TY - JOUR
T1 - Illustrating the overall reaction network of the synthesis-gas-to-hydrocarbons process over iron-zeolite bifunctional catalysis
AU - Gong, Xuan
AU - Ramirez, Adrian
AU - Abou-Hamad, Edy
AU - Shoinkhorova, Tuiana B.
AU - Çağlayan, Mustafa
AU - Ye, Yiru
AU - Wang, Wei
AU - Wehbe, Nimer
AU - Khairova, Rushana
AU - Chowdhury, Abhishek Dutta
AU - Gascon, Jorge
N1 - Publisher Copyright:
© 2022 Elsevier Inc.
PY - 2022/9/15
Y1 - 2022/9/15
N2 - 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.
AB - 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.
KW - bifunctional catalysis
KW - C1-chemistry
KW - Fischer-Tropsch process
KW - reaction mechanism
KW - SDG9: Industry, innovation, and infrastructure
KW - zeolite
UR - http://www.scopus.com/inward/record.url?scp=85137751813&partnerID=8YFLogxK
U2 - 10.1016/j.checat.2022.07.026
DO - 10.1016/j.checat.2022.07.026
M3 - Article
AN - SCOPUS:85137751813
SN - 2667-1107
VL - 2
SP - 2328
EP - 2345
JO - Chem Catalysis
JF - Chem Catalysis
IS - 9
ER -