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Atomically dispersed Fe3+ sites catalyze efficient CO2 electroreduction to CO
Jun Gu1, Chia-Shuo Hsu2, Lichen Bai1
1Laboratory of Inorganic Synthesis and Catalysis, Institute of Chemical Sciences and Engineering, Ecole Polytechnique Fédérale de Lausanne (EPFL), EPFL-ISIC-LSCI, BCH 3305, Lausanne CH 1015, Switzerland.
Science (New York, N.Y.)
|June 15, 2019
Summary
This study introduces a novel iron-based catalyst for efficient carbon dioxide (CO2) conversion to carbon monoxide (CO). The single-atom iron catalyst achieves high activity at low overpotentials, outperforming precious metal alternatives.
Area of Science:
- Electrochemistry
- Materials Science
- Catalysis
Background:
- Gold nanomaterials are the most active electrocatalysts for CO2 to CO conversion.
- Non-precious metal catalysts exhibit limited activity for this reaction.
Purpose of the Study:
- To develop a highly active and cost-effective catalyst for CO2 electroreduction.
- To investigate the performance of single-atom iron sites for CO2 to CO conversion.
Main Methods:
- Electrochemical testing to measure catalytic activity and overpotential.
- Operando X-ray absorption spectroscopy to identify active sites and oxidation states.
- Electrochemical data analysis to understand reaction mechanisms.
Main Results:
- A catalyst with dispersed single-atom iron sites achieved CO production at an 80 mV overpotential.
- Partial current density reached 94 mA/cm² at 340 mV overpotential.
- Active sites identified as discrete Fe3+ ions coordinated with pyrrolic nitrogen on a carbon support, maintaining the +3 oxidation state.
Conclusions:
- Single-atom Fe3+ sites coordinated with N atoms in a carbon support exhibit superior electrocatalytic activity for CO2 to CO conversion.
- The enhanced activity is attributed to faster CO2 adsorption and weaker CO adsorption compared to Fe2+ sites.
- This catalyst offers a promising non-precious metal alternative to gold-based catalysts.
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