The role of H2 in Fe carburization by CO in Fischer-Tropsch catalysts
Jiachun Chai (Eindhoven University of Technology)
Robert Pestman (Eindhoven University of Technology)
Wei Chen (Eindhoven University of Technology)
A. Iulian Dugulan (TU Delft - RID/TS/Instrumenten groep)
Bo Feng (National Institute of Clean-and-Low-Carbon Energy, Shenhua NICE, Future Science and Technology City, Changping District, Beijing 102211, People's Republic of China)
Zhuowu Men (National Institute of Clean-and-Low-Carbon Energy, Shenhua NICE, Future Science and Technology City, Changping District, Beijing 102211, People's Republic of China)
Peng Wang (Eindhoven University of Technology, National Institute of Clean-and-Low-Carbon Energy, Shenhua NICE, Future Science and Technology City, Changping District, Beijing 102211, People's Republic of China)
Emiel J.M. Hensen (Eindhoven University of Technology)
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Abstract
The formation of Fe-carbide phases is relevant to the synthesis of Fischer-Tropsch synthesis catalysts. We investigated the carburization of Raney Fe as a model catalyst using spectroscopic and temperature-programmed techniques. IR spectroscopy shows that CO dissociation already occurs at −150 °C, while C diffusion into metallic Fe requires much higher temperature (~180 °C). The carburization rate increases with increasing H2/CO ratio, which can be attributed to the lower overall barrier for O removal as H2O as compared to CO2. O removal frees vacancies that are needed for CO dissociation. The resulting higher C coverage increases the driving force for Fe-carbide formation. A higher driving force leads to predominant formation of the more carbon-rich ε(́)-carbide, while χ-Fe5C2 is formed at lower H2/CO ratio. The removal of surface O appears to be the rate-limiting step under all conditions. Initially, most of deposited C is used for Fe-carbide formation with a small contribution to hydrocarbons formation.
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