Dynamic structural evolution of iron catalysts involving competitive oxidation and carburization during CO ₂ hydrogenation

2022/02/04 by Jie Zhu, Peng Wang, Xiaoben Zhang +11 · 1 citation
Chemical Engineering · Engineering · Materials Science · #Catalysis and Hydrodesulfurization Studies #Catalysts for Methane Reforming #Catalytic Processes in Materials Science

paper · doi:10.1126/sciadv.abm3629

openalex publication_date 2022/02/04 · openalex created_date 2022/02/08 · openalex updated_date 2026/07/28

Abstract

Identifying the dynamic structure of heterogeneous catalysts is crucial for the rational design of new ones. In this contribution, the structural evolution of Fe(0) catalysts during CO 2 hydrogenation to hydrocarbons has been investigated by using several (quasi) in situ techniques. Upon initial reduction, Fe species are carburized to Fe 3 C and then to Fe 5 C 2 . The by-product of CO 2 hydrogenation, H 2 O, oxidizes the iron carbide to Fe 3 O 4 . The formation of Fe 3 O 4 @(Fe 5 C 2 +Fe 3 O 4 ) core-shell structure was observed at steady state, and the surface composition depends on the balance of oxidation and carburization, where water plays a key role in the oxidation. The performance of CO 2 hydrogenation was also correlated with the dynamic surface structure. Theoretical calculations and controll experiments reveal the interdependence between the phase transition and reactive environment. We also suggest a practical way to tune the competitive reactions to maintain an Fe 5 C 2 -rich surface for a desired C 2+ productivity.

Citations

• Projector augmented-wave method
• Effect of potassium on the active phases of Fe catalysts for carbon dioxide conversion to liquid fuels through hydrogenation
• Recent Advances in Carbon Dioxide Hydrogenation to Methanol via Heterogeneous Catalysis
• Rationally designed indium oxide catalysts for CO ₂ hydrogenation to methanol with high activity and selectivity
• Highly Selective Olefin Production from CO₂ Hydrogenation on Iron Catalysts: A Subtle Synergy between Manganese and Sodium Additives
• Novel Heterogeneous Catalysts for CO₂ Hydrogenation to Liquid Fuels
• CO₂ Hydrogenation to Methanol over In₂O₃-Based Catalysts: From Mechanism to Catalyst Development
• A hydrophobic FeMn@Si catalyst increases olefins from syngas by suppressing C1 by-products

Cited by

• Hydrogenation of CO ₂ for sustainable fuel and chemical production

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