Fischer-Tropsch Synthesis: The Characterization and Testing of Pt-Co/SiO2 Catalysts Prepared with Alternative Cobalt Precursors

Mehrbod, Mohammad; Martinelli, Michela; Watson, Caleb D.; Cronauer, Donald C.; Kropf, A. Jeremy; Jacobs, Gary

doi:10.3390/reactions2020011

Fischer-Tropsch Synthesis: The Characterization and Testing of Pt-Co/SiO₂ Catalysts Prepared with Alternative Cobalt Precursors

Journal Article · Tue Jun 01 00:00:00 EDT 2021 · Reactions

DOI:https://doi.org/10.3390/reactions2020011· OSTI ID:1828966

Mehrbod, Mohammad ^[1]; Martinelli, Michela ^[2]; ^[1]; Cronauer, Donald C. ^[3]; Kropf, A. Jeremy ^[3]; Jacobs, Gary ^[1]

UTSA, San Antonio, TX (United States)
Univ. of Kentucky, Lexington, KY (United States)
Argonne National Lab. (ANL), Argonne, IL (United States)

Different low-cost cobalt precursors (acetate, chloride) and thermal treatments (air calcination/H₂ reduction versus direct H₂-activation) were investigated to alter the interaction between cobalt and silica. H₂-activated catalysts prepared from cobalt chloride had large Co⁰ particles (XRD, chemisorption) formed by weak interactions between cobalt chloride and silica (temperature programmed reduction (TPR), TPR with mass spectrometry (TPR-MS), TPR with extended X-ray absorption fine structure (EXAFS) and X-ray absorption near edge spectroscopy (XANES) techniques) and retained Cl-blocked active sites, resulting in poor activity. In contrast, unpromoted Co/SiO₂ catalysts derived from cobalt acetate had strong interactions between Co species and silica (TPR/TPR-MS, TPR-EXAFS/XANES); adding Pt increased the extent of the Co reduction. For these Pt-promoted catalysts, the reduction of uncalcined catalysts was faster, resulting in larger Co⁰ clusters (19.5 nm) in comparison with the air-calcined/H₂-activated catalyst (7.8 nm). Both catalysts had CO conversions 25% higher than that of the Pt-promoted catalyst prepared in the traditional manner (air calcination/H₂ reduction using cobalt nitrate) and three times higher than that of the traditional unpromoted Co/silica catalyst. The retention of residual cobalt carbide (observed in XANES) from cobalt acetate decomposition impacted performance, resulting in a higher C₁–C₄ selectivity (32.2% for air-calcined and 38.7% for uncalcined) than that of traditional catalysts (17.5–18.6%). The residual carbide also lowered the α-value and olefin/paraffin ratio. Future work will focus on improving selectivity through oxidation–reduction cycles.

View Accepted Manuscript (DOE)

Research Organization:: Argonne National Laboratory (ANL), Argonne, IL (United States)

Sponsoring Organization:: Materials Research Collaborative Access Team (MRCAT); National Science Foundation (NSF); USDOE Office of Fossil Energy (FE); USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1828966

Journal Information:: Reactions, Journal Name: Reactions Journal Issue: 2 Vol. 2; ISSN 2624-781X

Publisher:: MDPICopyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
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cobalt acetate
cobalt chloride
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Fischer-Tropsch Synthesis: The Characterization and Testing of Pt-Co/SiO2 Catalysts Prepared with Alternative Cobalt Precursors

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Fischer-Tropsch Synthesis: The Characterization and Testing of Pt-Co/SiO₂ Catalysts Prepared with Alternative Cobalt Precursors