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Understanding the morphology and chemical activity of model ZrOx/Au (111) catalysts for CO2 hydrogenation

Journal Article · · Surface Science
 [1];  [2];  [3];  [2];  [2];  [3];  [4]
  1. Stony Brook Univ., NY (United States)
  2. Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  3. Brookhaven National Laboratory (BNL), Upton, NY (United States)
  4. Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)
+ Show Author Affiliations
In this study, the growth of ZrOx on Au (111) was investigated using scanning tunneling microscopy (STM) and synchrotron-based ambient pressure X-ray photoelectron spectroscopy (AP-XPS). Nanostructures of ZrOx (x= 1,2) at the sub-monolayer (≤ 0.3 ML) level were prepared by vapor depositing Zr metal onto Au (111) followed by oxidation with O2 or CO2. At low coverages of the admetal (< 0.05 ML), the formed ZrOx nanostructures were dispersed randomly on the terraces and steps of the Au(111) substrate. Strong oxide-metal interactions prevented the formation of islands of zirconia. The ZrOx nanostructures displayed a reactivity towards CO2 and H2 not seen for bulk zirconia. C 1 s AP-XPS results indicated that CO2 molecules adsorbed on Zr/ZrOx/Au(111) surfaces could undergo partial decomposition on Zr (CO2, gas → COgas + Oads), or react with oxygen sites from ZrOx to yield carbonates (Zr-CO3, ads). Further, after exposing ZrO2/Au (111) surfaces to 1:3 mixtures of CO2:H2, the formation of HCOO, CO3, and CH3O was detected in AP-XP spectra. These chemical species decomposed at temperatures in the range of 400-600 K, making them possible reaction intermediates for methanol synthesis.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Sponsoring Organization:
USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES)
Grant/Contract Number:
SC0012704
OSTI ID:
2448239
Alternate ID(s):
OSTI ID: 2438364
Report Number(s):
BNL--226187-2024-JAAM
Journal Information:
Surface Science, Journal Name: Surface Science Vol. 750; ISSN 0039-6028
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
Ambient pressure X-ray photoelectron spectroscopy
CO2 hydrogenation
Inverse oxide/metal catalysts
Scanning tunneling microscopy
Zirconium catalyst