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Activity and selectivity for CO2 methanation of clusters and nanoplates of ruthenium dispersed on ceria: In-situ studies with XAFS and DRIFTS

Journal Article · · Catalysis Today
 [1];  [2];  [1];  [3];  [1];  [4];  [5];  [1];  [2];  [6]
  1. Brookhaven National Laboratory (BNL), Upton, NY (United States)
  2. Consejo Superior de Investigaciones Cientificas (CSIC), Madrid (Spain). Inst. de Catalisis y Petroleoquimica
  3. Universidade Federal do Paraná (UFPR), Palotina (Brazil)
  4. Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
  5. Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
  6. Brookhaven National Laboratory (BNL), Upton, NY (United States); Stony Brook University, NY (United States)
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The performance of Ru/CeO2 catalysts under CO2 hydrogenation conditions was studied using in situ X-ray absorption fine structure (XAFS) and diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) to understand the structural evolution and chemical nature of each component under reaction conditions. The catalysts were prepared using a reverse microemulsion method that maximized the dispersion of RuOx particles on ceria. A RuOx → Ru transformation was observed upon exposure of the RuOx/CeO2 systems to H2 at 250 °C. For a sample with 5% molar Ru, two-dimensional clusters (2-4 atoms) of Ru formed on top of the ceria support. An increase in the loading of ruthenium to 20% molar led to the formation of nanoplates of the metal 2-3 atomic layers thick. Both Ru structures were highly dispersed on ceria. They were oxidized after exposure to CO2 at 250 °C. However, under CO2/H2 mixture, they remained in a metallic state as two-dimensional clusters and nanoplates. In situ DRIFTS studies, the 5% and 20% Ru/CeO2 catalysts showed distinct reaction intermediates when exposed to CO2 or CO2/H2 (1/4) reaction mixtures. Normalized to the Ru molar percentage, the 5% Ru/CeO2 system was the most active catalyst exhibiting a selectivity of ~ 60% CH4 and 40% CO at 250 °C. On the other hand, under the same reaction conditions, the 20% Ru/CeO2 system was less active but had a CH4 selectivity close to 80%. In conclusion, these results highlight the importance of the structure of the metallic Ru particles as a factor that determines the catalytic performance.
Research Organization:
Brookhaven National Laboratory (BNL), Upton, NY (United States)
Sponsoring Organization:
USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences & Biosciences Division (CSGB); USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)
Grant/Contract Number:
SC0012704
OSTI ID:
2572356
Report Number(s):
BNL--228406-2025-JAAM
Journal Information:
Catalysis Today, Journal Name: Catalysis Today Vol. 459; ISSN 0920-5861
Publisher:
ElsevierCopyright Statement
Country of Publication:
United States
Language:
English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CO2 hydrogenation
Ruthenium
ceria
methane production