Illustrating the overall reaction network of the synthesis-gas-to-hydrocarbons process over iron-zeolite bifunctional catalysis

Xuan Gong, Adrian Ramirez, Edy Abou-Hamad, Tuiana B. Shoinkhorova, Mustafa Çağlayan, Yiru Ye, Wei Wang, Nimer Wehbe, Rushana Khairova, Abhishek Dutta Chowdhury*, Jorge Gascon*

*Corresponding author for this work

Research output: Contribution to journalArticlepeer-review

5 Scopus citations

Abstract

Since its discovery in the early 20th century, Fischer-Tropsch synthesis (FTS) has opened a path, as an alternative to crude oil, to produce fuels and chemicals. When classical FTS catalysts are combined with acidic zeolites, the scope of this gas-phase polymerization can be narrowed, thus maximizing the production of value-added commodities and eliminating energy-consuming separation steps. However, from a mechanistic standpoint, even now, little is known about the role of the different reaction intermediates. Here, we present a comprehensive, in-depth, mechanistic investigation using solid-state NMR spectroscopy and well-designed control experiments on combining a classical Fe-based FTS catalyst and zeolites with different topologies to establish the impact of “co-catalytic” key organic carbon-based reaction intermediates, including carbonylated/oxygenated species (ester/ketone/alcohol/ether/epoxide/ketene). Consequently, this work provides experimental evidence supporting the “co-existence” of oxygenate (cf. surface-enol and CO-insertion) mechanisms (together with the traditional carbide-based FTS mechanism). The significance of “supramolecular reactive centers” within zeolite and host-guest chemistry has also been illuminated.

Original languageEnglish (US)
Pages (from-to)2328-2345
Number of pages18
JournalChem Catalysis
Volume2
Issue number9
DOIs
StatePublished - Sep 15 2022

Keywords

  • bifunctional catalysis
  • C1-chemistry
  • Fischer-Tropsch process
  • reaction mechanism
  • SDG9: Industry, innovation, and infrastructure
  • zeolite

ASJC Scopus subject areas

  • Chemistry (miscellaneous)
  • Physical and Theoretical Chemistry
  • Organic Chemistry

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