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The Surface Chemistry of Methanol on Pd(111) and H–Pd(111) Surfaces: C–O Bond Cleavage and the Effects of Metal Hydride Formation

Journal Article · · Journal of Physical Chemistry Letters
 [1];  [2];  [3];  [4];  [2];  [2];  [5];  [6]
  1. Brookhaven National Laboratory (BNL), Upton, NY (United States); Pohang Univ. of Science and Technology (POSTECH) (Korea, Republic of)
  2. Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  3. Stony Brook Univ., NY (United States)
  4. Charles Univ., Prague (Czech Republic)
  5. Brookhaven National Laboratory (BNL), Upton, NY (United States)
  6. Brookhaven National Laboratory (BNL), Upton, NY (United States); Stony Brook Univ., NY (United States)

Palladium catalysts are frequently employed in processes where methanol is an energy vector or carrier, being useful for the synthesis of methanol from mixtures of carbon dioxide and hydrogen (CO2/H2) or its steam reforming on demand. Results of synchrotron-based ambient pressure X-ray photoelectron spectroscopy for the adsorption of methanol on a Pd(111) model catalyst show a rich surface chemistry and complex phenomena that strongly depend on pressure and temperature. At low pressures (< 10-6 Torr) and temperatures (< 300 K), CO is the dominant decomposition product. Further, as the pressure increases, cleavage of C-H, O-H and C-O bonds is observed, and at elevated temperatures (400-600 K) the formation of CO and CHx/C fragments compete on the surface. Thus, existing reaction networks for methanol decomposition must be modified. Furthermore, surface and subsurface hydrogen (coming from PdHx) play a significant role in the stability and removal of CHx and C species.

Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB)
Grant/Contract Number:
SC0012704
OSTI ID:
2372824
Report Number(s):
BNL-225716-2024-JAAM
Journal Information:
Journal of Physical Chemistry Letters, Vol. 15, Issue 23; ISSN 1948-7185
Publisher:
American Chemical SocietyCopyright Statement
Country of Publication:
United States
Language:
English

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