g., PdNaY and Al/sub 2/O/sub 3/), but much lower than those observed on highly active La/sub 2/O/sub 3/-supported Pd. In addition, no dimethyl ether product was detected on Pd(110), though it is a significant product on many acidic supports. Thus, Pd metal is an active methanol synthesis catalyst, and no specific support interaction is required. Highly interacting supports exhibit rates and/or selectivities substantially different from those of Pd(110).
Research Organization:
Sandia National Labs., Albuquerque, NM (USA)
DOE Contract Number:
AC04-76DP00789
OSTI ID:
5206247
Journal Information:
J. Catal.; (United States), Journal Name: J. Catal.; (United States) Vol. 108:2; ISSN JCTLA
Country of Publication:
United States
Language:
English