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Surface characterization and methane activation on SnOx/Cu2O/Cu(111) inverse oxide/metal catalysts

Journal Article · · Physical Chemistry Chemical Physics. PCCP
DOI:https://doi.org/10.1039/d1cp02829d· OSTI ID:1812502
 [1];  [2];  [1];  [1];  [2];  [1];  [1];  [1];  [2];  [3];  [3]
  1. Stony Brook Univ., NY (United States)
  2. Brookhaven National Lab. (BNL), Upton, NY (United States)
  3. Stony Brook Univ., NY (United States); Brookhaven National Lab. (BNL), Upton, NY (United States)
+ Show Author Affiliations
To activate methane at low or medium temperatures is a difficult task and a pre-requisite for the conversion of this light alkane into high value chemicals. In this work, we report the preparation and characterizations of novel SnOx/Cu2O/Cu(111) interfaces that enable low-temperature methane activation. Scanning tunneling microscopy identified small, well-dispersed SnOx nanoclusters on the Cu2O/Cu(111) substrate with an average size of 8 Å, and such morphology was sustained up to 450 K in UHV annealing. Ambient pressure X-ray photoelectron spectroscopy showed that hydrocarbon species (CHx groups), the product of methane activation, were formed on SnOx/Cu2O/Cu(111) at a temperature as low as 300 K. An essential role of the SnOx–Cu2O interface was evinced by the SnOx coverage dependence. Systems with a small amount of tin oxide, 0.1–0.2 ML coverage, produced the highest concentration of adsorbed CHx groups. Calculations based on density functional theory showed a drastic reduction in the activation barrier for C–H bond cleavage when going from Cu2O/Cu(111) to SnOx/Cu2O/Cu(111). On the supported SnOx, the dissociation of methane was highly exothermic (ΔE ~ –35 kcal mol–1) and the calculated barrier for activation (~20 kcal mol–1) could be overcome at 300–500 K, target temperatures for the conversion of methane to high value chemicals.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
National Science Foundation (NSF); USDOE; USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division
Grant/Contract Number:
AC02-05CH11231; SC0012704
OSTI ID:
1812502
Alternate ID(s):
OSTI ID: 1811944
Report Number(s):
BNL--221960-2021-JAAM
Journal Information:
Physical Chemistry Chemical Physics. PCCP, Journal Name: Physical Chemistry Chemical Physics. PCCP Journal Issue: 32 Vol. 23; ISSN 1463-9076
Publisher:
Royal Society of ChemistryCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

36 MATERIALS SCIENCE
copper oxide
methane
tin oxide