skip to main content

DOE PAGESDOE PAGES

Title: Active sites for CO 2 hydrogenation to methanol on Cu/ZnO catalysts

The active sites over commercial copper/zinc oxide/aluminum oxide (Cu/ZnO/Al 2O 3) catalysts for carbon dioxide (CO 2) hydrogenation to methanol, the Zn-Cu bimetallic sites or ZnO-Cu interfacial sites, have recently been the subject of intense debate. Here, we report a direct comparison between the activity of ZnCu and ZnO/Cu model catalysts for methanol synthesis. By combining x-ray photoemission spectroscopy, density functional theory, and kinetic Monte Carlo simulations, we can identify and characterize the reactivity of each catalyst. Both experimental and theoretical results agree that ZnCu undergoes surface oxidation under the reaction conditions so that surface Zn transforms into ZnO and allows ZnCu to reach the activity of ZnO/Cu with the same Zn coverage. These results highlight a synergy of Cu and ZnO at the interface that facilitates methanol synthesis via formate intermediates.
Authors:
ORCiD logo [1] ; ORCiD logo [2] ; ORCiD logo [3] ; ORCiD logo [4] ; ORCiD logo [4]
  1. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division
  2. Univ. of Central Venezuela, Caracas (Venezuela)
  3. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division; Columbia Univ., New York, NY (United States). Dept. of Chemical Engineering
  4. Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Division; State Univ. of New York (SUNY), Stony Brook, NY (United States). Dept. of Chemistry
Publication Date:
Report Number(s):
BNL-114202-2017-JA
Journal ID: ISSN 0036-8075; R&D Project: CO040; KC0302010
Grant/Contract Number:
SC00112704; AC02-05CH11231; 276047
Type:
Published Article
Journal Name:
Science
Additional Journal Information:
Journal Volume: 355; Journal Issue: 6331; Journal ID: ISSN 0036-8075
Publisher:
AAAS
Research Org:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1434385
Alternate Identifier(s):
OSTI ID: 1377055