An Investigation into the Effects of Mn Promotion on the Activity and Selectivity of Co/SiO 2 for Fischer–Tropsch Synthesis: Evidence for Enhanced CO Adsorption and Dissociation

Johnson, Gregory R.; Werner, Sebastian; Bell, Alexis T.

doi:10.1021/acscatal.5b01578

An Investigation into the Effects of Mn Promotion on the Activity and Selectivity of Co/SiO ₂ for Fischer–Tropsch Synthesis: Evidence for Enhanced CO Adsorption and Dissociation

Journal Article · Thu Aug 27 00:00:00 EDT 2015 · ACS Catalysis

DOI:https://doi.org/10.1021/acscatal.5b01578· OSTI ID:1416909

Johnson, Gregory R. ^[1]; Werner, Sebastian ^[1]; Bell, Alexis T. ^[2]

Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering
Univ. of California, Berkeley, CA (United States). Dept. of Chemical and Biomolecular Engineering; Lawrence Berkeley National Lab. (LBNL), Berkeley, CA (United States)

Mn is an effective promoter for improving the activity and selectivity of Co-based Fischer-Tropsch synthesis (FTS) catalysts, but the mechanism by which this promoter functions is poorly understood. The work reported here was aimed at defining the manner in which Mn interacts with Co and determining how these interactions affect the activity and selectivity of Co. Detailed measurements are reported for the kinetics of FTS as a function of Mn/Co ratio, temperature, and reactant partial pressure. These data are described by a single, two-parameter rate expression. Mn promotion was found to increase both the apparent rate constant for CO consumption and the CO adsorption constant. Further evidence for enhanced CO adsorption and dissociation was obtained from measurements of temperature-programmed desorption of CO and CO disproportionation rates, respectively. Quantitative analysis of elemental maps obtained by STEM-EDS revealed that the promoter accumulates preferentially on the surface of Co nanoparticles at low Mn loadings, resulting in a rapid onset of improvements in the product selectivity as the Mn loading increases. Furthermore, for catalysts prepared with loadings higher than Mn/Co = 0.1, the additional Mn accumulates in the form of nanometer-scale particles of MnO on the support. In situ IR spectra of adsorbed CO show that Mn promotion increases the abundance of adsorbed CO with weakened C-O bonds. It is proposed that the cleavage of the C-O bond is promoted through Lewis acid-base interactions between the Mn ²⁺ cations located at the edges of MnO islands covering the Co nanoparticles and the O atom of CO adsorbates adjacent to the MnO islands. Finally, the observed decrease in selectivity to CH ₄ and the increased selectivity to C ⁵⁺ products with increasing Mn/Co ratio are attributed to a decrease in the ratio of adsorbed H to CO on the surface of the supported Co nanoparticles.

View Accepted Manuscript (DOE)

Research Organization:: Lawrence Berkeley National Laboratory (LBNL), Berkeley, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)

Grant/Contract Number:: AC02-05CH11231; AC02-06CH11357

OSTI ID:: 1416909

Alternate ID(s):: OSTI ID: 1225093

Journal Information:: ACS Catalysis, Journal Name: ACS Catalysis Journal Issue: 10 Vol. 5; ISSN 2155-5435

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
cobalt
fischer-tropsch synthesis
heterogeneous catalysis
manganese
promotion