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Domino Effect of Catalysis: Coherence between Reaction Network and Catalyst Restructuring Accelerating Surface
Pengfei Du1, Yafeng Zhang1, Rui Qi2,3
1CAS Key Laboratory of Science and Technology on Applied Catalysis, Dalian Institute of Chemical Physics, Chinese Academy of Sciences, Dalian 116023, China.
Journal of the American Chemical Society
|May 29, 2025
Summary
Dynamic carburization on palladium-iron oxide (Pd-FeOx) catalysts is controlled by in situ alloying, not particle size. This discovery optimizes catalyst performance in CO2 hydrogenation by forming active iron carbide (Fe5C2) phases.
Area of Science:
- Catalysis
- Materials Science
- Chemical Engineering
Background:
- Dynamic carburization is crucial in industrial reactions, but catalyst optimization is complex due to intertwined catalyst and reaction dynamics.
- Understanding the factors governing dynamic carburization is key for improving catalytic processes.
Purpose of the Study:
- To investigate the critical factors controlling dynamic carburization on Pd-FeOx catalysts during CO2 hydrogenation.
- To reveal the domino effect between reaction networks and catalyst restructuring for optimized catalyst design.
Main Methods:
- Preparation of Pd-FeOx catalysts with varying Pd nanoparticle sizes (5Pd-FeOx, 0.5Pd-FeOx, 0.05Pd-FeOx).
- In situ characterization of catalyst evolution during long-term CO2 hydrogenation.
- Design and testing of a presynthesized Pd3Fe alloy catalyst for proof of concept.
Main Results:
- Large Pd nanoparticle size (5Pd-FeOx) induced reactive metal-support interaction, leading to in situ Pd3Fe formation.
- In situ alloying, specifically Pd3Fe formation, was identified as crucial for the rapid formation of the active iron carbide (Fe5C2) phase.
- Presynthesized Pd3Fe alloy catalysts showed enhanced activity with reduced Pd loading due to controlled fast carburization.
Conclusions:
- In situ alloying, rather than Pd particle size, is the critical factor governing fast carburization and catalytic performance in Pd-FeOx systems.
- This study demonstrates the controllability of dynamic carburization and provides a strategy for catalyst optimization via understanding in situ transformations.
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