4.6 Article

CO2 Hydrogenation to Hydrocarbons over Fe/BZY Catalysts

Journal

CHEMCATCHEM
Volume 14, Issue 19, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/cctc.202200802

Keywords

CO2 hydrogenation; Fe catalyst; Redox-active support; Bi-functional catalyst; de-facto Fischer-Tropsch

Funding

  1. U.S. Department of Energy, Office of Fossil Energy and Carbon Management [DE-FE0031716, DOE-FWP-FEAA421]
  2. Karlsruhe Institute of Technology Collaborative Research Center/Transregio -SFB/TRR
  3. National Science Foundation
  4. Colorado School of Mines Foundation, via the Angel Research Fund

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This manuscript reports a CO2 hydrogenation process using Fe/BZY15 catalysts, in which the effects of temperature, feed composition, and residence time on CO2 conversion and carbon selectivity are studied. The results indicate that the residence time has a significant impact on higher-carbon selectivity and yield, while CO2 activation depends on the redox activity of the catalyst.
This manuscript reports a CO2 hydrogenation process in a catalytic laboratory-scale packed-bed reactor using an Fe/BZY15 (BaZr0.85Y0.15O3-delta) catalyst to form hydrocarbons (e. g., CH4, C2+) at elevated pressure of 30 bar and temperatures in the range 270 <= T <= 375 degrees C. The effects of temperature, feed composition (i. e., CO2/H-2 ratio, and residence time (i. e., Weight Hourly Space Velocity (WHSV) are studied to understand the relationship between CO2 conversion and carbon selectivity. Catalyst characterization elucidates the relationships between the catalyst structure, surface adsorbates, and reaction pathways. Thermodynamic analyses guide the experimental conditions and assist in interpreting results. While the feed composition and temperature influence the product distribution, the results suggest that the higher-carbon (C2+) selectivity and yield depend strongly on residence time. The results suggest that the CO2 hydrogenation reaction pathway is similar to Fischer-Tropsch (FT) synthesis. The reaction begins with CO2 activation to form CO, followed by chain-growth reactions similar to the FT process. The CO2 activation depends on the redox activity of the catalyst. However, the carbon chain growth depends primarily on the residence time. as is the case for the FT synthesis, high residence time (on the orders of hours) is required to achieve high C2+ yield.

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