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Effect of Pretreatment Method on the Nanostructure and Performance of Supported Co Catalysts in Fischer−Tropsch Synthesis

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Author(s)

  • Robert Mitchell
  • david lloyd
  • Leon van de Water
  • Peter Ellis
  • Kirsty Metcalfe
  • Connor Sibbald
  • Laura Davies
  • Dan Enache
  • Gordon Kelly
  • Edward Boyes
  • Pratibha L Gai

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Publication details

JournalACS Catalysis
DateAccepted/In press - 8 Aug 2018
DateE-pub ahead of print - 23 Aug 2018
DatePublished (current) - 7 Sep 2018
Volume8
Number of pages14
Pages (from-to)8816-8829
Early online date23/08/18
Original languageEnglish

Abstract

ABSTRACT: Understanding precursor transformation to active catalysts is crucial to heterogeneous Fischer−Tropsch (FT) catalysis directed toward production of hydrocarbons for transportation fuels. Despite considerable literature on FT catalysis, the effect of pretreatment of supported cobalt catalysts on cobalt dispersion, dynamic atomic structure, and the activity of the catalysts is not well understood. Here we present systematic studies into the formation of active catalyst phases in supported Co catalyst precursors in FT catalysis using in situ environmental (scanning) transmission electron microscopy (E(S)TEM) with single-atom resolution under controlled reaction environments for in situ visualization, imaging, and analysis of reacting atomic species in real time, EXAFS, XAS, DRIFTS analyses, and catalytic activity measurements. We have synthesized and analyzed dried reduced (D) and dried calcined reduced (DC) Co real catalysts on reducible and nonreducible supports, such as SiO2, Al2O3, TiO2, and ZrO2. Comparisons of dynamic in situ atomic structural observations of reacting single atoms, atomic clusters, and nanoparticles of Co and DRIFTS, XAS, EXAFS, and catalytic activity data of the D and DC samples reveal in most cases better dispersion in the D samples, leading to a larger number of low-coordination Co0 sites and a higher number of active sites for CO adsorption. The experimental findings on the degree of reduction of D and 27 DC catalysts on reducible and nonreducible supports and correlations between hexagonal (hcp) Co sites and the activity of the catalysts generate structural insights into the catalyst dynamics, important to the development of efficient FT catalysts.

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© 2018 American Chemical Society. This is an author-produced version of the published paper. Uploaded in accordance with the publisher’s self-archiving policy. Further copying may not be permitted; contact the publisher for details.

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