Journal
POLYHEDRON
Volume 209, Issue -, Pages -Publisher
PERGAMON-ELSEVIER SCIENCE LTD
DOI: 10.1016/j.poly.2021.115461
Keywords
Carbynes; Carbides; Thiocarbonyls; Fischer-Tropsch; CO cleavage
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Funding
- NIH [GM-075757]
- Dow Next Generation Instrumentation Grant/Educator Funds
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The article describes the synthesis of Fe-CS complexes and the possibility of further producing Fe-carbynes. Strategies for achieving C-S bond cleavage from these complexes are discussed, as well as the limitations that have so far prevented the generation of terminal Fe-carbide in this system.
The remarkable catalytic transformation of CO to liquid hydrocarbons by Fe and Co catalysts in the industrial Fischer-Tropsch process motivates interest in developing well-defined systems to model aspects of this chemistry. One of the most interesting potential intermediates in this chemistry is a terminally-bound, first row metal carbide, yet a molecular model of this species remains elusive. With this in mind, we targeted the synthesis of highly-activated Fe-thiocarbonyl complexes, as prospective precursors to S-functionalization, C-S bond cleavage, and carbide generation. Herein, we describe the synthesis of three Fe-CS complexes that can be alkylated to generate a series of terminal Fe-carbynes that could be characterized across three oxidation states. Strategies to access C-S bond scission from these species are discussed, including limitations that, thus far, have precluded the generation of a terminal Fe-carbide for this system.
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